Construction of Highly Active Fe5C2–FeCo Interfacial Sites for Oriented Synthesis of Light Olefins from CO2 Hydrogenation

IF 11.3 1区 化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2025-01-03 DOI:10.1021/acscatal.4c06001
Teng Li, Heng Zhao, Lisheng Guo, Guangbo Liu, Jinhu Wu, Tao Xing, Tao Li, Qiang Liu, Jiancai Sui, Yitong Han, Jiaming Liang, Yingluo He, Noritatsu Tsubaki
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Abstract

The hydrogenation of CO2 into high-value chemistry is seen as one of the viable strategies for solving the energy crisis of the future. Light olefins have attracted considerable attention as basic feedstocks in the industry. In this work, a series of Fe–Co bimetallic active site catalysts were constructed by a typical sol–gel strategy. The synergistic regulation layout of the Fe–Co bimetallic active site catalyst constructed highly active interfaces and exhibited high conversion (56.9%) of CO2, low CO selectivity (3.6%), high selectivity (40.5%) of light olefins, and remarkable light olefins yield (22.2%). The results of the associated characterization analysis indicate that the high activity interfaces formed by the synergistic regulation layout of the Fe–Co bimetallic active sites are the fundamental reason for the high yield of light olefins. The high activity interfaces formed by the introduction of cobalt drive the RWGS reaction forward (Le Chatelier’s Principle), which further enhances the CO2 conversion. In addition, the dynamic evolution of the physical phase structure, elemental composition and valence, CO2 and H2 adsorption ability, and the formation process of light olefins during the reaction of Fe–Co bimetallic catalysts were analyzed by in situ DRIFT spectra and other characterizations, and a potential mechanism for the high selectivity of CO2 hydrogenation to light olefins is further proposed. This work provides an effective and rational design strategy for the synergistic regulation layout of Fe–Co bimetals with highly active interfaces to promote efficient hydrogenation of CO2 for the oriented synthesis of light olefins.

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ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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