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

被引:96
作者
Cao, Sufeng [1 ]
Zhao, Yanyan [2 ]
Lee, Sungsik [3 ]
Yang, Shize [4 ]
Liu, Jilei [1 ]
Giannakakis, Georgios [1 ]
Li, Mengwei [1 ]
Ouyang, Mengyao [1 ]
Wang, Dunwei [2 ]
Sykes, E. Charles H. [5 ]
Flytzani-Stephanopoulos, Maria [1 ]
机构
[1] Tufts Univ, Dept Chem & Biol Engn, Medford, MA 02155 USA
[2] Boston Coll, Merkert Chem Ctr, Dept Chem, Chestnut Hill, MA 02467 USA
[3] Argonne Natl Lab, Xray Sci Div, Lemont, IL 60439 USA
[4] Brookhaven Natl Lab, Ctr Funct Nanomat, Upton, NY 11973 USA
[5] Tufts Univ, Dept Chem, 62 Talbot Ave, Medford, MA 02155 USA
来源
SCIENCE ADVANCES | 2020年 / 6卷 / 25期
关键词
SUPPORTED PLATINUM CATALYSTS; CARBON-MONOXIDE; PREFERENTIAL OXIDATION; H-2; OXIDATION; GAS; HYDROGEN; MECHANISM; MIXTURES; SODIUM; XPS;
D O I
10.1126/sciadv.aba3809
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
The preferential oxidation of CO (PROX) in hydrogen-rich fuel gas streams is an attractive option to remove CO while effectively conserving energy and H-2. 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 (similar to 99.8% conversion, 70% selectivity at 110 degrees 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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页数:7
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