优化NiCo-LDH助催化剂的形成能垒促进光电氧化苯甲醇

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

{"title":"优化NiCo-LDH助催化剂的形成能垒促进光电氧化苯甲醇","authors":"Bin Gao, Xiaowei Mu, Jianming Liu, Jianyong Feng, Huiting Huang, Zhigang Zou, Zhaosheng Li","doi":"10.1021/acs.jpclett.4c03065","DOIUrl":null,"url":null,"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.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"88 1","pages":""},"PeriodicalIF":4.8000,"publicationDate":"2024-12-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Optimizing Formation Energy Barrier of NiCo-LDH Cocatalyst to Enhance Photoelectrochemical Benzyl Alcohol Oxidation\",\"authors\":\"Bin Gao, Xiaowei Mu, Jianming Liu, Jianyong Feng, Huiting Huang, Zhigang Zou, Zhaosheng Li\",\"doi\":\"10.1021/acs.jpclett.4c03065\",\"DOIUrl\":null,\"url\":null,\"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.\",\"PeriodicalId\":62,\"journal\":{\"name\":\"The Journal of Physical Chemistry Letters\",\"volume\":\"88 1\",\"pages\":\"\"},\"PeriodicalIF\":4.8000,\"publicationDate\":\"2024-12-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"The Journal of Physical Chemistry Letters\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.jpclett.4c03065\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"The Journal of Physical Chemistry Letters","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.jpclett.4c03065","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}

引用次数: 0

摘要

利用有机氧化反应取代析氧反应是生产高价值有机产品和氢气的一种很有前途的方法。在这里，我们报道了一种基于α-Fe2O3光阳极涂覆nico层双氢氧化物（NiCo-LDH）助催化剂的电化学苯甲醇氧化体系。通过调整NiCo-LDH中Ni和Co的相对含量，优化后的光阳极苯甲醇转化率为99.1%，苯甲酸选择性为90.9%。实验研究表明，苯甲醇氧化反应是通过NiCo-LDH助催化剂的高价种间接催化机制进行的。Co在NiCo-LDH中降低了高价态的形成能垒和氧化能力，从而影响了光阳极的性能。这项工作提供了对助催化剂组成在有机反应氧化中的关键作用的见解，并有助于开发各种光电化学有机氧化系统。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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

查看原文本刊更多论文

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

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.

求助全文

通过发布文献求助，成功后即可免费获取论文全文。去求助

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.