Neighboring Pd single atoms surpass isolated single atoms for selective hydrodehalogenation catalysis

Chu, Chiheng; Huang, Dahong; Gupta, Srishti; Weon, Seunghyun; Niu, Junfeng; Stavitski, Eli; Muhich, Christopher; Kim, Jae-Hong

doi:10.1038/s41467-021-25526-2

Neighboring Pd single atoms surpass isolated single atoms for selective hydrodehalogenation catalysis

Journal Article · Mon Aug 30 00:00:00 EDT 2021 · Nature Communications

DOI:https://doi.org/10.1038/s41467-021-25526-2· OSTI ID:1825733

Chu, Chiheng ^[1]; Huang, Dahong ^[2]; ^[3]; ^[4]; ^[5]; Stavitski, Eli ^[6]; ^[3]; ^[7]

Zhejiang Univ., Hangzhou (China); Yale Univ., New Haven, CT (United States); NSF Nanosystems Engineering Research Center for Nanotechnology Enabled Water Treatment (NEWT), Houston, TX (United States)
Yale Univ., New Haven, CT (United States); NSF Nanosystems Engineering Research Center for Nanotechnology Enabled Water Treatment (NEWT), Houston, TX (United States); Dongguan Univ. of Technology, Guangdong (China)
NSF Nanosystems Engineering Research Center for Nanotechnology Enabled Water Treatment (NEWT), Houston, TX (United States); Arizona State Univ., Tempe, AZ (United States)
Yale Univ., New Haven, CT (United States); NSF Nanosystems Engineering Research Center for Nanotechnology Enabled Water Treatment (NEWT), Houston, TX (United States); Korea Univ., Seoul (Korea)
Dongguan Univ. of Technology, Guangdong (China)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Yale Univ., New Haven, CT (United States); NSF Nanosystems Engineering Research Center for Nanotechnology Enabled Water Treatment (NEWT), Houston, TX (United States)

Single atom catalysts have been found to exhibit superior selectivity over nanoparticulate catalysts for catalytic reactions such as hydrogenation due to their single-site nature. However, improved selectively is often accompanied by loss of activity and slow kinetics. Here we demonstrate that neighboring Pd single atom catalysts retain the high selectivity merit of sparsely isolated single atom catalysts, while the cooperative interactions between neighboring atoms greatly enhance the activity for hydrogenation of carbon-halogen bonds. Experimental results and computational calculations suggest that neighboring Pd atoms work in synergy to lower the energy of key meta-stable reactions steps, i.e., initial water desorption and final hydrogenated product desorption. The placement of neighboring Pd atoms also contribute to nearly exclusive hydrogenation of carbon-chlorine bond without altering any other bonds in organohalogens. The promising hydrogenation performance achieved by neighboring single atoms sheds light on a new approach for manipulating the activity and selectivity of single atom catalysts that are increasingly studied in multiple applications.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1825733

Report Number(s):: BNL--222251-2021-JAAM

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 12; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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