How light-harvesting semiconductors can alter the bias of reversible electrocatalysts in favor of H2 production and CO2 reduction.
How light-harvesting semiconductors can alter the bias of reversible electrocatalysts in favor of H2 production and CO2 reduction.
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DOI：
10.1021/ja4042675
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发表时间：
2013-10-09
影响因子：
15
通讯作者：
Armstrong, Fraser A.
中科院分区：
文献类型：
--
作者：
Bachmeier, Andreas;Wang, Vincent C. C.;Woolerton, Thomas W.;Bell, Sophie;Fontecilla-Camps, Juan C.;Can, Mehmet;Ragsdale, Stephen W.;Chaudhary, Yatendra S.;Armstrong, Fraser A.
用于太阳能燃料生产的最有效的催化剂应该在接近可逆电势的情况下操作，但对燃料形成方向具有偏置。蛋白质膜电化学研究含镍的一氧化碳脱氢酶和[NiFeSe]-氢化酶，每一个可逆的电催化剂，表明电极的电子状态强烈偏置的CO2/CO和H+/H2相互转化的电催化的方向。附着在石墨电极上，这些酶表现出高活性的氧化和还原，但有一个显着的偏移偏置，有利于CO2或H+还原，当相应的酶连接，而不是从CdS和TiO 2纳米粒子构造的n-型半导体电极。如果电极在与电催化电流在氧化和还原之间切换相同的窄电位范围（<0.25 V）内在半导体和金属类行为之间转换，则对于附着到半导体电极的可逆电催化剂，可以产生这种催化整流效应。
The most efficient catalysts for solar fuel production should operate close to reversible potentials, yet possess a bias for the fuel-forming direction. Protein film electrochemical studies of Ni-containing carbon monoxide dehydrogenase and [NiFeSe]-hydrogenase, each a reversible electrocatalyst, show that the electronic state of the electrode strongly biases the direction of electrocatalysis of CO2/CO and H+/H2 interconversions. Attached to graphite electrodes, these enzymes show high activities for both oxidation and reduction, but there is a marked shift in bias, in favor of CO2 or H+ reduction, when the respective enzymes are attached instead to n-type semiconductor electrodes constructed from CdS and TiO2 nanoparticles. This catalytic rectification effect can arise for a reversible electrocatalyst attached to a semiconductor electrode if the electrode transforms between semiconductor- and metallic-like behavior across the same narrow potential range (<0.25 V) that the electrocatalytic current switches between oxidation and reduction.
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DOI：
10.1016/s0969-2126(99)80072-0
发表时间：
1999-05-01
期刊：
STRUCTURE WITH FOLDING & DESIGN
影响因子：
--
作者：
Garcin, E;Vernede, X;Fontecilla-Camps, JC
通讯作者：
Fontecilla-Camps, JC
影响因子：
2.9
作者：
Seravalli, Javier;Ragsdale, Stephen W.
通讯作者：
Ragsdale, Stephen W.
影响因子：
3.9
作者：
Boschloo, G;Fitzmaurice, D
通讯作者：
Fitzmaurice, D
影响因子：
56.9
作者：
Helm, Monte L.;Stewart, Michael P.;DuBois, Daniel L.
通讯作者：
DuBois, Daniel L.
影响因子：
15
作者：
Brown, Katherine A.;Wilker, Molly B.;King, Paul W.
通讯作者：
King, Paul W.