质子调谐表面化学促进酸性CO2电还原中多碳的形成。

IF 4.6 2区化学 Q2 CHEMISTRY, PHYSICAL

The Journal of Physical Chemistry Letters Pub Date : 2025-10-02 DOI:10.1021/acs.jpclett.5c02529

Qingqing Song,Feng Li,Aoni Xu,Chenchen Zhang,Yuanming Xie,Junjun Mao,Ying Zhang,Yong Zhao

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引用次数: 0

摘要

在强酸性介质中，二氧化碳电还原成多碳（C2+）产物是一种很有前途的方法，可以减轻在碱性和中性电解质中观察到的碳损失。然而，在节能电流密度下实现高C2+选择性仍然具有挑战性，因为有竞争的单碳（C1）产物生成。在这里，我们报告了在中等电流密度下，质子可用性促进酸性CO2电还原中C2+的产生。我们发现，通过将质子浓度从pH 2提高到pH 1，可以显著提高C2+的产量──C2+的法拉第效率从23.9±2.7%提高到48.1±0.6%，C2+/C1比值从0.4提高到1.6。我们的原位拉曼光谱和模拟研究表明，较高的质子浓度增加了铜表面的*CO覆盖率，有利于铜表面的低频*CO结合构型，从而促进C-C耦合，促进C2+产物的形成。

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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Proton-Tuned Surface Chemistry Promotes Multicarbon Formation in Acidic CO2 Electroreduction.

Carbon dioxide electroreduction to multicarbon (C2+) products in strongly acidic media offers a promising approach to mitigate carbon loss observed in alkaline and neutral electrolytes. However, achieving high C2+ selectivity at energy-efficient current densities remains challenging due to competing one-carbon (C1) product generation. Here, we report a proton-availability-promoted C2+ production in acidic CO2 electroreduction within a moderate current density regime. We demonstrated a remarkably enhanced C2+ production─C2+ faradaic efficiency increasing from 23.9 ± 2.7% to 48.1 ± 0.6% and C2+/C1 ratio from 0.4 to 1.6─by increasing the proton concentration from pH 2 to pH 1 in the bulk acidic electrolyte. Our in situ Raman spectroscopy and simulation studies revealed that higher proton concentration enhances *CO coverage and favors a low-frequency *CO binding configuration on copper surface, thereby facilitating C-C coupling and promoting C2+ product formation.

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来源期刊

The Journal of Physical Chemistry Letters CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY

CiteScore

9.60

自引率

7.00%

发文量

1519

审稿时长

1.6 months

期刊介绍： The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.