Optimizing Formation Energy Barrier of NiCo-LDH Cocatalyst to Enhance Photoelectrochemical Benzyl Alcohol Oxidation

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters Pub Date : 2024-12-21 DOI:10.1021/acs.jpclett.4c03065

Bin Gao, Xiaowei Mu, Jianming Liu, Jianyong Feng, Huiting Huang, Zhigang Zou, Zhaosheng Li

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Abstract

Using organic oxidation reactions to replace the oxygen evolution reaction is a promising approach for producing high-value organic products and hydrogen. Here, we report a photoelectrochemical benzyl alcohol oxidation system based on an α-Fe₂O₃ photoanode coated with a NiCo-layered double hydroxide (NiCo-LDH) cocatalyst. By adjustment of the relative content of Ni and Co in the NiCo-LDH, the optimized photoanode achieved a benzyl alcohol conversion efficiency of 99.1% and benzoic acid selectivity of 90.9%. Experimental studies revealed that the benzyl alcohol oxidation reaction proceeds via an indirect catalytic mechanism involving high-valence species of the NiCo-LDH cocatalyst. Co in NiCo-LDH reduced the formation energy barrier and oxidative capability of the high-valence species, thereby influencing the performance of the photoanode. This work provides insights into the crucial role of cocatalyst composition in organic reaction oxidation and contributes to developing various photoelectrochemical organic oxidation systems.

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来源期刊

The Journal of Physical Chemistry Letters CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY

CiteScore

9.60

自引率

7.00%

发文量

1519

审稿时长

1.6 months

期刊介绍： The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.