Interface Manipulation to Improve Plasmon-Coupled Photoelectrochemical Water Splitting on alpha-Fe2O3 Photoanodes
Interface Manipulation to Improve Plasmon-Coupled Photoelectrochemical Water Splitting on alpha-Fe2O3 Photoanodes
复制标题
界面操纵改善 α-Fe2O3 光阳极上的等离激元耦合光电化学水分解
DOI：
10.1002/cssc.201701679
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发表时间：
2018
期刊：
影响因子：
8.4
通讯作者：
Zou Zhigang
中科院分区：
文献类型：
--
作者：
Xu Zhe;Fan Zhongwen;Shi Zhan;Li Mengyu;Feng Jianyong;Pei Lang;Zhou Chenguang;Zhou Junkang;Yang Lingxia;Li Wenchao;Xu Guangzhou;Yan Shicheng;Zou Zhigang
金属纳米粒子的等离子体共振效应为提高半导体的太阳能转换效率提供了一条很有前途的途径。研究表明，Au纳米粒子的等离子体共振效应产生的超热电子容易注入Fe 2 O3光阳极的表面态，而不是导带，从而发生严重的表面复合.这样的电子转移过程似乎与外部施加的电势无关，但对金属-半导体界面性质敏感。用非催化的Al 2 O3层钝化Fe 2 O3的表面态可以在Ti掺杂的Fe 2 O3（Ti-Fe 2 O3）和Au NPs之间构建有效的共振能量转移界面。在这样的Ti-Fe 2 O3/Al 2 O3/Au电极配置中，增强的光电化学（PEC）水裂解性能可以归因于以下两个因素：1）在Au NP的非光响应波长范围内，Al 2 O3钝化层的弛豫费米钉扎效应和Au的较高功函数都扩大了能带弯曲;从而促进电荷分离;以及2）在Au NP的光响应波长范围内，有效的共振能量转移有助于光捕获和转换。 本文提出的界面操纵可以提供一种新的途径来设计用于能量转换的有效等离子体PEC装置。
The plasmon resonance effect of metal nanoparticles (NPs) offers a promising route to improve the solar energy conversion efficiency of semiconductors. In this study, it is revealed that hot electrons generated by the plasmon resonance effect of Au NPs tend to inject into the surface states instead of the conduction band of Fe2O3photoanodes, and then severe surface recombination occurs. Such an electron‐transfer process seems to be independent of external applied potentials, but is sensitive to metal–semiconductor interface properties. Passivating the surface states of Fe2O3with a noncatalytic Al2O3layer can construct an effective resonant energy‐transfer interface between Ti‐doped Fe2O3(Ti‐Fe2O3) and Au NPs. In such a Ti‐Fe2O3/Al2O3/Au electrode configuration, the enhanced photoelectrochemical (PEC) water‐splitting performance can be attributed to the following two factors: 1) in the non‐light‐responsive wavelength range of Au NPs, both the relaxing Fermi pinning effect of the Al2O3passivation layer and the higher work function of Au enlarge band bending; thus promoting the charge separation; and 2) in the light‐responsive wavelength range of Au NPs, the effective resonant energy transfer contributes to light harvesting and conversion. The interface manipulation proposed herein may provide a new route to design efficient plasmonic PEC devices for energy conversion.