| Single-Atom Catalysts through Pressure-Controlled Metal Diffusion | |
AlHilfi, Samir H1,2; Jiang XK(蒋玺恺)3; Heuer, Julian2; Akula, Srinu4; Tammeveski, Kaido4; Hu, Guoqing5 ; Yang, Juan1; Wang, Hai I2,6; Bonn, Mischa2; Landfester, Katharina2; Muellen, Klaus2; Zhou, Yazhou1,2
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| Corresponding Author | Bonn, Mischa([email protected]) ; Muellen, Klaus() ; Zhou, Yazhou([email protected]) |
| Source Publication | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
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| 2024-07-11 | |
| Volume | 146Issue:29Pages:19886-19895 |
| ISSN | 0002-7863 |
| Abstract | 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. |
| DOI | 10.1021/jacs.4c03066 |
| Indexed By | SCI ; EI |
| Language | 英语 |
| WOS ID | WOS:001266684200001 |
| WOS Keyword | ARYL HALIDES ; IDENTIFICATION ; COMPLEXES ; AMINATION ; EFFICIENT ; SITES |
| WOS Research Area | Chemistry |
| WOS Subject | Chemistry, Multidisciplinary |
| Funding Project | Natural Science Foundation of China[51702129] ; Natural Science Foundation of China[51972150] ; DFG[514772236] ; Estonian Research Council[PRG723] ; EU through the European Regional Development Fund[MOBJD671] ; EU through the European Regional Development Fund[TK141] |
| Funding Organization | Natural Science Foundation of China ; DFG ; Estonian Research Council ; EU through the European Regional Development Fund |
| Classification | 一类 |
| Ranking | 2 |
| Contributor | Bonn, Mischa ; Muellen, Klaus ; Zhou, Yazhou |
| Citation statistics | |
| Document Type | 期刊论文 |
| Identifier | http://dspace.imech.ac.cn/handle/311007/95978 |
| Collection | 非线性力学国家重点实验室 |
| Affiliation | 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 |
| Recommended Citation GB/T 7714 | AlHilfi, Samir H,Jiang XK,Heuer, Julian,et al. Single-Atom Catalysts through Pressure-Controlled Metal Diffusion[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2024,146,29,:19886-19895.Rp_Au:Bonn, Mischa, Muellen, Klaus, Zhou, Yazhou |
| APA | AlHilfi, Samir H.,蒋玺恺.,Heuer, Julian.,Akula, Srinu.,Tammeveski, Kaido.,...&Zhou, Yazhou.(2024).Single-Atom Catalysts through Pressure-Controlled Metal Diffusion.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,146(29),19886-19895. |
| MLA | AlHilfi, Samir H,et al."Single-Atom Catalysts through Pressure-Controlled Metal Diffusion".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 146.29(2024):19886-19895. |
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