Unveiling the role of N species in Co/NC catalysts for photothermal CO2 hydrogenation

IF 3.9 2区 化学 Q2 CHEMISTRY, PHYSICAL Molecular Catalysis Pub Date : 2024-11-14 DOI:10.1016/j.mcat.2024.114686
Pengcheng Wang , Qingqing Jiang , XingYu Li, Xuedong Wang, Juncheng Hu
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Abstract

Generally, researchers focus on the regulation of metal sites rather than surrounding nonmetals in photothermal CO2 hydrogenation reaction. Herein, concerning the role of non-metallic N species, a series of Co/NC-T catalysts have been fabricated via high-temperature pyrolysis of Zeolitic Imidazolate Frameworks-67. The CO2 conversion rate shows a consistent tendency with the ratio of graphitized-N species while the product selectivity is closely related to the coordination state of Co-Nx species. Co/NC-800 catalyst achieves high CO2 conversion rate of 758 mmol gcat-1 h-1 with CH4 selectivity of 99.6 %. After adding extra graphitized-N species, the CO2 conversion rate could further enhance to 80.2 % for N-Co/NC-2. The role of N species in photothermal CO2 hydrogenation reaction has been investigated in details, providing new insights for the design of metal organic frameworks derived metal/N-doped carbon catalysts.

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揭示用于二氧化碳光热加氢的 Co/NC 催化剂中 N 物种的作用
一般来说,研究人员关注的是光热二氧化碳加氢反应中金属位点的调控,而不是周围非金属的调控。本文针对非金属 N 物种的作用,通过高温热解沸石咪唑啉框架-67 制备了一系列 Co/NC-T 催化剂。二氧化碳转化率与石墨化 N 物种的比例呈一致趋势,而产物选择性则与 Co-Nx 物种的配位状态密切相关。Co/NC-800 催化剂的 CO2 转化率高达 758 mmol gcat-1 h-1,CH4 选择性为 99.6%。添加额外的石墨化 N 物种后,N-Co/NC-2 的 CO2 转化率进一步提高到 80.2%。详细研究了 N 物种在光热 CO2 加氢反应中的作用,为设计金属有机框架衍生的金属/N 掺杂碳催化剂提供了新的见解。
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来源期刊
Molecular Catalysis
Molecular Catalysis Chemical Engineering-Process Chemistry and Technology
CiteScore
6.90
自引率
10.90%
发文量
700
审稿时长
40 days
期刊介绍: Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are: Heterogeneous catalysis including immobilized molecular catalysts Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis Photo- and electrochemistry Theoretical aspects of catalysis analyzed by computational methods
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