Comparison of experimental and calculated M-ligand bond lengths (Å) of complexes (1–3).
\r\n\tHydrogen gas is the key energy source for hydrogen-based society. Ozone dissolved water is expected as the sterilization and cleaning agent that can comply with the new law enacted by the US Food and Drug Administration (FDA). The law “FDA Food Safety Modernization Act” requires sterilization and washing of foods to prevent food poisoning and has a strict provision that vegetables, meat, and fish must be washed with non-chlorine cleaning agents to make E. coli adhering to food down to “zero”. If ozone dissolved water could be successively applied in this field, electrochemistry would make a significant contribution to society.
\r\n\r\n\t
\r\n\tOxygen-enriched water is said to promote the growth of farmed fish. Hydrogen dissolved water is said to be able to efficiently remove minute dust on the silicon wafer when used in combination with ultrasonic irradiation.
\r\n\tAt present researches on direct water electrolysis have shown significant progress. For example, boron-doped diamonds and complex metal oxides are widely used as an electrode, and the interposing polymer electrolyte membrane (PEM) between electrodes has become one of the major processes of water electrolysis.
\r\n\t
\r\n\tThe purpose of this book is to show the latest water electrolysis technology and the future of society applying it.
Psoriasis has a profound impact on patients’ everyday life. The burden of the disease extends beyond physical manifestations and includes significant physical, social and psychological impairment. Numerous studies have demonstrated the significant negative impact of psoriasis on quality of life (QoL) [1-5]. Furthermore, as a chronic disease, psoriasis affects the QoL of both patients and their close relatives in a cumulative way [6]. The family members of patients with psoriasis experience a wide range of detrimental effects on their lives with regards to psychological social and lifestyle modifications, interpersonal relationships, financial issues, family activities, sleep and issues related to the practical care of the patients.
\nVarious factors may contribute to the lower QoL of patients with psoriasis. The chronic nature of the disease and the lack of control over unexpected outbreaks of the symptoms are among the most bothersome aspects of psoriasis [7]. Patients may feel humiliated when they need to expose their bodies during intimate relationships, swimming, using public showers, or anyway living in conditions that do not provide adequate privacy [8]. Thus psoriasis affects patients’ social life, daily activities, and sexual functioning [9]. Treatment of psoriasis, as it may be associated with risk for adverse effects, is also an important component of the QoL of psoriasis patients [10]. By utilizing the Short Form-36 (SF-3 6), a generic QoL instrument, it has been demonstrated that psoriasis may cause as much disability as other major medical diseases, including heart disease, diabetes, and cancer [11].
\nPsoriasis is also related to several co-morbidities, especially cardiovascular diseases and psychiatric disorders. Moreover, cardiovascular risk factors are strongly associated with the severity of inflammation and the duration of disease [12-14].
\nImproving the QoL in psoriasis patients is an extremely important goal. Therefore, the interventions to improve the process of care of this population should also assess QoL outcomes, such as social functioning and emotional well-being, adjusting for the effects of co-existing chronic conditions. Disease-specific measures may be sensitive enough to detect and quantify small changes that are important to clinicians and patients [15]. Healthcare professionals have a crucial role in identifying and supporting affected patients and families. In order to establish a good relationship with family members and to be able to improve patients’ compliance, dermatologists should develop greater insight into the lives of psoriasis patients and their relatives.
\nIn this chapter, the impact of the different aspects of psoriasis on QoL will be reviewed.
\nResearch found that large percentages of patients with psoriasis reported considerably skin pain and discomfort [16,17]. Skin pain was reported by up to 42%, and skin discomfort by up to 37% of psoriasis patients [16, 18,19]. Skin pain and discomfort had a negative impact on functions such as sleep, mood and enjoyment of life [16]. Studies suggested that other psoriasis-related sensory skin symptoms were associated with sleep disturbances, psychological distress and impaired health related QoL (HRQoL) [20-25].
\nLjosaa et al. [17] showed that physiological factors such as skin pain and disease severity were significantly associated with HRQoL and that the association between skin pain and HRQoL was partly mediated by sleep disturbance, while less by psychological distress.
\nOther skin symptoms of psoriasis can significantly affect physical functioning, perception of disease, and QoL. These symptoms include itching, “skin shedding”, tightness, redness, dryness, and bleeding [2, 21]. In particular, a direct correlation between pruritus severity and depression has been shown [26]. Psoriatic lesions of the vulva were found in women with psoriasis, resulting in itching, burning and vulvar discomfort, and women with these symptoms more frequently demonstrated depressive symptoms [27].
\nPsoriatic skin lesions are often perceived by patients as making their physical appearance unsightly; skin lesions make them feeling disfigured and apprehensive that others will avoid or exclude them, resulting in low self-esteem and self-confidence [28, 29].
\nWhen psoriasis involves the palms and soles, which occurs in approximately 40% of patients, the pain and discomfort result in significantly greater physical disability than is experienced by patients without palmoplantar involvement [30]. Nail involvement, which is present in up to 50% of patients, may also limit daily activities such as basic self-care activities and housekeeping [31, 32].
\nPsoriatic arthritis (PsA) is a painful disease of the joints and connective tissue affecting 10-30% of patients with psoriasis, and is mainly localized at fingers, toes, wrists, hips and back [2, 3, 31, 33]. PsA can result in damage to bone and synovial membranes, pronounced disability, and increased mortality [33]. Patients with PsA have a significantly worse QoL than those without PsA, as measured by different questionnaires [31, 34].
\nPsoriasis is associated with a variety of psychological difficulties, including poor self-esteem, sexual dysfunction, anxiety, depression, and suicidal ideation [35]. The psychiatric morbidity in psoriasis may be primary or secondary to the impact of the disease upon the patients’ QoL.
\nHigh depression/anxiety scores, obsessionality and difficulties with verbal expression of emotions, especially anger, social stigmatization, high stress levels, depression, and other psychosocial co-morbidities experienced by patients with psoriasis are not always proportional to, or predicted by, other measurements of disease severity, such as body surface area involvement or plaque severity [36-46]. In general, psychological disturbances, including perception of stigmatization and depression, are stronger determinants of disability in psoriasis patients than are disease severity, location and duration [47]. The Italian PSYCHAE study, which measured psychological distress (PD) in 1580 patients with psoriasis by the General Health Questionnaire-12 (GSQ-12) and the Brief Symptom Inventory (BSI), found that there was no association between disease severity and PD [48].
\nIt is not surprising that perceived stress in patients with psoriasis, as well as with other chronic disease, predicts poorer QoL [49]. On the other hand psoriasis is generally thought to be made worse by stress. Various studies have reported an association between stress and psoriasis. In a study of 132 patients with psoriasis, 39% recalled a significant stressful event within one month before the first episode of psoriasis [50]. In contrast, a more recent prospective clinical study demonstrated that there was no direct relationship between stress and exacerbation of psoriasis, showed no clear relationship between stress levels and worsening of psoriasis and found no time relationships between stress and the appearance of psoriasis [51]. A factor analysis of the Psoriasis Life Stress Inventory revealed two stress-related factors contributing to the psychosocial impact of psoriasis: stress associated with anticipation of the reaction and avoidance by others, and stress associated with patients’ experience or beliefs about being evaluated exclusively on the basis of their skin [52]. So, stress is largely secondary to the cosmetic disfigurement associated with psoriasis, with great impact on QoL and possibly resulting in psychological morbidity.
\nStudies on the relationship between psychological factors and psoriasis severity have primarily been focused on depression, with conflicting results: some authors have found depression correlated with objective measures of disease severity [49], while others have not [53]. Anyway, relatively high rates of depression are reported in patients with psoriasis [54, 55]. Controlled studies found notably higher degree of depression in patients with psoriasis than in controls [56-58].
\nSuicidal ideation and cases of completed suicide have been reported in psoriasis. The prevalence of suicidal ideation has been reported to be 2.5% among less severely affected outpatients with <30% of their body surface involved and 7.2% among the more severely affected inpatients as compared to 5.2% in acne patients, 2.1% in atopic dermatitis patients and 0% in alopecia areata patients [57, 59]. Death wishes and suicidal ideation were associated with higher depression scores.
\nSome reports suggest a higher prevalence of alcohol abuse and cigarette smoking among psoriatic patients [60,61]. In one study, there was an 18% prevalence of alcoholism in patients with psoriasis compared to 2% among dermatologic controls [60]. Several studies have shown that treatment outcomes are worse in heavy drinkers [62-64]. Abstinence alone has been shown to possibly induce psoriasis remission, whereas restarting drinking may cause disease relapse [62, 65].
\nConcerning the evolution of PD in psoriasis, the longitudinal phase of the PSYCHAE study, that specifically evaluated this aspect in 1500 psoriatic patients during up to 12 months, showed that minor PD halved during the observation period, possibly due to improvement of clinical symptoms, while major PD remained stable [66]. The same authors investigated patients’ coping strategies and found that planning, active coping and acceptance were strategies most commonly employed by their patients while denial, behavioural disengagement, and substance abuse were the least frequent attitudes [48]. During the 12-month follow-up, active coping and avoiding dramatization by recourse to humor were predictive factors of amelioration of PD [66].
\nA stigma is severe social disapproval of a person based on a distinguishing characteristics [67]. It has also been defined as a biologic or social mark that sets a person off from others [68]. Visible lesions cause feelings of stigmatization which can lead to psychological stress and social withdrawal [69]. Psoriasis patients, even those with relatively mild symptoms, experience high stigmatization as compared to sufferers of other skin diseases, with significant impact on outcomes such as QoL, depression and disability [70-72]. Stigmatization has many forms: Ginsburg and Link identified different dimensions, including anticipation of rejection, feeling of being flawed, sensitivity to others’ attitude, guilt and shame, reduction of self-esteem [73].
\nAmong the themes at the basis of the stigma experience, shame has an important role. In different studies, patients with psoriasis reported feelings of embarrassment and shame compared to healthy controls [74, 75]. Shame is one of the most reported emotions, especially by women and by patients with a long disease duration [74]. Feelings of shame can have a strong impact on social life, since they can result in avoidance of public spaces, thus reducing social opportunities, even concerning employment [76].
\nBoehm et al. [67] have found that it is stigmatization that mediates between symptom severity and QoL, in particular the stigmatization parameters ‘reduction of self-esteem’ and ‘rejection’.
\nPsoriasis does not discriminate by gender. Studies generally show no difference in the severity of physical symptoms suffered by men and women. However, women and men have different subjective perceptions of how symptoms affect their social interactions, emotional states and, ultimately, their QoL.
\nMen can find it easier to distance themselves from the social effects of psoriasis. Women, in contrast, are more likely to report feeling ‘upset’, ‘disturbed’ or ‘ashamed’ in social settings [77]. Stress research provides another way of understanding differences between men and women’s reactions to psoriasis. Women may be more prone to perceive stress and may be more likely to perceive a greater impact on mental QoL [78].Other authors have shown that women may have a higher likelihood of being stress-reactors [79]. Boehm et al. [67] have found that women reported higher discomfort levels and higher stigmatization, and that, in general, gender differences are observable in the mental component summary score, but not in general-physical or skin-related QoL. The PSYCHAE study, conducted on nearly 1600 Italian psoriasis patients, found that the female gender was the most important predictive factor for psychological distress [48].
\nPsoriasis may involve genital skin. In a Netherlands study, of 1943 patients with psoriasis, over 45% reported genital involvement at some time during the course of the disease [80]. Relatively few studies have evaluated the impact of psoriasis on sexual health, however, according to these studies, psoriasis interferes with sexual relations in 35-50% of patients [76, 81, 82]. Sexual dysfunction and distress are particularly high when genital skin is affected.
\nPsoriasis has a negative influence on a patient’s desire for physical intimacy [83] and causes decreased libido in a substantial proportion of patients [81]. Feelings of shame and embarrassment about physical appearance and reduced sexual desire might play a major role in high distress and dysfunction scores in specific sexual indexes [84]. Impairment of sexual activity is more profound in patients with more severe psoriatic symptoms [85], and appears to be more prevalent in women [1]. The patients who believe psoriasis has a negative effect on their sexual lives have more symptoms of depression [81].
\nAlso the treatments used by patients with psoriasis may cause sexual dysfunction: some publications report that antipsoriatic medication such as methotrexate and etretinate might cause sexual impotence and erectile dysfunction [86-88].
\nPsoriasis causes significant occupational disability. Over 17% of patients aged 18-54 report psychologic effects in the workplace due to their disease [2], 6% of employed patients with severe psoriasis reported workplace discrimination [2], and 23% reported that psoriasis affected their choice of career [9]. Problems in work were more frequent in patients with palmoplantar psoriasis. Thus, it appears that psoriasis may have a negative impact on work both for psychological and clinical reasons [2, 9]. Wu et al [89] showed that psoriasis patients were more likely to have missed work for health-related reasons, had significantly more health-related work productivity impairment, and more overall work impairment [90]. This can have financial consequences and may limit lifetime earning potential and career. One study found that 86% of patients with severe psoriasis were ‘moderately’ or ‘a lot’ concerned with the time and costs of treating psoriasis [91]. Moreover, psoriasis prevents some patients from obtaining employment altogether [92]. Two studies in the UK found a lower rate of employment in patients with severe psoriasis [41, 92]. Patients with psoriasis who are working, however, tend to have a low work QoL [91]. Fleischer et al [93] theorized that the effect of psoriasis on a patient’s work life might result in reduced socio-economical standing and limitations and 34% of the study patients reported hardships due to the financial burden of the disease.
\nPoorer QoL of psoriasis patients is associated with increased healthcare resource utilization, independent of the clinical severity of the disease [94]. As stated previously in this chapter, measuring clinical severity of skin lesions does not fully capture the effect of the disease on patient QoL [47, 95].
\nThe study by Sato et al. [94] showed that healthcare resource utilization by European patients with plaque psoriasis, in terms of dermatologist visits and hospitalizations, is greater for those with poorer QoL, independent of clinical disease severity, and may decrease if QoL improves. These authors also found that poor QoL is also associated with employment disadvantages, even when controlling for disease severity, suggesting that indirect costs of psoriasis may also be augmented for patients who have a poor QoL.
\nIn childhood, QoL is greatly influenced by psoriasis. Data on QoL in juvenile psoriasis are limited, however some studies demonstrated the negative influence of psoriasis on the QoL of children by means of the Children’s Dermatology Life Quality Index (CDLQI) [96-100].The social development domain, which is one of the developmental milestones in a child, is particularly impaired [101]. Moreover, psoriasis in childhood causes a high degree of limitations on recreational activities in at least 15-30% of patients [101]. Itching and problems with treatments were shown to have the highest impact on the children’s QoL. The same authors showed that QoL in the long term is not determined by the age of onset of psoriasis.
\nOther authors demonstrated that the significant negative impact of plaque psoriasis on QoL of children with psoriasis is generally comparable to the impact of other serious pediatric chronic diseases, as arthritis, asthma, and diabetes [102]. The impairment in QoL impacts particularly emotional and school functioning [102].
\nOnly a few clinical trials have been conducted on the effect of treatments for psoriasis on QoL and some of them were not specifically designed to measure QoL but rather inferred the drug impact on QoL from its effect on the clinical symptoms of the disease.
\nAmong topical treatments, calcipotriol-betamethasone gel was reported to improve QoL in patients with scalp psoriasis [103]. Narrowband ultraviolet B (NBUVB) phototherapy administered three times a week for 6 months significantly improved QoL in 95 plaque-type psoriasis patients [104].
\nLow-dose (3 mg/kg/day), short-term cyclosporine therapy was effective in improving QoL as measured by Skindex-16 and GHQ-28 in 41 patients with mild to severe psoriasis [105]. An Italian longitudinal study on psoriasis patients followed up for 12 months observed that treatment with cyclosporine significantly reduced by 30% the risk for minor psychological distress, while methotrexate and topical corticosteroids were associated with significantly increased risks (33% and 185%, respectively) [66]. Additionally, results from a small study indicate that the use of cyclosporine for the treatment of nail psoriasis can lead to an improvement in QoL [106].
\nIn a Canadian randomized, placebo-controlled trial on 451 plaque psoriasis patients, voclosporin was reported to improve QoL, assessed by DLQI and Psoriasis Disability Index (PDI) [107].
\nA recent analysis of Japanese trials on infliximab demonstrates that a Psoriasis Area and Severity Index (PASI) 90 response is necessary to achieve a DLQI of 0 or 1. Since infliximab showed to achieve nearly 50% of PASI 90 responses, the authors infer that it might be useful in meeting the goal of a DLQI of 0 or 1 [108].
\nAn analysis of pooled data from two randomized, placebo-controlled trials evaluated the effects of adalimumab on the risk of symptom worsening in psoriasis and the subsequent impact on HRQoL. The analysis pointed out that clinically relevant worsening of psoriasis symptoms was associated with substantial worsening of HRQoL. Adalimumab treatment was associated with a reduction in risk of clinical worsening of psoriasis, but its specific effect on HRQoL was not reported [109].
\nA metanalysis of randomized, controlled trials of etanercept in patients with rheumatoid arthritis, psoriatic arthritis and psoriasis, evaluating among other outcome measures the effect of the drug on HRQoL, treatment with etanercept resulted in improvements in the physical and mental component summary scores (PCS and MCS), as well as in individual SF-36 domains across all indications [110]. The PRESTA trial, conducted in Germany, evaluated the effect of etanercept on a composite measure of skin symptoms, joint manifestations, and QoL [111]. At 24 weeks, around 30% of patients met the triad of efficacy outcomes. In juvenile plaque psoriasis, one randomized, controlled, longitudinal study described a significant positive effect of etanercept on QoL [100].
\nIn a subanalysis of the PHOENIX 1 and 2 trials on ustekinumab in psoriasis, aimed at evaluating the effect on HRQoL and sexual difficulties, ustekinumab treatment was associated with significant improvement in HRQoL and sexual difficulties due to psoriasis [112]. Another post-hoc analysis of the PHOENIX 2 trial showed that ustekinumab decreases work limitations, improves work productivity and reduces work days missed in the 1230 study patients with moderate-to-severe psoriasis [113]. The efficacy of ustekinumab was also evaluated in nail psoriasis and nail-associated QoL in a population treated for cutaneous psoriasis. Together with a statistically significant reduction of the nail psoriasis severity index (NAPSI), a significant improvement of the international onychomycosis QoL scores was observed at all time points up to 40 weeks [114].
\nIn children, in a psoriatic cohort treated in daily clinical practice, QoL was assessed by CDLQI. The results showed that all psoriasis treatments contributed to a significant improvement in children’s QoL, which was greatest with dithranol and systemic treatments. The highest positive impact with all treatments was observed on itching and sleep disturbances [115].
\nPsoriasis is associated with significant psychological distress, psychiatric morbidity, experience of stigmatization and decreased QoL. Several studies have demonstrated the significant negative impact of psoriasis on QoL, which is similar to the impact of other major chronic diseases as heart diseases, diabetes and cancer. Presence of psoriatic arthritis, psychiatric disorders, and other co-morbidities may further worsen QoL and should be taken into account. The association between symptom severity and QoL, though observed by some studies [98,116], is not always strong, and other studies found no significant association at all [48, 95]. Symptom severity has been shown to have a greater direct impact on the physical rather than the mental components of QoL, while the effects of stigmatization on QoL are more strongly mental [67]. Some research has concluded that ‘subjective experience of psoriasis is a more powerful determinant of QoL’ in comparison to clinical measures [117].
\nStudies have shown that dermatologists employ a problem-orientated coping style in caring’ for their patients, and often appear much more interested in investigating the superficial skin rather than the deep emotions of their patients [48]. On the contrary, it is essential that measures of psychosocial morbidity are included when assessing psoriasis severity.
\nIn clinical practice there is a great challenge for dermatologists to improve the QoL of adults and children with psoriasis. Greater attention should be paid to the possible limitations that these patients experience. The outcome of QoL measurements should be taken into account when deciding on treatment strategies. Dermatology professionals should be encouraged to identify patients, irrespective of gender and of severity of clinical manifestations, who perceive especially high levels of discomfort, indicate problems in maintaining self-esteem and/or have experienced instances of rejection. Specific therapeutic strategies that address issues of self-esteem and social rejection are appropriate especially for these patients. Optimal therapy that leads to long-lasting remission can only be achieved by addressing both the physical and psychosocial effects of psoriasis. The choice of the optimal psoriasis treatment should also take into account the effect of the drug on the patient’s psychosocial well-being, and adjunctive psychological interventions before and during treatment may be of benefit for selected patients. It is recommended that psoriasis patients, especially those with severe disease, receive a more holistic, multitarget approach that encompasses both medical and psychological measures.
\nThe alkali and alkaline earth metal cations have inert gas electronic structures and are not expected to show any stereochemical requirements in their complex formation as do transition metal cations. They may be considered spherical even in the complex state. Their complexation is thus treated as recognition of spherical cations by organic ligands [1]. Depending upon the nature of the organic ligand and the anion, the metal ions can be separated as solvated ions, solvent separate, loose and tight ion pairs.
Alkali and alkaline earth metal ions form a large number of solid complexes with podands [2, 3, 4, 5, 6]. The podands are inherently flexible because the two ends of the molecule are not tied simultaneously. Polypodal ligands are acyclic multidentate ligands containing more than three arms. They form an unlimited family of structures which finally give rise to dendrimers. A predominant 1:1 complexation has also been observed in alkali and alkaline earth metal complexes of the tetra- and pentapodands. The stability constants of the terapodands are generally lower than those of the corresponding tripodands because of more severe steric hindrance to complexation [7]. Vögtle and coworkers have indicated that the ligands resembling tetrapodands are capable of forming 1:1 complexes with s-block metal ions [8, 9].
The s-block elements present a usual challenge in the molecular modeling, because the metal-ligand interactions in both cases are principally electrostatic. The types of alkali and alkaline earth metal complexes subjected to molecular modeling can be divided into five categories: crown ethers [10, 11, 12, 13, 14, 15, 16], cryptands [17, 18], spherands [19, 20], podands and other biologically important ligands, such as ionophores and cyclic antibiotics [21, 22, 23, 24] . The present work has been undertaken with the aim to computationally characterize the structure and nature of complexes of s-block metal ions with the tetrapodands THEEN and THPEN. Recently the computational studies of these tetrapodal ligands with Cu(II), Ag(I) and La(III) have been reported. Recently, synthesis, crystal structure and biological properties of [Co(edtp)Cl]·NO3·H2O complex was also determined, where edtp is N,N,N′,N′-Tetrakis(2-hydroxypropyl) ethylenediamine in which Co2+ ion is coordinated by the N,N′,O,O′,O″-pentadentate edtp ligand and a chloride to generate a distorted CoClN2O3 octahedron [25, 26, 27, 28].
From the last 3 decades density functional theory has been the dominant method for the quantum mechanical simulation of periodic systems. In recent years it has also been adopted by quantum chemists and is now very widely used for the simulation of energy surfaces in molecules. The quantum-chemical calculations (DFT calculations) giving molecular geometries of minimum energies, molecular orbitals (HOMO-LUMO), 13C-NMR and vibrational spectra were performed using the Gaussian 09 [29]. Molecular orbitals were visualized using “Gauss view”. The method used was Becke’s three-parameter hybrid-exchange functional, the nonlocal correlation provided by the Lee, Yang and Parr expression, and the Vosko, Wilk, and Nuair 1980 local correlation functional (III) (B3LYP) [30, 31]. The 6-31 g + (d,p) basis set was used for C, N and O. The LANL2DZ basis set [32] and pseudopotentials of Hay and Wadt were used for Ca, Sr, Ba and Na metal atoms [33, 34]. DFT calculations were performed in the gaseous phase and the input coordinates were obtained from and then compared with crystal structure data of already reported complexes: [Ca(THEEN)(PIC)](PIC),[Ca(THPEN)(H2O)2](PIC)2, Ba(THPEN)(PIC)2, [Na(THPEN)]2(PIC)2, [Sr(THPEN)(H2O)2]2(DNP)4 and [Ba(THPEN)(H2O)2]2(DNP)4 (where DNP is 3,5-dinitrophenolate) [35]. The structural parameters were adjusted until an optimal agreement between calculated and experimental structure obtained throughout the entire range of available structures. HOMO-LUMO analyses and spectroscopic calculations were performed on the optimized geometries of the title complexes (1–6) using B3LYP/6-31 g + (d,p)/LANL2DZ level of theory.
Complexes (1–6) were successfully modeled by using the input coordinates of crystal data. Tables 1 and 2 represent comparison of calculated and experimental M-Ligand bond lengths (Å) of complexes (1–3) and (4–6), respectively. The picrates and dinitrophenolates that are excluded from the primary coordination spheres of metal atoms in the crystallographic determinations, are not optimized in the computed structures. Tables 3 and 4 represent comparison of calculated and experimental torsion angles of ligand in complexes (1–3) and (4–6) respectively.
Complex 1 (M = Ca) | Complex 2 (M = Ca) | Complex 3 (M = Ba) | |||||||
---|---|---|---|---|---|---|---|---|---|
Theo. | Exp. | Dev. | Theo. | Exp. | Dev. | Theo. | Exp. | Dev. | |
M-O1 | 2.450 | 2.410 | 0.040 | 2.389 | 2.341 | 0.048 | 2.720 | 2.722 | −0.002 |
M-O2 | 2.450 | 2.380 | 0.070 | 2.495 | 2.498 | −0.003 | 2.807 | 2.812 | −0.006 |
M-O3 | 2.410 | 2.480 | 0.070 | 2.753 | 2.753 | 0.000 | |||
M-O4 | 2.410 | 2.370 | 0.040 | 2.812 | 2.816 | −0.004 | |||
M-O5 | 2.681 | 2.687 | −0.006 | ||||||
M-O6 | 3.127 | 3.135 | −0.008 | ||||||
M-O12 | 2.310 | 2.30 | 0.01 | 2.728 | 2.735 | −0.007 | |||
M-O13 | 2.470 | 2.73 | 0.26 | ||||||
M-O18 | 2.977 | 2.990 | −0.013 | ||||||
M-O1W | 2.440 | 2.442 | −0.002 | ||||||
M-O2W | |||||||||
M-N1 | 2.824 | 2.591 | 0.233 | 2.601 | 2.603 | −0.002 | 3.038 | 3.042 | 0.004 |
M-N2 | 2.738 | 2.658 | 0.08 | 3.026 | 3.032 | −0.006 |
Comparison of experimental and calculated M-ligand bond lengths (Å) of complexes (1–3).
Complex 4 (M = Na) | Complex 5 (M = Sr) | Complex 6 (M = Ba) | |||||||
---|---|---|---|---|---|---|---|---|---|
Theo. | Exp. | Dev. | Theo. | Exp. | Dev. | Theo. | Exp. | Dev. | |
M-O1 | 2.412 | 2.416 | −0.004 | 2.617 | 2.628 | −0.011 | 2.736 | 2.743 | −0.007 |
M-O2 | 2.393 | 2.396 | −0.003 | 2.611 | 2.618 | −0.007 | 2.763 | 2.767 | −0.004 |
M-O3 | 2.505 | 2.508 | −0.003 | 2.506 | 2.516 | −0.010 | 2.756 | 2.762 | −0.006 |
M-O4 | 2.628 | 2.632 | −0.004 | 2.618 | 2.626 | −0.008 | 2.658 | 2.668 | −0.010 |
M-O1W | 2.701 | 2.711 | −0.010 | 2.880 | 2.884 | −0.004 | |||
M-O2W | 2.699 | 2.705 | −0.006 | 2.988 | 2.995 | −0.007 | |||
M-O2WA | 2.726 | 2.732 | −0.006 | ||||||
M-N1 | 2.835 | 2.842 | −0.007 | 3.009 | 3.008 | −0.001 | |||
M-N2 | 2.849 | 2.857 | −0.008 | 3.010 | 3.010 | 0.000 |
Comparison of experimental and calculated M-ligand bond lengths (Å) of complexes (4–6).
Name of the | Complex (1) | Complex (2) | Complex (3) | ||||||
---|---|---|---|---|---|---|---|---|---|
Atoms | Theo. | Exp. | Dev. | Theo. | Exp. | Dev. | Theo. | Exp. | Dev. |
O1-C1-C2-N1 | −55.1 | −55.05 | 0.05 | 57.9 | 58.0 | 0.1 | −32.3 | −32.4 | −0.1 |
C1-C2-N1-C5 | 165.1 | 165.1 | 0.0 | 82.8 | 82.7 | 0.1 | 161.9 | 162.0 | 0.1 |
C2-N1-C5-C6 | −159.0 | −159.0 | 0.0 | −165.5 | −165.5 | 0.0 | −157.6 | −157.8 | −0.2 |
N1-C5-C6-N2 | 65.4 | 65.3 | 0.1 | 60.4 | 60.5 | 0.1 | 65.9 | 66.1 | 0.2 |
C5-C6-N2-C8 | −159.1 | −159.0 | 0.1 | −159.3 | −159.4 | 0.1 | |||
C6-N2-C8-C7 | 89.1 | 89.1 | 0.0 | 163.6 | 163.7 | 0.1 | |||
N2-C8-C7-O3 | 60.9 | 60.9 | 0.0 | −34.1 | −34.2 | −0.1 | |||
O2-C3-C4-N1 | 36.5 | 36.7 | 0.2 | 55.5 | 55.6 | 0.1 | 46.8 | 46.9 | −0.1 |
C3-C4-N1-C5 | −121.6 | −121.7 | −0.1 | −161.0 | −161.0 | 0.0 | −132.6 | −132.7 | −0.1 |
C4-N1-C5-C6 | 77.2 | 77.2 | 0.0 | 72.6 | 72.6 | 0.0 | 83.7 | 83.8 | 0.1 |
C5-C6-N2-C10 | 79.4 | 79.4 | 0.0 | 79.0 | 79.1 | 0.1 | |||
C6-N2-C10-C9 | −151.8 | −151.8 | 0.0 | −134.9 | −134.9 | 0.0 | |||
N2-C10-C9-O4 | 61.3 | 61.4 | 0.1 | 52.1 | 52.2 | 0.1 |
Comparison of calculated and experimental torsion angles (°) of ligand in the complexes (1–3).
Name of the | Complex (4) | Complex (5) | Complex (6) | ||||||
---|---|---|---|---|---|---|---|---|---|
Atoms | Theo. | Exp. | Dev. | Theo. | Exp. | Dev. | Theo. | Exp. | Dev. |
Complex | −55.6 | −55.7 | −0.1 | 32.3 | 32.3 | 0.0 | −43.4 | −43.5 | 0.1 |
O1-C1-C2-N1 | 152.7 | 152.6 | 0.1 | −143.9 | −143.9 | 0.0 | 162.3 | 162.4 | 0.1 |
C1-C2-N1-C5 | −80.2 | −80.2 | 0.0 | 86.1 | 86.1 | 0.0 | −92.7 | −92.8 | 0.1 |
C2-N1-C5-C6 | −64.0 | −63.9 | −0.1 | 43.6 | 43.6 | 0.0 | −50.1 | −50.1 | 0.0 |
N1-C5-C6-N2 | 165.5 | 165.4 | 0.1 | −146.4 | −146.4 | 0.0 | 156.5 | 156.7 | 0.2 |
C5-C6-N2-C8 | −85.7 | −85.7 | 0.0 | 156 | 155.9 | 0.1 | −89.6 | −89.9 | 0.3 |
C6-N2-C8-C7 | −60.3 | −60.4 | −0.1 | −44.7 | −44.7 | 0.0 | −30.4 | −30.4 | 0.0 |
N2-C8-C7-O3 | −59.7 | −59.8 | −0.1 | −17.4 | −17.4 | 0.0 | 47.8 | 48.1 | 0.3 |
O2-C3-C4-N1 | −91.0 | −91.1 | −0.1 | 112.7 | 112.7 | 0.0 | −135.1 | −135.2 | 0.1 |
C3-C4-N1-C5 | 156.0 | 156.0 | 0.0 | −159.1 | −159.2 | 0.1 | 151.9 | 151.9 | 0.0 |
C4-N1-C5-C6 | −72.4 | −72.5 | −0.1 | 97.4 | 97.4 | 0.0 | −92.1 | −92.4 | 0.3 |
C5-C6-N2-C10 | 156.6 | 156.6 | 0.0 | −151.8 | −151.8 | 0.0 | 143.4 | 143.9 | 0.5 |
C6-N2-C10-C9 | −59.2 | −59.3 | −0.1 | 41.6 | 41.7 | 0.1 | 5.1 | 4.9 | 0.3 |
N2-C10-C9-O4 | −55.6 | −55.7 | −0.1 | 32.3 | 32.3 | 0.0 | −43.4 | −43.5 | 0.1 |
Comparison of experimental and calculated and torsion angles (°) of ligand in the complexes (4–6).
The coordination number of Ca(II) ion is eight with distorted cube geometry in the optimized geometry of cationic complex (1) (Figure 1). THEEN is interacting with Ca(II) ion through all the six potential donor atoms. The seventh and eighth coordination sites of Ca(II) are occupied by picrate anion through phenolic oxygen and one of the o-nitro oxygen. The observed and calculated positions of calcium and donor atoms are in agreement. A comparison of bond lengths and bond angles provided a maximum tolerance of 0.27 Å and 16.33°Å, respectively (Table 1 and Table S1; Figure S1a,b) of computed title complex (1) and crystallographically determined complex [Ca(THEEN)(PIC)](PIC). The torsion angles of the ligand THEEN in theoretically determined and experimental complex are also in well consistency with each other (Table 3). The HOMO-LUMO analysis has indicated that there is maximum distribution of HOMO over the carbon atoms and to a lesser extent on the oxygen of the coordinated picrate. LUMO is mainly distributed or concentrated on all the atoms of coordinated picrate except p-nitro group. Neither HOMO nor LUMO distribution is found either on calcium ion or on any ligand atom. The HOMO-LUMO gap (ΔE) is found to be 0.852 eV (Figure S1c).
(a) Optimized geometric structure of [Ca(THEEN)(PIC)]+ (1) (b) distorted cube geometry.
Ca(II) is eight coordinated in monomeric cationic complex with a distorted square-antiprismatic geometry in complex (2) as is observed in crystal structure of [Ca(THPEN)(H2O)2] (PIC)2. H2O (Figure 2). THPEN is acting as hexadentate ligand towards the metal ion. Two remaining sites around the metal ion are occupied by two water molecules. The observed and calculated positions of calcium and donor atoms are in agreement. All strain energy minimized structures reproduced the observed X-ray structures with almost no deviation in M-L bond length and torsion angle of the ligand (Table 3). The maximum tolerance of L-M-L bond angle is 15.8° (Tables 1 and Table S1, Figure S2a,b). Complex 2 is displaying the main distribution of HOMO as well as LUMO only on water molecules. There is slight distribution of HOMO and LUMO on hydroxyl oxygen of THPEN ligand also with HOMO-LUMO gap (HLG) of 0.419 eV (Figure S2c).
(a) Optimized geometric structure of [Ca(THPEN)(H2O)2]2+ (2) (b) distorted square-antiprismatic geometry.
Ba(II) is ten-coordinate in its monomeric complex (3) (Figure 3). The ligand THPEN coordinates through both its nitrogen atoms and all the four hydroxyl oxygen. The two picrate ions are also directly coordinated to Ba2+ ion through the phenolic oxygen and one oxygen of the o-nitro group. Since both the picrates are directly interacting with the cation, the complex is termed as tight ion-paired complex as is found in the crystallographically determined complex. The observed and calculated positions of barium and donor atoms are in agreement. There is negligible deviation found in bond length, bond angle (0.11°) and torsion angle of ligand THPEN for calculated title complex (3) and experimental Ba(THPEN)(PIC)2 (Tables 1 and 3 and S1, Figure S3a,b). An analysis of HOMO-LUMO has illustrated that HOMO is mainly distributed on the ligand THPEN with a small distribution on coordinated picrates. In contrast to this LUMO is mainly distributed on coordinated picrates with no distribution over the ligand or metal atom. The complex is showing HLG of 0.118 eV (Figure S3c).
(a) Optimized geometric structure of Ba(THPEN)(PIC)2 (3) (b) bicapped square-antiprismatic geometry.
Figure 4a shows the optimized structure of the cationic complex of sodium (4). This structure is centrosymmetric dimer. The coordination number around each Na+ ion is seven. Each THPEN ligand coordinates to Na(I) ion in a heptadenate fashion (Figure 4). In other words, one hydroxyl group of the THPEN ligand acts as a bridge between two Na+ ions. The geometry of the complex is distorted monocapped octahedron. The Na…Na non bridging distance is 3.429 Å. Almost no deviation has been observed in bond length (M-L), torsion angle of ligand THPEN and bond angles (L-M-L) of computed title complex (4) and crystallographically determined complex [Na(THPEN)]2(PIC)2 (Tables 2 and 4 and Table S1, Figures S4a,b). The HOMO-LUMO study has revealed that in the title complex (4) HOMO is mainly concentrated on bridged hydroxyl oxygens and sodium metal but to a smaller extent on the other coordinated hydroxyl oxygens and amine nitrogens. LUMO is mainly concentrated on bridged hydroxyl oxygens and to a smaller extent on other coordinated oxygen atoms. The HOMO-LUMO gap is 0.261 eV (Figure S4c).
(a) Optimized geometric structure of [Na(THPEN)]22+(4) (b) distorted monocapped octahedron geometry.
Sr(II) is nine-coordinated in its dimeric complex (5) (Figure 5). This cationic complex is having tricapped trigonal-prismatic geometry as is found in crystallographically determined complex [Sr(THPEN)(H2O)2]2(DNP)4. Each Sr2+ ion in the complex is coordinated by six potential donor sites of the ligand THPEN and four water molecules. Out of four water molecules, two are bridging and the third one is non-bridging. Sr…Sr non bridging distance is 4.346 Å indicating the existence of van der Waals contact. All strain energy minimized structures reproduced the observed X-ray structures to a maximum tolerance of 9.07° bond angle (Table 2 and Table S1, Figure S5a,b). Almost no deviation of M-L bond length and torsion angle of ligand THPEN has been observed for the title complex (5) and crystallographically determined complex (Tables 2 and 4). The HOMO-LUMO analysis has shown that the complex (5) is having maximum distribution of HOMO and LUMO on bridged coordinated water molecules and there is HLG of 0.0225 eV (Figure S5c).
(a) Optimized geometric structure of [Sr(THPEN)(H2O)2]2(DNP)4 (b) Trigonal- prismatic geometry.
Ba(II) is ten-coordinate in the cationic title complex (6) as is found in the crystallographic determined complex [Ba(THPEN)(H2O)2](DNP)4. The geometry around Ba(II) is bicapped cubic. Each Ba(II) in dimer is interacting with THPEN through all its six potential donor sites and four water molecules. The latter are bridging in nature. The existence of van der Waals contact between non-bridging Ba…Ba is indicated by their larger distance (4.196 Å). The observed and calculated positions of the metal and donor atoms are in agreement as almost negligible deviation of M-L bond length and torsion angle of THPEN. A deviation of 0.14° of bond angle L-M-L has been observed for complex (6) [Ba(THPEN)(H2O)2](DNP)4 (Tables 2 and 4 and Table S1; Figures S6a,b and S7). The region of distribution of HOMO and LUMO is only over two of the bridged water molecules in complex (6) with a very small HOMO-LUMO gap (ΔE = 0.0375 eV) indicating the soft nature of complex (Figure 6).
(a) Optimized geometric structure of [Ba(THPEN)(H2O)2]22+ (6) (b) Bicapped cubic geometry.
Smaller is the HUMO-LUMO gap (HLG) softer is the complex [36, 37]. The frontier orbitals HOMO and LUMO are very important parameters for chemical reaction and take part in chemical stability [38, 39, 40]. It is predicted from the HOMO-LUMO gaps that the title complexes are soft as is obvious from their smaller HUMO-LUMO energy gaps (HLG) relative to the similar reported complexes of copper, silver and lanthanoid [25, 26, 27] (Table 5). It has been observed in the present computational study that the dinitrophenolate complexes are softer than trinitrophenolate and among the latter, [Ca(THEEN)(PIC)]+ (1) is displaying least softness. It is pertinent to mention here that the complex (1) is having THEEN ligand whereas THPEN is ligand in rest of the complexes (2–6).
HLG (eV) | Reported complexes | HLG (eV) | Reported complexes | HLG (eV) | |
---|---|---|---|---|---|
[Ca(THEEN)(PIC)]+ (1) | 0.852 | [Cu(THEEN)(H2O)](PIC)2 | 3.537 | [La(THEEN)(PIC) (H2O)2] (PIC)2.2H2O | 3.428 |
[Ca(THPEN)(H2O)2]2+ (2) | 0.419 | [Cu(THPEN)](PIC)2.C3H8O | 3.467 | [La(TEAH3)(H2O)2] (PIC)3 | 3.673 |
Ba(THPEN)(PIC)2 (3) | 0.118 | [Cu(TEAH3)(PIC)](PIC).H2O | 3.619 | ||
[Na(THPEN)]22+ (4) | 0.261 | [Ag (THEEN)]2 (PIC)2 | 2.530 | ||
[Sr(THPEN)(H2O)2]22+ (5) | 0.0225 | [Ag (THPEN)]2 (PIC)2 | 2.640 | ||
[Ba(THPEN)(H2O)2]22+ (6) | 0.0375 | [Ag(TEAH3)2] (PIC) | 1.061 |
Nuclear magnetic resonance spectra (NMR) and infrared (IR) spectroscopy can be useful for studying the coordination of various ligating sites. The 13C-NMR spectra were predicted for complexes (1–6) using DFT/B3LYP/6-31G** method and the spectral data was compared with experimental data reported in literature [35]. The computed NMR spectral data is fairly in agreement with experimental data (Tables 6 and 7). Small deviations are due to the fact that H-bonding interactions or any type of lattice interactions are not modeled in theoretically computed structures. The terminal methyl groups in theoretically predicted complexes (2–5) are displaying quiet high upfield shifts relative to the experimentally obtained due to more free movements in the gaseous phase than in solution or solid phase.
Assignments (δ) | [Ca(THEEN)(PIC)]+ (1) | Ba(THPEN)(PIC)2 (3) | ||
---|---|---|---|---|
Theo. | Exp. | Theo. | Exp. | |
▬CH3 | * | * | 4.22 | 19.61 |
▬CH3 | 4.49 | 19.89 | ||
▬NCH2 | 52.31 | 55.03 | 51.73 | 55.34 |
▬NCH2 | 43.35 | 55.20 | ||
▬OCH2, ▬OCH | 59.03 | 57.47 | 50.75 | 63.00 |
▬ArCH | 113.63 | 124.33 | 117.85 | 124.36 |
p-ArCN | 134.75 | 123.60 | 122.06 | 123.68 |
o-ArCN | 140.68 | 140.78 | 140.98 | 140.78 |
▬ArCO | 161.57 | 160.20 | 150.21 | 160.20 |
Comparison of calculated and experimental 13C-NMR spectral data for complexes (1 and 3).
* Group absent.
Assignment (δ) | [Ca(THPEN)(H2O)2]2+ (2) | [Na(THPEN)]22+ (4) | [Sr(THPEN)(H2O)2]22+ (5) | [Ba(THPEN)(H2O)2]22+ (6) | ||||
---|---|---|---|---|---|---|---|---|
Theo. | Exp. | Theo. | Exp. | Theo. | Exp. | Theo. | Exp. | |
▬CH3 | 11.35 | 18.79 | 4.01 | 20.30 | 3.77 | 18.31 | 27.02 | 18.35 |
▬CH3 | 11.38 | 19.02 | 5.63 | 20.36 | 3.85 | 18.59 | 27.69 | 18.63 |
▬NCH2 | 39.60 | 50.99 | 43.05 | 50.42 | 43.60 | 48.31 | 61.69 | 59.80 |
▬NCH2 | 39.61 | 51.76 | 44.05 | 52.90 | 57.81 | 59.68 | 61.69 | 60.59 |
▬OCH | * | * | 50.73 | 55.73 | 41.85 | 60.62 | 60.37 | 60.66 |
▬OCH | 69.24 | 61.74 | 57.90 | 55.95 | 51.91 | 61.08 | 60.38 | 62.53 |
Comparison of calculated and experimental 13C-NMR spectral data for complexes (2, 4–6).
* Group absent.
The computed IR spectral peaks that appear in the range of 1370–600 cm−1 are fairly in agreement with the experimental data (Tables 8 and 9). The absorption peaks due to the presence of hydroxyl groups were observed only for complexes (1) and (6) in the computed IR spectra. It is pertinent to mention here that both of these complexes possess the picrate anion in their coordination sphere. The less extent of H-bonding is reported in the crystallographic description of these complexes [35]. The theoretical absorption band appears at 3223 and 3235 cm−1 for both complexes (1) and (6) whereas the experimental band is reported at 3300 cm−1 for both of them [35].
Assignments (cm−1) | [Ca(THEEN)(PIC)]+ (1) | [Ca(THPEN)(H2O)2]2+ (2) | Ba(THPEN)(PIC)2 (3) | |||
---|---|---|---|---|---|---|
Theo. | Exp. | Theo. | Exp. | Theo. | Exp. | |
ν (NO2) | 1363.56 | 1360 m | 1320.81 | 1360 vs | 1384.20 | 1370 |
δ (〓CH) | 696.80 | 700 m | 784.16 | 790 m | 800 | 800 |
Comparison of calculated and experimental IR spectral data for complexes (1–3).
Assignments (cm−1) | [Na(THPEN)]22+ (4) | [Sr(THPEN)(H2O)2]22+ (5) | [Ba(THPEN)(H2O)2]22+ (6) | |||
---|---|---|---|---|---|---|
Theo. | Exp. | Theo. | Exp. | Theo. | Exp. | |
ν (NO2) | 1366 | 1371.21 | 1330 | 1329.24 | 1340 | 1329.43 |
δ (〓CH) | 790 | 784.54 | 760 | 762.52 | 790 | 787.17 |
Comparison of calculated and experimental IR spectral data for complexes (4–6).
The coordination number of the title s-block complexes is varying from 7 to 10 in the present work. As the size of the metal increases, coordination number of central metal ion also increases. Out of the six complexes presented, three are monomeric (1–3) and three are dimeric (4–6). The longer distances between two M…M distances in the dinuclear complexes indicate the existence of van der Waals contacts between the two s-block metal ions. All the title complexes are cationic except Ba(THPEN)(PIC)2 (3). The latter is tight ion-paired complex. All strain energy minimized structures obtained using quantum-chemical approach reproduced the observed X-ray structures with geometric parameters in well agreement. HOMO-LUMO studies suggest the softness of the title s-block complexes relative to the similar already reported copper, silver and lanthanoid complexes. The theoretical spectral data (13C-NMR and IR) computed using DFT and experimental data is fairly in agreement with each other. The accuracy of the results predicts that the DFT studies performed using B3LYP/6-31 g + (d,p)/LANL2DZ level of theory is the appropriate quantum-chemical method for reproducing the experimental results for the title s-block complexes. This quantum-chemical approach has potential for molecular modeling of other s-block complexes and exploring their chemistry.
Small deviations in geometric as well as spectral parameters may be attributed to the lack of H-bonding and packing interactions within lattice which were not modeled during the computational study of the entitled s-block complexes. Moreover, the quantum-chemical approach of DFT studies has been carried out in the gaseous phase whereas the already reported experimental crystal and IR spectral data is in the solid phase while 13C-NMR spectral data is in the solution phase.
Plot showing the deviations of theoretical and experimental (a) bond lengths (Å) and (b) bond angles (°) for the complex (1) and (c) (HOMO-LUMO) of the complex (1) with energy gap.
Plot showing the deviations of theoretical and experimental (a) bond lengths (Å) and (b) bond angles (°) for the complex (2) (c) (HOMO-LUMO) of the complex (2) with energy gap.
Plot showing the deviations of theoretical and experimental (a) bond lengths (Å) and (b) bond angles (°) for the complex (3) (c) (HOMO-LUMO) of the complex (3) with energy gap.
Plot showing the deviations of theoretical and experimental (a) bond lengths (Å) and (b) bond angles (°) for the complex (4) (c) (HOMO-LUMO) of the complex (4) with energy gap.
Plot showing the deviations of theoretical and experimental (a) bond lengths (Å) and (b) bond angles (°) for the complex (5) (c) (HOMO-LUMO) of the complex (5) with energy gap.
Plot showing the deviations of theoretical and experimental (a) bond lengths (Å) and (b) bond angles (°) for the complex (6) (c) (HOMO-LUMO) of the complex (6) with energy gap.
R = H, THEEN; R = CH3, THPEN.
Bond distances (Å) | Theoretical | Experimental | Dev. | Bond angles (°) | Theoretical | Experimental | Dev. |
---|---|---|---|---|---|---|---|
Complex (1) | |||||||
Ca-N1 | 2.600 | 2.600 | 0.000 | N1-Ca-N1A | 71.54 | 71.60 | 0.06 |
Ca-O1 | 2.387 | 2.388 | 0.001 | N1-Ca-O2A | 81.41 | 65.52 | 15.89 |
Ca-O2 | 2.495 | 2.496 | 0.001 | N1-Ca-O1W | 119.08 | 119.09 | 0.01 |
Ca-O1W | 2.439 | 2.439 | 0.000 | N1-Ca-O1WA | 143.89 | 143.89 | 0.00 |
O1-Ca-O2 | 102.93 | 102.95 | 0.02 | ||||
O1-Ca-N1 | 67.80 | 67.79 | 0.01 | ||||
O1-Ca-O1W | 79.82 | 79.85 | 0.03 | ||||
O1-Ca-N1A | 132.22 | 132.22 | 0.00 | ||||
O1-Ca-O2A | 84.37 | 84.36 | 0.01 | ||||
O1-Ca-O1A | 159.11 | 159.10 | 0.01 | ||||
O1-Ca-O1WA | 83.52 | 83.54 | 0.02 | ||||
O2-Ca-N1 | 65.50 | 65.52 | 0.02 | ||||
O2-Ca-O1W | 74.11 | 74.10 | 0.01 | ||||
O2-Ca-N1A | 81.42 | 81.40 | 0.02 | ||||
O2-Ca-O2A | 139.33 | 139.89 | 0.56 | ||||
O2A-Ca-O1W | 145.88 | 145.90 | 0.02 | ||||
Complex (2) | |||||||
Ca-O1 | 2.45 | 2.41 | 0.04 | O1-Ca-O2 | 94.43 | 102.08 | 7.65 |
Ca-O2 | 2.45 | 2.38 | 0.07 | O1-Ca-O3 | 172.00 | 175.21 | 3.21 |
Ca-O3 | 2.41 | 2.48 | 0.07 | O1-Ca-O4 | 85.56 | 74.35 | 11.21 |
Ca-O4 | 2.41 | 2.37 | 0.04 | O1-Ca-O12 | 107.80 | 104.18 | 3.62 |
Ca-O12 | 2.31 | 2.30 | 0.01 | O1-Ca-O13 | 61.91 | 64.85 | 2.94 |
Ca-O13 | 2.47 | 2.73 | 0.26 | O1-Ca-N1 | 65.93 | 68.50 | 2.57 |
Ca-N1 | 2.74 | 2.59 | 0.15 | O1-Ca-N2 | 104.33 | 115.49 | 11.16 |
Ca-N2 | 2.82 | 2.65 | 0.17 | O2-Ca-O3 | 90.99 | 79.27 | 11.72 |
O2-Ca-O4 | 180.00 | 168.65 | 11.35 | ||||
O2-Ca-O12 | 108.06 | 107.20 | 0.86 | ||||
O2-Ca-O13 | 61.38 | 69.92 | 8.54 | ||||
O2-Ca-N1 | 64.20 | 68.43 | 4.23 | ||||
O2-Ca-N2 | 114.39 | 105.72 | 8.67 | ||||
O3-Ca-O4 | 89.01 | 105.24 | 16.23 | ||||
O3-Ca-O12 | 75.95 | 71.06 | 4.89 | ||||
O3-Ca-O13 | 126.03 | 110.69 | 15.34 | ||||
O3-Ca-N1 | 111.54 | 116.18 | 4.64 | ||||
O3-Ca-N2 | 67.97 | 68.26 | 0.29 | ||||
O4-Ca-O12 | 71.93 | 84.20 | 12.27 | ||||
O4-Ca-O13 | 118.62 | 116.91 | 1.71 | ||||
O4-Ca-N1 | 115.80 | 100.38 | 15.42 | ||||
O4-Ca-N2 | 65.61 | 67.36 | 1.75 | ||||
O12-Ca-O13 | 71.32 | 62.19 | 9.13 | ||||
O12-Ca-N1 | 168.56 | 169.55 | 0.99 | ||||
O12-Ca-N2 | 123.47 | 120.54 | 2.93 | ||||
O13-Ca-N1 | 97.26 | 107.46 | 10.2 | ||||
O13-Ca-N2 | 163.73 | 175.60 | 11.87 | ||||
N1-Ca-N2 | 67.95 | 69.92 | 1.97 | ||||
Complex (3) | |||||||
Ba-O1 | 2.720 | 2.720 | 0.000 | O1-Ba-O2 | 86.95 | 87.00 | 0.05 |
Ba-O2 | 2.807 | 2.801 | 0.006 | O1-Ba-O3 | 172.87 | 173.00 | 0.13 |
Ba-O3 | 2.753 | 2.750 | 0.003 | O1-Ba-O4 | 88.55 | 88.50 | 0.05 |
Ba-O4 | 2.812 | 2.812 | 0.000 | O1-Ba-O6 | 72.90 | 72.90 | 0.00 |
Ba-O5 | 2.681 | 2.683 | 0.002 | O1-Ba-O12 | 61.79 | 61.80 | 0.01 |
Ba-O6 | 3.127 | 3.128 | 0.001 | O1-Ba-O18 | 109.63 | 109.70 | 0.07 |
Ba-O12 | 2.728 | 2.729 | 0.001 | O1-Ba-N1 | 58.12 | 58.10 | 0.02 |
Ba-O18 | 2.977 | 2.979 | 0.002 | O1-Ba-N2 | 114.85 | 114.80 | 0.05 |
Ba-N1 | 3.038 | 3.038 | 0.000 | O2-Ba-O4 | 129.37 | 129.40 | 0.03 |
Ba-N2 | 3.026 | 3.028 | 0.002 | O2-Ba-O6 | 64.79 | 64.80 | 0.01 |
O2-Ba-O18 | 161.62 | 160.60 | 0.02 | ||||
O2-Ba-N2 | 79.36 | 79.40 | 0.03 | ||||
O2-Ba-N1 | 57.03 | 57.12 | 0.05 | ||||
O3-Ba-O2 | 92.08 | 92.10 | 0.02 | ||||
O3-Ba-O4 | 86.61 | 86.70 | 0.09 | ||||
O3-Ba-O6 | 113.02 | 113.10 | 0.08 | ||||
O3-Ba-O18 | 72.70 | 72.80 | 0.10 | ||||
O3-Ba-N1 | 115.63 | 115.60 | 0.03 | ||||
O3-Ba-N2 | 58.06 | 58.20 | 0.14 | ||||
O4-Ba-O6 | 156.82 | 156.80 | 0.02 | ||||
O4-Ba-O18 | 63.13 | 63.20 | 0.07 | ||||
O4-Ba-N1 | 78.20 | 78.20 | 0.00 | ||||
O4-Ba-N2 | 57.43 | 57.40 | 0.03 | ||||
O5-Ba-O1 | 123.12 | 123.20 | 0.08 | ||||
O5-Ba-O2 | 85.94 | 85.90 | 0.04 | ||||
O5-Ba-O3 | 63.80 | 63.90 | 0.10 | ||||
O5-Ba-O4 | 135.92 | 135.90 | 0.02 | ||||
O5-Ba-O6 | 53.26 | 53.30 | 0.03 | ||||
O5-Ba-O12 | 84.0 | 84.00 | 0.00 | ||||
O5-Ba-O18 | 76.67 | 76.90 | 0.13 | ||||
O5-Ba-N1 | 142.90 | 142.90 | 0.00 | ||||
O5-Ba-N2 | 118.97 | 118.90 | 0.07 | ||||
O12-Ba-O2 | 133.15 | 133.20 | 0.05 | ||||
O12-Ba-O3 | 123.02 | 123.00 | 0.02 | ||||
O12-Ba-O4 | 86.45 | 86.40 | 0.05 | ||||
O12-Ba-O6 | 72.69 | 72.70 | 0.01 | ||||
O12-Ba-O18 | 54.05 | 54.00 | 0.05 | ||||
O12-Ba-N1 | 117.95 | 117.96 | 0.01 | ||||
O12-Ba-N2 | 143.78 | 143.80 | 0.02 | ||||
O18-Ba-O6 | 109.54 | 109.60 | 0.06 | ||||
O18-Ba-N1 | 140.27 | 140.40 | 0.13 | ||||
O18-Ba-N2 | 101.49 | 101.50 | 0.01 | ||||
N2-Ba-N1 | 61.27 | 61.30 | 0.03 | ||||
N2-Ba-O6 | 143.21 | 143.20 | 0.01 | ||||
N1-Ba-O6 | 102.39 | 102.40 | 0.01 | ||||
Complex (4) | |||||||
Na-N1 | 2.552 | 2.554 | 0.002 | O1-Na-O2 | 99.56 | 99.50 | 0.06 |
Na-N2 | 2.565 | 2.566 | 0.001 | O1-Na-O3 | 86.59 | 86.60 | 0.01 |
Na-O1 | 2.412 | 2.412 | 0.000 | O1-Na-O4 | 174.34 | 174.30 | 0.04 |
Na-O2 | 2.393 | 2.393 | 0.000 | O1-Na-O4A | 90.18 | 9023 | 0.05 |
Na-O3 | 2.505 | 2.505 | 0.000 | O1-Na-N1 | 69.82 | 69.82 | 0.00 |
Na-O4 | 2.628 | 2.629 | 0.001 | O1-Na-N2 | 109.13 | 109.10 | 0.03 |
Na-O4A | 2.442 | 2.443 | 0.001 | O2-Na-O3 | 164.10 | 164.13 | 0.03 |
Na-NaA | 3.429 | 3.430 | 0.001 | O2-Na-O4 | 78.26 | 78.31 | 0.05 |
O2-Na-O4A | 88.56 | 88.57 | 0.01 | ||||
O2-Na-N1 | 70.69 | 70.70 | 0.01 | ||||
O2-Na-N2 | 121.68 | 121.71 | 0.03 | ||||
O3-Na-O4 | 96.86 | 96.87 | 0.01 | ||||
O3-Na-N1 | 125.19 | 125.17 | 0.02 | ||||
O3-Na-N2 | 68.93 | 68.91 | 0.02 | ||||
O3-Na-O4A | 76.69 | 76.72 | 0.03 | ||||
O4-Na-O4A | 94.96 | 95.00 | 0.03 | ||||
O4-Na-N1 | 68.25 | 68.25 | 0.00 | ||||
O4-Na-N2 | 68.25 | 68.25 | 0.00 | ||||
N1-Na-N2 | 73.38 | 73.37 | 0.01 | ||||
N1-Na-O4A | 147.48 | 147.51 | 0.03 | ||||
N2-Na-O4A | 138.85 | 138.87 | 0.02 | ||||
Complex(5) | |||||||
Sr-O1 | 2.617 | 2.618 | 0.001 | O3-Sr-O2 | 151.28 | 158.70 | 7.42 |
Sr-O2 | 2.611 | 2.610 | 0.001 | O3-Sr-O1 | 73.24 | 77.20 | 3.96 |
Sr-O3 | 2.506 | 2.505 | 0.001 | O2-Sr-O1 | 113.98 | 114.30 | 0.32 |
Sr-O4 | 2.618 | 2.618 | 0.000 | O3-Sr-O4 | 87.91 | 88.20 | 0.29 |
Sr-O1W | 2.701 | 2.702 | 0.001 | O2-Sr-O4 | 77.89 | 73.50 | 4.39 |
Sr-O2W | 2.699 | 2.699 | 0.000 | O1-Sr-O4 | 158.36 | 151.60 | 6.76 |
Sr-O2WA | 2.726 | 2.699 | 0.000 | O3-Sr-N1 | 102.34 | 113.60 | 11.26 |
Sr-N1 | 2.835 | 2.835 | 0.000 | O4-Sr-N1 | 113.34 | 102.50 | 10.84 |
Sr-N2 | 2.849 | 2.849 | 0.000 | O3-Sr-N2 | 61.38 | 64.40 | 3.02 |
O2-Sr-N2 | 89.92 | 97.10 | 7.18 | ||||
O1-Sr-N2 | 96.80 | 90.2 | 6.60 | ||||
O4-Sr-N2 | 64.13 | 61.60 | 2.53 | ||||
O3-Sr-O2W | 106.07 | 106.40 | 0.33 | ||||
O2-Sr-O2W | 70.58 | 77.10 | 6.52 | ||||
O1-Sr-O2W | 129.35 | 140.50 | 11.15 | ||||
O4-Sr-O2W | 70.80 | 67.90 | 2.90 | ||||
O2-Sr-O1W | 79.52 | 65.40 | 14.12 | ||||
O1-Sr-O1W | 65.11 | 79.80 | 14.69 | ||||
O4-Sr-O1W | 136.42 | 127.40 | 9.02 | ||||
O3’-Sr-O1W | 126.14 | 127.90 | 1.76 | ||||
O2W-Sr-O1W | 70.75 | 71.00 | 0.25 | ||||
O2W-Sr-N2 | 128.11 | 128.40 | 0.29 | ||||
O1W-Sr-N2 | 152.06 | 152.40 | 0.34 | ||||
N1-Sr-N2 | 64.77 | 65.00 | 0.23 | ||||
O2W-Sr-N1 | 139.03 | 139.30 | 0.27 | ||||
O1W-Sr-N1 | 87.52 | 87.80 | 0.28 | ||||
Complex (6) | |||||||
Ba-O1 | 2.736 | 2.738 | 0.002 | O4-Ba-O1 | 162.70 | 162.90 | 0.20 |
Ba-O2 | 2.763 | 2.761 | 0.002 | O4-Ba-O3 | 92.45 | 92.70 | 0.25 |
Ba-O3 | 2.756 | 2.757 | 0.001 | O1-Ba-O3 | 79.69 | 80.00 | 0.31 |
Ba-O4 | 2.658 | 2.657 | 0.001 | O4-Ba-O2 | 84.25 | 84.60 | 0.35 |
Ba-O1W | 2.880 | 2.880 | 0.000 | O1-Ba-O2 | 94.22 | 94.50 | 0.28 |
Ba-O2W | 2.988 | 2.990 | -0.002 | O3-Ba-O2 | 148.19 | 148.40 | 0.21 |
Ba-N1 | 3.009 | 3.002 | 0.007 | O4-Ba-N1 | 107.19 | 107.50 | 0.31 |
Ba-N2 | 3.010 | 3.004 | 0.006 | O1-Ba-N1 | 58.19 | 58.40 | 0.21 |
O3-Ba-N1 | 91.90 | 92.00 | 0.01 | ||||
O2-Ba-N1 | 59.43 | 59.60 | 0.17 | ||||
O4-Ba-N2 | 59.95 | 61.10 | 1.15 | ||||
O1-Ba-N2 | 103.03 | 103.20 | 0.17 | ||||
O3-Ba-N2 | 58.68 | 58.80 | 0.12 | ||||
O2-Ba-N2 | 93.2 | 93.40 | 0.20 | ||||
N1-Ba-N2 | 61.84 | 62.00 | 0.16 | ||||
O4-Ba-O1W | 126.17 | 126.50 | 0.33 | ||||
O1-Ba-O1W | 66.29 | 66.50 | 0.23 | ||||
O3-Ba-O1W | 72.53 | 72.80 | 0.27 | ||||
O2-Ba-O1W | 133.50 | 133.80 | 0.30 | ||||
O1-Ba-O2W | 73.43 | 73.70 | 0.27 | ||||
O3-Ba-O2W | 131.18 | 131.50 | 0.32 | ||||
O2-Ba-O2W | 74.74 | 75.00 | 0.26 | ||||
O2W-Ba-O1WA | 59.36 | 59.50 | 0.14 | ||||
N1-Ba-O1WA | 137.03 | 137.20 | 0.17 | ||||
N1-Ba-O1W | 124.19 | 124.19 | 0.00 | ||||
N1-Ba-O2W | 106.68 | 106.90 | 0.22 | ||||
N2-Ba-O1WA | 123.73 | 124.00 | 0.27 | ||||
N2-Ba-O1W | 131.21 | 131.50 | 0.29 | ||||
N2-Ba-O2W | 166.91 | 167.00 | 0.10 | ||||
N2-Ba-O2WA | 100.84 | 100.87 | 0.03 |
Comparison of selected experimental and calculated geometric parameters bond lengths (Å) and bond angles (°) for complexes (1–6).
Authors are listed below with their open access chapters linked via author name:
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\\n\\nMohamed Oukka 2016-18
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\\n\\nUlrike Ravens-Sieberer 2016-18
\\n\\nYexiang Tong 2017, 2018
\\n\\nJim Van Os 2015-18
\\n\\nLong Wang 2017, 2018
\\n\\nFei Wei 2016-18
\\n\\nIoannis Xenarios 2017, 2018
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\\n\\nXin-She Yang 2017, 2018
\\n\\nYulong Yin 2015, 2017, 2018
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\n\n\n\n\n\n\n\n\n\nJocelyn Chanussot (chapter to be published soon...)
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