Aiming at the trade-off effect between activity and selectivity of the selective hydrogenation of trace acetylene in ethylene stream. Yanan Liu and Dianqing Li group in collaboration with Professor Shubo Tian and Xin Zhang from our institute ingeniously leveraged the structural characteristics of molybdenum disulfide nanoflakes (MoS2-NF) including periodically arranged basal planes and abundant edge sulfur vacancies to successfully construct a single-atom Ni catalyst with dual coordination environments (Ni1-S6/Ni1-Mo2). This enables efficiently and selectively convert residual acetylene in C2 streams into polymer-grade ethylene.
This work titled as "Engineering Heterogeneous Dual-Coordination Environments for Single-Atom Nickel Catalysts: A Synergistic Strategy to Enhance Selective Hydrogenation", were published in J. Am. Chem. Soc. on 2nd December. The first author is Yanan Liu from Beijing University of Chemical Technology (BUCT), and the corresponding authors are Yanan Liu, Xin Zhang, and Shubo Tian from BUCT.
Through the combination of experiments and theoretical calculations, the research group clarified the function of Ni sites in different coordination environments. Specifically, the edge Ni1-Mo2 sites can efficiently activate hydrogen molecules, while the basal plane Ni1-S6 sites can selectively adsorb acetylene in a di-σ configuration that is favorable for ethylene generation. The spatial distance between these two sites is approximately 0.63 nm, which generates a strong synergistic effect, effectively ensuring the efficient transfer of active hydrogen species from the edge sites to the basal plane sites. At mild reaction conditions (~145°C), the complete conversion of acetylene in ethylene stream was achieved with the ethylene selectivity of 91.9%. Meanwhile, this synergistic catalyst exhibited excellent anti-coking and anti-sintering stability, maintaining stable performance without significant deactivation even after 100 hours. This overcomes the problem of easy agglomeration and deactivation of active metals caused by the strong exothermic nature of the reaction, breaking the activity-selectivity-stability trade-off effect in acetylene selective hydrogenation.
Original link: https://doi.org/10.1021/jacs.5c12183
Author introductions
Yanan Liu, is associate professor and doctoral supervisor at School of Chemistry, Beijing University of Chemical Technology. The main research focuses on the design and construction of selective hydrogenation catalysts. She has published more than 60 papers in prestigious journals in the fields of chemical engineering and chemistry, such as Chem. Soc. Rev., J. Am. Chem. Soc., AIChE J., and ACS Catal., and has participated in the compilation of 1 monograph. She has 1 authorized U.S. invention patent and more than 20 authorized Chinese invention patents, among which 3 patent achievements have been successfully transformed, thus constructing 2 sets of catalyst preparation devices and forming 2 enterprise standards. She has successively presided more than 10 projects, including National Natural Science Foundation of China, provincial and ministerial-level key research and development projects, and technical development projects of PetroChina. The relevant achievements have been applied in enterprises such as PetroChina Lanzhou Petrochemical and Liming Research Institute.
Xin Zhang is Professor, Doctoral Supervisor and Deputy Director of the Academic Affairs Office in Beijing University of Chemical Technology. She was awarded the National high-level talents (2022) and the "Young Teaching Master Award" of Beijing Higher Education Institutions (2021). Her research interests focus on theoretical and computational catalysis, as well as data-driven catalyst design. Currently, she has published more than 120 papers in well-known academic journals including Nat. Catal., Nat. Commun., and PNAS. She has presided over 4 projects of the National Natural Science Foundation of China, and participated in a number of key research and development projects of the state as well as key projects of China Petrochemical Corporation as a core member. She has long served as a reviewer for the National Natural Science Foundation of China, China Scholarship Council, and a popular science expert of the China Association for Science and Technology.
Shubo Tian is professor at the School of Chemistry, Beijing University of Chemical Technology, and a Young Changjiang Scholar. His main research field is atomic-scale heterogeneous catalysis. So far, he has published more than 40 academic papers, which have been cited more than 5,000 times. These papers include those published in top journals such as Nat. Catal., Nat. Commun., J. Am. Chem. Soc., Angew. Chem. Int. Ed., and Chem. He has applied for 13 national invention patents, 6 of which have been authorized. He has presided over a variety of vertical and horizontal projects, including the General Program of the National Natural Science Foundation of China, the Youth Program of the National Natural Science Foundation of China, key projects of Beijing, sub-tasks of the Young Scientists Program of the Ministry of Science and Technology, sub-projects of key research and development projects of the Ministry of Science and Technology, and projects of university-enterprise joint research centers.