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
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
收藏
页数:9
相关论文
共 51 条
[1]   Imine Metathesis Catalyzed by a Silica-Supported Hafnium Imido Complex [J].
Aljuhani, Maha A. ;
Barman, Samir ;
Abou-Hamad, Edy ;
Gurinov, Andrei ;
Ould-Chikh, Samy ;
Guan, Erjia ;
Jedidi, Abdesslem ;
Cavallo, Luigi ;
Gates, Bruce C. ;
Pelletier, Jeremie D. A. ;
Basset, Jean-Marie .
ACS CATALYSIS, 2018, 8 (10) :9440-9446
[2]  
[Anonymous], J CHEM PHYS
[3]  
[Anonymous], 1979, Adv. Organomet. Chem
[4]   Controlling catalytic activity and selectivity for partial hydrogenation by tuning the environment around active sites in iridium complexes bonded to supports [J].
Babucci, Melike ;
Fang, Chia-Yu ;
Perez-Aguilar, Jorge E. ;
Hoffman, Adam S. ;
Boubnov, Alexey ;
Guan, Erjia ;
Bare, Simon R. ;
Gates, Bruce C. ;
Uzun, Alper .
CHEMICAL SCIENCE, 2019, 10 (09) :2623-2632
[5]   An investigation of a new regeneration method of commercial aged three-way catalysts [J].
Birgersson, Henrik ;
Boutonnet, Magali ;
Klingstedt, Fredrik ;
Murzin, Dmitry Yu. ;
Stefanov, Plamen ;
Naydenov, Anton .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2006, 65 (1-2) :93-100
[6]   Relating Rates of Catalyst Sintering to the Disappearance of Individual Nanoparticles during Ostwald Ripening [J].
Challa, Sivakumar R. ;
Delariva, Andrew T. ;
Hansen, Thomas W. ;
Helveg, Stig ;
Sehested, Jens ;
Hansen, Poul L. ;
Garzon, Fernando ;
Datye, Abhaya K. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2011, 133 (51) :20672-20675
[7]   Effects of oxidation/reduction and oxychlorination/reduction cycles on CO adsorption by Pt-Re/Al2O3 catalysts [J].
Chong, FK ;
Anderson, JA ;
Rochester, CH .
JOURNAL OF CATALYSIS, 2000, 190 (02) :327-337
[8]   Bridging homogeneous and heterogeneous catalysis by heterogeneous single-metal-site catalysts [J].
Cui, Xinjiang ;
Li, Wu ;
Ryabchuk, Pavel ;
Junge, Kathrin ;
Beller, Matthias .
NATURE CATALYSIS, 2018, 1 (06) :385-397
[9]   Size controllable redispersion of sintered Au nanoparticles by using iodohydrocarbon and its implications [J].
Duan, Xinping ;
Tian, Xuelin ;
Ke, Jinhuo ;
Yin, Yan ;
Zheng, Jianwei ;
Chen, Jin ;
Cao, Zhenming ;
Xie, Zhaoxiong ;
Yuan, Youzhu .
CHEMICAL SCIENCE, 2016, 7 (05) :3181-3187
[10]  
Feller D, 1996, J COMPUT CHEM, V17, P1571, DOI 10.1002/(SICI)1096-987X(199610)17:13<1571::AID-JCC9>3.0.CO