Harnessing strong metal–support interactions via a reverse route

Peiwen Wu, Shuai Tan, Jisue Moon, Zihao Yan, Victor Fung, Na Li, Shi-Ze Yang, Yongqiang Cheng, Carter W. Abney, Zili Wu, Aditya Savara, Ayyoub M. Momen, Jiang De-en, Dong Su, Huaming Li, Wenshuai Zhu (), Sheng Dai () and Huiyuan Zhu ()
Additional contact information
Peiwen Wu: Oak Ridge National Laboratory
Shuai Tan: Oak Ridge National Laboratory
Jisue Moon: Oak Ridge National Laboratory
Zihao Yan: Virginia Polytechnic Institute and State University
Victor Fung: University of California
Na Li: Brookhaven National Laboratory
Shi-Ze Yang: Oak Ridge National Laboratory
Yongqiang Cheng: Oak Ridge National Laboratory
Carter W. Abney: Oak Ridge National Laboratory
Zili Wu: Oak Ridge National Laboratory
Aditya Savara: Oak Ridge National Laboratory
Ayyoub M. Momen: Oak Ridge National Laboratory
Jiang De-en: University of California
Dong Su: Brookhaven National Laboratory
Huaming Li: Jiangsu University
Wenshuai Zhu: Jiangsu University
Sheng Dai: Oak Ridge National Laboratory
Huiyuan Zhu: Oak Ridge National Laboratory

Nature Communications, 2020, vol. 11, issue 1, 1-10

Abstract: Abstract Engineering strong metal–support interactions (SMSI) is an effective strategy for tuning structures and performances of supported metal catalysts but induces poor exposure of active sites. Here, we demonstrate a strong metal–support interaction via a reverse route (SMSIR) by starting from the final morphology of SMSI (fully-encapsulated core–shell structure) to obtain the intermediate state with desirable exposure of metal sites. Using core–shell nanoparticles (NPs) as a building block, the Pd–FeOx NPs are transformed into a porous yolk–shell structure along with the formation of SMSIR upon treatment under a reductive atmosphere. The final structure, denoted as Pd–Fe3O4–H, exhibits excellent catalytic performance in semi-hydrogenation of acetylene with 100% conversion and 85.1% selectivity to ethylene at 80 °C. Detailed electron microscopic and spectroscopic experiments coupled with computational modeling demonstrate that the compelling performance stems from the SMSIR, favoring the formation of surface hydrogen on Pd instead of hydride.

Date: 2020
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DOI: 10.1038/s41467-020-16674-y

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