Catalytic Metallopolymers from [2Fe‐2S] Clusters: Artificial Metalloenzymes for Hydrogen Production
Catalytic Metallopolymers from [2Fe‐2S] Clusters: Artificial Metalloenzymes for Hydrogen Production
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[2Fe-2S] 簇催化金属聚合物：用于制氢的人工金属酶
DOI：
10.1002/ange.201813776
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发表时间：
2019
影响因子：
--
通讯作者：
Pyun, Jeffrey
中科院分区：
文献类型：
--
作者：
Karayilan, Metin;Brezinski, William P.;Clary, Kayla E.;Lichtenberger, Dennis L.;Glass, Richard S.;Pyun, Jeffrey
本文综述了用于电催化和光催化析氢反应的新型聚合物负载的[2Fe-2S]催化剂体系的发展。[FeFe]氢化酶是最著名的天然存在的金属酶，用于产生氢，并且这些金属酶的活性位点（H簇）的小分子含[2Fe-2S]的模拟物已经合成多年。 这些小的[2Fe-2S]复合物还没有达到与酶相同的制氢能力。最近，现代高分子化学已被用于在[2Fe-2S]簇周围构建外配位球，以提供位点隔离、水溶性和改善的催化活性。本文综述了这些聚合物负载的[2Fe-2S]材料的各种大分子结构及其催化性能。最新的催化剂包含单一的[2Fe-2S]络合物，称为单位点[2Fe-2S]金属聚合物，表现出上级的H2生产活性。
Reviewed herein is the development of novel polymer‐supported [2Fe‐2S] catalyst systems for electrocatalytic and photocatalytic hydrogen evolution reactions. [FeFe] hydrogenases are the best known naturally occurring metalloenzymes for hydrogen generation, and small‐molecule, [2Fe‐2S]‐containing mimetics of the active site (H‐cluster) of these metalloenzymes have been synthesized for years. These small [2Fe‐2S] complexes have not yet reached the same capacity as that of enzymes for hydrogen production. Recently, modern polymer chemistry has been utilized to construct an outer coordination sphere around the [2Fe‐2S] clusters to provide site isolation, water solubility, and improved catalytic activity. In this review, the various macromolecular motifs and the catalytic properties of these polymer‐supported [2Fe‐2S] materials are surveyed. The most recent catalysts that incorporate a single [2Fe‐2S] complex, termed single‐site [2Fe‐2S] metallopolymers, exhibit superior activity for H2production.