{"title":"在强酸性介质中,在800毫安厘米- 2下电还原稀释的二氧化碳到高碳利用率的多碳产品","authors":"Xue-Rong Qin, Jing-Jing Li, Lin-Lin Wang, Huan Liu, Zuo-Tao Yang, Guo-Jin Feng, Xiao-Ran Wang, Xuan-Xuan Cheng, Chao Zhang, Zi-You Yu, Tong-Bu Lu","doi":"10.1038/s41467-025-59783-2","DOIUrl":null,"url":null,"abstract":"<p>Acidic CO<sub>2</sub> electroreduction using diluted CO<sub>2</sub> (as in flue gas) as the feedstock can simultaneously circumvent the CO<sub>2</sub> purification step and lower the carbon loss in conventional alkaline or neutral electrolyte, and thus is highly desired but has rarely been achieved thus far. Herein, we report a simple and general strategy using an imidazolium-based anion-exchange ionomer as the coating layer, which could enrich the diluted CO<sub>2</sub> to generate a high local CO<sub>2</sub> concentration, and simultaneously block the proton transport to the cathode surface to suppress the competing hydrogen evolution reaction. As a result, the ionomer-modified Cu catalyst can achieve an efficient electroreduction of diluted CO<sub>2</sub> (15 vol% CO<sub>2</sub>) to multicarbon (C<sub>2+</sub>) products in strong acid (pH 0.8), with a high C<sub>2+</sub> Faradaic efficiency of 70.5% and a high single-pass carbon efficiency of 73.6% at a current density of 800 mA cm<sup>–2</sup>, competitive with that obtained with pure CO<sub>2</sub>. These findings provide opportunity for the direct electrochemical conversion of flue gas into valuable products with high efficiency.</p>","PeriodicalId":19066,"journal":{"name":"Nature Communications","volume":"817 1","pages":"4447"},"PeriodicalIF":14.7000,"publicationDate":"2025-05-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Electroreduction of diluted CO2 to multicarbon products with high carbon utilization at 800 mA cm–2 in strongly acidic media\",\"authors\":\"Xue-Rong Qin, Jing-Jing Li, Lin-Lin Wang, Huan Liu, Zuo-Tao Yang, Guo-Jin Feng, Xiao-Ran Wang, Xuan-Xuan Cheng, Chao Zhang, Zi-You Yu, Tong-Bu Lu\",\"doi\":\"10.1038/s41467-025-59783-2\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Acidic CO<sub>2</sub> electroreduction using diluted CO<sub>2</sub> (as in flue gas) as the feedstock can simultaneously circumvent the CO<sub>2</sub> purification step and lower the carbon loss in conventional alkaline or neutral electrolyte, and thus is highly desired but has rarely been achieved thus far. Herein, we report a simple and general strategy using an imidazolium-based anion-exchange ionomer as the coating layer, which could enrich the diluted CO<sub>2</sub> to generate a high local CO<sub>2</sub> concentration, and simultaneously block the proton transport to the cathode surface to suppress the competing hydrogen evolution reaction. As a result, the ionomer-modified Cu catalyst can achieve an efficient electroreduction of diluted CO<sub>2</sub> (15 vol% CO<sub>2</sub>) to multicarbon (C<sub>2+</sub>) products in strong acid (pH 0.8), with a high C<sub>2+</sub> Faradaic efficiency of 70.5% and a high single-pass carbon efficiency of 73.6% at a current density of 800 mA cm<sup>–2</sup>, competitive with that obtained with pure CO<sub>2</sub>. These findings provide opportunity for the direct electrochemical conversion of flue gas into valuable products with high efficiency.</p>\",\"PeriodicalId\":19066,\"journal\":{\"name\":\"Nature Communications\",\"volume\":\"817 1\",\"pages\":\"4447\"},\"PeriodicalIF\":14.7000,\"publicationDate\":\"2025-05-13\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nature Communications\",\"FirstCategoryId\":\"103\",\"ListUrlMain\":\"https://doi.org/10.1038/s41467-025-59783-2\",\"RegionNum\":1,\"RegionCategory\":\"综合性期刊\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MULTIDISCIPLINARY SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Communications","FirstCategoryId":"103","ListUrlMain":"https://doi.org/10.1038/s41467-025-59783-2","RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}
引用次数: 0
摘要
使用稀释的二氧化碳(如在烟气中)作为原料的酸性二氧化碳电还原可以同时绕过二氧化碳净化步骤并降低传统碱性或中性电解质中的碳损失,因此非常需要,但迄今为止很少实现。本文采用咪唑基阴离子交换离聚体作为包覆层,可以富集稀释后的CO2,从而产生较高的局部CO2浓度,同时阻断质子向阴极表面的输移,抑制竞争性析氢反应。结果表明,离子聚体修饰的Cu催化剂在强酸(pH = 0.8)条件下,可将稀释后的CO2 (15 vol% CO2)高效电还原为多碳(C2+)产物,在电流密度为800 mA cm-2时,C2+的法拉第效率高达70.5%,单次碳效率高达73.6%,可与纯CO2相竞争。这些发现为直接电化学将烟气高效转化为有价值的产品提供了机会。
Electroreduction of diluted CO2 to multicarbon products with high carbon utilization at 800 mA cm–2 in strongly acidic media
Acidic CO2 electroreduction using diluted CO2 (as in flue gas) as the feedstock can simultaneously circumvent the CO2 purification step and lower the carbon loss in conventional alkaline or neutral electrolyte, and thus is highly desired but has rarely been achieved thus far. Herein, we report a simple and general strategy using an imidazolium-based anion-exchange ionomer as the coating layer, which could enrich the diluted CO2 to generate a high local CO2 concentration, and simultaneously block the proton transport to the cathode surface to suppress the competing hydrogen evolution reaction. As a result, the ionomer-modified Cu catalyst can achieve an efficient electroreduction of diluted CO2 (15 vol% CO2) to multicarbon (C2+) products in strong acid (pH 0.8), with a high C2+ Faradaic efficiency of 70.5% and a high single-pass carbon efficiency of 73.6% at a current density of 800 mA cm–2, competitive with that obtained with pure CO2. These findings provide opportunity for the direct electrochemical conversion of flue gas into valuable products with high efficiency.
期刊介绍:
Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.