Surfactants Used in Colloidal Synthesis Modulate Ni Nanoparticle Surface Evolution for Selective CO 2 Hydrogenation

Year: 2023

Type: article

Abstract: Colloidal chemistry holds promise to prepare uniform and size-controllable pre-catalysts; however, it remains a challenge to unveil the atomic-level transition from pre-catalysts to active catalytic surfaces under the reaction conditions to enable the mechanistic design of catalysts. Here, we report an ambient-pressure X-ray photoelectron spectroscopy study, coupled with in situ environmental transmission electron microscopy, infrared spectroscopy, and theoretical calculations, to elucidate the surface catalytic sites of colloidal Ni nanoparticles for CO 2 hydrogenation. We show that Ni nanoparticles with phosphine ligands exhibit a distinct surface evolution compared with amine-capped ones, owing to the diffusion of P under oxidative (air) or reductive (CO 2 + H 2 ) gaseous environments at elevated temperatures. The resulting NiP x surface leads to a substantially improved selectivity for CO production, in contrast to the metallic Ni, which favors CH 4 . The further elimination of surface metallic Ni sites by designing multi-step P incorporation achieves unit selectivity of CO in high-rate CO 2 hydrogenation.

Source: Journal of the American Chemical Society

DOI: 10.1021/jacs.3c02739

Authors: Xiangru Wei, Grayson Johnson, Yifan Ye, Meiyang Cui, Shen-Wei Yu, Yihua Ran, Jun Cai, Zhi Liu, Xi Chen, Wenpei Gao, Paul J. L. Bean, Weijie Zhang, Tommy Yunpu Zhao, Frédéric A. Perras, Ethan J. Crumlin, Xu Zhang, Robert J. Davis, Zhangxiong Wu, Sen Zhang

Institutions: Soochow University, University of Virginia, University of Science and Technology of China, Lawrence Berkeley National Laboratory, National Synchrotron Radiation Laboratory, Advanced Light Source, ShanghaiTech University, North Carolina State University, Ames National Laboratory, California State University, Northridge

Language: English

Topic: Catalysts for Methane Reforming

Subfield: Catalysis

Field: Chemical Engineering

Domain: Physical Sciences

Open Access status: green

Funders: National Science Foundation, U.S. Department of Energy, North Carolina State University, National Natural Science Foundation of China, Chinese Academy of Sciences, China Scholarship Council, University of Science and Technology of China, Office of Science, Division of Electrical, Communications and Cyber Systems, Basic Energy Sciences, Bioenergy Technologies Office, Chemical Sciences, Geosciences, and Biosciences Division

OpenAlex ID: W4381598569