王昱沆教授与程涛教授合作在Nat. Commun.上发表论文

发布时间:2025-12-03访问量:10设置


题目:

Polymer-tethered pyridine tunes activities of the two distinct CO2 electroreduction sites on Cu

作者:

Fan Zeng1,2#, Xuan Wang1,2#, Tianxiu Yin1,2#, Jinglei Shen1,2, Binbin Pan1,2, Wenzhi Teng1,2, Tao Cheng,1,2*, Yuhang Wang1,2*

单位:

1State Key Laboratory of Bioinspired Interfacial Materials Science, Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou 215123, China

2Jiangsu Key Laboratory for Advanced Negative Carbon Technologies, Soochow University,199 Ren’ai Road, Suzhou, Jiangsu, 215123, China

摘要:

CO2 electroreduction (CO2RR) to multi-carbon products on Cu was found to occur via a two-site mode: one site is more active for CO2-to-CO conversion, and the other is primarily responsible for CO reduction. However, it remains unclear whether the activities of these two sites can be modulated independently. Here, we show that polyvinylpyridine, a pyridine-functionalized polymer, preferentially enhances the activity toward multi-carbon products at the CO2-to-CO site by a factor of 3 while reducing that of the CO reduction site. Poly-4-vinylpyridine-(P4VP)-modified Cu2O-derived Cu (OD-Cu) increases the multi-carbon product Faradaic efficiency by a factor of 1.3 to 3 across a current density range of 60 to 260mAcm-2. Moreover, the CO reduction reaction (CORR) activity decreases by up to 40% in the same range when P4VP is introduced. Isotopic labeling, in-situ Raman spectroscopy, contact angle tests, and theoretical calculations reveal that this phenomenon arises from CO2 enrichment, increased hydrophilicity, and Cu surface charge redistribution in the presence of polyvinylpyridine. These findings demonstrate the potential to independently control CO2 reduction at different active sites.

影响因子:

15.7

分区情况:

一区

链接:

https://doi.org/10.1038/s41467-025-66673-0



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