High selectivity and abundant active sites in atomically dispersed TM2C12 monolayer for CO2 reduction

IF 7.2 2区 工程技术 Q1 CHEMISTRY, APPLIED
Shu-Long Li , Yu Song , Guo Tian , Qiaoling Liu , Liang Qiao , Yong Zhao , Li-Yong Gan
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Abstract

Developing highly efficient single-atom catalysts (SACs) for electrocatalytic carbon dioxide reduction reaction (CO2RR) is a promising approach to promoting carbon neutrality. However, challenges such as low activity, selectivity and high costs hinder industrial scaling, attributed to the lack of innate activity or insufficient transition metal (TM) active site density in current catalysts. Therefore, the focus of CO2RR research remains on developing SACs with intrinsic catalytic activity, high TM coverage and cost-effectiveness. This study presents the design of carbon-based materials with ultra-high TM coverage (TM2C12) (TM = Mo, Ru, Rh, W, Re, Os and Ir) as electrocatalyst SACs for CO2RR using density functional theory calculations. Among these materials, W2C12 (W represents tungsten) demonstrates superior selectivity and catalytic activity for CO2RR to carbon monoxide (CO) products with overpotentials of 0.45 V and a W coverage of up to 71.84 wt%. To further enhance its catalytic activity, non-metallic (NM) coordination modification (NM = B, N, O, P doping and C vacancy) was explored on W2C12. The results indicate that N-doped W2C12 (N-W2C12) can significantly improve selectivity and catalytic activity, achieving an extremely low overpotential of 0.34 V. This research offers valuable insights into designing SACs with high activity, selectivity and stability for CO2RR and other catalytic reactions.

Abstract Image

用于二氧化碳还原的原子分散 TM2C12 单层具有高选择性和丰富的活性位点
开发用于电催化二氧化碳还原反应(CO2RR)的高效单原子催化剂(SACs)是促进碳中和的一种可行方法。然而,由于目前的催化剂缺乏先天活性或过渡金属(TM)活性位点密度不足,低活性、选择性和高成本等挑战阻碍了工业规模的扩大。因此,CO2RR 研究的重点仍然是开发具有内在催化活性、高 TM 覆盖率和成本效益的 SAC。本研究利用密度泛函理论计算设计了具有超高 TM 覆盖率(TM2C12)(TM = Mo、Ru、Rh、W、Re、Os 和 Ir)的碳基材料,作为 CO2RR 的电催化剂 SAC。在这些材料中,W2C12(W 代表钨)在 CO2RR 到一氧化碳(CO)产物的过程中表现出卓越的选择性和催化活性,过电位为 0.45 V,W 覆盖率高达 71.84 wt%。为了进一步提高其催化活性,研究人员对 W2C12 进行了非金属(NM)配位修饰(NM = B、N、O、P 掺杂和 C 空位)。结果表明,掺杂 N 的 W2C12(N-W2C12)可显著提高选择性和催化活性,实现 0.34 V 的超低过电位。这项研究为设计具有高活性、高选择性和高稳定性的 SACs 用于 CO2RR 及其他催化反应提供了宝贵的见解。
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来源期刊
Fuel Processing Technology
Fuel Processing Technology 工程技术-工程:化工
CiteScore
13.20
自引率
9.30%
发文量
398
审稿时长
26 days
期刊介绍: Fuel Processing Technology (FPT) deals with the scientific and technological aspects of converting fossil and renewable resources to clean fuels, value-added chemicals, fuel-related advanced carbon materials and by-products. In addition to the traditional non-nuclear fossil fuels, biomass and wastes, papers on the integration of renewables such as solar and wind energy and energy storage into the fuel processing processes, as well as papers on the production and conversion of non-carbon-containing fuels such as hydrogen and ammonia, are also welcome. While chemical conversion is emphasized, papers on advanced physical conversion processes are also considered for publication in FPT. Papers on the fundamental aspects of fuel structure and properties will also be considered.
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