Abrading bulk metal into single atoms

被引:165
作者
Han, Gao-Feng [1 ]
Li, Feng [1 ,2 ]
Rykov, Alexandre, I [3 ]
Im, Yoon-Kwang [1 ]
Yu, Soo-Young [1 ]
Jeon, Jong-Pil [1 ]
Kim, Seok-Jin [1 ]
Zhou, Wenhui [3 ]
Ge, Rile [3 ]
Ao, Zhimin [4 ]
Shin, Tae Joo [5 ]
Wang, Junhu [3 ]
Jeong, Hu Young [5 ]
Baek, Jong-Beom [1 ]
机构
[1] Ulsan Natl Inst Sci & Technol UNIST, Ctr Dimens Controllable Organ Frameworks, Sch Energy & Chem Engn, Ulsan, South Korea
[2] Fudan Univ, Lab Adv Mat, Shanghai Key Lab Mol Catalysis & Innovat Mat, Shanghai, Peoples R China
[3] Chinese Acad Sci, Mossbauer Effect Data Ctr, Dalian Inst Chem Phys, Dalian, Peoples R China
[4] Guangdong Univ Technol, Sch Environm Sci & Engn, Inst Environm Hlth & Pollut Control, Guangzhou, Peoples R China
[5] Ulsan Natl Inst Sci & Technol UNIST, Grad Sch Semicond Mat & Devices Engn, Ulsan, South Korea
基金
新加坡国家研究基金会; 中国国家自然科学基金;
关键词
ACTIVE-SITES; CATALYSTS; IDENTIFICATION; SPECTROSCOPY; OXIDATION; OXYGEN; IRON; ORR;
D O I
10.1038/s41565-022-01075-7
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
A solvent-free and zero-waste method was reported for the synthesis of single-atom catalysts via abrading bulk metal into single atoms. This strategy works for different metals (iron, cobalt, nickel and copper or their alloys) and supports (carbons, oxides or nitrides). Single-atom catalysts have recently attracted considerable attention because of their highly efficient metal utilization and unique properties. Finding a green, facile method to synthesize them is key to their widespread commercialization. Here we show that single-atom catalysts (including iron, cobalt, nickel and copper) can be prepared via a top-down abrasion method, in which the bulk metal is directly atomized onto different supports, such as carbon frameworks, oxides and nitrides. The level of metal loading can be easily tuned by changing the abrasion rate. No synthetic chemicals, solvents or even water were used in the process and no by-products or waste were generated. The underlying reaction mechanism involves the mechanochemical force in situ generating defects on the supports, then trapping and stably sequestering atomized metals.
引用
收藏
页码:403 / +
页数:7
相关论文
共 35 条
[1]   Towards dense single-atom catalysts for future automotive applications [J].
Beniya, Atsushi ;
Higashi, Shougo .
NATURE CATALYSIS, 2019, 2 (07) :590-602
[2]   Identification of single-atom active sites in carbon-based cobalt catalysts during electrocatalytic hydrogen evolution [J].
Cao, Linlin ;
Luo, Qiquan ;
Liu, Wei ;
Lin, Yue ;
Liu, Xiaokang ;
Cao, Yuanjie ;
Zhang, Wei ;
Wu, Yuen ;
Yang, Jinlong ;
Yao, Tao ;
Wei, Shiqiang .
NATURE CATALYSIS, 2019, 2 (02) :134-141
[3]   Direct atomic-level insight into the active sites of a high-performance PGM-free ORR catalyst [J].
Chung, Hoon T. ;
Cullen, David A. ;
Higgins, Drew ;
Sneed, Brian T. ;
Holby, Edward F. ;
More, Karren L. ;
Zelenay, Piotr .
SCIENCE, 2017, 357 (6350) :479-483
[4]   First principles methods using CASTEP [J].
Clark, SJ ;
Segall, MD ;
Pickard, CJ ;
Hasnip, PJ ;
Probert, MJ ;
Refson, K ;
Payne, MC .
ZEITSCHRIFT FUR KRISTALLOGRAPHIE, 2005, 220 (5-6) :567-570
[5]   Migration and Localization of Metal Atoms on Strained Graphene [J].
Cretu, Ovidiu ;
Krasheninnikov, Arkady V. ;
Rodriguez-Manzo, Julio A. ;
Sun, Litao ;
Nieminen, Risto M. ;
Banhart, Florian .
PHYSICAL REVIEW LETTERS, 2010, 105 (19)
[6]   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
[7]   General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities [J].
Fei, Huilong ;
Dong, Juncai ;
Feng, Yexin ;
Allen, Christopher S. ;
Wan, Chengzhang ;
Volosskiy, Boris ;
Li, Mufan ;
Zhao, Zipeng ;
Wang, Yiliu ;
Sun, Hongtao ;
An, Pengfei ;
Chen, Wenxing ;
Guo, Zhiying ;
Lee, Chain ;
Chen, Dongliang ;
Shakir, Imran ;
Liu, Mingjie ;
Hu, Tiandou ;
Li, Yadong ;
Kirkland, Angus I. ;
Duan, Xiangfeng ;
Huang, Yu .
NATURE CATALYSIS, 2018, 1 (01) :63-72
[8]   Facile Synthesis of Kilogram-Scale Co-Alloyed Pt Single-Atom Catalysts via Ball Milling for Hydrodeoxygenation of 5-Hydroxymethylfurfural [J].
Gan, Tao ;
Liu, Yifei ;
He, Qian ;
Zhang, Hao ;
He, Xiaohui ;
Ji, Hongbing .
ACS SUSTAINABLE CHEMISTRY & ENGINEERING, 2020, 8 (23) :8692-8699
[9]   Unveiling the kilogram-scale gold single-atom catalysts via ball milling for preferential oxidation of CO in excess hydrogen [J].
Gan, Tao ;
He, Qian ;
Zhang, Hao ;
Xiao, Huajian ;
Liu, Yifei ;
Zhang, Ying ;
He, Xiaohui ;
Ji, Hongbing .
CHEMICAL ENGINEERING JOURNAL, 2020, 389
[10]   Catalyst deactivation via decomposition into single atoms and the role of metal loading [J].
Goodman, Emmett D. ;
Johnston-Peck, Aaron C. ;
Dietze, Elisabeth M. ;
Wrasman, Cody J. ;
Hoffman, Adam S. ;
Abild-Pedersen, Frank ;
Bare, Simon R. ;
Plessow, Philipp N. ;
Cargnello, Matteo .
NATURE CATALYSIS, 2019, 2 (09) :748-755