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

被引：76

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

来源：

NATURE COMMUNICATIONS | 2019年 / 10卷 / 1期

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

页数：9