高等学校化学学报 ›› 2022, Vol. 43 ›› Issue (5): 20220043.doi: 10.7503/cjcu20220043
收稿日期:
2022-01-18
出版日期:
2022-05-10
发布日期:
2022-02-22
通讯作者:
王定胜
E-mail:wangdingsheng@mail.tsinghua.edu.cn
基金资助:
ZHUANG Jiahao, WANG Dingsheng()
Received:
2022-01-18
Online:
2022-05-10
Published:
2022-02-22
Contact:
WANG Dingsheng
E-mail:wangdingsheng@mail.tsinghua.edu.cn
Supported by:
摘要:
单原子催化剂(SACs)兼具均相与多相催化剂的双重优势, 表现出最大化的原子利用率、 超高的本征活性与选择性以及易与产物分离的特点, 受到人们的广泛关注. 然而, 由于单个原子较高的表面能以及不稳定性, 设计与制备单原子催化剂仍是一大挑战. 本文综合评述了近年来单原子催化剂的稳定化策略、 高载量催化剂的制备方法以及批量制备技术等方面的关键研究进展, 并简要分析了单原子催化剂未来发展所面临的问题与挑战, 最后对单原子催化的发展方向进行了展望.
中图分类号:
TrendMD:
庄嘉豪, 王定胜. 单原子催化的关键进展与未来挑战. 高等学校化学学报, 2022, 43(5): 20220043.
ZHUANG Jiahao, WANG Dingsheng. Current Advances and Future Challenges of Single-atom Catalysis. Chem. J. Chinese Universities, 2022, 43(5): 20220043.
Fig.2 Stabilizing single metal atoms by non?metallic atom(A) ADF image of single niobium atoms(bright dots) doped in the carbon shell and theoretical simulation of charge flows from the niobium atom(blue) into the O atoms(yellow)[44]. Copyright 2013, Macmillan Publishers Limited. (B) Scheme of the formation of Co SAs/N-C[45]. Copyright 2016, Wiley-VCH. (C) Scheme of the transformation of nanoparticles to Pd single atoms[46]. Copyright 2018, Springer Nature. (D) Discharge polarization curves, power density plots, chemical state and atomic local structure of S-Cu-ISA/SNC[51]. Copyright 2020, Springer Nature.
Fig.3 Stabilizing single metal atoms by metal oxides(A) Schematic illustration of the atom?trapping process for preparing a single?atom Pt catalyst[55]. Copyright 2016, American Association for the Advancement of Science. (B) Synthesis process for isolated Au atoms stabilized on defective TiO2 nanosheets[56]. Copyright 2018, Wiley?VCH. (C) Schematic illustration of Au atoms anchored on ZnO layer?stacking ladder[58]. Copyright 2020, Elsevier. (D) Illustration of Pt NP sintering/dispersing on different supports[59]. Copyright 2019, Springer Nature.
Fig.4 Stabilizing single metal atoms by metal?metal bond(A) Atomically resolved elemental mapping of Ru1?Pt3Cu[68]. Copyright 2019, Springer Nature. (B) Models and catalytic performance of alkynes semi?hydrogenation reaction of Pd1/Cu(111) and Pd1/Cu(100) surface[69]. Copyright 2020, Springer Nature. (C) High?resolution STEM Z?contrast images and approaching “real” APRM of fresh and used Pt/α?MoC catalyst[71]. Copyright 2017, Springer Nature.
Fig.5 Synthesis of SACs with high metal loadings(A) AC?HAADF?STEM images and structure model of SAS?Fe[72]. Copyright 2020, Wiley?VCH. (B) The proposed method based on the crosslinking and self?assembly of GQDs[73]. Copyright 2021, Springer Nature. (C) Strategy for the preparation of UHD?SACs[74]. Copyright 2021, Springer Nature.
Fig.6 Vapor transport strategies for SACs preparation(A) Schematic of the top?down synthesis of the preparation of Cu?SAs/N?C[75]. Copyright 2018, Springer Nature. (B) AC?HAADF?STEM images of Ru1/MAFO?900 sample[76]. Copyright 2020, Springer Nature.
Fig.7 Solid synthesis strategies for SACs preparation(A) Scheme of the solid synthesis of Fe?doped?ZIF?8 crystal and carbonization for final Fe?N?C catalyst[77]. Copyright 2018, Wiley?VCH. (B) Fabrication process of Pd1/ZnO?10[83]. Copyright 2019, the authors.
Fig.9 In situ fine structure characterizations for SACs(A) In situ ETEM and in situ XRD characterization of the thermal transformation and surface reconstruction from AgNP/MnO2 to Ag1/MnO2[89]. Copyright 2020, Wiley?VCH. (B) In situ XAFS spectra change of the Ru K?edge[68]. Copyright 2019, Springer Nature.
Fig.10 Construction of complex single?atom system[95](A) O2 adsorption models and Gibbs free energy diagram for ORR on Fe?N4 and Fe?N4/Pt?N4; (B) synthesis process of Fe?N4/Pt?N4@NC. Copyright 2021, Wiley?VCH.
Fig.11 Unique catalytic performances of SACs(A) HAADF?STEM image, corresponding surface model and elemental mapping of RuNi1 NCs, and the histograms of mass activities of Pt/C, Ru, Ru?Ni, and RuNi1 before and after stability tests[97]. Copyright 2020, American Chemical Society. (B) Illustration of the preparation process of FeN3P?SAzyme, and cell viability of HepG2 hepatoma cells and time?dependent cell death with FeN3P? SAzyme, FeN4?SAzyme and Fe3O4 nanozyme[100]. Copyright 2021, Springer Nature.
Fig.12 Stability of SACs under reaction conditions(A) Schematic overview of the SACs evolution during CO oxidation[101]. Copyright 2021, Springer Nature. (B) The charge density differences and stability of FeCoN5P1 and FeCoN6[102]. Copyright 2021, Springer Nature.
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