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MOF-assisted Synthesis of Dual-atom Palladium Catalysts for acetylene semi-hydrogenation

China Petroleum Processing & Petrochemical Technology 2024年第3期26卷 42-52页

作者： Chen Jie Xu Yuebing Qi Jian Liu Bing Liu Xiaohao Department of Chemical Engineering School of Chemical and Material EngineeringJiangnan UniversityWuxi 214122China State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China

The selective removal of trace acetylene in ethylene feed gas is of great significance in the petrochemicalindustry;however, there are still challenges in designing and developing high-performance catalysts. Here, a MOFassistedencapsulation strategy was adopted for the precise synthesis of diatomic Pd2 sites on a ZnO support. When usedfor the acetylene semi-hydrogenation reaction, the dual-atom Pd2-ZnO catalyst exhibited improved catalytic performance,achieving complete conversion of acetylene at 125 °C with an 89% selectivity to ethene, as compared to Pd single-atom andnanoparticles. This enhancement was mainly attributed to the catalyst’s ability to dissociate H2 and facilitate the desorptionof intermediate C2H4. Moreover, the strong interaction between the support and the diatomic Pd sites was responsible for thecatalyst’s excellent stability during the long-term reaction.

关键词： dual-atom palladium acetylene semi-hydrogenation MOFs hydrogen dissociation intermediate

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Pd/ZnO catalysts with different origins for high chemoselectivity in acetylene semi-hydrogenation

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Chinese Journal of Catalysis 2016年第5期37卷 692-699页

作者：周慧然杨小峰王爱琴苗澍刘晓艳潘晓丽苏杨李林谭媛张涛中国科学院大连化学物理研究所催化基础国家重点实验室能源材料化学协同创新中心辽宁大连116023 中国科学院大学北京100049

The heterogeneity of active sites is the main obstacle for selectivity control in heterogeneous *** atom catalysts（SACs） with homogeneous isolated active sites are highly desired in chemoselective transformations. In this work, a Pd1/ZnO catalyst with single‐atom dispersion of Pd active sites was achieved by decreasing the Pd loading and reducing the sample at a relatively low temperature. The Pd1/ZnO SAC exhibited excellent catalytic performance in the chemoselective hydrogenation of acetylene with comparable chemoselectivity to that of PdZn intermetallic catalysts and a greatly enhanced utilization of Pd metal. Such unusual behaviors of the Pd1/ZnO SAC in acetylene semi‐hydrogenation were ascribed to the high‐valent single Pd active sites, which could promote electrostatic interactions with acetylene but restrain undesired ethylene hydrogenation via the spatial restrictions of σ‐chemical bonding toward ethylene.

关键词： Single atom catalyst acetylene semi-hydrogenation Chemoselectivity Palladium Zinc oxide

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Structural and Kinetics Understanding of Support Effects in Pd-Catalyzed semi-hydrogenation of acetylene

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Engineering 2021年第1期7卷 103-110页

作者： Yueqiang Cao Xiaohu Ge Yurou Li Rui Si Zhijun Sui Jinghong Zhou Xuezhi Duan Xinggui Zhou State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China Shanghai Synchrotron Radiation Facility Shanghai Institute of Applied PhysicsChinese Academy of SciencesShanghai 201800China

In this study,the support effects on the Pd-catalyzed semi-hydrogenation of acetylene have been investigated from the structural and kinetic *** to the results of kinetic analysis and X-ray photoelectron spectroscopy,hydrogen temperature-programmed reduction,temperature-programmed hydride decomposition,and in situ X-ray diffraction measurements,using carbon nanotubes as support for Pd nanocatalysts with various sizes instead of a-Al_(2)O_(3) decreases the Pd^(0)3d binding energy and suppresses the formation of undesirable palladium hydride species,thus increasing the ethylene ***,X-ray absorption spectroscopy,high-resolution transmission electron microscopy,and C_(2)H_(4) temperature-programmed desorption studies combined with density-functional theory calculations reveal the existence of a unique Pd local environment,containing subsurface carbon atoms,that produces positive geometric effects on the acetylene conversion ***,tailoring the Pd local environment and electronic properties represents an effective strategy for the fabrication and design of highly active and selective Pd semi-hydrogenation catalysts.

关键词： acetylene semi-hydrogenation Reaction kinetics Support effects Electronic effects Pd local environment

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Graphdiyne anchoring to construct highly dense palladium trimer active sites for the selective hydrogenation of acetylene

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Nano Research 2023年第5期16卷 6167-6177页

作者： Rongrong Li Yuxue Yue Xianlang Chen Renqin Chang Jiaxin Zhang Bo Zhao Jieyu Zhang Di Cai Yihan Zhu Deman Han Jia Zhao Xiaonian Li Engineering Research Center of Recycling and Comprehensive Utilization of Pharmaceutical and Chemical Waste of Zhejiang Province Taizhou UniversityTaizhou 318000China Industrial Catalysis Institute of Zhejiang University of Technology Hangzhou 310014China Research Center of Analysis Measurement of Zhejiang University of Technology Hangzhou 310014China School of Science Zhejiang Sci-Tech UniversityHangzhou 310018China

semi-hydrogenation of acetylene is of growing interest and popularity but subjects to a major challenge in selective hydrogenation to ***,we report a strategy that uses graphdiyne(GDY)as a carrier to prepare single-cluster catalysts(SCCs),which on average clusters composed of three atoms(denoted as Pd3 trimer)and applied it to the acetylene semihydrogenation in the presence of large amounts of *** on experimental results and systematic quantum chemical research and computational screening,we found that there are multiple active Pd structures on GDY and the Pd3 trimer anchored on GDY is a specific and durable cluster with great potential for accurate and efficient heterogeneous *** synergetic effects between neighboring atoms in Pd trimer guarantee easy desorption of ethylene and the absence of unselective hydride species thereby preventing excessive hydrogenation to generate unwanted byproducts,which is a crucial mechanism for the excellent selectivity of the *** new method for precise synthesis Pd clusters provides accurate ways for designing selective hydrogenation catalysts at the atomic scale.

关键词： Pd cluster catalysts acetylene semi-hydrogenation Pd trimer

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