Boosting Electrocatalytic Hydrogen Evolution over Metal-Organic Frameworks by Plasmon-Induced Hot-Electron Injection

Boosting Electrocatalytic Hydrogen Evolution over Metal-Organic Frameworks by Plasmon-Induced Hot-Electron Injection
复制标题

通过等离激元诱导热电子注入促进金属有机框架电催化析氢

DOI:
10.1002/anie.201906134
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发表时间:
2019-07-29
影响因子:
16.6
通讯作者:
Jiang, Hai-Long
Jiang, Hai-Long
中科院分区:
化学1区
文献类型:
--
作者:
Wang, Shan-Shan;Jiao, Long;Jiang, Hai-Long

文献摘要

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通过电催化水分解实现高效析氢在现代能源设备中具有广阔的前景。在此,我们证明Au纳米棒(NR)的局域表面等离子体共振(LSPR)激发显着提高了CoFe-金属有机骨架纳米片(CoFe-MOFN)的电催化析氢活性,导致-0.236 V(相对于RHE)下的电流密度增加了4倍以上 Au/CoFe-MOFN 复合材料在光照射下与在黑暗下的比较。机理研究表明,析氢增强很大程度上归因于热电子从 AuNR 注入 CoFe-MOFN,提高了 CoFe-MOFN 的费米能​​级,促进 H2O 的还原并降低 HER 的活化能。这项研究强调了等离激元激发在提高MOF电催化效率方面的优越性,并为光照射下高效水分解系统的设计提供了一条新途径。
Efficient hydrogen evolution via electrocatalytic water splitting holds great promise in modern energy devices. Herein, we demonstrate that the localized surface plasmon resonance (LSPR) excitation of Au nanorods (NRs) dramatically improves the electrocatalytic hydrogen evolution activity of CoFe-metal-organic framework nanosheets (CoFe-MOFNs), leading to a more than 4-fold increase of current density at -0.236 V (vs. RHE) for Au/CoFe-MOFNs composite under light irradiation versus in dark. Mechanistic investigations reveal that the hydrogen evolution enhancement can be largely attributed to the injection of hot electrons from AuNRs to CoFe-MOFNs, raising the Fermi level of CoFe-MOFNs, facilitating the reduction of H2O and affording decreased activation energy for HER. This study highlights the superiority of plasmonic excitation on improving electrocatalytic efficiency of MOFs and provides a novel avenue towards the design of highly efficient water-splitting systems under light irradiation.