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.
引用
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页数:7
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共 48 条
  • [41] Water-Mediated Mars-Van Krevelen Mechanism for CO Oxidation on Ceria-Supported Single-Atom Pt1 Catalyst
    Wang, Chunlei
    Gu, Xiang-Kui
    Yan, Huan
    Lin, Yue
    Li, Junjie
    Liu, Dandan
    Li, Wei-Xue
    Lu, Junling
    [J]. ACS CATALYSIS, 2017, 7 (01): : 887 - 891
  • [42] Synthesis of silicon complexes from rice husk derived silica nanoparticles
    Wang, Weixing
    Martin, Jarett C.
    Huang, Rongcai
    Huang, Wenxi
    Liu, Anhua
    Han, Aijie
    Sun, Luyi
    [J]. RSC ADVANCES, 2012, 2 (24) : 9036 - 9041
  • [43] Preferential oxidation of carbon monoxide in the presence of hydrogen (PROX) over ceria-zirconia and alumina-supported Pt catalysts
    Wootsch, A
    Descorme, C
    Duprez, D
    [J]. JOURNAL OF CATALYSIS, 2004, 225 (02) : 259 - 266
  • [44] A Common Single-Site Pt(II)-O(OH)x- Species Stabilized by Sodium on "Active" and "Inert" Supports Catalyzes the Water-Gas Shift Reaction
    Yang, Ming
    Liu, Jilei
    Lee, Sungsik
    Zugic, Branko
    Huang, Jun
    Allard, Lawrence F.
    Flytzani-Stephanopoulos, Maria
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2015, 137 (10) : 3470 - 3473
  • [45] Atomically Dispersed Au-(OH)x Species Bound on Titania Catalyze the Low-Temperature Water-Gas Shift Reaction
    Yang, Ming
    Allard, Lawrence F.
    Flytzani-Stephanopoulos, Maria
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2013, 135 (10) : 3768 - 3771
  • [46] Alkali-Stabilized Pt-OHx Species Catalyze Low-Temperature Water-Gas Shift Reactions
    Zhai, Yanping
    Pierre, Danny
    Si, Rui
    Deng, Weiling
    Ferrin, Peter
    Nilekar, Anand U.
    Peng, Guowen
    Herron, Jeffrey A.
    Bell, David C.
    Saltsburg, Howard
    Mavrikakis, Manos
    Flytzani-Stephanopoulos, Maria
    [J]. SCIENCE, 2010, 329 (5999) : 1633 - 1636
  • [47] Probing the Low-Temperature Water-Gas Shift Activity of Alkali-Promoted Platinum Catalysts Stabilized on Carbon Supports
    Zugic, Branko
    Zhang, Shiran
    Bell, David C.
    Tao, Franklin
    Flytzani-Stephanopoulos, Maria
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2014, 136 (08) : 3238 - 3245
  • [48] Activation of carbon-supported platinum catalysts by sodium for the low-temperature water-gas shift reaction
    Zugic, Branko
    Bell, David C.
    Flytzani-Stephanopoulos, Maria
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 2014, 144 : 243 - 251