Enhanced Performance of Si MIS Photocathodes Containing Oxide-Coated Nanoparticle Electrocatalysts.
Enhanced Performance of Si MIS Photocathodes Containing Oxide-Coated Nanoparticle Electrocatalysts.
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DOI：
10.1021/acs.nanolett.6b02909
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发表时间：
2016-10-12
期刊：
影响因子：
10.8
通讯作者：
Esposito DV
中科院分区：
文献类型：
--
作者：
Labrador NY;Li X;Liu Y;Tan H;Wang R;Koberstein JT;Moffat TP;Esposito DV
将低负载量的金属纳米粒子催化剂电沉积到半导体光电极的表面上是降低催化剂成本和最小化光学损失的一种非常有吸引力的方法。然而，将纳米粒子安全地锚定到光电极表面可能具有挑战性，尤其是当表面被薄绝缘覆盖层覆盖时。在此，我们报告了用于析氢反应的硅基光电阴极，通过使用沉积在 Pt 纳米颗粒催化剂顶部的 2-10 nm 厚的氧化硅 (SiOx) 层克服了这个问题，该催化剂首先电沉积在 1.5 nm SiO2|p-Si(100) 吸收层上。与缺乏二次 SiOx 覆盖层的金属-绝缘体-半导体 (MIS) 对照样品相比，这种绝缘体-金属-绝缘体-半导体 (IMIS) 光电极表现出优异的耐用性和电荷转移特性。对颗粒负载、SiOx 层厚度和光照强度影响的系统研究表明，SiOx 层具有适度的电导率，从而降低了与 p-Si 和 Pt 纳米颗粒之间的高局部隧道电流密度相关的电荷转移电阻。重要的是，IMIS架构被证明是一种非常有效的方法，可以稳定沉积在绝缘覆盖层上的电催化纳米颗粒，而不会对与析氢反应相关的反应物和产物种类的质量传输产生不利影响。
Electrodepositing low loadings of metallic nanoparticle catalysts onto the surface of semiconducting photoelectrodes is a highly attractive approach for decreasing catalyst costs and minimizing optical losses. However, securely anchoring nanoparticles to the photoelectrode surface can be challenging—especially if the surface is covered by a thin insulating overlayer. Herein, we report on Si-based photocathodes for the hydrogen evolution reaction that overcome this problem through the use of a 2–10 nm thick layer of silicon oxide (SiOx) that is deposited on top of Pt nanoparticle catalysts that were first electrodeposited on a 1.5 nm SiO2|p-Si(100) absorber layer. Such insulator–metal–insulator–semiconductor (IMIS) photoelectrodes exhibit superior durability and charge transfer properties compared to metal–insulator–semiconductor (MIS) control samples that lacked the secondary SiOx overlayer. Systematic investigation of the influence of particle loading, SiOx layer thickness, and illumination intensity suggests that the SiOx layer possesses moderate conductivity, thereby reducing charge transfer resistance associated with high local tunneling current densities between the p-Si and Pt nanoparticles. Importantly, the IMIS architecture is proven to be a highly effective approach for stabilizing electrocatalytic nanoparticles deposited on insulating overlayers without adversely affecting mass transport of reactant and product species associated with the hydrogen evolution reaction.
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