Photochemical hydrogen evolution from cobalt microperoxidase-11.
Photochemical hydrogen evolution from cobalt microperoxidase-11.
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DOI：
10.1016/j.jinorgbio.2021.111384
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发表时间：
2021-04
影响因子：
3.9
通讯作者：
Bren, Kara L.
中科院分区：
文献类型：
--
作者：
Edwards, Emily H.;Jelusic, Jana;Chakraborty, Saikat;Bren, Kara L.
关键词：
利用半合成生物分子催化剂乙酰化钴微过氧化物酶-11（CoMP 11-Ac）沿着[Ru（bpy）3]2+作为光敏剂和抗坏血酸作为电子供体的光化学系统显示在可见光驱动的反应中从水产生氢。光激发[Ru（bpy）3]2+促进的还原淬灭途径克服了CoMP 11-Ac在电催化中观察到的高过电位，产生的转换数范围为606至2390（2 μM - 0.1 μM CoMP 11-Ac）。CoMP 11-Ac在光化学系统中的寿命（持续催化超过20小时）与其先前报道的在电化学系统中的行为（其中催化在15分钟后减慢）形成对比。质子还原转换数和速率在中性pH下最高，这是类似光化学系统中钴催化剂的罕见特征，其通常在酸性条件下发挥最佳作用。将生物分子组分引入光化学系统的催化剂设计中可以解决从中性pH水源产生氢的需求。
A photochemical system utilizing the semisynthetic biomolecular catalyst acetylated cobalt microperoxidase-11 (CoMP11-Ac) along with [Ru(bpy)3]2+ as a photosensitizer and ascorbic acid as an electron donor is shown to generate hydrogen from water in a visible light-driven reaction. The reductive quenching pathway facilitated by photoexcited [Ru(bpy)3]2+ overcomes the high overpotential observed for CoMP11-Ac in electrocatalysis, yielding turnover numbers ranging from 606 to 2390 (2 μM – 0.1 μM CoMP11-Ac). The longevity of CoMP11-Ac in the photochemical system, sustaining catalysis for over twenty hours, is in contrast to its previously reported behavior in an electrochemical system where catalysis slows after fifteen minutes. Proton reduction turnover number and rate are highest at a neutral pH, a rare feature among cobalt catalysts in similar photochemical systems, which typically function best under acidic conditions. Incorporating biomolecular components into the design of catalysts for photochemical systems may address the need for hydrogen generation from neutral-pH water sources.
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影响因子：
4
作者：
Deponti, Elisa;Luisa, Alessandra;Scandola, Franco
通讯作者：
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影响因子：
15
作者：
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影响因子：
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Brunold, Thomas C.
DOI：
10.1126/science.36.926.385
发表时间：
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期刊：
Science (New York, N.Y.)
影响因子：
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作者：
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通讯作者：
Ciamician, G
影响因子：
4.6
作者：
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通讯作者：
Eisenberg, Richard