Pub Date : 2025-09-07DOI: 10.1016/j.apcatb.2025.125939
Yuhou Pei, Di Li, Y. P. Pei, Zongmiao Li, Yuting Liu, Xiang Ling, Yingying Lü, Bing Zhang
Urea synthesis by co-electroreduction of CO 2 and nitrate provides a promising strategy for sustainable fertilizer production. Despite advances in catalyst exploration, it is of significance to figure out the microenvironment on the electrode interface toward the kinetically matched C-N coupling. Here, we fabricated a hydrophobic triple-phase catalytic interface through a simply blending of commercial CuZn alloy and polytetrafluoroethylene (PTFE) particles for proof of concept. Incorporating PTFE boosted the Faradaic efficiency of urea from 8 % to 49 % and tripled the urea production rate. Kinetics and in-situ spectra studies reveal that hydrophobicity slows the proton/electron transfer during nitrate reduction, accelerates CO₂ diffusion at the triple-phase interface, and preserves high-valent asymmetric adsorption sites. This synergy extends the lifetime and surface coverage of critical C-/N-intermediates, and thus kinetically-matched asymmetric C-N coupling. Low catalytic selectivity incurred by kinetically mismatched electroreduction of C- and N-source, and hence inefficient chemical C-N coupling is the major limitation for urea electrosynthesis. Here, we investigated the hydrophobicity effect on the triple-phase interface upon urea electrosynthesis, and found that a hydrophobic interface promotes gas diffusion as well as decelerates the electro-hydrogenation of N-source, which balances the kinetically matched electrochemical C-N coupling process. • Hydrophobic microenvironment impacts the kinetic matching during the C-N coupling. • Hydrophobicity influences proton/electron transfer processes for NO 3 RR and CO 2 diffusion for CO 2 RR. • The kinetics of CO 2 -to-*CO and NO 3 - -to-*NH 2 can thus be simultaneously tuned on the hydrophobic interface. • FE urea can be greatly improved from 8 % to 49 % by adding 40 % PTFE to the CuZn catalyst.
{"title":"Tailoring the triple-phase microenvironment for kinetically matched C-N coupling in urea electrosynthesis","authors":"Yuhou Pei, Di Li, Y. P. Pei, Zongmiao Li, Yuting Liu, Xiang Ling, Yingying Lü, Bing Zhang","doi":"10.1016/j.apcatb.2025.125939","DOIUrl":"https://doi.org/10.1016/j.apcatb.2025.125939","url":null,"abstract":"Urea synthesis by co-electroreduction of CO 2 and nitrate provides a promising strategy for sustainable fertilizer production. Despite advances in catalyst exploration, it is of significance to figure out the microenvironment on the electrode interface toward the kinetically matched C-N coupling. Here, we fabricated a hydrophobic triple-phase catalytic interface through a simply blending of commercial CuZn alloy and polytetrafluoroethylene (PTFE) particles for proof of concept. Incorporating PTFE boosted the Faradaic efficiency of urea from 8 % to 49 % and tripled the urea production rate. Kinetics and in-situ spectra studies reveal that hydrophobicity slows the proton/electron transfer during nitrate reduction, accelerates CO₂ diffusion at the triple-phase interface, and preserves high-valent asymmetric adsorption sites. This synergy extends the lifetime and surface coverage of critical C-/N-intermediates, and thus kinetically-matched asymmetric C-N coupling. Low catalytic selectivity incurred by kinetically mismatched electroreduction of C- and N-source, and hence inefficient chemical C-N coupling is the major limitation for urea electrosynthesis. Here, we investigated the hydrophobicity effect on the triple-phase interface upon urea electrosynthesis, and found that a hydrophobic interface promotes gas diffusion as well as decelerates the electro-hydrogenation of N-source, which balances the kinetically matched electrochemical C-N coupling process. • Hydrophobic microenvironment impacts the kinetic matching during the C-N coupling. • Hydrophobicity influences proton/electron transfer processes for NO 3 RR and CO 2 diffusion for CO 2 RR. • The kinetics of CO 2 -to-*CO and NO 3 - -to-*NH 2 can thus be simultaneously tuned on the hydrophobic interface. • FE urea can be greatly improved from 8 % to 49 % by adding 40 % PTFE to the CuZn catalyst.","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"382 1","pages":"125939-125939"},"PeriodicalIF":0.0,"publicationDate":"2025-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147332320","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-08-28DOI: 10.1016/j.apcatb.2025.125896
Shaojian Jiang, Yuhang Liu, Ruidong Yang, Kai Deng, Ziqiang Wang, You Xu, Liang Wang, Hongjie Yu, Hongjing Wang
{"title":"Unveiling the role of lattice oxygen in promoting direct electrochemical propylene oxidation to propylene glycol","authors":"Shaojian Jiang, Yuhang Liu, Ruidong Yang, Kai Deng, Ziqiang Wang, You Xu, Liang Wang, Hongjie Yu, Hongjing Wang","doi":"10.1016/j.apcatb.2025.125896","DOIUrl":"https://doi.org/10.1016/j.apcatb.2025.125896","url":null,"abstract":"","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"381 1","pages":"125896-125896"},"PeriodicalIF":0.0,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147333966","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-08-25DOI: 10.1016/j.apcatb.2025.125891
Hongman Sun, Yuanyuan Wen, Yaqian Li, Rong Fan, Yonglian Lu, Chao Feng, Hao Liu, Youhe Wang, Zhipeng Ma, Yu Zhang, Rose Amal, Zifeng Yan
{"title":"Steering the reaction pathway of CO2 electroreduction and stabilizing Cu+ species by constructing the Cu2+/Cu+ valence state fluctuation buffer zone","authors":"Hongman Sun, Yuanyuan Wen, Yaqian Li, Rong Fan, Yonglian Lu, Chao Feng, Hao Liu, Youhe Wang, Zhipeng Ma, Yu Zhang, Rose Amal, Zifeng Yan","doi":"10.1016/j.apcatb.2025.125891","DOIUrl":"https://doi.org/10.1016/j.apcatb.2025.125891","url":null,"abstract":"","PeriodicalId":244,"journal":{"name":"Applied Catalysis B: Environmental","volume":"381 1","pages":"125891-125891"},"PeriodicalIF":0.0,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147333669","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
京公网安备 11010802042870号
京ICP备2023020795号-1
扫码关注我们
求助内容：
应助结果提醒方式：