题目： | substituent tuning of cu coordination polymers enables carbon-efficient co2 electroreduction to multi-carbon products |
作者： | huiying deng1,2#, tingting liu2,3#, wenshan zhao4#, jundong wang1,2, yuesheng zhang1,2, shuzhen zhang5, yu yang5, chao yang6, wenzhi teng1,2, zhuo chen1,2, gengfeng zheng6, fengwang li 5, yaqiong su4*, jingshu hui 2,3* & yuhang wang 1,2* |
单位： | 1institute of functional nano & soft materials (funsom), soochow university, suzhou, jiangsu, china. 2jiangsu key laboratory for advanced negative carbon technologies, soochow university, suzhou, jiangsu, china. 3soochow institute for energy and materials innovations (siemis), college of energy, soochow university, suzhou, jiangsu, china. 4xi'an key laboratory of sustainable energy materials chemistry, school of chemistry, xi'an jiaotong university, xi'an, shanxi, china. 5school of chemical and biomolecular engineering and arc centre of excellence for green electrochemical transformation of carbon dioxide, the university of sydney, sydney, nsw, australia. 6laboratory of advanced materials, fudan university, shanghai, china. |
摘要： | co2 electroreduction is a potential pathway to achieve net-zero emissions in the chemical industry. yet, co2 loss, resulting from (bi)carbonate formation, renders the process energy-intensive. acidic environments can address the issue but at the expense of compromised product faradaic efficiencies (fes), particularly for multi-carbon (c2 ) products, as rapid diffusion and migration of protons (h) favors competing h2 and co production. here, we present a strategy of tuning the 2-position substituent length on benzimidazole (bim)-based copper (cu) coordination polymer (cucp) precatalyst – to enhance co2 reduction to c2 products in acidic environments. lengthening the substituent from h to nonyl enhances h diffusion retardation and decreases cu-cu coordination numbers (cns), favoring further reduction of co. this leads to a nearly 24× enhancement of selectivity towards co hydrogenation and c-c coupling at 60 ma cm−2. we report the highest c2 product fe of more than 70% at 260 ma cm−2 on pentyl-cucp and demonstrate a co2-to-c2 single-pass conversion (spc) of ~54% at 180 ma cm−2 using pentyl-cucp in zero-gap electrolyzers. |
影响因子： | 14.7 |
分区情况： | 一区 |
链接： | 责任编辑：杜欣 |
