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Adsorption Site Regulation to Guide Atomic Design of Ni–Ga Catalysts for Acetylene Semi-Hydrogenation |
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| Authors: | Dr Yueqiang Cao Hao Zhang Dr Shufang Ji Prof Zhijun Sui Prof Zheng Jiang Prof Dingsheng Wang Prof Francisco Zaera Prof Xinggui Zhou Prof Xuezhi Duan Prof Yadong Li |
| Institution: | 1. State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237 China
These authors contributed equally to this work.;2. Shanghai Institute of Applied Physics, Chinese Academy of Science, Shanghai, 201800 China University of Chinese Academy of Sciences, Beijing, 100049 China These authors contributed equally to this work.;3. Department of Chemistry, Tsinghua University, Beijing, 100084 China;4. State Key Laboratory of Chemical Engineering, School of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237 China;5. Shanghai Institute of Applied Physics, Chinese Academy of Science, Shanghai, 201800 China Shanghai Synchrotron Radiation Facility, Zhangjiang Lab, Shanghai Advanced Research Institute, Chinese Academy of Science, Shanghai, 201210 China;6. Department of Chemistry and UCR Center for Catalysis, University of California, Riverside, CA, 92521 USA |
| Abstract: | Atomic regulation of metal catalysts has emerged as an intriguing yet challenging strategy to boost product selectivity. Here, we report a density functional theory-guided atomic design strategy for the fabrication of a NiGa intermetallic catalyst with completely isolated Ni sites to optimize acetylene semi-hydrogenation processes. Such Ni sites show not only preferential acetylene π-adsorption, but also enhanced ethylene desorption. The characteristics of the Ni sites are confirmed by multiple characterization techniques, including aberration-corrected high-resolution scanning transmission electron microscopy and X-ray absorption spectrometry measurements. The superior performance is also confirmed experimentally against a Ni5Ga3 intermetallic catalyst with partially isolated Ni sites and against a Ni catalyst with multi-atomic ensemble Ni sites. Accordingly, the NiGa intermetallic catalyst with the completely isolated Ni sites shows significantly enhanced selectivity to ethylene and suppressed coke formation. |
| Keywords: | acetylene heterogeneous catalysis Ni–Ga intermetallic catalyst semi-hydrogenation site regulation |