Single-Atom Catalysts through Pressure-Controlled Metal Diffusion

被引:9
作者
Al-Hilfi, Samir H. [1 ,2 ]
Jiang, Xikai [3 ]
Heuer, Julian [2 ]
Akula, Srinu [4 ]
Tammeveski, Kaido [4 ]
Hu, Guoqing [5 ]
Yang, Juan [1 ]
Wang, Hai. I. [2 ,6 ]
Bonn, Mischa [2 ]
Landfester, Katharina [2 ]
Muellen, Klaus [2 ]
Zhou, Yazhou [1 ,2 ]
机构
[1] Jiangsu Univ, Sch Mat Sci & Engn, Zhenjiang 212013, Jiangsu, Peoples R China
[2] Max Planck Inst Polymer Res, D-55128 Mainz, Germany
[3] Chinese Acad Sci, Inst Mech, State Key Lab Nonlinear Mech, Beijing 100190, Peoples R China
[4] Univ Tartu, Inst Chem, EE-50411 Tartu, Estonia
[5] Zhejiang Univ, Dept Engn Mech, State Key Lab Fluid Power & Mechatron Syst, Hangzhou 310027, Zhejiang, Peoples R China
[6] Univ Utrecht, Debye Inst Nanomat Sci, Nanophoton, NL-3584 CC Utrecht, Netherlands
关键词
ARYL HALIDES; IDENTIFICATION; COMPLEXES; AMINATION; EFFICIENT; SITES;
D O I
10.1021/jacs.4c03066
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Single-atom catalysts (SACs) open up new possibilities for advanced technologies. However, a major complication in preparing high-density single-atom sites is the aggregation of single atoms into clusters. This complication stems from the delicate balance between the diffusion and stabilization of metal atoms during pyrolysis. Here, we present pressure-controlled metal diffusion as a new concept for fabricating ultra-high-density SACs. Reducing the pressure inhibits aggregation substantially, resulting in almost three times higher single-atom loadings than those obtained at ambient pressure. Molecular dynamics and computational fluid dynamics simulations reveal the role of a metal hopping mechanism, maximizing the metal atom distribution through an increased probability of metal-ligand binding. The investigation of the active site density by electrocatalytic oxygen reduction validates the robustness of our approach. The first realization of Ullmann-type carbon-oxygen couplings catalyzed on single Cu sites demonstrates further options for efficient heterogeneous catalysis.
引用
收藏
页码:19886 / 19895
页数:10
相关论文
共 63 条
  • [1] Mechanistic studies of the palladium-catalyzed amination of aryl halides and the oxidative addition of aryl bromides to Pd(BINAP)2 and Pd(DPPF)2:: An unusual case of zero-order kinetic behavior and product inhibition
    Alcazar-Roman, LM
    Hartwig, JF
    Rheingold, AL
    Liable-Sands, LM
    Guzei, IA
    [J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2000, 122 (19) : 4618 - 4630
  • [2] Allen M. P., 2017, COMPUTER SIMULATIONO, DOI [10.1093/oso/9780198803195.001.0001, DOI 10.1093/OSO/9780198803195.001.0001]
  • [3] Molecular dynamics simulation of rotating carbon nanotube in uniform liquid argon flow
    Arabghahestani, M.
    Karimian, S. M. H.
    [J]. JOURNAL OF MOLECULAR LIQUIDS, 2017, 225 : 357 - 364
  • [4] Copper(I)-creatine complex on magnetic nanoparticles as a green catalyst for N- and O-arylation in deep eutectic solvent
    Bagheri, Sepideh
    Pazoki, Farzane
    Radfar, Iman
    Heydari, Akbar
    [J]. APPLIED ORGANOMETALLIC CHEMISTRY, 2020, 34 (03)
  • [5] Bird R.B., 2002, Appl. Mech. Rev., V55, pR1, DOI DOI 10.1115/1.1424298
  • [6] Expanding the medicinal chemistry synthetic toolbox
    Bostrom, Jonas
    Brown, Dean G.
    Young, Robert J.
    Keseru, Gyorgy M.
    [J]. NATURE REVIEWS DRUG DISCOVERY, 2018, 17 (10) : 709 - 727
  • [7] Single-Atom Catalysts: Synthetic Strategies and Electrochemical Applications
    Chen, Yuanjun
    Ji, Shufang
    Chen, Chen
    Peng, Qing
    Wang, Dingsheng
    Li, Yadong
    [J]. JOULE, 2018, 2 (07) : 1242 - 1264
  • [8] Dobkin D. M., 2003, PRINCIPLES CHEM VAPO, DOI [10.1007/978-94-017-0369-7, DOI 10.1007/978-94-017-0369-7]
  • [9] General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities
    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
    [J]. NATURE CATALYSIS, 2018, 1 (01): : 63 - 72
  • [10] Single-Atom Catalysts Designed and Prepared by the Atomic Layer Deposition Technique
    Fonseca, Javier
    Lu, Junling
    [J]. ACS CATALYSIS, 2021, 11 (12) : 7018 - 7059