Effective ensemble of pt single atoms and clusters over the (Ni,Co)(OH)2 substrate catalyzes highly selective, efficient, and stable hydrogenation reactions

DOI: 10.1021/acscatal.2c01901

Authors: Lihua Zhu (The University of Hong Kong; Jiangxi University of Science and Technology) , Yilun Sun (Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences (CAS)) , Huaze Zhu (Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences) , Guoliang Chai (State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences (CAS)) , Zhiqing Yang (Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences) , Congxiao Shang (The University of Hong Kong) , Hengqiang Ye (Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences) , Bing Hui Chen (College of Chemistry and Chemical Engineering, Xiamen University) , Anna Kroner (Diamond Light Source) , Zhengxiao Guo (The University of Hong Kong)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Acs Catalysis

State: Published (Approved)
Published: June 2022
Diamond Proposal Number(s): 29684

Abstract: A Pt–Ni–Co catalyst was synthesized with Pt single atoms and atomic clusters (SAACs) dispersed over (Ni,Co)(OH)2 nanoparticles on a carbon matrix, which leads to high catalytic activity, up to 100% conversion, and selectivity in the hydrogenation of nitroaromatics under moderate conditions (H2 ∼ 1.0 MPa and ≤40 °C). A synergistically coordinated ensemble effect of the Pt SAACs is identified with the strongly polarized Pt single atoms preferentially adsorbing the −NO2 and the Pt clusters adsorbing and homolytically dissociating H2 molecules, and the H species then readily move to the adsorbed −NO2 group, overcoming a much reduced energy barrier on the (Ni,Co)(OH)2, enhancing the reaction rate by ca. 50 times. The approach not only reveals the coordinated ensemble catalysis mechanism of SAACs but also provides a strategy of developing highly efficient and selective catalysts by fine tuning of the electronic microenvironment from single atoms to atomic clusters co-located over a multimetallic substrate. The demonstrated case for nitroarenes can be readily applied for other species containing −NO2 or other easily hydrogenated groups (such as C═C, C≡N, and C═O).

Journal Keywords: Pt single atoms and atomic clusters (SAACs); (Ni,Co)(OH)2; nanoparticles; hydrogenation reactions; synergistic effect

Subject Areas: Chemistry


Instruments: B18-Core EXAFS

Added On: 27/06/2022 08:23

Discipline Tags:

Physical Chemistry Catalysis Chemistry

Technical Tags:

Spectroscopy X-ray Absorption Spectroscopy (XAS) Extended X-ray Absorption Fine Structure (EXAFS)