{"title":"CNTs Coordination-Embedded into Copper–Pyrazole MOFs for Selective Electrocatalytic CO2 to C2H4","authors":"Zi Wan, Yunxin Dai, Jiajun Ma, Yunxia Zhao","doi":"10.1007/s10562-025-05008-6","DOIUrl":null,"url":null,"abstract":"<div><p>Selective electrolytic CO<sub>2</sub> to C<sub>2</sub>H<sub>4</sub> is a meaningful pathway to alleviate both energy and environmental concerns. Copper–pyrazole MOFs (CuPz) has emerged as a highly promising and ideal catalytic material for C<sub>2</sub>H<sub>4</sub> production from electrocatalytic CO<sub>2</sub> reduction. Here, short carbon nanotubes (CNTs) or functionalized CNTs were in situ embedded into CuPz to enhance its electrical conductivity and to regulate the direct coordination microenvironment of the Cu active center. Following a pre-reduction at − 1.3 V vs. reversible hydrogen electrode (RHE), a further increase in low-valent Cu was observed on the surface of CuPz, particularly in the case of CuPz@FCNT-A, with Cu<sup>+</sup> accounting for over 50%. This resulted in the highest C<sub>2</sub>H<sub>4</sub> selectivity (55.3% FE<sub>C2H4</sub>) at − 1.1 V vs. RHE and excellent stability. The embedding of short CNTs or functionalized CNTs exposed more active sites, and, at the same time, enhanced the catalysts’ electron transfer ability. Notably, functionalized CNTs exhibited a more pronounced positive impact than pristine CNTs. The reaction mechanism responsible for C<sub>2</sub>H<sub>4</sub> production was elucidated through in situ attenuated total reflection-fourier transform infrared spectroscopy (ATR-FTIR) analysis, which revealed that *CO dimerization was the primary pathway and *CO–*COH coupling was the secondary one.</p><h3>Graphical Abstract</h3><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"155 5","pages":""},"PeriodicalIF":2.3000,"publicationDate":"2025-04-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysis Letters","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s10562-025-05008-6","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Selective electrolytic CO2 to C2H4 is a meaningful pathway to alleviate both energy and environmental concerns. Copper–pyrazole MOFs (CuPz) has emerged as a highly promising and ideal catalytic material for C2H4 production from electrocatalytic CO2 reduction. Here, short carbon nanotubes (CNTs) or functionalized CNTs were in situ embedded into CuPz to enhance its electrical conductivity and to regulate the direct coordination microenvironment of the Cu active center. Following a pre-reduction at − 1.3 V vs. reversible hydrogen electrode (RHE), a further increase in low-valent Cu was observed on the surface of CuPz, particularly in the case of CuPz@FCNT-A, with Cu+ accounting for over 50%. This resulted in the highest C2H4 selectivity (55.3% FEC2H4) at − 1.1 V vs. RHE and excellent stability. The embedding of short CNTs or functionalized CNTs exposed more active sites, and, at the same time, enhanced the catalysts’ electron transfer ability. Notably, functionalized CNTs exhibited a more pronounced positive impact than pristine CNTs. The reaction mechanism responsible for C2H4 production was elucidated through in situ attenuated total reflection-fourier transform infrared spectroscopy (ATR-FTIR) analysis, which revealed that *CO dimerization was the primary pathway and *CO–*COH coupling was the secondary one.
期刊介绍:
Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis.
The high-quality original research articles published in Catalysis Letters are subject to rigorous peer review. Accepted papers are published online first and subsequently in print issues. All contributions must include a graphical abstract. Manuscripts should be written in English and the responsibility lies with the authors to ensure that they are grammatically and linguistically correct. Authors for whom English is not the working language are encouraged to consider using a professional language-editing service before submitting their manuscripts.