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

IF 13.1 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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CO2加氢定向合成轻烯烃的高活性fec_2 - feco界面位的构建
将二氧化碳加氢转化为高价值的化学物质被视为解决未来能源危机的可行策略之一。轻质烯烃作为基础原料在工业上受到了广泛的关注。本文采用典型的溶胶-凝胶策略,构建了一系列Fe-Co双金属活性位点催化剂。Fe-Co双金属活性位催化剂的协同调控布局构建了高活性界面,具有高CO2转化率(56.9%)、低CO选择性(3.6%)、高轻烯烃选择性(40.5%)和显著的轻烯烃收率(22.2%)。相关表征分析结果表明,Fe-Co双金属活性位协同调控布局形成的高活性界面是轻质烯烃产率高的根本原因。引入钴形成的高活性界面推动RWGS反应正向进行(勒夏特列原理),进一步提高了CO2的转化率。此外,通过原位漂移光谱等表征手段,分析了Fe-Co双金属催化剂在反应过程中物理相结构、元素组成和价态、CO2和H2吸附能力以及轻质烯烃形成过程的动态演变,并进一步提出了CO2加氢对轻质烯烃具有高选择性的潜在机理。本研究为具有高活性界面的Fe-Co双金属协同调控布局提供了一种有效合理的设计策略,以促进定向合成轻烯烃中CO2的高效加氢。
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来源期刊
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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