A single site ruthenium catalyst for robust soot oxidation without platinum or palladium

被引:44
作者
Li, Yuanfeng [1 ]
Qin, Tian
Wei, Yuechang [1 ]
Xiong, Jing [1 ]
Zhang, Peng [1 ]
Lai, Kezhen [1 ]
Chi, Hongjie [1 ]
Liu, Xi [2 ]
Chen, Liwei
Yu, Xiaolin [3 ]
Zhao, Zhen [1 ]
Li, Lina [4 ]
Liu, Jian [1 ]
机构
[1] China Univ Petr, State Key Lab Heavy Oil Proc, Key Lab Opt Detect Technol Oil & Gas, Beijing 102249, Peoples R China
[2] Shanghai Jiao Tong Univ, Sch Chem & Chem, In Situ Ctr Phys Sci, Shanghai 200240, Peoples R China
[3] Chinese Acad Sci, Beijing Natl Lab Mol Sci BNLMS, Inst Chem, State Key Lab Struct Chem Unstable & Stable Speci, Beijing 100190, Peoples R China
[4] Shanghai Adv Res Inst, Shanghai Synchrotron Radiat Facil, Shanghai, Peoples R China
基金
北京市自然科学基金;
关键词
TOTAL-ENERGY CALCULATIONS; ELASTIC BAND METHOD; CO OXIDATION; CERIA; NANOPARTICLES; COMBUSTION; SURFACE; TEMPERATURE; RU/CEO2; ROLES;
D O I
10.1038/s41467-023-42935-7
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 quest for efficient non-Pt/Pd catalysts has proved to be a formidable challenge for auto-exhaust purification. Herein, we present an approach to construct a robust catalyst by embedding single-atom Ru sites onto the surface of CeO2 through a gas bubbling-assisted membrane deposition method. The formed single-atom Ru sites, which occupy surface lattice sites of CeO2, can improve activation efficiency for NO and O-2. Remarkably, the Ru-1/CeO2 catalyst exhibits exceptional catalytic performance and stability during auto-exhaust carbon particle oxidation (soot), rivaling commercial Pt-based catalysts. The turnover frequency (0.218h(-1)) is a nine-fold increase relative to the Ru nanoparticle catalyst. We further show that the strong interfacial charge transfer within the atomically dispersed Ru active site greatly enhances the rate-determining step of NO oxidation, resulting in a substantial reduction of the apparent activation energy during soot oxidation. The single-atom Ru catalyst represents a step toward reducing dependence on Pt/Pd-based catalysts. Here, the authors report a study exploring surface lattice-confined single-atom ruthenium sites which demonstrate remarkable stability and exceptional catalytic performance for auto-exhaust purification, making them a promising alternative to costly Pt/Pd-based catalysts.
引用
收藏
页数:11
相关论文
共 65 条
  • [1] Ceria-supported small Pt and Pt3Sn nanoparticles for NOx-assisted soot oxidation
    Andana, Tahrizi
    Piumetti, Marco
    Bensaid, Samir
    Veyre, Laurent
    Thieuleux, Chloe
    Russo, Nunzio
    Fino, Debora
    Quadrelli, Elsje Alessandra
    Pirone, Raffaele
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 2017, 209 : 295 - 310
  • [2] Shape-Dependent Activity of Ceria in Soot Combustion
    Aneggi, Eleonora
    Wiater, Dawid
    de Leitenburg, Carla
    Llorca, Jordi
    Trovarelli, Alessandro
    [J]. ACS CATALYSIS, 2014, 4 (01): : 172 - 181
  • [3] Simultaneous oxidation of carbon black and volatile organic compounds over Ru/CeO2 catalysts
    Aouad, Samer
    Abi-Aad, Edmond
    Aboukais, Antoine
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 2009, 88 (3-4) : 249 - 256
  • [4] Insights into the Mechanism of Methanol Steam Reforming Tandem Reaction over CeO2 Supported Single-Site Catalysts
    Chen, Luning
    Qi, Zhiyuan
    Peng, Xinxing
    Chen, Jeng-Lung
    Pao, Chih-Wen
    Zhang, Xibo
    Dun, Chaochao
    Young, Melissa
    Prendergast, David
    Urban, Jeffrey J.
    Guo, Jinghua
    Somorjai, Gabor A.
    Su, Ji
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2021, 143 (31) : 12074 - 12081
  • [5] Holey Co-Ce oxide nanosheets as a highly efficient catalyst for diesel soot combustion
    Cui, Bing
    Zhou, Lingjie
    Li, Kai
    Liu, Yun-Quan
    Wang, Duo
    Ye, Yueyuan
    Li, Shuirong
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 2020, 267
  • [6] Catalytic combustion of chlorobenzene over Ru-doped ceria catalysts
    Dai, Qiguang
    Bai, Shuxing
    Wang, Zhengyi
    Wang, Xingyi
    Lu, Guanzhong
    [J]. APPLIED CATALYSIS B-ENVIRONMENTAL, 2012, 126 : 64 - 75
  • [7] Active nonmetallic Au and Pt species on ceria-based water-gas shift catalysts
    Fu, Q
    Saltsburg, H
    Flytzani-Stephanopoulos, M
    [J]. SCIENCE, 2003, 301 (5635) : 935 - 938
  • [8] Mechanistic Insights into Oxygen Dynamics in Soot Combustion over Cryptomelane Catalysts in Tight and Loose Contact Modes via 18O2/16O2 Isotopic Variable Composition Measurements - A Hot Ring Model of the Catalyst Operation
    Grybos, Joanna
    Fedyna, Monika
    Legutko, Piotr
    Leszczynski, Bartosz
    Janas, Janusz
    Wach, Anna
    Szlachetko, Jakub
    Yu, Xuehua
    Kotarba, Andrzej
    Zhao, Zhen
    Sojka, Zbigniew
    [J]. ACS CATALYSIS, 2021, 11 (15) : 9530 - 9546
  • [9] Unraveling the electronegativity-dominated intermediate adsorption on high-entropy alloy electrocatalysts
    Hao, Jiace
    Zhuang, Zechao
    Cao, Kecheng
    Gao, Guohua
    Wang, Chan
    Lai, Feili
    Lu, Shuanglong
    Ma, Piming
    Dong, Weifu
    Liu, Tianxi
    Du, Mingliang
    Zhu, Han
    [J]. NATURE COMMUNICATIONS, 2022, 13 (01)
  • [10] Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points
    Henkelman, G
    Jónsson, H
    [J]. JOURNAL OF CHEMICAL PHYSICS, 2000, 113 (22) : 9978 - 9985