Isolating contiguous Pt atoms and forming Pt-Zn intermetallic nanoparticles to regulate selectivity in 4-nitrophenylacetylene hydrogenation

Aijuan Han; Jian Zhang; Wenming Sun; Wenxing Chen; Shaolong Zhang; Yunhu Han; Quanchen Feng; Lirong Zheng; Lin Gu; Chen Chen; Qing Peng; Dingsheng Wang; Yadong Li

doi:10.1038/s41467-019-11794-6

Isolating contiguous Pt atoms and forming Pt-Zn intermetallic nanoparticles to regulate selectivity in 4-nitrophenylacetylene hydrogenation

Nat Commun. 2019 Aug 22;10(1):3787. doi: 10.1038/s41467-019-11794-6.

Authors

Aijuan Han^{1

2}, Jian Zhang², Wenming Sun³, Wenxing Chen^{2

4}, Shaolong Zhang², Yunhu Han², Quanchen Feng², Lirong Zheng⁵, Lin Gu⁶, Chen Chen², Qing Peng², Dingsheng Wang⁷, Yadong Li²

Affiliations

¹ State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029, China.
² Department of Chemistry, Tsinghua University, Beijing, 100084, China.
³ College of Science, China Agricultural University, Beijing, 100193, China.
⁴ Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081, China.
⁵ Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, Chinese Academy of Sciences, Beijing, 100049, China.
⁶ Institute of Physics, Chinese Academy of Sciences, Beijing, 100190, China.
⁷ Department of Chemistry, Tsinghua University, Beijing, 100084, China. wangdingsheng@mail.tsinghua.edu.cn.

Abstract

Noble metals play a momentous role in heterogeneous catalysis but still face a huge challenge in selectivity control. Herein, we report isolating contiguous Pt atoms and forming Pt-Zn intermetallic nanoparticles as an effective strategy to optimize the selectivity of Pt catalysts. Contiguous Pt atoms are isolated into single atoms and Pt-Zn intermetallic nanoparticles are formed which are supported on hollow nitrogen-doped carbon nanotubes (PtZn/HNCNT), as confirmed by aberration-corrected high-resolution transmission electron microscopy and X-ray absorption spectrometry measurements. Interestingly, this PtZn/HNCNT catalyst promotes the hydrogenation of 4-nitrophenylacetylene to 4-aminophenylacetylene with a much higher conversion ( > 99%) and selectivity (99%) than the comparison samples with Pt isolated-single-atomic-sites (Pt/HNCNT) and Pt nanoparticles (Pt/CN). Further density functional theory (DFT) calculations disclose that the positive Zn atoms assist the adsorption of nitro group and Pt-Zn intermetallic nanoparticles facilitate the hydrogenation on nitro group kinetically.

Abstract

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