摘要
The severe bulk recombination and sluggish oxygen evolution reaction(OER)dynamics of photoanodes severely restrict the application of photoelectrochemical(PEC)devices.To solve these two problems,crystallographic facet orientation and cocatalyst emergence with a high-quality photoanode/cocatalyst interface were realized through an air annealing-assisted strategy to treat atomic layer deposition(ALD)-modified SnSnanosheet arrays.Based on experimental observations and theoretical calculations,the reduced(001)crystal facet of SnSdecreases the recombination of photogenerated carriers in the bulk and improves the carrier separation of the photoanode.Moreover,the unexpectedly formed ZnTiOSfilm decreases the overpotential of the surface OER,reduces interface recombination,and extends the carrier lifetime.These synergistic effects lead to significantly enhanced PEC performance,with a high photocurrent density of 1.97 mA cm^(-2)at 1.23 V vs.reversible hydrogen electrode(RHE)and a low onset potential of 0.21 V vs.RHE,which are superior to reported mostly SnS-based photoanodes.
光阳极内部严重的体相复合和缓慢的析氧反应(OER)动力学严重限制了光电化学(PEC)水分解器件的应用.为解决这2个问题,本文对原子层沉积修饰的SnS纳米片阵列进行空气退火处理,实现了晶面取向的调控并获得了具有高质量光阳极/助催化剂界面的复合光阳极器件.基于实验观测和理论计算分析,SnS中(001)晶面的降低减少了光生载流子的体相复合,提高了载流子的体相分离能力.此外,形成的ZnTiOS薄膜作为高效的助催化剂降低了表面OER反应势垒,减少了界面复合,延长了载流子寿命.这些协同效应显著增强了SnS的PEC性能,在1.23 V vs.RHE下得到1.97 mA cm^(-2)的光电流密度,起始电位达到0.21 V vs.RHE.该工作不仅提供了一种简便有效的策略,可以同时减少光阳极中的体相和表面复合,也为通过后处理或非原位策略制备高效助催化剂提供了新思路.
作者
Linxing Meng
Cheng Cheng
Run Long
Weiwei Xu
Shengnan Li
Wei Tian
Liang Li
孟林兴;程成;龙闰;许卫卫;李胜男;田维;李亮(School of Physical Science and Technology,Jiangsu Key Laboratory of Thin Films,Center for Energy Conversion Materials&Physics(CECMP),Soochow University,Suzhou 215006,China;College of Chemistry,Key Laboratory of Theoretical&Computational Photochemistry of Ministry of Education,Beijing Normal University,Beijing 100875,China)
基金
support from the National Key Research and Development Program of China(2021YFA1500800)
the National Natural Science Foundation of China(52025028)
the Priority Academic Program Development(PAPD)of Jiangsu Higher Education Institutions
support of the National Natural Science Foundation of China(21973006)。
