A General Strategy for Fabricating Isolated Single Metal Atomic Site Catalysts in Y Zeolite

Yiwei Liu; Zhi Li; Qiuying Yu; Yanfei Chen; Ziwei Chai; Guofeng Zhao; Shoujie Liu; Weng-Chon Cheong; Yuan Pan; Qinghua Zhang; Lin Gu; Lirong Zheng; Yu Wang; Yong Lu; Dingsheng Wang; Chen Chen; Qing Peng; Yunqi Liu; Limin Liu; Jiesheng Chen; Yadong Li

doi:10.1021/jacs.9b02936

A General Strategy for Fabricating Isolated Single Metal Atomic Site Catalysts in Y Zeolite

J Am Chem Soc. 2019 Jun 12;141(23):9305-9311. doi: 10.1021/jacs.9b02936. Epub 2019 May 30.

Authors

Yiwei Liu¹, Zhi Li¹, Qiuying Yu², Yanfei Chen³, Ziwei Chai⁴, Guofeng Zhao⁵, Shoujie Liu⁶, Weng-Chon Cheong¹, Yuan Pan¹, Qinghua Zhang⁷, Lin Gu⁷, Lirong Zheng⁸, Yu Wang⁹, Yong Lu⁵, Dingsheng Wang¹, Chen Chen¹, Qing Peng¹, Yunqi Liu³, Limin Liu⁴, Jiesheng Chen², Yadong Li¹

Affiliations

¹ Department of Chemistry , Tsinghua University , Beijing 100084 , China.
² School of Chemistry and Chemical Engineering , Shanghai Jiao Tong University , Shanghai 200240 , China.
³ State Key Laboratory of Heavy Oil Processing, Key Laboratory of Catalysis , China University of Petroleum , Qingdao , Shandong 266580 , China.
⁴ Beijing Computational Science Research Center , Beijing 100193 , China.
⁵ School of Chemistry and Molecular Engineering , East China Normal University , Shanghai 200062 , China.
⁶ College of Chemistry and Materials Science , Anhui Normal University , Wuhu , Anhui 241000 , China.
⁷ Institute of Physics, Chinese Academy of Sciences , Beijing 100190 , China.
⁸ Beijing Synchrotron Radiation Facility , Institute of High Energy Physics, Chinese Academy of Sciences , Beijing 100049 , China.
⁹ Shanghai Synchrotron Radiation Facility , Shanghai Institute of Applied Physics, Chinese Academy of Sciences , Shanghai 201800 , China.

PMID: 31117651
DOI: 10.1021/jacs.9b02936

Abstract

Exploring high-performance zeolite-supported metal catalysts is of great significance. Herein, we develop a strategy for fabricating isolated single metal atomic site catalysts in Y zeolite (M-ISAS@Y, M = Pt, Pd, Ru, Rh, Co, Ni, Cu) by in situ separating and confining a metal-ethanediamine complex into β-cages during the crystallization process followed by thermal treatment. The M-ISAS are stabilized by skeletal oxygens of Y zeolite, and the crystallinity, porosity, and large surface area are well inherited in M-ISAS@Y. As a demonstration, acidic Pt-ISAS@Y is used for n-hexane isomerization involving consecutive catalytic dehydrogenation/hydrogenation on Pt-ISAS and isomerization on Brønsted acid sites. The turnover frequency value of Pt-ISAS reaches 727 h^-1, 5 times more than Pt nanoparticles (∼3.5 nm), with a total isomer selectivity of more than 98%. This strategy provides a convenient route to fabricate promising zeolite-based M-ISAS catalysts for industrial applications.