Anti-poisoning of CO and carbonyl species over Pd catalysts during the electrooxidation of ethylene glycol to glycolic acid at elevated current density†

IF 7.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Chemical Science Pub Date : 2025-02-01 DOI:10.1039/D4SC08579E
Jia Cheng, Yunchuan Tu, Yang Xiang, Jingtian Ni, Tao Guo, Xun Huang, Bin Liu and Zidong Wei
{"title":"Anti-poisoning of CO and carbonyl species over Pd catalysts during the electrooxidation of ethylene glycol to glycolic acid at elevated current density†","authors":"Jia Cheng, Yunchuan Tu, Yang Xiang, Jingtian Ni, Tao Guo, Xun Huang, Bin Liu and Zidong Wei","doi":"10.1039/D4SC08579E","DOIUrl":null,"url":null,"abstract":"<p >The electrocatalytic oxidation of ethylene glycol (EG) to produce valuable glycolic acid (GLYA) is a promising strategy to tackle EG overcapacity. Despite the good selectivity of Pd for EG oxidation, its performance is constrained by limited mass activity and toxicity of intermediates like CO or CO-analogues. This study reports the alloying of Pd with Ni and Mo metals to enhance the activity and durability of EG oxidation in alkaline media. Notably, the peak current density reached up to 2423 mA mg<small><sup>−1</sup></small>, double that of pristine Pd/C, accompanied by a GLYA Faraday efficiency up to 87.7%. Moreover, PdNiMo/C exhibited a 5-fold slower activity decline compared to Pd/C. <em>In situ</em> experiments and theoretical analysis reveal that Ni and Mo synergistically strengthen the oxygen affinity of the catalyst, facilitating the generation of *OH radicals at lower potentials, thereby accelerating EG oxidation kinetics. Additionally, Ni incorporation prevents C–C bond cleavage and weakens CO adsorption, effectively mitigating catalyst poisoning.</p>","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":" 10","pages":" 4303-4310"},"PeriodicalIF":7.4000,"publicationDate":"2025-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/sc/d4sc08579e?page=search","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Science","FirstCategoryId":"92","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2025/sc/d4sc08579e","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0

Abstract

The electrocatalytic oxidation of ethylene glycol (EG) to produce valuable glycolic acid (GLYA) is a promising strategy to tackle EG overcapacity. Despite the good selectivity of Pd for EG oxidation, its performance is constrained by limited mass activity and toxicity of intermediates like CO or CO-analogues. This study reports the alloying of Pd with Ni and Mo metals to enhance the activity and durability of EG oxidation in alkaline media. Notably, the peak current density reached up to 2423 mA mg−1, double that of pristine Pd/C, accompanied by a GLYA Faraday efficiency up to 87.7%. Moreover, PdNiMo/C exhibited a 5-fold slower activity decline compared to Pd/C. In situ experiments and theoretical analysis reveal that Ni and Mo synergistically strengthen the oxygen affinity of the catalyst, facilitating the generation of *OH radicals at lower potentials, thereby accelerating EG oxidation kinetics. Additionally, Ni incorporation prevents C–C bond cleavage and weakens CO adsorption, effectively mitigating catalyst poisoning.

Abstract Image

查看原文
分享 分享
微信好友 朋友圈 QQ好友 复制链接
本刊更多论文
高电流密度下乙二醇电氧化制乙醇酸过程中CO和羰基对Pd催化剂的抗中毒作用
电催化氧化乙二醇生产有价乙醇酸是解决乙二醇产能过剩的一种很有前途的策略。尽管Pd对EG氧化具有良好的选择性,但其性能受到CO或CO类似物等中间体有限的质量活性和毒性的限制。本文研究了Pd与Ni和Mo合金在碱性介质中氧化EG的活性和耐久性。值得注意的是,峰值电流密度高达2423 mA mg-1,是原始Pd/C的两倍,同时GLYA法拉第效率高达87.7%。此外,PdNiMo/C的活性下降速度比Pd/C慢5倍。原位实验和理论分析表明,Ni和Mo协同增强了催化剂的氧亲和力,促进了*OH自由基在较低电位下的生成,从而加速了EG的氧化动力学。此外,Ni的掺入阻止了C-C键的断裂,减弱了CO的吸附,有效地减轻了催化剂中毒。
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 去求助
来源期刊
Chemical Science
Chemical Science CHEMISTRY, MULTIDISCIPLINARY-
CiteScore
14.40
自引率
4.80%
发文量
1352
审稿时长
2.1 months
期刊介绍: Chemical Science is a journal that encompasses various disciplines within the chemical sciences. Its scope includes publishing ground-breaking research with significant implications for its respective field, as well as appealing to a wider audience in related areas. To be considered for publication, articles must showcase innovative and original advances in their field of study and be presented in a manner that is understandable to scientists from diverse backgrounds. However, the journal generally does not publish highly specialized research.
期刊最新文献
Silver-Catalysed Intermolecular Benzylic-Selective C–H Amidation via Nitrene Transfer A Brønsted Acid-Base Approach for the Net Monoselective C-F Substitution of (Trifluoromethyl)alkanes Computational redesign and directed evolution of a lanthanide-dependent photoredox enzyme for enantioselective diol cleavage Molecular Engineering of Metalloporphyrins and Phthalocycanines for Homogeneous and Heterogeneous CO 2 Electroreduction Stealing from a distant neighbor: an unexpectedly fast long-span peroxy radical hydrogen-shift reaction in a long-chain diether
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
已复制链接
已复制链接
快去分享给好友吧!
我知道了
×
扫码分享
扫码分享
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1