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<p>CO<sub>2</sub> electroreduction (CO<sub>2</sub>RR) to multi-carbon products on Cu was found to occur via a two-site mode: one site is more active for CO<sub>2</sub>-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 CO<sub>2</sub>-to-CO site by a factor of 3 while reducing that of the CO reduction site. Poly-4-vinylpyridine-(P4VP)-modified Cu<sub>2</sub>O-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 260 mA cm<sup>-2</sup>. 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 CO<sub>2</sub> enrichment, increased hydrophilicity, and Cu surface charge redistribution in the presence of polyvinylpyridine. These findings demonstrate the potential to independently control CO<sub>2</sub> reduction at different active sites.</p>

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

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年11月20日

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  • Fan Zeng,
  • Xuan Wang,
  • Tianxiu Yin,
  • Jinglei Shen,
  • Binbin Pan,
  • Wenzhi Teng,
  • Tao Cheng,
  • Yuhang Wang

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 260 mA cm-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.