zr基金属有机骨架集成双核铜簇选择性电还原CO2制CH4

IF 13.3 1区工程技术 Q1 ENGINEERING, CHEMICAL

Chemical Engineering Journal Pub Date : 2025-01-23 DOI:10.1016/j.cej.2025.159858

Xuejing Zhai, Shanshan Liu, Luyang Zuo, Qi Liu, Bo Li, Liya Wang

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引用次数: 0

摘要

电催化二氧化碳还原（ECO2RR）技术对于实现碳调峰、实现碳中和、缓解能源和环境危机具有重要意义。在ECO2RR中实现甲烷（CH4）的高选择性仍然是一个巨大的挑战，因为可能的产物具有相似的还原潜力和缓慢的二氧化碳（CO2）活化动力学。铜及其氧化物是目前最有效的电催化剂之一。本研究通过对zr基金属有机骨架（MOF） NU-1000的合成后修饰（PSM）得到NU-1000- cu，不仅提高了NU-1000的稳定性，而且提高了其电催化性能。在酸性电解液中，CO2可还原为CH4，法拉第效率（FE）为82.4 %，局部电流密度为21.4 mA cm−2。此外，通过密度泛函理论（DFT）计算进一步研究了催化机理，揭示了铜活性位点在促进CO2还原为CH4中的关键作用。

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Selective electroreduction of CO2 to CH4 by Zr-based metal–organic framework integrated binuclear copper cluster

Electrocatalytic carbon dioxide reduction (ECO₂RR) technology is of great significance for achieving carbon peaking, carbon neutralization, and alleviating energy and environmental crises. Achieving high selectivity of methane (CH₄) in ECO₂RR is still a huge challenge, because the possible products have similar reduction potential and slow carbon dioxide (CO₂) activation kinetics. Cu and its oxides are one of the most effective electrocatalysts at present. In this study, NU-1000-Cu was obtained by post-synthetic modification (PSM) of Zr-based metal–organic framework (MOF), NU-1000, which not only improved the stability of NU-1000, but also improved its electrocatalytic performance. CO₂ can be reduced to CH₄ in an acidic electrolyte with a Faraday efficiency (FE) of 82.4 % and a local current density of 21.4 mA cm⁻². In addition, the catalytic mechanism was further studied by density functional theory (DFT) calculation to reveal the key role of copper active sites in promoting the reduction of CO₂ to CH₄.

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来源期刊

Chemical Engineering Journal 工程技术-工程：化工

CiteScore

21.70

自引率

9.30%

发文量

6781

审稿时长

2.4 months

期刊介绍： The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.