Pivotal Role and Regulation of Proton Transfer in Water Oxidation on Hematite Photoanodes
文献类型：期刊论文
| 作者 | Zhang, Yuchao; Zhang, Hongna; Ji, Hongwei; Ma, Wanhong; Chen, Chuncheng; Zhao, Jincai |
| 刊名 | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
 |
| 出版日期 | 2016-03-02 |
| 卷号 | 138期号:8页码:2705-2711 |
| 英文摘要 | Hematite is a promising material for solar water splitting; however, high efficiency remains elusive because of the kinetic limitations of interfacial charge transfer. Here, we demonstrate the pivotal role of proton transfer in water oxidation on hematite photoanodes using photoelectrochemical (PEC) characterization, the H/D kinetic isotope effect (KIE), and electrochemical impedance spectroscopy (EIS). We observed a concerted proton-electron transfer (CPET) characteristic for the rate-determining interfacial hole transfer, where electron transfer (ET) from molecular water to a surface-trapped hole was accompanied by proton transfer (PT) to a solvent water molecule, demonstrating a substantial KIE (similar to 3.5). The temperature dependency of KIE revealed a highly flexible proton transfer channel along the hydrogen bond at the hematite/electrolyte interface. A mechanistic transition in the rate-determining step from CPET to ET occurred after OH- became the dominant hole acceptor. We further modified the proton electron transfer sequence with appropriate proton acceptors (buffer bases) and achieved a greater than 4-fold increase in the PEC water oxidation efficiency on a hematite photoanode. |
| 收录类别 | SCI |
| 语种 | 英语 |
| 源URL | [http://ir.iccas.ac.cn/handle/121111/35880]  |
| 专题 | 化学研究所_光化学实验室 |
| 作者单位 | Chinese Acad Sci, Inst Chem, Beijing Natl Lab Mol Sci, Key Lab Photochem, Beijing 100190, Peoples R China |
| 推荐引用方式 GB/T 7714 | Zhang, Yuchao,Zhang, Hongna,Ji, Hongwei,et al. Pivotal Role and Regulation of Proton Transfer in Water Oxidation on Hematite Photoanodes[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2016,138(8):2705-2711. |
| APA | Zhang, Yuchao,Zhang, Hongna,Ji, Hongwei,Ma, Wanhong,Chen, Chuncheng,&Zhao, Jincai.(2016).Pivotal Role and Regulation of Proton Transfer in Water Oxidation on Hematite Photoanodes.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,138(8),2705-2711. |
| MLA | Zhang, Yuchao,et al."Pivotal Role and Regulation of Proton Transfer in Water Oxidation on Hematite Photoanodes".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 138.8(2016):2705-2711. |
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来源：化学研究所
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