Controlled C-C coupling of CO on borophene as a non-metallic catalyst: A DFT study on solvent water effects

IF 3.9 2区材料科学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY

Vacuum Pub Date : 2025-08-28 DOI:10.1016/j.vacuum.2025.114702

Pengfei Liu , Wanfei Hu , Xing Gao , Tiantian Liu , Junying Zhang

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引用次数: 0

Abstract

C-C controllable coupling is a key factor in the electrocatalytic reduction of CO₂ (CO₂RR) to C₂ compounds, but the influence of solvent water on C-C coupling in theoretical research lags far behind experiments. Herein, we systematically study the C-C coupling mechanism of CO generated OCCO on borophene surface through DFT, while considering the influence of solvent water. The results indicate that CO can be chemically adsorbed on borophene surface, followed by direct C-C coupling to form chemically adsorbed ∗OCCO. The activation energy barrier for ∗CO to form ∗OCCO on the surface of 2pmmn-borophene is the lowest, at 0.11 eV ∗OCCO can also be directly generated by C-C coupling of CO in both implicit and explicit solvent water models. The trend of energy barrier variation in implicit water models is consistent with that in vacuum environments. In the explicit water model, the activation energy barrier for ∗CO to generate ∗OCCO on the surface of α-borophene is the lowest, with an activation energy of 0.23 eV. The results indicate that the explicit solvent water is crucial in the electrocatalytic reduction of CO₂ in theoretical research. This study provides a new perspective for understanding the efficient C-C coupling of solvent effects in CO₂RR.

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非金属催化剂硼罗芬上CO的可控C-C偶联：溶剂水效应的DFT研究

C-C可控耦合是电催化还原CO2 （CO2RR）制C2化合物的关键因素，但理论研究中溶剂水对C-C耦合的影响远远落后于实验。本文在考虑溶剂水影响的情况下，通过DFT系统研究了CO生成的OCCO在硼罗芬表面的C-C耦合机理。结果表明，CO可以在硼苯表面进行化学吸附，然后通过C-C直接偶联形成化学吸附的OCCO。在隐式和显式溶剂水模型中，CO在2pmn -硼苯表面形成* OCCO的活化能垒最低，为0.11 eV * OCCO，也可由CO的C-C耦合直接产生。隐式水模型中能量势垒的变化趋势与真空环境中一致。在显式水模型中，α-硼苯表面上的* CO生成* OCCO的活化能垒最低，为0.23 eV。结果表明，在理论研究中，外显溶剂水是电催化还原CO2的关键。本研究为理解CO2RR中溶剂效应的高效C-C耦合提供了新的视角。

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来源期刊

Vacuum 工程技术-材料科学：综合

CiteScore

6.80

自引率

17.50%

发文量

审稿时长

34 days

期刊介绍： Vacuum is an international rapid publications journal with a focus on short communication. All papers are peer-reviewed, with the review process for short communication geared towards very fast turnaround times. The journal also published full research papers, thematic issues and selected papers from leading conferences. A report in Vacuum should represent a major advance in an area that involves a controlled environment at pressures of one atmosphere or below. The scope of the journal includes: 1. Vacuum; original developments in vacuum pumping and instrumentation, vacuum measurement, vacuum gas dynamics, gas-surface interactions, surface treatment for UHV applications and low outgassing, vacuum melting, sintering, and vacuum metrology. Technology and solutions for large-scale facilities (e.g., particle accelerators and fusion devices). New instrumentation ( e.g., detectors and electron microscopes). 2. Plasma science; advances in PVD, CVD, plasma-assisted CVD, ion sources, deposition processes and analysis. 3. Surface science; surface engineering, surface chemistry, surface analysis, crystal growth, ion-surface interactions and etching, nanometer-scale processing, surface modification. 4. Materials science; novel functional or structural materials. Metals, ceramics, and polymers. Experiments, simulations, and modelling for understanding structure-property relationships. Thin films and coatings. Nanostructures and ion implantation.