Acetylene hydrochlorination to vinyl chloride monomer on Au(I) centers stabilized by pyrrole N in active carbon

IF 6.5 1区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2025-02-01 Epub Date: 2024-12-22 DOI:10.1016/j.jcat.2024.115918
Fujun Ren , Jianian Cheng , Junqi Tian , Xiaojing Wu , Ruihui Zhang , Xingxing Zhou , Zelong Li , Can Li
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Abstract

The urgent need to replace the toxic mercuric chloride (HgCl2/AC) catalyst used in current industry for the production of vinyl chloride monomer (VCM) through acetylene hydrochlorination has been a great challenge. Although Au catalyst has been regarded as a potential catalyst for the reaction, it is unstable under reaction conditions. In this work, we report that atomically dispersed Au+ atoms supported on nitrogen doped carbon (Au/NC) can show high performance in the production of VCM. This catalyst achieves a C2H2 conversion of 94.2% and a VCM selectivity of 99.9%, superior to Au catalyst supported on active carbon (Au/AC) without nitrogen doping. These active centers were identified to be the Au+ active centers, and the enhanced performance of the Au/NC catalyst is attributed to the presence of pyrrole nitrogen species, which strongly coordinate to the Au+ active centers promoting the adsorption and activation of C2H2. This research offers a promising way to stabilize the Au+ active centers and enhances the catalytic performance.

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乙炔在活性炭中以吡咯N稳定的Au(I)中心上加氢氯化制氯乙烯单体
用乙炔加氢氯化法生产氯乙烯单体(VCM),迫切需要取代目前工业上使用的有毒的氯化汞(HgCl2/AC)催化剂,这是一个巨大的挑战。虽然金催化剂一直被认为是反应的潜在催化剂,但在反应条件下,金催化剂是不稳定的。在这项工作中,我们报道了原子分散的Au+原子负载在氮掺杂碳(Au/NC)上,可以在氯乙烯单体的生产中表现出高性能。该催化剂的C2H2转化率为94.2 %,VCM选择性为99.9 %,优于未掺杂氮的Au/AC催化剂。这些活性中心被鉴定为Au+活性中心,Au/NC催化剂性能的增强归因于吡咯氮的存在,吡咯氮与Au+活性中心强配合,促进了C2H2的吸附和活化。该研究为稳定Au+活性中心和提高催化性能提供了一条有希望的途径。
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来源期刊
Journal of Catalysis
Journal of Catalysis 工程技术-工程:化工
CiteScore
12.30
自引率
5.50%
发文量
447
审稿时长
31 days
期刊介绍: The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.
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