Ag/Pt co-modified FeCoNiOx spinel oxides enhancing interface water dissociation to boost selective ethanol electrooxidation to acetate

IF 7.4 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Science China Materials Pub Date : 2025-06-06 DOI:10.1007/s40843-025-3411-3

Chunqi Yang (, ), Rui Yang (, ), Yue Fan (, ), Dantong Du (, ), Yuxuan Dong (, ), Yifan Hu (, ), Kaiyue Zhang (, ), Lingli Luo (, ), Yuhang Li (, ), Chunzhong Li (, )

{"title":"Ag/Pt co-modified FeCoNiOx spinel oxides enhancing interface water dissociation to boost selective ethanol electrooxidation to acetate","authors":"Chunqi Yang \n (, ), Rui Yang \n (, ), Yue Fan \n (, ), Dantong Du \n (, ), Yuxuan Dong \n (, ), Yifan Hu \n (, ), Kaiyue Zhang \n (, ), Lingli Luo \n (, ), Yuhang Li \n (, ), Chunzhong Li \n (, )","doi":"10.1007/s40843-025-3411-3","DOIUrl":null,"url":null,"abstract":"<div><p>Electrochemical catalysis offers a promising approach for biomass valorization, enabling the production of value-added chemicals. Acetate (CH<sub>3</sub>COOH), regarded as a fundamental and versatile chemical, holds significant marker potential. The electrooxidation of ethanol (CH<sub>3</sub>CH<sub>2</sub>OH) can generate valuable acetate while coupling with the cathodic reaction to produce green hydrogen, thus enhancing the electron efficiency and atom economy of the entire system. However, most electrocatalysts typically operate at low current densities and suffer from poor stability, which are unsuitable for industrial-scale applications. Therefore, we have designed and synthesized the FeCoNiO<sub><i>x</i></sub> spinel oxides complexed with Pt and Ag (FeCoNiO<sub><i>x</i></sub>-PtAg). The FeCoNiO<sub><i>x</i></sub>-PtAg catalyst can achieve the maximum Faradaic efficiency (FE) of 98.1% under 100 mA cm<sup>−2</sup>, the maximum partial current density of 291.2 mA cm<sup>−2</sup> and superior stability over 100 h. Besides, we have also conducted <i>in-situ</i> attenuated total reflection surface-enhanced infrared absorption spectroscopy to study the reaction pathway, which can demonstrate the regulation of water dissociation for moderate *OH generation and inhibit the *OH to *O through compounding of Pt and Ag. Furthermore, technoeconomic analysis confirms that this paired system is a cost-effective and low-carbon route for the production of acetate and green hydrogen.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":773,"journal":{"name":"Science China Materials","volume":"68 7","pages":"2375 - 2380"},"PeriodicalIF":7.4000,"publicationDate":"2025-06-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Science China Materials","FirstCategoryId":"88","ListUrlMain":"https://link.springer.com/article/10.1007/s40843-025-3411-3","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}

引用次数: 0

Abstract

Electrochemical catalysis offers a promising approach for biomass valorization, enabling the production of value-added chemicals. Acetate (CH₃COOH), regarded as a fundamental and versatile chemical, holds significant marker potential. The electrooxidation of ethanol (CH₃CH₂OH) can generate valuable acetate while coupling with the cathodic reaction to produce green hydrogen, thus enhancing the electron efficiency and atom economy of the entire system. However, most electrocatalysts typically operate at low current densities and suffer from poor stability, which are unsuitable for industrial-scale applications. Therefore, we have designed and synthesized the FeCoNiO_x spinel oxides complexed with Pt and Ag (FeCoNiO_x-PtAg). The FeCoNiO_x-PtAg catalyst can achieve the maximum Faradaic efficiency (FE) of 98.1% under 100 mA cm⁻², the maximum partial current density of 291.2 mA cm⁻² and superior stability over 100 h. Besides, we have also conducted in-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy to study the reaction pathway, which can demonstrate the regulation of water dissociation for moderate *OH generation and inhibit the *OH to *O through compounding of Pt and Ag. Furthermore, technoeconomic analysis confirms that this paired system is a cost-effective and low-carbon route for the production of acetate and green hydrogen.

查看原文本刊更多论文

Ag/Pt共改性FeCoNiOx尖晶石氧化物增强界面水解离，促进选择性乙醇电氧化成乙酸酯

电化学催化为生物质增值提供了一种很有前途的方法，使生产增值化学品成为可能。醋酸酯（CH3COOH）被认为是一种基础的、用途广泛的化学物质，具有重要的标记潜力。乙醇（CH3CH2OH）的电氧化可以生成有价值的乙酸，同时与阴极反应偶联产生绿色氢，从而提高了整个体系的电子效率和原子经济性。然而，大多数电催化剂通常在低电流密度下工作，稳定性差，不适合工业规模的应用。因此，我们设计并合成了FeCoNiOx尖晶石氧化物与Pt和Ag络合（feconox - ptag）。FeCoNiOx-PtAg催化剂在100 mA cm−2条件下的最大法拉第效率（FE）为98.1%，最大分电流密度为291.2 mA cm−2，在100 h内具有优异的稳定性。此外，我们还通过原位衰减全反射表面增强红外吸收光谱研究了反应途径，证明了通过Pt和Ag的复合，水解离调节适度的*OH生成，抑制*OH生成*O。此外，技术经济分析证实，这种配对系统是一种成本效益高、低碳的醋酸盐和绿色氢生产途径。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

Science China Materials Materials Science-General Materials Science

CiteScore

11.40

自引率

7.40%

发文量

949

期刊介绍： Science China Materials (SCM) is a globally peer-reviewed journal that covers all facets of materials science. It is supervised by the Chinese Academy of Sciences and co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China. The journal is jointly published monthly in both printed and electronic forms by Science China Press and Springer. The aim of SCM is to encourage communication of high-quality, innovative research results at the cutting-edge interface of materials science with chemistry, physics, biology, and engineering. It focuses on breakthroughs from around the world and aims to become a world-leading academic journal for materials science.