Solar-Driven Water Oxidation and Decoupled Hydrogen Production Mediated by an Electron-Coupled-Proton Buffer.
Solar-Driven Water Oxidation and Decoupled Hydrogen Production Mediated by an Electron-Coupled-Proton Buffer.
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DOI：
10.1021/jacs.6b03187
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发表时间：
2016-06-01
影响因子：
15
通讯作者：
Cronin L
中科院分区：
文献类型：
--
作者：
Bloor LG;Solarska R;Bienkowski K;Kulesza PJ;Augustynski J;Symes MD;Cronin L
太阳能-氢光电化学电池（佩奇）已经被提出作为将太阳光转化为H2燃料的手段。然而，在传统的佩奇中，析氧反应和析氢反应是耦合的，因此这两者的速率受到可以从太阳能通量产生的光电流的限制。这反过来导致缓慢的气体析出速率，这有利于H2进入O2流的交叉，反之亦然，即使通过表面上不可渗透的膜，如Nafion。在此，我们表明，使用的电子耦合质子缓冲（ECPB）H3 PMo 12 O 40允许太阳能驱动的O2从水的演变，以超过1 mA cm-2的速率进行WO 3光阳极，而不需要任何额外的电化学偏压。在PEC中不产生H2，而是将H3 PMo 12 O 40还原为H5 PMo 12 O 40。如果还原的ECPB经受单独的电化学再氧化，则以完全的总法拉第效率产生H2。
Solar-to-hydrogen photoelectrochemical cells (PECs) have been proposed as a means of converting sunlight into H2 fuel. However, in traditional PECs, the oxygen evolution reaction and the hydrogen evolution reaction are coupled, and so the rate of both of these is limited by the photocurrents that can be generated from the solar flux. This in turn leads to slow rates of gas evolution that favor crossover of H2 into the O2 stream and vice versa, even through ostensibly impermeable membranes such as Nafion. Herein, we show that the use of the electron-coupled-proton buffer (ECPB) H3PMo12O40 allows solar-driven O2 evolution from water to proceed at rates of over 1 mA cm–2 on WO3 photoanodes without the need for any additional electrochemical bias. No H2 is produced in the PEC, and instead H3PMo12O40 is reduced to H5PMo12O40. If the reduced ECPB is subjected to a separate electrochemical reoxidation, then H2 is produced with full overall Faradaic efficiency.
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