Clinical evidence demonstrating the use of stem cells in cerebral palsy.
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by",editors:[{id:"37194",title:"Dr.",name:"Theophanides",surname:"Theophile",slug:"theophanides-theophile",fullName:"Theophanides Theophile"}],productType:{id:"1",chapterContentType:"chapter",authoredCaption:"Edited by"}},{type:"book",id:"3161",title:"Frontiers in Guided Wave Optics and Optoelectronics",subtitle:null,isOpenForSubmission:!1,hash:"deb44e9c99f82bbce1083abea743146c",slug:"frontiers-in-guided-wave-optics-and-optoelectronics",bookSignature:"Bishnu Pal",coverURL:"https://cdn.intechopen.com/books/images_new/3161.jpg",editedByType:"Edited by",editors:[{id:"4782",title:"Prof.",name:"Bishnu",surname:"Pal",slug:"bishnu-pal",fullName:"Bishnu Pal"}],productType:{id:"1",chapterContentType:"chapter",authoredCaption:"Edited by"}}]},chapter:{item:{type:"chapter",id:"55171",title:"Stem Cell Therapy in Pediatric Neurological Disabilities",doi:"10.5772/67656",slug:"stem-cell-therapy-in-pediatric-neurological-disabilities",body:'\nNeurodevelopmental disorders (NDD) are characterized by an abnormal development of the brain during the early development phase, leading to a myriad of symptoms and diseases, including delayed milestones and deficits in personal and social functioning [1]. The developmental deficits can vary from specific limitations of adaptive, behavioral and cognitive functioning, motor dysfunction, to global impairments of social skills [2]. Some of the common neurodevelopmental disorders are cerebral palsy (CP), autism spectrum disorders, attention deficit hyperactivity disorder, intellectual disability (ID) or intellectual and developmental disability (IDD), learning disabilities, muscular dystrophies, Down’s syndrome, genetic disorders such as fragile‐X syndrome, spinal muscular atrophy (SMA) and metabolic disorders.
\nPediatric neurological disorders represent a major part of the disabilities worldwide. In over 10 decades of research to find a cure for these disorders, medical science has not been able to repair the underlying brain injury [3]. The causes of NDD can be classified as congenital (present at birth) or acquired (developed after birth). The various etiologies are genetic defects, metabolic disorders, nutritional deficiencies, exposure to toxins, infections, hypoxia/asphyxia, low birth weight, perinatal complications leading to traumatic brain injury or spinal cord injury in children [4]. This may affect language and speech, motor skills, behavior, memory, learning or other neurological functions affecting activities of daily life. While the severity of symptoms often change or evolve as the child’s age progresses, these disabilities remain permanent. As these are lifelong disabilities, they pose a substantial economic burden on the society [5]. Hence, finding a treatment for them is the need of the hour. Improvement in the performance of these children would be of great significance to the quality of life of patients and their families.
\nTherapeutic strategies and clinical expectations of patients and medical professionals have not yet been met. Currently, available treatments such as physiotherapy, occupational therapy, behavioral therapy, psychological intervention, speech therapy and pharmacological intervention only focus on alleviating the symptoms of these disabilities and do not address the underlying neuropathophysiology. However, the advent of stem cell therapy has opened new avenues for treatment of pediatric neurological disorders. In recent years, extensive research has been done to explore the potential of stem cells for the treatment of pediatric neurological disabilities. Until now, it was believed that once injured, the cells of the central nervous system cannot regenerate. However, owing to the distinct properties of stem cells to repair and regenerate, they can be considered as a potential therapeutic strategy.
\nThis chapter focuses on recent advances in the application of stem cells as a therapeutic tool for some of the common NDDs (cerebral palsy, autism, intellectual disability and muscular dystrophy). The mechanism of action of stem cells in each disorder has been explained. A review of clinical data has been described giving a clear understanding of current status of stem cell therapy in these disorders. Various factors influencing the outcome of stem cell therapy such as different types of cells, different routes of administration and dosage and frequency of transplantation have also been discussed. Our experience of treating these disorders is exhibited in the form of our published data. Use of novel monitoring tools such as MRI MSK and PET‐CT scan brain to track the changes occurring at cellular level after stem cell therapy is described. We also highlight the importance of a multidisciplinary approach of combining rehabilitation with stem cell therapy. Adverse effects of stem cell therapy are also enumerated.
\nStem cells are blank, immature cells which have a capacity to self‐renew and differentiate into host‐specific multiple lineage cells [6]. Several types of stem cells are being explored for the treatment of neurological disorders such as bone marrow stem cells, embryonic stem cells, olfactory ensheathing cells and umbilical cord blood cells. The main aim of stem cell therapy is replacement of injured/dead neuronal cells and recovery of lost functions [7]. These cells perform repair process directly by regeneration of new cells or indirectly through paracrine activity. The chief underlying mechanisms of stem cells include neuroregeneration, neuroreplacement, neuroprotection, immunomodulation, axon sprouting and neural circuit reconstruction [8] (Figure 1).
\nPediatric neurological disorders are caused due to mechanisms affecting the molecular, cellular and tissue plasticity of the brain and nervous system [9].
\nMechanism of action of stem cells in pediatric neurological disorders.
Stem cells when transplanted migrate and home towards the injured areas of the brain [10]. This homing property is attributed to the expression of growth factors, chemokine and extracellular matrix receptors on the surface of cells such as stromal cell–derived factor 1 (SDF‐1), monocyte chemo attractant protein‐3 (MCP‐3), stem cell factor (SCF) and/or IL‐8. They differentiate into the host tissue cells and replace the injured/dead neuronal tissue [11]. Through paracrine mechanisms they halt further injury and stimulate endogenous cells to carry out the repair and restoration process [12]. Stem cells secrete a vast array of neuroprotective growth factors including brain‐derived neurotrophic factor (BDNF), nerve growth factor (NGF), neurotrophin‐3 (NT‐3), glial cell line–derived neurotrophic factor (GDNF) and insulin‐like growth factor type 1. These growth factors activate a number of signaling pathways and help in enhancing differentiation, survival of neurons and maintaining neuronal functions [13]. They also produce vascular endothelial growth factor (VEGF), hepatocyte growth factor (HGF) and basic fibroblast growth factor (FGF‐2) which improve perfusion and enhance angiogenesis [14]. Anti‐inflammatory paracrine factors such as Interleukin 10 (IL 10) and Transforming growth factor (TGF)‐β help in immunomodulation [15].
\nIn this section, we discuss the literature review of various stem cell therapy studies in each disorder followed by our experience.
\nWe published a study of 71 children diagnosed with different incurable neurological disorders. Autologous bone marrow–derived mononuclear cells were transplanted intrathecally and intramuscularly. Improvements were noted in muscle power, functional independent measure (FIM) and Brooke and Vignos scale. Imaging and electrophysiological investigations also showed improvement. Overall 97% muscular dystrophy cases showed subjective, functional and investigational improvement. Eighty‐five percent of cases of cerebral palsy cases showed improvements. Eighty‐eight percent of cases of other incurable neurological disorders such as autism, Retts syndrome and giant axonal neuropathy also showed improvement. No major adverse events were noted.
\nIn cerebral palsy, white matter injury also known as periventricular leukomalacia (PVL) is one of the major pathologies observed [16]. Stem cells differentiate into neurons, oligodendrocytes and astrocytes which replace and repair the white matter injury in CP [17] (Figure 2). The growth factors secreted by these cells also help in remyelination, synaptogenesis, cytoprotection and angiogenesis which reverse the cellular injury in CP [18, 19]. Numerous preclinical studies have demonstrated the potential of stem cell transplantation in cerebral palsy. The homing property of these cells was confirmed by Chen et al., who transplanted magnetically labeled mesenchymal stem cells in a model of perinatal brain injury and found that these cells migrate to lesion sites and proliferate [20]. Studies have demonstrated the differentiation of bone marrow, umbilical cord blood, neural and other progenitor stem cells into neurons and oligodendrocytes in experimental animal models [21–25]. Transplantation of stem cells in rat models have resulted in improved cognition and sensorimotor deficits along with functional recovery [26].
\nStem cell therapy in cerebral palsy.
In cerebral palsy, around 26 studies have been published explaining the effect of stem cell therapy. Overall, 579 (90%) out of 646 patients have shown improvements (Table 1) [20, 27–51].
\nSr. no | \nCitations | \nCells used | \nRoute of administration | \nSample size | \nPatient improved | \nAdverse events | \n
---|---|---|---|---|---|---|
1. | \nSharma et al. [27] | \nAutologous bone marrow mononuclear cells (BMMNCs) | \nIntrathecal | \n40 | \nNone | \n\n |
2. | \nMin et al. [28] | \nAllogenic umbilical cord blood | \nIntravenous | \n96 | \n86 | \nPneumonia and irritability | \n
3. | \nLee et al. [29] | \nAutologous umbilical cord blood | \nIntravenous | \n20 | \n5 | \nNausea, hemoglobinuria or urticaria | \n
4. | \nPurandare et al. [30] | \nAutologous BMMNCs | \nIntrathecal | \n1 | \n1 | \nNone | \n
5. | \nChen et al. [20] | \nAutologous bone marrow mesenchymal cells | \nSubarachnoid | \n60 | \n60 | \nIncreased frequency of crying | \n
6. | \nLi et al. [31] | \nAutologous bone marrow mesenchymal cells | \nSubarachnoid | \n1 | \n1 | \nNone | \n
7. | \nLuan et al. [32] | \nNeural progenitor cells | \nIntracranial | \n45 | \n45 | \nNone | \n
8. | \nChen et al. [33] | \nOlfactory ensheathing cells | \nIntracranial | \n33 | \n33 | \nNone | \n
9. | \nRamirez et al. [34] | \nUmbilical cord blood cells | \nIntramuscular injection | \n8 | \n8 | \nLocalized mild pain at the site of injection. | \n
10. | \nPayne [35] | \nUmbilical cord blood cells | \nSubcutaneous | \n16 | \n16 | \nNone | \n
11. | \nSharma et al. [36] | \nAutologous BMMNCs | \nIntrathecal | \n1 | \n1 | \nNone | \n
12. | \nSharma et al. [37] | \nAutologous BMMNCs | \nIntrathecal | \n1 | \n1 | \nNone | \n
13. | \nPapadopoulos et al. [38] | \nAutologous BMMNCs | \nIntrathecal | \n2 | \n2 | \nNone | \n
14. | \nSharma et al. [39] | \nAutologous BMMNCs | \nIntrathecal | \n1 | \n1 | \nNone | \n
15. | \nJensen and Hamelmann [40] | \nAutologous umbilical cord blood cells | \nIntravenous | \n1 | \n1 | \nNone | \n
16. | \nWang et al. [41] | \nUmbilical cord mesenchymal stem cells | \nIntravenous and intrathecal administration | \n1 | \n1 | \nTemporary low‐grade fever | \n
17. | \nLuan et al. [42] | \nHuman neural stem cells | \nIntracerebral | \n7 | \n4 | \nNone | \n
18. | \nWang et al. [43] | \nBone marrow mesenchymal stromal cells | \n– | \n52 | \n52 | \nnone | \n
19. | \nYang et al. [44] | \nUmbilical cord mesenchymal stem cell | \nIntravenous and intrathecal | \n25 | \n22 | \nnone | \n
20. | \nZali et al. [45] | \nCD133‐positive enriched bone marrow progenitor cells | \nIntrathecal | \n12 | \n12 | \nseizure | \n
21. | \nMancías‐Guerra et al. [46] | \nAutologous bone marrow–derived total nucleated cell (TNC) | \nIntrathecal and intravenous injection | \n18 | \n18 | \nHeadache, vomiting, fever and stiff neck | \n
22. | \nRomanov et al. [47] | \nAllogenic umbilical cord blood cells | \nIntravenous | \n80 | \n80 | \nNone | \n
23. | \nZang et al. [48] | \nUmbilical cord blood mesenchymal stem cells | \nIntravenous | \n1 | \n1 | \nNone | \n
24. | \nWang et al. [49] | \nUmbilical cord–derived mesenchymal stromal cell | \nSubarachnoid | \n16 (8 pair of twins) | \n16 (8 pair of twins) | \nNone | \n
25. | \nShroff et al. [50] | \nHuman embryonic stem cells | \nIntravenous | \n91 | \n63 | \nSeizures | \n
26. | \nAbi Chahine et al. [51] | \nBone marrow mononuclear cells | \nIntrathecal | \n17 | \n11 | \nHeadaches, transient fever and vomiting | \n
Clinical evidence demonstrating the use of stem cells in cerebral palsy.
In 2015, we published a nonrandomized study demonstrating the benefits of autologous bone marrow mononuclear cells (BMMNCs) in cerebral palsy [27]. These patients were followed up at 3 and 6 months. Six months after intervention, 38 out of 40 (95%) patients showed improvements and 2 did not show any improvement but remained stable without any deterioration (Figure 3). No major adverse events were noted except for seizures in two patients which were controlled by medications.
\nGraph showing improvement in children with cerebral palsy after stem cell therapy.
We have also published three case reports demonstrating the safety and efficacy of BMMNC transplantation in cerebral palsy [36, 37, 39]. In these case reports, the functional improvements are supported by improved brain metabolism recorded in comparative PET‐CT scans performed before and after the intervention.
\nIn autism, immune dysfunction, hypoperfusion, oxidative stress, decreased number of Purkinje cells (PCs), cerebellum alterations, defective cortical organization and altered plasticity of dendritic spine morphology are the underlying neuropathologies (Figure 4) [52, 53]. Stem cells modulate the immune dysfunction by releasing anti‐inflammatory molecules and inhibiting pro‐inflammatory molecules, which further reduces neural injury [54]. They also facilitate angiogenesis which increases blood and oxygen supply to the brain thus reversing the hypoperfusion [55]. Stem cells may also reinforce cortical plasticity, promote synaptic plasticity and restore cerebellar PCs [56]. These mechanisms collectively may improve the lost neural connectivity and restore lost functions in autism. In an experimental model of mice, H Segal Gavish et al. transplanted mesenchymal stem cells, which resulted in reduction of stereotypical behaviors, decrease in cognitive rigidity and improvement in social behavior. Tissue analysis revealed elevated BDNF protein levels in the hippocampus accompanied by increased hippocampal neurogenesis in the MSC‐transplanted mice compared with sham treated mice [57].
\nStem cell therapy in autism.
A total of 11 studies (3 case series and 8 case reports) have been published all over the world demonstrating the benefits of stem cell therapy in autism. Overall, 122 patients were administered with cellular therapy and 90 showed improvements (Table 2) [58–68].
\nAuthor | \nType of cells used | \nRoute of administration | \nSample size | \nHow many patients improved | \nDemonstrated safety | \n
---|---|---|---|---|---|
Sharma et al. [58] | \nAutologous bone marrow mononuclear cells (BMMNCs) | \nIntrathecal | \n32 | \n29 | \nYes | \n
Lv et al. [59] | \nHuman cord blood mononuclear cells (CBMNCs) and umbilical cord–derived mesenchymal stem cells (UCMSCs) | \nIntravenous and intrathecal | \n37 | \n18 | \nYes | \n
Bradstreet et al. [60] | \nFetal stem cells | \nSubcutaneous | \n45 | \n35 | \nYes | \n
Sharma et al. [61] | \nAutologous BMMNCs | \nIntrathecal | \n1 | \n1 | \nYes | \n
Sharma et al. [62] | \nAutologous BMMNCs | \nIntrathecal | \n1 | \n1 | \nYes | \n
Sharma et al. [63] | \nAutologous BMMNCs | \nIntrathecal | \n1 | \n1 | \nYes | \n
Sharma et al. [64] | \nAutologous BMMNCs | \nIntrathecal | \n1 | \n1 | \nYes | \n
Sharma et al. [65] | \nAutologous BMMNCs | \nIntrathecal | \n1 | \n1 | \nYes | \n
Sharma et al. [66] | \nAutologous BMMNCs | \nIntrathecal | \n1 | \n1 | \nYes | \n
Sharma et al. [67] | \nAutologous BMMNCs | \nIntrathecal | \n1 | \n1 | \nYes | \n
Sharma et al. [68] | \nAutologous BMMNCs | \nIntrathecal | \n1 | \n1 | \nYes | \n
Clinical evidence demonstrating the use of stem cells in autism.
In 2013, we published an open label proof of concept study which included 32 patients of autism [58] (Figure 5). These patients were followed up for 26 months (mean 12.7). The outcome measures used were Childhood Autism Rating Scale (CARS), Indian Scale for Autism Assessment (ISAA), Clinical Global Impression (CGI) and Functional Independence Measure (FIM/Wee‐FIM) scales. It was found that out of 32 patients, a total of 29 (91%) patients improved on total ISAA scores and 20 patients (62%) showed decreased severity on CGI‐I. On CGI‐II 96% of patients showed global improvement. Improvements in brain metabolism were also observed on positron emission tomography‐computed tomography (PET‐CT) scan brain. All 32 patients were monitored through the duration of follow‐up for any major adverse events. Incidence of seizures was recorded in three patients, which were reversible and easily controlled with medications.
\nGraph showing percentage improvement in various symptoms of autism post stem cell therapy.
In addition to the above study, we have also published eight case reports demonstrating the safety, efficacy and objective improvements on PET‐CT scan brain in patients with autism following stem cell therapy [61–68].
\nIn intellectual disability (ID), the neuronal connectivity in the brain is impaired along with disrupted cell migration, cell multiplication, axon growth, brain plasticity and synaptogenesis (Figure 6) [9]. Studies have recorded defects in hippocampus and cerebral cortex areas of the brain leading to faulty information processing, consecutively affecting cognition and adaptive behavior in ID. Stem cells restore the synaptic transmitters released and provide local reinnervations to the area affected. It also integrates existing neural and synaptic network and re‐establishes connections of functional afferent and efferent cells which may have contributed in restoring the cognitive and functional deficit in IDs [69].
\nStem cell therapy in intellectual disabilities.
We are currently under process of analyzing the data of a prospective study conducted to demonstrate the effect of autologous bone marrow mononuclear cells in intellectual disability. However, in 2015, we published a report of a 13‐year‐old boy with intellectual disability who exhibited improvements after stem cell therapy [70]. He was followed up after 3 and 6 months of intervention. No major adverse events were recorded post intervention. Over a period of 6 months, he showed improved eye contact, cognition, learning ability, behavior and ability to perform activities of daily living. His score on Functional Independence Measure (FIM) increased from 67 to 76. On comparing the pre and post PET‐CT scan, improvement in metabolic activity of hippocampus, left amygdala and cerebellum was recorded. These changes correlated to the functional outcome.
\nThe underlying pathogenic mechanism of muscular dystrophy is an imbalance between muscle degeneration and resident satellite cell–mediated regeneration [71]. Satellite cells, the adult skeletal muscle progenitor cells, are considered to be the main cell type involved in skeletal muscle regeneration. Continuous cycles of degeneration and regeneration of muscle fibers exhausts the muscle stem cell pool, leading to muscle being replaced by adipose and fibrotic tissue. Stem cell therapy holds great promise as a treatment for Duchenne muscular dystrophy by providing cells that can both deliver functional muscle proteins and replenish the stem cell pool [72].
\nStem cells are known to enhance angiogenesis, contribute to neovascularization, promote tissue remodeling, prevent apoptosis, decrease inflammation, release growth factors and activate the satellite cells [73] (Figure 7). In animal models, these cells have shown to produce the deficient proteins and make new muscle cells which fuse with the host fibers. Further, stem cell–derived exosomes which are small membrane vesicles and are responsible for inter‐cellular communication, promote muscle regeneration by enhancing myogenesis and angiogenesis [74].
\nRole of stem cells in muscular dystrophy.
A total of 14 studies have been conducted demonstrating the efficacy of stem cells in muscular dystrophy. Various types of stem cells such as bone marrow–derived cells, umbilical cord stem cells and muscle‐derived cells were used. Out of a total of 346 patients who underwent stem cell therapy, 296 showed a positive outcome (Table 3) [75–90].
\nAuthor | \nSample size | \nType of cells used | \nRoute of administration | \nNumber of patients improved | \nLevel of evidence | \n
---|---|---|---|---|---|
Torrente et al. [75] | \n8 | \nMuscle‐derived CD133+ cell | \nIntramuscular | \n8 | \n4 | \n
Yang et al. [76] | \n82 | \nAutologous bone marrow mesenchymal stem cells (BMSC) and umbilical cord mesenchymal stem cells (UMSC) | \nIntravenous and intramuscular | \nEffective in 68 [82.9%] cases. | \n4 | \n
Mendell et al. [77] | \n12 | \nMuscle precursor cells | \nIntramuscular | \nIn one patient, 10.3% of muscle fibers expressed donor‐derived dystrophin after myoblast transfer. Three other patients also had a low level of donor dystrophin; eight had none. | \n4 | \n
Sharma et al [78] | \n150 | \nBMMNCs | \nIntrathecal, Intramuscular | \n130 [86.67%] cases showed symptomatic and functional improvements | \n4 | \n
Rajput et al. [79] | \n16 | \nHuman umbilical cord mesenchymal stem cells | \nIV and IM injection | \n9 out of 11 patients were stable no deterioration. | \n\n |
Sharma et al. [80] | \n65 | \nBMMNCs | \nIntrathecal, Intramuscular | \n65 (plateau phase, no further progression) | \n4 | \n
Skuk et al. [81] | \n1 | \nMuscle‐precursor cells | \nIntramuscular | \n27.5% of the myofiber profiles expressed donor‐derived dystrophin, 1 month post‐transplantation and 34.5%, 18 months post‐transplantation | \n5 | \n
Sharma et al. [82–87] | \n6 case reports | \nBMMNCs | \nIntrathecal, Intramuscular | \n6 | \n5 | \n
Kang et al. [88] | \n1 | \nUmbilical cord–derived hematopoietic stem cell | \nIntrathecal | \nnot effective | \n5 | \n
Skuk et al. [89] | \n3 | \nMyogenic cells | \nIntramuscular | \ndystrophin‐positive myofibers in the cell‐grafted sites amounting to 9 (patient 1), 6.8 (patient 2) and 11% (patient 3). | \n\n |
Zhang et al. [90] | \n1 | \nAllogeneic cord blood stem cells | \nIntravenous | \n1 | \n5 | \n
Clinical evidence demonstrating the use of stem cells in muscular dystrophy.
We conducted a study on 150 patients diagnosed with muscular dystrophy. On a mean follow up period of 12 months ± 1 month, 86.67% cases showed symptomatic and functional improvements, with six patients showing muscle regeneration and decrease in fatty infiltration on musculoskeletal magnetic resonance imaging (MRI MSK) and nine showing improved muscle electrical activity on electromyography (EMG). Fifty‐three percent cases showed increase in trunk muscle strength, 48% an increase in upper limb (UL) strength, 59% an increase in lower limb (LL) strength and about 10% showed an improved gait pattern (Figures 8 and 9).
\nGraph showing improvements in muscular dystrophy patients after stem cell therapy. y‐axis = number of patients (n = 150).
Graph showing symptomatic improvements in muscular dystrophy patients after stem cell therapy. Number of patients showing improvements in trunk strength, upper limb (UL) strength, lower limb (LL) strength, gait pattern, and standing function are shown. y‐axis = number of patients (n = 150).
The adverse events following stem cell transplantation mainly depends on the type of stem cell and the route of administration. Other factors like dosage of cells, frequency of transplantation and age of the patient may also contribute. Fetal stem cells are known to be potentially tumorigenic [91]. Use of umbilical cord stem cells is limited due to slow or incomplete immune reconstitution, resulting in a high transplantation‐related mortality (TRM) due to infections. Most studies have demonstrated a predominance of Gram‐positive bacteria (GPB) bloodstream infections [92]. On the contrary, adult stem cell has not shown any serious adverse events. Autologous cell transplantation is safer than allogenic.
\nAdverse events of stem cell therapy can be categorized into minor and major adverse events. Minor adverse events include procedure related events such as spinal headache, nausea, diarrhea, vomiting, pain or bleeding at the site of aspiration/injection and fever amongst others. These are treated using medications. Anesthetic complications and allergic reactions may also occur depending on the procedure. Major adverse events include episodes of seizures occurring after intervention. These can be managed prophylactically. Pre‐existing epileptogenic focus in Electroencephalogram (EEG) also predicts the occurrence of seizures. Evidence suggests that antiepileptic prophylactic regimen decreases the incidence of seizures as an adverse event after stem cell therapy [93].
\nThe route of delivery of cells plays an important role in maximizing the clinical output of cellular therapy. Intrathecal route of administration is a relatively minimally invasive and targeted route of administration of cells. It is devoid of any major side effects [94]. In neurological disorders, intrathecal transplantation enhances the accessibility of the injected cells into the CNS [95]. Intramuscular injections are administered at the motor points plotted on the affected muscles. Motor points are the points where the innervating nerve enters the muscle. Thus, implantation of cells in the muscles enhances the effect of stem cells on the degenerating muscles [96]. Intravenous administration is the least invasive route. However, evidence suggests that majority of cells get trapped in the pulmonary passage and only few cells reach the injured site [97]. An alternate route of administration is via intra‐cerebral route. But, it is an invasive technique and might result in secondary complications such as bleeding and neural tissue injury [98]. Hence, as compared to all the delivery routes, intrathecal administration is most efficacious.
\nCells used from allogenic sources have an inherent risk of immunogenicity and may potentially cause immune rejection of graft versus host disease. Autologous cells have the least possibility of immune reaction and so far clinical studies with autologous minimally manipulated cells have shown no immunogenic reactions in the host post transplantation. Autologous cells may therefore be a safer option in children with NDD.
\nGenetic factors play a major part in the pathology of neurological disorders and gene therapy has provided novel insights in treating the underlying genetic aberrations. But gene therapy cannot replace the lost neurons and practical difficulties have prevented it from being a clinically feasible and viable option at present. The sporadic nature of the disease is also an important factor influencing the outcome, where the etiology of the disease is unknown. Stem cell therapy addresses the core injury occurring in the brain. The multiple mechanism of action of the stem cells addresses the multifactorial pathology of the NDD.
\nIt has been observed that the mild cases of neurodevelopment disorders have a better recovery curve than the chronic cases. In mild cases, axonal function remains intact and recovery can be rapid if remyelination occurs. In severe cases, axonal degeneration occurs and recovery depends on axonal regeneration. Recovery becomes much slower, and there is a greater degree of residual injury. Mild cases require lesser dosage of cells and the frequency of doses required is less to attain potential recovery than the severe cases.
\nOne of postulated hypothesis is that the neural circuits, that form the basis for learning, behavior and health, are more plastic during the initial years of life. They become increasingly difficult to alter over time. Age‐related decline in the potency of the stem cells is observed which might also affect the remodeling of CNS by these cells. Early intervention is advised for better outcome of stem cell therapy.
\nNeurorehabilitation aims at restoration and maximization of functions that have been lost due to impairments caused by injury or disease of nervous system making the patient functionally independent. The rehabilitation regime promotes and facilitates neural plasticity [99]. Studies have shown that exercise enhances the effect of injected stem cells by inducing mobility of the cells, activating and proliferating the local stem cells, promoting muscle angiogenesis and release of cytokines and nerve growth factors. Hence, neurorehabilitation compliments with the stem cell therapy [100].
\nNeuroimaging techniques enable the quantitative measurement of various biological markers which may serve as a powerful tool for optimizing the use of stem cells for clinical applications.
\nPET‐CT scan brain can be used efficiently as a monitoring tool to study the outcome of stem cell therapy. One of the advantages of using PET‐CT is its extreme sensitivity enabling it to detect molecules at the nanomolar level [101]. Brain 18F‐FDG PET allows studying the cerebral glucose metabolism, indicating the neuronal and synaptic activity. It dynamically measures the energy metabolism along with blood oxygenation and blood flow [102]. The alteration in neuronal activity caused by disease is reflected in change of glucose metabolism and can be revealed in the PET‐CT scan brain. As mentioned previously in the clinical results, there were improvements recorded in the brain metabolism of patients included in the clinical studies. The changes seen on PET‐CT scan brain correlated with the clinical improvement indicating that it can identify alteration occurring at the tissue levels (Figures 10–12).
\n(A) Pre SCT PET‐CT scan images with blue areas indicating hypometabolism. (B) These areas have almost disappeared after SCT as seen in the post PET‐CT scan image. This shows improvement in the metabolism/functioning in the affected areas of the brain after SCT.
Findings in PET‐CT scan before and after cellular therapy. (a) PET‐CT scan before intervention showing reduced FDG uptake in the areas of frontal lobe, cerebellum, amygdala, hippocampus, parahippocampus, and mesial temporal lobe. (b) PET‐CT scan six months after intervention comparison shows increased FDG uptake in the areas of frontal lobe, cerebellum, amygdala, hippocampus, parahippocampus, and mesial temporal lobe.
(A) Pre stem cell therapy PET‐CT scan showing blue areas with hypometabolism. (B) Post stem cell therapy PET‐CT scan showing decrease in blue areas which is replaced by green areas indicating improved functioning of the brain.
Magnetic resonance imaging (MRI) is gaining popularity because of its capacity to reveal characteristic findings that address the diagnosis and support therapeutic interventions. Since MRI is devoid of ionizing radiations, it has turned out to be a valuable imaging method in children, although sometimes sedation might be necessary. In the past few years, studies have reported on the detection of muscle involvement pattern in various muscular dystrophies through MRI musculoskeletal imaging (MRI/MSK). The images provide a high soft tissue contrast allowing assessment of affected striated muscles in terms of shape, volume (hypotrophy and hypertrophy) and architecture [103, 104]. MRI MSK was used as a tool to assess the therapeutic efficacy of stem cell therapy in muscular dystrophy. In our published data, images of MRI MSK performed after intervention has revealed stabilization of disease progression in muscular dystrophy.
\nIn children, the brain is still at a developing stage and not fully matured resulting in maximal neural plasticity during childhood. Hence, likelihood of improvement in affected areas of the brain increases manifold with early intervention. Stem cell therapy has recently gained lot of importance as a therapeutic strategy for various disorders including NDDs. In this review, we have demonstrated the outcome of stem cell therapy in NDDs mainly cerebral palsy, autism, intellectual disability and muscular dystrophy supported by our published data. Through its neurorestorative and neuroregenerative property, stem cells have the capacity of repairing the underlying neural and muscular dysfunction. This property can augment neurodevelopment, facilitating achievement of milestones earlier as compared to the current conventional treatment modalities. In progressive developmental disorders like muscular dystrophies, stem cell therapy has shown to slow down the disease progression. The data also establishes the fact that autologous stem cell therapy is a safe and efficacious treatment which helps in recovery of lost functions and neural plasticity.
\nThough stem cell therapy is not a cure, the gap between normalcy and disability can be minimized. Stem cells in combination with the multidisciplinary medical and rehabilitative modalities can enhance and hasten the recovery from NDD which will help the patient to lead a productive and respectable life in the society.
\nStem cell therapy is still in its developing stage. There are still numerous uncertainties prevailing with respect to optimum volume of cells to be injected, number of doses, route of administration, types of cells amongst others. The advent of induced pluripotent stem cells (iPSCs) has provided opportunities for the study of human neurodevelopmental diseases in a controlled environment. Reprogramming cells from patients with neurological diseases will allow the study of disease‐specific cellular and molecular pathways causing these diseases. Also, the establishment of neural stem cells (NSCs), a life‐long source of neurons and glia, has contradicted the dogma that the nervous system lacked regenerative power. Future studies need to focus on the precautionary pre‐intervention assessments to identify patients with high risk for seizures and related adverse events after stem cell therapy. A better knowledge of all these factors will improve the therapeutic effectiveness of stem cell therapy. Future studies should consider the use of modern radiological tools as monitoring tool and substantiate the effects of cellular therapy in NDDs. Large scale, multicentre and randomized controlled trials are recommended to further establish the safety and efficacy of cellular therapy.
\nRedox flow batteries (RFB) are electrochemical reactors suitable for storing electrical energy by chemical reactions. [1] Depending on the technology used, this reaction can take place at elevated temperatures and/or in aggressive media, with an electrochemical potential superimposed. In recent years, the technical requirements on materials and components of the reactor of the Redox flow battery have therefore become more and more demanding. The battery unit consists of many stacked cells which are connected in series to a Flow battery stack. Each cell in turn consists of various components such as the proton exchange membrane, seals, frames and the conductive bipolar plate which provides the connection from cell to cell up to the end of the stack where the generated current is collected.
RFBs, in particular vanadium redox flow batteries (VRFBs), have now reached a considerable degree of technical maturity and the systems are available on the market through many suppliers. However, due to a high remaining cost structure - partly due to a lack of economies of scale - the profitable market introduction of flow batteries still suffers from a high market acceptance.
On the one hand the membrane is considered the heart of a redox flow battery. On the other hand, the bipolar plate is one of the key components of an RFB. However, the Bipolar plate is important, since the plate has an impact on the complete systems, as far as total dimensions, total weight, thermal and electrical properties of the stack and thus of the system is determined by the bipolar plate technology. [2]
As already mentioned, the chemical conditions for the materials used in redox flow batteries are challenging. [3] Most systems are operated between 40°C and 60°C in a liquid of dissolved vanadium salts in sulfuric acid. Besides the Vanadium-technology, there also some other technologies (metallobased or organic RFBs), which will not be further considered.
Due to these harsh conditions, superimposed by an electrochemical potential, graphite-based bipolar plates with polymeric binders are used in almost all applications in these battery stacks. The graphite composite plates are an unbeatable material in terms of stability under the above-mentioned corrosive conditions, and the cost-intensive coated metal plates have no chance.
They have been operated very adequately several times over the years. However, due to an intrinsic fragility caused by a high filling load with graphite, graphite composite plates require a greater thickness than metal plates, resulting in more weight and volume of the stack. From a cost point of view, the membrane is certainly considered the dominant part of the redox flow battery stack. However, the bipolar plates tend to be underestimated both in terms of their technical requirements and, in particular, their contribution to the cost structure.
Graphite composite based bipolar plates are manufactured using highly filled compounds [2]. They contain fillers like graphite and/or other electrically conductive carbons incorporated in polymers performing as a gluing binding matrix. The key challenge is the competing interaction between electrical conductivity - achieved by the carbon component - and mechanical stability as well as liquid tightness which is provided by the binding polymer.
The compounding process is the first step to produce highly filled, electrically and thermally conductive pellets for the subsequently following step of forming bipolar plates.
Both compounding and molding processes, which can be injection molding, compression molding or continuously extrusion, are very sensitive to process parameters and need to be carefully controlled. The objective is to manufacture bipolar plates in large volumes and high quality more or less like standard plastic parts. Only by using price cost attractive materials and the consequent focus on process automation by higher volume, the bipolar plate can contribute significantly to a better market acceptance of RFB.
Besides the bipolar plate, the gasket is a very important component of the battery stack and tends to be heavily underestimated. It plays a key role in the mechanical properties of the stack. Inappropriately selected gasket materials may cause cracks in the bipolar plates or may affect the membrane-structure negatively. Despite the fact that the gasket has to seal the stack, the cooperation with other stack components and their cumulative tolerance effects have to be on focus for the stack design and for the operation of its.
The same which is evident for each component is also obviously for the gasket; they have to be cost attractive. Therefore, in some research projects, it is the objective is to suspend gaskets completely and use welding or bonding processes instead.
Technically, the bipolar plate of a RFB stack has to accomplish the following functions [3, 4]:
conduct electrical current,
conduct heat and distribute coolant in a eventually incorporated cooling flow field,
provide mechanical stability of the stack,
prevent permeation and leakage
However, the functions of the gasket are completely different. The main functions of gaskets in a RFB stack are [5, 6]:
sealing and leakage prevention of anode and cathode area,
sealing and leakage prevention of cooling plates,
compensate tolerances and dimensional changes during stack-assembling caused by interaction with all stack components.
Based on the technical functions described above, a comparison to other technologies is necessary: The Fuel Cells: The US department of energy (DoE) suggested development targets for fuel cell components as shown in the Table 1 for bipolar plates [8]. Although these data are based on communication and data from conventional low temperature PEM fuel cell developers, most of the targeted values can be directly transferred to Redox-Flow technology.
Technical property | Units | Targeted value |
---|---|---|
Plate weight | < | |
Electrical conductivity Depending on type | > | |
Thermal conductivity | > | |
Flexural strength | > | |
Shore D hardness | > | |
Temperature resistance Thermo-mechanical test | > | |
Acid uptake Depends on application or technology | low |
Benchmarks for bipolar plates in redox-flow applications defined by DoE [7] and experiences from customer requirements from Eisenhuth GmbH & Co. KG.
Additionally, the chemical resistance of the bipolar plate can be characterized by measuring the corrosion current under a potential typical for RFB and using sulfuric acid or something suitable (depending on application as an electrolyte). The detailed parameters and development objectives of this corrosion test are still subject to technical discussions and depend on the anticipated application of the plate. A similar table of functional requirements can be set-up also for gasket materials in RFB.
The gasket material has to be resistant against the selected electrolyte and environment under operating conditions. This is qualified for example by comparison the mechanical properties of recently produced and altered samples. It has to be noted that the values mentioned in Table 2 are for orientation and refer to standard elastomer materials available on the market. Based on these technical requirements, an appropriate feedstock respectively materials for both bipolar plates and gaskets have to be selected.
Technical property | Units | Targeted value |
---|---|---|
Density | ||
Electrical conductivity Depending on type | < | |
Shore D hardness | < | |
Compression set | < | |
Temperature resistance Thermo-mechanical test | > | |
Chemical stability Depends on RFB-type | Resistant against the used chemical environment; no or low changes in properties (typically mechanical) |
Proposed benchmarks for gaskets in RFB based on fuel cell requirements [9] and experiences from customer requirements from Eisenhuth GmbH & Co. KG.
As mentioned above, composite bipolar plates consist of a binder polymer, which is highly filled with a conductive carbon component. Typical compositions are >80 wt.% conductive filler and < 20 wt.% binder polymer. Compounding, processing and manufacturing is substantially different from conventional polymers due to the high content of filler material in the compound [10]. The function of the carbon filler is to provide electrical and thermal conductivity.
Therefore, a three-dimensional percolating carbon structure is required. Usually, the main carbon component of the plate is synthetic graphite and the second material is carbon black. For producing plates, several options are possible:
Compression molding
Injection molding
Plate Extrusion
Foil Extrusion
In all methods, after removal from the process certain after treatment procedures may be necessary. Either to remove the ‘skin’ of the mold release agent from the surface of the plate or as noted in Derieth et al. [9, 10] to remove an accumulation of polymer from the injection. Or compression molding skin.
In general, two different concepts of polymer binders can be applied in bipolar plates. First, the binder material can be polymerized or cross-linked in-situ in the composite during molding of the plate (resin method). The used polymer is thermosetting, which provides good mechanical properties at elevated temperatures and often a relatively easy processing. [11]
Second, a thermoplastic polymer material can be used in the compounding process (thermoplast method). Since the most materials in RFB are thermoplastic materials, in the following the focus will be also in this consideration. The polymer has to be selected with sufficient chemical, mechanical and thermal stability (e.g. data from [11]). Several material candidates are available on the market in high quality and well-defined configurations for different processing methods and applications due to the usage of additives like waxes, minerals or fibers.
Figure 1 shows the well know pyramidal classification for more than a handful of popular plastics.
The plastics pyramid preferred materials for RFB applications are semi-crystalline materials such as PP, PE and PVDF [9].
While graphite is generally the major filler for bipolar plates to achieve a sufficient conductivity, several other carbon additives can be employed in order to boost conductivity properties of the composite material. Examples for such additives are highly conductive carbon nano tubes (CNT), high surface carbon blacks (CB) or multi-layer graphene nanoplatelets. [7]
Due to its crystalline layer structure graphite is inherently anisotropic in its physical properties e.g. electrical conductivity or its mechanical behavior. Electrical conductivity is being provided by the mobility of electrons within the graphite layers of each platelet. Contrary to the conductivity along the layers, graphite is perpendicular to these layers an electrical insulator. Thus, the bipolar plate manufacturing process should ‘promote’ different orientations of the platelets forming isotropic physical properties of the macroscopic plate material. Some additives such as carbon blacks are helpful to increase the number of conductive paths in the carbon-polymer-system. The nano-sized carbon blacks do function as a ‘gap-filler’ in the insulating polymeric matrix between the micro-sized graphite particles and this in consequence increases the overall material conductivity significantly. [7]
The overall conductivity in a bipolar plate is generated by a three-dimensional percolating network which consists of conductive particles. The carbon-binder system is always inhomogeneous and can be considered as a two-phase system of conductive carbon paths bonded in a polymer matrix as shown in Figure 2. The structure of the material highly depends on the chemical composition and not less important on the kind of the chosen processing-approach (compounding, molding, extruding…) and the therefore used parameters. The complete processing chain – from the raw material to the molded plate – has to be carefully controlled to ensure consistency and reproducibility of the bipolar plates.
Polarization microscopy of polished surface from bipolar plate with 80 wt.% graphite content. Particles (black) are locatable in polymer matrix (white).
Carbon blacks can be formed in the gas phase by thermal decomposition of hydrocarbons under different conditions [11] and this results in a broad variety of materials with differences in surface area, hydrophobicity and conductivity. The different carbon black grades are then available for the adequate application and function.
Keeping this in mind it has to be considered that high surface carbons are more disposed to (undesired) carbon corrosion effects than graphite-based materials, thus their positive conductivity effect has to be balanced against long term stability requirements.
Another important aspect of carbon materials is purity. Since most fuel cell membranes and catalysts are highly sensitive against contamination with Iron-ions and other metal residuals, the raw materials for bipolar plates have to be carefully characterized with respect to their contamination level. The carbon or graphite type also mainly determines bipolar plate’s properties like porosity, phosphoric acid uptake or corrosion and hydrophobicity, both regarding the surface and the bulk. [11, 12]
At status quo, the amount of waste caused by the production of bipolar plates – an inhomogeneous system consisting of plastic and carbon –is significantly higher when compared to a fully implemented commodity plastic production process. [13] The waste accrues in form of rejects from production, which can be lowered by optimization processes, but also in form of gates, which are necessary for production and dimensioned by material properties. In addition, the systems in which the material is used have a limited lifespan, so the demand of reusage of the parts made of graphite compound or the compound itself is conceivable.
On the other hand, there is the possibility to use secondary materials as feedstock of the graphite compounds to substitute fully or partially the conventional fillers. Conductive fillers like synthetic graphite are valuable resources being produced via different thermal processes, which are similar to other thermal processes e.g. some recycling processes for various other wastes. Some of these processes generate in some degree useful carbon materials. [13]
These circumstances and opportunities result in an increasing development of recycling methods with the consequence of a property upgrade of the carbon by combining lower general production costs. In the best case these carbons are suitable for bipolar plates. In Figure 3 the principle of the different recycling opportunities are being described.
Scratch of flow diagram for resources from recycling and secondary sources. The primal structure is from plastic treatment [14, 15, 16]. The obvious barriers are the contaminations and changes in material properties caused by multiplied processing.
Certainly, the final criteria of success for any bipolar plate is the in-situ control of performance and stability under real RFB conditions. However, RFB are highly complex systems with numerous sources of inconsistency. Thus, standardized ex-situ bipolar plate characterization is required for material development and quality control. Several test methods are well established for bipolar plates and some are presented below. The list of test methods is not considered to be complete.
Clearly, electrical conductivity both in-plane and through-plane is one of the most important properties of the bipolar plate. Despite most fuel cell (component) and battery laboratories have access to electrical conductivity testing equipment, by now there is no generally standardized test method for bipolar plates for RFB, and comparing results from different sources can show significant differences, even though the same samples are tested. One of the main reasons may be surface effects and pre-treatment of the sample. As shown in the Figure 4, Eisenhuth has implemented a testing system for this application, which is suited for local in-plane conductivity testing with the option to measure several times at different locations on the plate.
Testing device and method for electrical conductivity measurement at Eisenhuth GmbH & Co. KG.
The in-plane conductivity device allows for a conductivity mapping over a sample area of 750x300 mm. Thus, the characterizing of the plates with respect to the degree of homogeneity during production is possible. Conductivity mapping is an important tool both for quality control as well as and furthermore for the material and process development.
For graphite composite plates it is well known that compounding and molding are highly sensitive to process details and may generate inhomogeneous structures on the surface and/or in the inner core of the material. Certainly, the development target is a homogeneous distribution of conductivity with only minimal deviations between different points on the bipolar plate.
For PPG86 and BMA5 or BMA6 plates the compounding and manufacturing process in hot pressing are established and well controlled, and the conductivity mapping shows an even distribution. Irregularities in the conductivity are in some processes unavoidable because of the process-depending-orientation of the particles through different processing influences. For example, in injection molding the filler particles orientate differently from the core to the surface of the produced parts, which results in different conductivities measured In-plane or through-plane. In addition, the regions which will be filled lastly in injection molding show a higher average conductivity compared to the gate region.
A conductivity mapping of a second process example for a PPG86 based plate is shown in Figure 5. This specific plate is produced by plate extrusion. The border area of the plate parallel to the flow direction during the extrusion process seem less conductive.
In-plane conductivity mapping of a PPG86 based bipolar plate made by extrusion by another company who is also active in the field of redox flow batteries. The material shows a higher resistivity at the outside areas caused by the manufacturing-process. The results are corrected with finite size corrections for 4-point probe measurements. [17].
In terms of hot pressing – a process with a certainly low flow – these described irregularities are more dependent from the overall process stability and experience of the manufacturer. Development in the field of hot pressing by Eisenhuth GmbH & Co. KG in the last years are focused mainly in material research with the aim of reaching higher conductivity, larger plate designs and simultaneously easier production.
In Table 3 technical properties for bipolar plates made by hot pressing are shown. The data is measured with the shown in-plane conductivity measurement device and specimen according DIN EN ISO 527 tested on a universal testing device and a microbalance.
Technical property values | 2018 | 2020 | ||
---|---|---|---|---|
PPG86 | BMA6 | PPG86 | BMA6 | |
Density ( | 1.8 | 2.1 | 1.8 | 2.0 |
Electrical conductivity ( Depending on type | 96.2 | 192.3 | 185.2 | 312.5 |
Flexural strength ( | 21.1 | 31.8 | 22.4 | 31.7 |
Technical properties from databases from Eisenhuth GmbH & Co. KG.
The comparison between the results shows that the improvement of the standard products from Eisenhuth GmbH & Co. KG has led to an increase of the electrical conductivity from around 75%. But the mechanical behavior seems similar. This is due to optimizing process parameters and periodic testing of new raw materials.
As described above the material used for the bipolar plates in RFB applications is made out of plastics and conductive fillers like graphite. During RFB operation the bipolar plates are exposed to normal temperatures, such as 40°C. Consequently, all raw materials used for plate manufacturing have to resist approximately 40°C.
Parallel to the shortage of the raw materials, the Vanadium-RFB technology has to compete regarding cost- and technology-aspects to other technologies, in particular with the lithium ion storage technology. Knowing this background, it is more than advisably to look out for alternative materials. Thus, the Eisenhuth GmbH & Co. KG is investigating together with a consortium alternative material sources, in particular from the recycling sector. Two potential processes which produces carbon materials are shown in Figure 6.
Principle of producing carbon black and graphite from used tires (A) and in a hydrogen production in a methane cracking process (B). [13, 16, 18].
Both processes separate carbon in form of agglomerated particles. Tyres consists of rubber filled with carbon pigments to strengthen the material. By the oxygen-less combustion of tyres the carbon will be released and during the pyrolysis process it is being formed to agglomerates.
During methane cracking – a process to produce hydrogen - carbon can agglomerate on particles, which function as. The particles consist of contaminations of the used feed gas or are part of the used catalyst. [17]
The samples are called CB-RC for the tyre recycling carbon black and CB-MC for the methane cracking carbon black. Resulting curves of the mass loss over the temperature of TGA from different carbon blacks are shown in Figure 7. Samples of conventional carbon blacks are called CB-C.
TGA data from different carbon blacks. Conventional CB (CB-C) and CB from secondary sources (CB-MC and CB-RC) are compared. The differences in combustion temperatures and contents of ash are significant.
The thermogravimetric analysis (TGA) can be used in order to determine the combustion and vaporization temperatures of the materials and allows to quantify the contents of different materials in the compound. [19]
During TGA a sample is heated under defined conditions such as gas environment and heating rate. The weight loss as well as the temperature (in correlation to the weight loss) of the sample in the oven is being determined. The TGA is used at Eisenhuth as an instrument of permanent quality control of the process. It also can be used, to get more information about the compound material.
The TGA curves show that the secondary materials contain a high content of ash. The influence of the ash is at that point unknown. At best it does not influence or at least it has a minor influence on the properties of the compound respectively the plates. In the worst case some critical contaminations are soluble or volatile and will damage the system, in which the material is used. The details are shown in Table 4. The average combustion temperature is extracted from the curves at the point at which 50% of the weight of the combustible mass is lost.
Carbon black type | Average combustion temperature / | Rest mass (Ash) / |
---|---|---|
CB-C-I | 784.4 | 0.13 |
CB-C-II | 691.4 | −0.29 |
CB-MC-I | 684.7 | 8.66 |
CB-MC-II | 666.4 | 14.86 |
CB-MC-III | 695.8 | 10.18 |
CB-RC-I | 558.4 | 19.52 |
CB-RC-II | 541.4 | 12.45 |
Results of TGA from different CB-types. The CB tested are conventional (CB-C), products from methane cracking (CB-MC) and products from Tyre recycling (CB-RC). The average combustion temperature is at the point of 50% weight loss of the combustible mass.
The second that stand out is the difference of the combustion temperatures of the tested CB. A lower combustion temperature under the assumption that the tested materials consists of similar carbon structures is an indication for a higher surface area [20]. It is described that the surface area – normally measured for CB according ASTM D 2414 with dibutyl phthalate (DBP) – has an influence in the percolation threshold and the resulting conductivity of the corresponding compound. The percolation threshold is the small zone in which the compound receives a mayor increase in its electrical conductivity by only adding a very less of filler content. [21]
In order to characterize the influence of the different CB types on the conductivity, the secondary CB are integrated and evaluated in various testing and production series to compare the new materials with the current neat carbon black. The Table 5 shows the results of conductivity measurements like described above from different compounds, in which the CB types are used. For comparison individual references from the mentioned testing and production series are listed in the same table. The compounds are made by combining different polymers mostly PP with graphite. Some of the graphite is replaced with the different CB to keep the recorded filler content at the same level for all.
CB used in compound | Filler content / | Compound conductivity / | Reference conductivity / | CB used in Ref. |
---|---|---|---|---|
CB-C-I | 78 | 28.3 ± 2.0 | 13.2 ± 2.5 | None |
CB-C-II | 75 | 12.9 ± 0.9 | < 1 | CB-C-I |
CB-MC-I | 80 | 11.3 ± 1.2 | < 1 | None |
CB-MC-II | 80 | 10.6 ± 2.5 | < 1 | None |
CB-MC-III | 80 | 12.0 ± 1.5 | < 1 | None |
CB-RC-I | 75 | 8.9 ± 0.7 | 18.7 ± 0.6 | CB-C-I |
CB-RC-II | 75 | 9.0 ± 0.8 | 18.7 ± 0.6 | CB-C-I |
Results of conductivity measurements from different compounds. Partially consisting of the described CB types from conventional and secondary sources compared to individual references produced parallel the tested compound mixtures.
It can be observed that the impact of the secondary CB on the electrical conductivity is noticeable, but far less for CB-MC and CB-RC-types than the qualification by the TGA suggests. The compounds consisting the CB-MC types have a relatively low conductivity compared to standard materials but the reference compound with the same filler content has no measurable conductivity, therefore the CB-MC types seem to reduce the percolation threshold for the filler in the compound. The CB-RC types have compared to conventional CB a smaller impact on the conductivity because half the value of the CB-C-I consisting reference compound with the filler content of 75 wt.% has been measured.
The qualification by the TGA was fitting for the conventional types. Whereas the high differences between the prognosis and the measurement results for the secondary CB types are unexpected and a high level of uncertainty remains. The reason of these differences can be the high content of probably non-conductive contamination or different carbon structures of the particles. Both reasons are possibly responsible for a way lesser combustion temperature during TGA-measurements. The higher the lever of amorphous carbon and impurities so lower the combustion temperature and the achievable level of conductivity.
Since many years the fuel cell developers invested tremendous efforts in improvement and technological readiness of the core components, such as membranes and electrodes configuration. However, within the last years the gasket material was recognized more and more as an underestimated component. Despite the gasket does not directly contribute to the electrochemical processes, inappropriate gaskets can cause leakages. [6]
The increased use and establishment of the systems on the market, primarily among consumers, has resulted in a focus on safety issues during consumption and error sources during mass production.
Common hard gaskets support well defined gaps, however may be compromised in their sealing properties, do not compensate tolerances very well and may put mechanical distortion on the bipolar plates, which can cause cracks or breaking after a long time. On the other hand, with soft gaskets it is more difficult to control the performance of the system cause of limitations in parameters like pressure. These descriptions are analogue to RFB systems.
In general, like the other RFB components the gaskets have to resist temperatures up to 70°C, electrolytes like sulfuric acid or other materials of RFB systems like bromine and contact to electricity. Fluoroelastomers (FKM) and ethylene propylene diene monomer rubber (EPDM) are most likely the materials of choice for several applications.
For certain applications EPDM might be a cost-efficient alternative for systems which can handle the stiffness of this rubbers. The arguments clearly show that gaskets are a highly customized component for each stack manufacturer. For overview, some typical gasket properties for a broad variety of materials are shown in the Table 6.
Description and Unit | TPS | TPV | TPU | TPO | EPDM | SI | FKM | HNBR |
---|---|---|---|---|---|---|---|---|
Hardness Shore A | 2–95 | 20–95 | 2–85 | 65–95 | 25–85 | 25–85 | 50–90 | 40–90 |
Temperature range | −50 / +120 | −40 / +130 | −40 / +85 | −40 / +70 | −50 / +100 | −70 / +200 | −20 / +220 | −30 / +150 |
Steam resistance | — | — | — | — | ++ | ++ | ++ | ++ |
Oil resistance | + | + | — | + | — | + | ++ | ++ |
Acid /bases resistance | ++ | ++ | 0 | ++ | ++ | — | ++ | + |
Gasket material overview with typical physical properties and behavior in system specific conditions used by Eisenhuth GmbH & Co. KG.
Along with the rubber materials like silicone (SI), hydrogenated nitrile butadiene rubber (HNBR), EPDM and FKM thermoplastic elastomers (TPE) in form of styrenic block copolymers (TPS), thermoplastic vulcanizates (TPV), thermoplastic polyurethanes (TPU) and thermoplastic polyolefin elastomers (TPO) are listed. These thermoplastic-elastomers have similar properties to rubber but can be processed like “common” thermoplastics and can be softer if required. This has the advantage of easier manufacturing and recycling of the material as well as a broader range for applications.
In order to supply consistent gaskets with appropriate tolerances the viscoelastic properties of the gasket prepolymers and thermoplastics are an important parameter. A low viscosity is beneficial for processing. For plastic materials usually the mold flow rate or mold flow index are specified by the supplier, supporting the manufacturer for plastic parts with processing-relevant- information and –parameters. However, these data are ‘standard data’ and not always compatible with the molding conditions or equipment at the part manufacturer.
In addition, for rubber materials or their pre-polymers and thermoplastic elastomers these data are not available in most cases, because of their impacting viscoelastic behavior. Therefore, Eisenhuth developed a phenomenological test method to characterize polymer materials with respect to processability. In this test, a melt of the used pre-polymer or thermoplastic is pressed into a spiral-shaped mold with a defined pressure under process-relevant temperatures.
The viscous melt flows into the spiral mold and finally stops, when the applied pressure is equal to the ‘back-pressure’ in the mold. The reason therefore is the higher lever of the progressing polymerization, vulcanization or solidification of the melt. The length of the helix can be correlated to the viscosity and consequently to the processability. The longer the helix the lower the viscosity. This is helpful to find the processing ranges of materials as far as the viscosity is concerned (Figure 8).
Spiral mold for characterization processability by injection molding by Eisenhuth GmbH & Co. KG.
As mentioned, the length of the spiral is an good indicator for the processability. This test has been performed with a variety of potential gasket materials to achieve a data baseline. The values are shown in Figure 9.
Results of injection molding in spiral mold.
The results show that processability depends strongly on the material but different types of the same material have also high differences. Exemplarily shown in the Figure the good processability of some types of thermoplastic elastomer materials cannot be reached by the measured processability of rubber materials.
The processability of the thermoplastic elastomers is convenient but it is necessary to qualify the mechanical and chemical stability of the materials. The called rubbers are commonly used in different applications such as fuel cells and chemical industries, and their long-life behavior is already known.
To ensure the stability of the materials specimen according DIN EN ISO 37 are made and treated in this example in vanadium electrolyte for VRFB applications. The electrolyte is positive charged, so the most aggressive species of vanadium ions is to 1.65 mol/L concentrated in 4 mol/L sulfuric acid. The specimens are treated the same time for around thousand hours and therefore stored in glasses with full surrounding electrolyte. The specimens are tested for tensile strength according DIN EN ISO 37 in a universal testing machine. The resulting Young’s modulus are shown in Figure 10 and are exemplary for the overall changes in mechanical properties of the treated specimens.
Results of tensile strength testing according DIN EN ISO 37. The tested materials are different rubbers and thermoplastic elastomers. The untreated specimens are directly tested after production. The second data is generated after exposure of specimens with aggressive vanadium electrolyte used in VRFB.
It is shown that the stability of the rubbers in the specific environment is good. The modulus is low but there are no major changes measured. In average the thermoplastic elastomers are different to the rubbers. Most of the materials and material types have a higher modulus with low changes. TPU seems not suited for the application, moreover one indication are high changes such as superficial cracks in the surface of the sealing.
In this chapter the basics and advantages of graphite bipolar plates could be presented in connection with current research topics at Eisenhuth regarding the reduction of production costs and the related easier market introduction of RFB. Furthermore the suitability of easy to process thermoplastic elastomers as sealing material in RFB was shown.
It was explained that the proposed targets for material properties are not fully achieved, but that progress in materials research is possible. For example, the electrical conductivity of standard materials for RFB could be optimized by about 75% in recent years.
Options to reduce costs through recycling methods and use of secondary resources were discussed. It could be shown that the substitution of commercial carbon types such as synthetic graphite by secondary materials for composite production is possible.
The differences in the processability of rubber types and thermoplastic elastomers were shown by tests in a correspondingly designed injection mold. The chemical stability of some types of thermoplastic elastomers is tested for VRFB.
The authors acknowledge fruitful collaboration, extensive test work and the positive relationship to Technical University of Clausthal, German Aerospace Center Oldenburg (Institute of Networked Energy Systems) and Research Center of Fuel Cell Technology (ZBT) in Duisburg.
Public funding is gratefully acknowledged from Federal Ministry for Economic Affairs and Energy (Germany) and Ministry of Education and Research (Germany) in cooperation with the project holder Forschungszentrum Jülich in the projects ‘Redox Flow Extrusion’, ‘Re3dox’, ‘Demo-Bio BZ’ and from the State of Lower Saxony in the project “Maleskues” and “Titan Porous Hybrid”.
The authors are part of the company Eisenhuth GmbH & Co. KG, which produces bipolar plates made of graphitic compounds and gaskets for fuel cell, redox-flow battery and heat exchanger purposes.
The shown data are part of the acknowledged public funded projects. The conclusions and statements made are based on the experience of the authors in their specific working fields in the said company.
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