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ZIF-8 pyrolized N-doped carbon-supported iron catalysts for enhanced CO2 hydrogenation activity to valuable hydrocarbons
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2024-07-31 , DOI: 10.1039/d4cy00810c
Chao Deng 1 , Xu Wang 1 , Xixi Chen 1 , Ruxing Gao 2 , Leiyu Zhang 1 , Chundong Zhang 1 , Ki-Won Jun 3, 4 , Seok Ki Kim 5 , Hui Wan 1 , Guofeng Guan 1, 6
Affiliation  

N-doped carbon (NC) material-supported Fe catalysts have been widely used in CO2 hydrogenation reactions; however, the interaction between iron active sites and NC supports is still unclear. Herein, we synthesized a series of ZIF-8-derived N-doped carbon-supported iron catalysts via varied pyrolysis temperatures (Fe/NC-T, T = 950, 1050 and 1150 °C), preserving different amounts of N-type and C-type and tunable surface N-content. N-doping increases the adsorption of CO2 and the electron density around the active phase Fe, thereby enhancing the dissociation of CO2 during the reaction and the subsequent conversion of the CO intermediate to the hydrocarbon product. Besides, the balance of surface N-containing pyrrolic and graphitized carbon-mediated electron transfer on the catalyst surface was responsible for the enhanced catalytic performances. XPS, Raman spectroscopy, and TPD techniques were used to verify these alterations. The findings of this study provide insights and guidance for optimizing the catalytic performance of N-doped carbon-supported Fe catalysts in CO2 hydrogenation reactions.

中文翻译:


ZIF-8 热解氮掺杂碳载铁催化剂,用于增强 CO2 加氢生成有价值碳氢化合物的活性



氮掺杂碳(NC)材料负载的Fe催化剂已广泛应用于CO 2加氢反应中;然而,铁活性位点和NC支持物之间的相互作用仍不清楚。在此,我们通过不同的热解温度(Fe/NC- TT = 950、1050 和 1150 °C)合成了一系列 ZIF-8 衍生的 N 掺杂碳载铁催化剂,保留了不同量的 N 型和C型和可调表面氮含量。 N掺杂增加了CO 2的吸附和活性相Fe周围的电子密度,从而增强了反应期间CO 2的解离以及随后CO中间体向烃产物的转化。此外,催化剂表面表面含氮吡咯和石墨化碳介导的电子转移的平衡是催化性能增强的原因。 XPS、拉曼光谱和 TPD 技术用于验证这些改变。本研究的结果为优化氮掺杂碳载铁催化剂在CO 2加氢反应中的催化性能提供了见解和指导。
更新日期:2024-07-31
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