Harnessing strong metal–support interactions via a reverse route

Wu, Peiwen; Tan, Shuai; Moon, Jisue; Yan, Zihao; Fung, Victor; Li, Na; Yang, Shi-Ze; Cheng, Yongqiang; Abney, Carter W.; Wu, Zili; Savara, Aditya; Momen, Ayyoub M.; Jiang, De-en; Su, Dong; Li, Huaming; Zhu, Wenshuai; Dai, Sheng; Zhu, Huiyuan

doi:10.1038/s41467-020-16674-y

Title: Harnessing strong metal–support interactions via a reverse route

Journal Article · Tue Jun 16 00:00:00 EDT 2020 · Nature Communications

DOI:https://doi.org/10.1038/s41467-020-16674-y· OSTI ID:1633478

; Tan, Shuai;

; Yan, Zihao; Fung, Victor; Li, Na;

; Cheng, Yongqiang; Abney, Carter W.; Wu, Zili;

; Momen, Ayyoub M.;

;

; Li, Huaming;

;

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.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Natural Science Foundation of China (NSFC)

Grant/Contract Number:: SC0012704; AC02-06CH11357; AC05-00OR22725; 21722604; BK20190852

OSTI ID:: 1633478

Alternate ID(s):: OSTI ID: 1642412; OSTI ID: 1761660

Report Number(s):: BNL-216190-2020-JAAM; 3042; PII: 16674

Journal Information:: Nature Communications, Journal Name: Nature Communications Vol. 11 Journal Issue: 1; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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Cited by: 70 works

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