Progress in the mass production of single-atom catalysts

doi:10.11949/0438-1157.20221574

Abstract

Abstract:

Single-atom catalysts (SACs) have the advantages of clear active sites (like homogeneous catalysts) and easy separation (like heterogeneous catalysts), which are regarded as the bridge between traditional homogeneous and heterogeneous catalysis. SACs exhibit excellent catalytic performance in a series of important reactions due to their high utilization of metal species and unique electronic/geometric structure, and have a great prospect of industrial application. The preparation scale of single-atom catalysts reported so far is still mostly limited to the gram or even milligram level, which is far from meeting the needs of future industrial applications. This review describes two typical synthesis strategies for large-scale preparation of SACs: batch type (e.g., pyrolysis, physical mixing, and gas migration) and continuous type (e.g., microencapsulation, precursor atomization, photochemical synthesis, two-stage microreactor, and electric field-assisted synthesis). It provides reference for industrial production and application of SACs.

Key words: mass production, single-atom catalysts, mass transfer, heat transfer, nanomaterial

摘要：

单原子催化剂兼备均相催化剂活性中心明确和多相催化剂易于分离等优点，被视为传统均相催化和多相催化之间的桥梁。单原子催化剂所具备的高原子利用率和独特的电子-几何结构等特性，使其在一系列重要反应中表现出相当优异的催化性能，具有较好的工业化应用前景。但目前报道的单原子催化剂的制备量级仍大多局限在克级甚至毫克级，远不能满足未来的工业应用需求。本文介绍了目前间歇式(热解法、物理混合法和气体迁移法)和连续式(前体微胶囊法、前体雾化法、光化学合成法、两段式微反应器法和电场辅助合成法)这两种大规模制备单原子催化剂的典型合成策略，可为单原子催化剂的工业化生产和应用提供借鉴。

关键词: 规模化制备, 单原子催化剂, 传质, 传热, 纳米材料

CLC Number:

TQ 13

Hao ZHANG, Ziyue WANG, Yujie CHENG, Xiaohui HE, Hongbing JI. Progress in the mass production of single-atom catalysts[J]. CIESC Journal, 2023, 74(1): 276-289.

张浩, 王子悦, 程钰洁, 何晓辉, 纪红兵. 单原子催化剂规模化制备的研究进展[J]. 化工学报, 2023, 74(1): 276-289.

Figures/Tables 11

Fig.1 Synthesis diagram of the synthesis of Sn δ+ single-atom catalyst (a); TEM image of Sn δ+ single-atom catalyst (b); AC HAADF-STEM image of Sn δ+ single-atom catalyst (c); FT-EXAFS spectra of Sn δ+ single-atom catalyst (d) [44]

Fig.2 Schematic diagram of the ligand-mediated strategy for the synthesis of single-atom catalysts (a); AC HAADF-STEM images of different Ni single-atom catalysts with 2.5% (b), 3.4% (c), 4.5% (d), and 5.3% (e) Ni loding; Photograph of a large-scale 2.5% metal-loaded Ni single-atom catalyst (f) [47]; Strategy for the preparation of UHD-SACs (g)[47-48]

Fig.3 Schematic diagram of the synthesis of Pd1/ZnO (a); AC HAADF-STEM images of different scales of Pd1/ZnO (b); FT-EXAFS spectra of Pd1/ZnO-10 and Pd1/ZnO-1000 (c); Pictures of different scales of single-atom catalysts (d) [53]

Fig.4 Schematic diagram of the synthesis of Pt1/Co (a); AC HAADF-STEM images of Pt1/Co and Pt1/Co-1000 [(b),(c)]; AC HAADF-STEM images of different scales of single-atom catalysts (d); AC HAADF-STEM images of different types of single-atom catalysts (e) [55-57]

Fig.5 Schematic diagram of the synthesis of kilogram-scale Ru single-atom catalysts (a); STEM image of Ru1/MAFO (b); AC HAADF-STEM images of Ru1/MAFO[ (c), (d)] [59]

Fig.6 Schematic diagram of gas migration method (a) and single-atom catalyst formation mechanism (b) [62]

Fig.7 Schematic diagram of the experimental setup and formation mechanism of the gas migration strategy (a); AC HAADF-STEM image of Cu1/N-C [(b), (c)]; FT-EXAFS spectra of Cu1/N-C (d) [67]

Fig.8 Schematic diagram for the quasi-continuous synthesis of Fe/SNC (a); Scanning electron microscopy image of microcapsules (b); AC AC HAADF-STEM image of Fe/SNC (c), Co/SNC (d), and Ni/SNC (e) [68]

Fig.9 Experimental plot of the preparation of Pd1/FeO x (a); Single-atom catalyst synthesis production line (b); AC HAADF-STEM image of Pd1/FeO x from different synthesis batches [(c)-(f)]; FT-EXAFS spectra of Pd1/FeO x -1 and Pd1/FeO x -4 (g)[70]

Fig.10 Scheme for the continuous synthesis of Pd1/TiO2 (a); STEM-EDS elemental mapping of a single Pd1/TiO2 nanosheet (b); AC HAADF-STEM image of Pd1/TiO2 (c) [2]

Fig.11 Schematic of the continuous synthesis of catalysts (a); Histogram of particle size distribution of catalysts (b); AC HAADF-STEM image of Rh single-atom catalyst (c)[71]

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