Ultrastable single-atom gold catalysts with strong covalent metal-support interaction (CMSI)

被引:443
作者
Qiao, Botao [1 ,2 ]
Liang, Jin-Xia [3 ,4 ,5 ]
Wang, Aiqin [2 ]
Xu, Cong-Qiao [3 ,4 ]
Li, Jun [3 ,4 ]
Zhang, Tao [2 ]
Liu, Jingyue [1 ]
机构
[1] Arizona State Univ, Dept Phys, Tempe, AZ 85287 USA
[2] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
[3] Tsinghua Univ, Minist Educ, Dept Chem, Beijing 100084, Peoples R China
[4] Tsinghua Univ, Minist Educ, Key Lab Organ Optoelect & Mol Engn, Beijing 100084, Peoples R China
[5] Guizhou Normal Coll, Guizhou Prov Key Lab Computat Nanomat Sci, Guiyang 550018, Peoples R China
基金
中国国家自然科学基金;
关键词
single-atom catalysis; gold catalyst; CO oxidation; covalent metal-support interaction; LOW-TEMPERATURE OXIDATION; CO OXIDATION; CHEMOSELECTIVE HYDROGENATION; ACTIVE GOLD; SITE; AU; NANOPARTICLES; PERFORMANCE; MECHANISMS; IR-1/FEOX;
D O I
10.1007/s12274-015-0796-9
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Supported noble metal nanoparticles (including nanoclusters) are widely used in many industrial catalytic processes. While the finely dispersed nanostructures are highly active, they are usually thermodynamically unstable and tend to aggregate or sinter at elevated temperatures. This scenario is particularly true for supported nanogold catalysts because the gold nanostructures are easily sintered at high temperatures, under reaction conditions, or even during storage at ambient temperature. Here, we demonstrate that isolated Au single atoms dispersed on iron oxide nanocrystallites (Au-1/FeOx) are much more sinteringresistant than Au nanostructures, and exhibit extremely high reaction stability for CO oxidation in a wide temperature range. Theoretical studies revealed that the positively charged and surface-anchored Au1 atoms with high valent states formed significant covalent metal-support interactions (CMSIs), thus providing the ultra-stability and remarkable catalytic performance. This work may provide insights and a new avenue for fabricating supported Au catalysts with ultra-high stability.
引用
收藏
页码:2913 / 2924
页数:12
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