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Iridium‐Coordinated Histidyl Bolaamphiphile Self‐Assemblies as Heterogeneous Catalysts for Water Oxidation
ChemSusChem ( IF 7.5 ) Pub Date : 2018-07-12 , DOI: 10.1002/cssc.201800461 Changjoon Keum 1 , Sang‐Yup Lee 1
ChemSusChem ( IF 7.5 ) Pub Date : 2018-07-12 , DOI: 10.1002/cssc.201800461 Changjoon Keum 1 , Sang‐Yup Lee 1
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Catalysts that can promote oxygen evolution from water are necessary for green energy production. In this study, colloidal heterogeneous catalysts for oxygen evolution were prepared by coordination of Ir species to self‐assemblies of histidyl bolaamphiphiles. When dissolved in water, the histidyl bolaamphiphiles self‐assembled to form particulate structures with the exposure of densely packed histidine imidazoles on their surface. Subsequent coordination of the Ir species to the bolaamphiphile assembly gave rise to catalytic activity toward the oxygen evolution reaction. The oxygen evolution was examined by using the catalytic assemblies in the presence of a sacrificial oxidant, cerium ammonium nitrate. The Ir‐coordinated assemblies showed a turnover frequency of 13 min−1, which was comparable to those previously reported for molecular water oxidation catalysts. The catalytic activity increased with increasing histidine imidazole/Ir molar ratio, which suggested that multiple coordination of Ir to imidazoles facilitated the formation of active Ir intermediates. This study demonstrates the feasibility of constructing catalytically active interfaces from colloidal bolaamphiphile assemblies with biochemical ligands.
中文翻译：
铱配位的组氨酰两亲基自组装体作为水氧化多相催化剂
可以促进从水中放出氧气的催化剂对于绿色能源的生产是必不可少的。在这项研究中，通过使Ir物种与组胺基Blaamphiphiles的自组装协调，制备了用于氧释放的胶体非均相催化剂。当溶解在水中时，组胺基两亲基团会自组装形成颗粒结构，并在其表面上暴露出密集堆积的组氨酸咪唑。Ir物种随后与亲两性菌组装体的配位引起了对氧释放反应的催化活性。在牺牲氧化剂硝酸铈铵的存在下，通过使用催化组件检查了氧气的释放。Ir协调的程序集的周转频率为13分钟-1，可与之前报道的分子水氧化催化剂相媲美。催化活性随组氨酸咪唑/ Ir摩尔比的增加而增加，这表明Ir与咪唑的多重配位促进了活性Ir中间体的形成。这项研究证明了从具有生化配体的胶体双亲亲组装体构建催化活性界面的可行性。
更新日期：2018-07-12
中文翻译：
铱配位的组氨酰两亲基自组装体作为水氧化多相催化剂
可以促进从水中放出氧气的催化剂对于绿色能源的生产是必不可少的。在这项研究中，通过使Ir物种与组胺基Blaamphiphiles的自组装协调，制备了用于氧释放的胶体非均相催化剂。当溶解在水中时，组胺基两亲基团会自组装形成颗粒结构，并在其表面上暴露出密集堆积的组氨酸咪唑。Ir物种随后与亲两性菌组装体的配位引起了对氧释放反应的催化活性。在牺牲氧化剂硝酸铈铵的存在下，通过使用催化组件检查了氧气的释放。Ir协调的程序集的周转频率为13分钟-1，可与之前报道的分子水氧化催化剂相媲美。催化活性随组氨酸咪唑/ Ir摩尔比的增加而增加，这表明Ir与咪唑的多重配位促进了活性Ir中间体的形成。这项研究证明了从具有生化配体的胶体双亲亲组装体构建催化活性界面的可行性。
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