In situ formation of mononuclear complexes by reaction-induced atomic dispersion of supported noble metal nanoparticles

被引:80
作者
Feng, Siquan [1 ,2 ]
Song, Xiangen [1 ]
Liu, Yang [2 ,3 ,4 ]
Lin, Xiangsong [5 ]
Yan, Li [1 ]
Liu, Siyue [6 ]
Dong, Wenrui [6 ]
Yang, Xueming [6 ,7 ]
Jiang, Zheng [3 ,4 ]
Ding, Yunjie [1 ,7 ,8 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
[4] Chinese Acad Sci, Shanghai Adv Res Inst, Shanghai 201204, Peoples R China
[5] Jiaxing Univ, Sch Mat & Text Engn, Jiaxing 314001, Peoples R China
[6] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China
[7] Zhejiang Normal Univ, Hangzhou Inst Adv Studies, Hangzhou 311231, Zhejiang, Peoples R China
[8] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
基金
国家重点研发计划;
关键词
INITIO MOLECULAR-DYNAMICS; TOTAL-ENERGY CALCULATIONS; HETEROGENEOUS CATALYSIS; ACTIVE-SITES; GOLD; CARBONYLATION; REDISPERSION; CHEMISTRY; METHANOL; RHODIUM;
D O I
10.1038/s41467-019-12965-1
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
Supported noble metal nanoclusters and single-metal-site catalysts are inclined to aggregate into particles, driven by the high surface-to-volume ratio. Herein, we report a general method to atomically disperse noble metal nanoparticles. The activated carbon supported nanoparticles of Ru, Rh, Pd, Ag, Ir and Pt metals with loading up to 5 wt. % are completely dispersed by reacting with CH3I and CO mixture. The dispersive process of the Rh nano-particle is investigated in depth as an example. The in-situ detected I center dot radicals and CO molecules are identified to promote the breakage of Rh-Rh bonds and the formation of mononuclear complexes. The isolated Rh mononuclear complexes are immobilized by the oxygen-containing functional groups based on the effective atomic number rule. The method also provides a general strategy for the development of single-metal-site catalysts for other applications.
引用
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页数:9
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