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Directional Construction of the Highly Stable Active-Site Ensembles at Sub-2 nm to Enhance Catalytic Activity and Selectivity.
Chen, Zemin; Chen, Yu; Shi, Lei; Li, Xinyu; Xu, Guangyue; Zeng, Xiang; Zheng, Xusheng; Qi, Zeming; Zhang, Kaihang; Li, Jiong; Zhang, Shuo; Zhao, Zhijian; Zhang, Ying.
Afiliación
  • Chen Z; Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China, Hefei, 230026, China.
  • Chen Y; Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201204, P. R. China.
  • Shi L; The Instruments Center for Physical Science, University of Science and Technology of China, Hefei, 230026, China.
  • Li X; Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China, Hefei, 230026, China.
  • Xu G; Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China, Hefei, 230026, China.
  • Zeng X; Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China, Hefei, 230026, China.
  • Zheng X; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230026, China.
  • Qi Z; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230026, China.
  • Zhang K; Brook Byers Institute of Sustainable Systems, School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, GA, 30332, USA.
  • Li J; Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201204, P. R. China.
  • Zhang S; Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201204, P. R. China.
  • Zhao Z; Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin, 300072, China.
  • Zhang Y; Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China, Hefei, 230026, China.
Adv Mater ; 36(35): e2405733, 2024 Aug.
Article en En | MEDLINE | ID: mdl-39003615
ABSTRACT
Precise control over the size, species, and breakthrough of the activity-selectivity trade-off are great challenges for sub-nano non-noble metal catalysts. Here, for the first time, a "multiheteroatom induced SMSI + in situ P activation" strategy that enables high stability and effective construction of sub-2 nm metal sites for optimizing selective hydrogenation performance is developed. It is synthesized the smallest metal phosphide clusters (<2 nm) including from unary to ternary non-noble metal systems, accompanied by unprecedented thermal stability. In the proof-of-concept demonstration, further modulation of size and species results in the creation of a sub-2 nm site platform, directionally achieving single atom (Ni1), Ni1+metal cluster (Ni1+Nin), or novel Ni1+metal phosphide cluster synergistic sites (Ni1+Ni2Pn), respectively. Based on thorough structure and mechanism investigation, it is found the Ni1+Ni2Pn site is motivated to achieve electronic structure self-optimizing through synergistic SMSI and site coupling effect. Therefore, it speeds up the substrate adsorption-desorption kinetics in semihydrogenation of alkyne and achieves superior catalytic activity that is 56 times higher than the Ni1 site under mild conditions. Compared to traditional active sites, this may represent the highly effective integration of atom utilization, thermal stability, and favorable site requirements for chemisorption properties and reactivities of substrates.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Adv Mater Asunto de la revista: BIOFISICA / QUIMICA Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Alemania
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Adv Mater Asunto de la revista: BIOFISICA / QUIMICA Año: 2024 Tipo del documento: Article País de afiliación: China Pais de publicación: Alemania