文献类型：期刊文献

英文题名：Syngas to Aromatics on Cu-Zn-Zr and HZSM-5: Modulating the Capability of Oxygenated Intermediate Formation to Improve Durene Selectivity

作者：Li, Shunshun[1];Wang, Zihao[1];He, Muqian[1];Xu, Yuanxiang[1];Wang, Xuguang[1];Liu, Dianhua[1]

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, Carbon Neutral Joint Lab East China Univ Sci Techn, Engn Res Ctr Large Scale Reactor Engn & Technol,Mi, Shanghai 200237, Peoples R China

年份：2025

卷号：64

期号：23

起止页码：11270

外文期刊名：INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH

收录：;EI(收录号：20252218529073);WOS:【SCI-EXPANDED(收录号:WOS:001498718600001)】；

基金：This work was supported by "the National Key Research and Development Program of China" (2024YFB4105404), "the National Natural Science Foundation of China" (22478108), "the Science and Technology Commission of Shanghai Municipality" (22dz1208400), and "the Fundamental Research Funds for the Central Universities" (JKCA1241105).

语种：英文

摘要：The maximum durene selectivity can be obtained by the cofeeding approach in the syngas to aromatics (STA) process. In this study, the capability of oxygenated intermediate formation was modulated via simple adjustment of Cu, Zn, and Zr molar ratios, maximizing the durene selectivity and CO conversion. The incorporation of the Zr element enhanced the adsorption for CO and the Zn element accelerated the depletion of active hydrogen from zeolites, which suppressed the excessive hydrogenation of intermediates to alkanes. Meanwhile, the synchronization between oxygenated intermediate formation and aromatization was accomplished through optimization of the active sites of zeolites, bifunctional catalyst coupling approaches, and process parameters. Under optimal conditions, a maximum durene space time yield (STY) of 232.0 mu mol/gCat/h at a CO conversion of 90.1% was achieved by CuZnZr642/HZSM-5. Furthermore, the deactivation mechanisms of bifunctional catalysts were primarily attributed to the thermal instability of Cu-based catalysts at high temperatures, wherein carbon deposition elimination of spent zeolites was achieved via calcination under an air atmosphere. This study offers experimental support and theoretical insight into optimizing the STA catalytic system.