ZIF-8 热解掺杂 N 的碳支撑铁催化剂,用于提高 CO2 加氢转化为有价值碳氢化合物的活性

IF 4.4 3区 化学 Q2 CHEMISTRY, PHYSICAL Catalysis Science & Technology Pub Date : 2024-09-16 DOI:10.1039/d4cy00810c
Chao Deng , Xu Wang , Xixi Chen , Ruxing Gao , Leiyu Zhang , Chundong Zhang , Ki-Won Jun , Seok Ki Kim , Hui Wan , Guofeng Guan
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摘要

掺杂 N 的碳(NC)材料支撑的铁催化剂已被广泛应用于二氧化碳加氢反应;然而,铁活性位点与 NC 支撑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-T,T = 950、1050 和 1150 °C)合成了一系列 ZIF-8 衍生的 N-掺杂碳支撑铁催化剂,保留了不同数量的 N 型和 C 型以及可调的表面 N-含量。掺杂 N 增加了活性相 Fe 周围的 CO2 吸附和电子密度,从而提高了反应过程中 CO2 的解离以及随后 CO 中间产物向碳氢化合物产物的转化。此外,催化剂表面含 N 的吡咯烷酮和石墨化碳介导的电子传递平衡也是催化性能增强的原因。XPS、拉曼光谱和 TPD 技术被用来验证这些变化。本研究的发现为优化 N 掺杂碳支撑铁催化剂在 CO2 加氢反应中的催化性能提供了启示和指导。
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ZIF-8 pyrolized N-doped carbon-supported iron catalysts for enhanced CO2 hydrogenation activity to valuable hydrocarbons†
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.
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来源期刊
Catalysis Science & Technology
Catalysis Science & Technology CHEMISTRY, PHYSICAL-
CiteScore
8.70
自引率
6.00%
发文量
587
审稿时长
1.5 months
期刊介绍: A multidisciplinary journal focusing on cutting edge research across all fundamental science and technological aspects of catalysis. Editor-in-chief: Bert Weckhuysen Impact factor: 5.0 Time to first decision (peer reviewed only): 31 days
期刊最新文献
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