Crucial role of hydroxyl in CO selectivity for integrated CO2 capture and electrocatalytic reduction

IF 11.2

Carbon Neutrality Pub Date : 2026-01-07 DOI:10.1007/s43979-025-00157-4

Shaona Wang, Yang Yang, Wenqing Xu, Zhuoshu Bai, Fabing Su, Yixi Wang, Dingrong Bai, Tingyu Zhu

{"title":"Crucial role of hydroxyl in CO selectivity for integrated CO2 capture and electrocatalytic reduction","authors":"Shaona Wang, Yang Yang, Wenqing Xu, Zhuoshu Bai, Fabing Su, Yixi Wang, Dingrong Bai, Tingyu Zhu","doi":"10.1007/s43979-025-00157-4","DOIUrl":null,"url":null,"abstract":"Abstract As an integrated CO 2 capture and utilization (ICCU) process, direct electrochemical reduction of amine captured-CO 2 reduction reaction (cCO 2 RR) has enormous advantages in energy efficiency and operating cost. The low product selectivity is an urgent issue. Here, we found that the hydroxyl (-OH) on CeO 2 can significantly enhance CO selectivity. After hydroxyl modification, the CO faraday efficiency (FE CO ) was surprisingly increased by 188% (relative increase rate). The correlation coefficient between -OH quantity and FE CO is as high as 0.98. Further study indicated that the presence of -OH can lead to a more compact electrochemical double layer (EDL) and charge transfer resistance by proton transfer. The -OH can also enhance CO 2 adsorption and stabilize the intermediate species (*COOH). DFT results further demonstrate that the rate-determining step was proton transfer from the surface -OH to MEACOO − , -OH modification can reduce the energy barrier to as low as 0.39 eV. This work provides additional insights into improving selectivity in amine-based cCO 2 RR, advancing the development of ICCU technology.","PeriodicalId":488328,"journal":{"name":"Carbon Neutrality","volume":"5 1","pages":""},"PeriodicalIF":11.2000,"publicationDate":"2026-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s43979-025-00157-4.pdf","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Carbon Neutrality","FirstCategoryId":"0","ListUrlMain":"https://doi.org/10.1007/s43979-025-00157-4","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}

引用次数: 0

Abstract

Abstract As an integrated CO 2 capture and utilization (ICCU) process, direct electrochemical reduction of amine captured-CO 2 reduction reaction (cCO 2 RR) has enormous advantages in energy efficiency and operating cost. The low product selectivity is an urgent issue. Here, we found that the hydroxyl (-OH) on CeO 2 can significantly enhance CO selectivity. After hydroxyl modification, the CO faraday efficiency (FE CO ) was surprisingly increased by 188% (relative increase rate). The correlation coefficient between -OH quantity and FE CO is as high as 0.98. Further study indicated that the presence of -OH can lead to a more compact electrochemical double layer (EDL) and charge transfer resistance by proton transfer. The -OH can also enhance CO 2 adsorption and stabilize the intermediate species (*COOH). DFT results further demonstrate that the rate-determining step was proton transfer from the surface -OH to MEACOO − , -OH modification can reduce the energy barrier to as low as 0.39 eV. This work provides additional insights into improving selectivity in amine-based cCO 2 RR, advancing the development of ICCU technology.

查看原文本刊更多论文

羟基在CO选择性中起着至关重要的作用，用于综合CO2捕获和电催化还原

摘要：直接电化学还原胺捕获- co2还原反应（cco2 RR）作为一种集成的co2捕集与利用（ICCU）工艺，在能源效率和运行成本方面具有巨大的优势。产品选择性低是一个亟待解决的问题。在这里，我们发现ceo2上的羟基（-OH）可以显著提高CO的选择性。羟基改性后，CO的法拉第效率（FE CO）提高了188%（相对提高率）。-OH量与FE - CO的相关系数高达0.98。进一步的研究表明-OH的存在可以使电化学双层（EDL）更加致密，并通过质子转移产生电荷转移阻力。-OH还能增强co2的吸附，稳定中间体（*COOH）。DFT结果进一步表明，质子从表面-OH转移到MEACOO−是决定速率的步骤，-OH修饰可以使能垒低至0.39 eV。这项工作为提高胺基cco2 RR的选择性提供了额外的见解，促进了ICCU技术的发展。

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

Carbon Neutrality

CiteScore

5.10

自引率

0.00%

发文量