Switching CO2 electroreduction selectivity between CO and HCOOH on poly(ionic liquid)-Ag hybrids

IF 5.1 3区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nanoscale Pub Date : 2025-10-09 DOI:10.1039/d5nr03602j

Ang Li, Guo-Yi Duan, Yue Pan, Xiao-Qiang Li, Ruo-Lan Li, Jian Fang, Yongmei Chen, Bao-Hua Xu

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引用次数: 0

Abstract

The electrocatalytic conversion of CO2 into CO and HCOOH is highly attractive due to its potential high energy efficiency. In this study, the selectivity switching from CO to HCOOH on Ag sites was achieved by finely fabricating poly(ionic liquid)-silver (PIL-Ag) hybrids containing alkyl chains. The length of the alkyl chain influenced the structure of Ag sites with different intrinsic activity of *COOH and *H (and thereby *OCHO) formation, as well as the mass transfer behavior of CO2 and H2O. During acidic CO2RR at –300 mA cm–2, Ag@PIL-C(4)-0.5 demonstrated a high Faradaic efficiency ratio of HCOOH to CO (FEHCOOH/FECO = 1.45), while Ag@PIL-C(6)-0.5 favored the production of CO. By contrast, Ag@PIL-C(12)-0.5, which possessed low activities and poor mass transfer, exhibited a high apparent FEHCOOH/FECO ratio of 1.35. Experiment combined mechanism studies demonstrated that the higher enrichment of *H versus *CO2 intermediates at the Ag sites is beneficial for *OCHO formation. In light of this point, the FEHCOOH/FECO ratio increased from 0.15 to 0.87 with a low FEH2 (<5.0%) on Ag@PIL-C(6)-2.0, which has high activity and good mass transfer of CO2, by increasing the current density from –100 mA cm–2 to –600 mA cm–2.

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切换CO和HCOOH在多离子液体-银杂化物上的CO2电还原选择性

电催化将CO2转化为CO和HCOOH因其潜在的高能效而具有很高的吸引力。在本研究中，通过精细制备含有烷基链的聚离子液体-银（PIL-Ag）杂化物，实现了Ag位点上CO到HCOOH的选择性转换。烷基链的长度影响了*COOH和*H（从而形成*OCHO）本征活性不同的Ag位的结构，以及CO2和H2O的传质行为。在-300 mA cm-2的酸性CO2RR条件下，Ag@PIL-C(4)-0.5表现出较高的HCOOH/FECO法拉第效率（FEHCOOH/FECO = 1.45），而Ag@PIL-C(6)-0.5有利于CO的生成。相比之下，Ag@PIL-C(12)-0.5具有较低的活性和较差的传质，其FEHCOOH/FECO的表观比为1.35。实验结合机理研究表明，相对于*CO2中间体，*H在Ag位点的富集更有利于*OCHO的形成。考虑到这一点，通过将电流密度从-100 mA cm-2提高到-600 mA cm-2，在Ag@PIL-C(6)-2.0的低FEH2 （<5.0%）条件下，FEHCOOH/FECO比值从0.15提高到0.87，具有高活性和良好的CO2传质性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nanoscale CHEMISTRY, MULTIDISCIPLINARY-NANOSCIENCE & NANOTECHNOLOGY

CiteScore

12.10

自引率

3.00%

发文量

1628

审稿时长

1.6 months

期刊介绍： Nanoscale is a high-impact international journal, publishing high-quality research across nanoscience and nanotechnology. Nanoscale publishes a full mix of research articles on experimental and theoretical work, including reviews, communications, and full papers.Highly interdisciplinary, this journal appeals to scientists, researchers and professionals interested in nanoscience and nanotechnology, quantum materials and quantum technology, including the areas of physics, chemistry, biology, medicine, materials, energy/environment, information technology, detection science, healthcare and drug discovery, and electronics.