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Tuning the reactivity of cobalt-based H2 production electrocatalysts via the incorporation of the peripheral basic functionalities
Coordination Chemistry Reviews ( IF 20.3 ) Pub Date : 2020-04-20 , DOI: 10.1016/j.ccr.2020.213335
Dependu Dolui , Santanu Ghorai , Arnab Dutta

The construction of an efficient, inexpensive, and durable H2 production electrocatalyst is considered as an indispensable tool for the inception of a hydrogen-mediated alternative energy technology. Recently, cobalt-based molecular complexes have emerged as one of the realistic candidates for this key role of H2 evolution catalyst due to their intrinsic oxygen tolerance and moderately efficient proton reduction ability. However, the issues pertaining to the water solubility and long-term stability of those cobalt complexes have limited their practical applications. Recently, several research groups have adopted an enzyme-inspired catalyst design strategy, where variable basic functionalities were appended around the existing core-cobalt complexes to improve their water solubility. Additionally, presence of these peripheral groups enhances catalytic H2 evolution activity of the modified complexes by boosting the proton transduction around the framework. Inclusion of this biomimetic outer coordination sphere feature also induced structural flexibility around the metal core to improve the stability of the complexes under demanding catalytic conditions. In this article, we have specifically portrayed the multi-dimensional regulatory roles effectuated by these fluxional basic functionalities during the catalytic H2 production by the cobalt-based molecular complexes.



中文翻译:

通过结合外围基本功能来调整钴基H 2生产电催化剂的反应性

高效,廉价和耐用的H 2生产电催化剂的构造被认为是开始氢介导的替代能源技术必不可少的工具。最近,基于钴的分子复合物已成为H 2关键作用的现实候选者之一。催化剂由于其固有的耐氧性和中等有效的质子还原能力。然而,与那些钴配合物的水溶性和长期稳定性有关的问题限制了它们的实际应用。最近,几个研究小组采用了一种酶激发的催化剂设计策略,该方法将可变的基本功能附加到现有的核心-钴络合物周围,以提高其水溶性。此外,这些外围基团的存在增强了催化H 2通过促进框架周围的质子转导来修饰复合物的进化活性。包含这种仿生外部配位球特征还诱导了金属核周围的结构柔性,以改善配合物在苛刻催化条件下的稳定性。在本文中,我们特别描绘了在钴基分子配合物催化生成H 2的过程中,这些通量基本功能实现的多维调节作用。

更新日期:2020-04-20
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