High-loading single Pt atom sites [Pt-O(OH)x] catalyze the CO PROX reaction with high activity and selectivity at mild conditions

Cao, Sufeng; Zhao, Yanyan; Lee, Sungsik; Yang, Shize; Liu, Jilei; Giannakakis, Georgios; Li, Mengwei; Ouyang, Mengyao; Wang, Dunwei; Sykes, E. Charles H.; Flytzani-Stephanopoulos, Maria

doi:10.1126/sciadv.aba3809

Title: High-loading single Pt atom sites [Pt-O(OH)_x] catalyze the CO PROX reaction with high activity and selectivity at mild conditions

Journal Article · 16 June 2020 · Science Advances

DOI: https://doi.org/10.1126/sciadv.aba3809 · OSTI ID:1635798

^[1];

^[2];

^[3];

^[4]; Liu, Jilei ^[5]; Giannakakis, Georgios ^[6]; Li, Mengwei ^[5];

^[5]; Wang, Dunwei ^[2];

^[5]; Flytzani-Stephanopoulos, Maria ^[5]

Tufts Univ., Medford, MA (United States); Tufts University
Boston College, Chestnut Hill, MA (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Tufts Univ., Medford, MA (United States)
Tufts Univ., Medford, MA (United States).

The preferential oxidation of CO (PROX) in hydrogen-rich fuel gas streams is an attractive option to remove CO while effectively conserving energy and H₂. However, high CO conversion with concomitant high selectivity to CO₂ but not H₂O is challenging. Here, we report the synthesis of high-loading single Pt atom (2.0 weight %) catalysts with oxygen-bonded alkaline ions that stabilize the cationic Pt. The synthesis is performed in aqueous solution and achieves high Pt atom loadings in a single-step incipient wetness impregnation of alumina or silica. Promisingly, these catalysts have high CO PROX selectivity even at high CO conversion (~99.8% conversion, 70% selectivity at 110°C) and good stability under reaction conditions. These findings pave the way for the design of highly efficient single-atom catalysts, elucidate the role of –OH species in CO oxidation, and confirm the absence of a support effect for our case.

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Research Organization:: Tufts Univ., Medford, MA (United States)

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

Grant/Contract Number:: FG02-05ER15730; SC0012704; AC02-06CH11357

OSTI ID:: 1635798

Alternate ID(s):: OSTI ID: 1638813; OSTI ID: 1773879; OSTI ID: 1662007

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 25 Vol. 6; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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Title: High-loading single Pt atom sites [Pt-O(OH)x] catalyze the CO PROX reaction with high activity and selectivity at mild conditions

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Title: High-loading single Pt atom sites [Pt-O(OH)_x] catalyze the CO PROX reaction with high activity and selectivity at mild conditions