Single-atom catalysts on metal-based supports for solar photoreduction catalysis

doi:10.1016/S1872-2067(21)63918-9

Abstract

Abstract:

Metal atoms atomically dispersed on an inorganic metal-based support compose a unique category of single atom catalysts (SACs) and have important applications in catalytic photoreduction reactions, including H₂ evolution reaction, CO₂ reduction reaction, and N₂ reduction reaction. In this minreview, we summarized the typical metal-support interaction (M-SI) patterns for successful anchoring of single-atom metals on metallic compound supports. Subsequently, the contribution of the dispersed single metal atoms and M-SI to photocatalytic reactions with improved activity, selectivity, and stability are highlighted, such as by accelerating charge transfer, regulating band structure of the support, acting as the reductive sites, and/or increasing catalytic selectivity. Finally, some challenges and perspectives of future development are proposed. We anticipate that this minireview will be a beneficial supplement for a comprehensive perception of metal-based material supported SACs and their application in heterogeneous photo-reductive catalysis.

Key words: Single atom catalyst, Metal-based support, Metal-support interaction, Photocatalysis, Solar energy conversion

Huayang Zhang, Wenjie Tian, Xiaoguang Duan, Hongqi Sun, Yingping Huang, Yanfen Fang, Shaobin Wang. Single-atom catalysts on metal-based supports for solar photoreduction catalysis[J]. Chinese Journal of Catalysis, 2022, 43(9): 2301-2315.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63918-9

https://www.cjcatal.com/EN/Y2022/V43/I9/2301

Figures/Tables 6

Fig. 1. (a) Schematic illustration of M-SI patterns for anchoring SA metals on metal-based supports. (b) The contributions of SA metals on metal-based supports for enhanced photocatalytic HER, CRR, and NRR.

Fig. 2. (a-c) Loading of SA metals via SCUS: (a) STM image of Pt species deposited CeO2 (111) surface (Pt single atom at the step edges (bright edges); Pt clusters on the Ovs (bright dots)). Adapted with permission from Ref. [23], Copyright 2016, Springer Nature. (b,c) High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) images of Pt SAs located on different Ovs of TiO2 (110) surface. Adapted with permission from Ref. [29], Copyright 2014, American Chemical Society. (d) Underpotential electrodeposition process for anchoring Mo SAs on an inert S site of MoS2. Adapted with permission from Ref. [19], Copyright 2020, Springer Nature. (e) SA metal loading via a bridging ligand. The -SH in L-cysteine bridged with Au clusters, while the C groups in L-cysteine coordinated with SA metal cations (Au-C-M). Adapted with permission from Ref. [36], Copyright 2018, American Chemical Society. (f) SA metal loading via spatial confinement. Interaction between [PtCl4]2- and surface cavities for confining the Pt SAs. Adapted with permission from Ref. [37], Copyright 2020, Springer Nature.

Fig. 3. (a) The synthesis process of defective TiO2 nanotube supported Pt SAs. (b) HAADF-STEM of Pt SAs/defective TiO2. Pt SAs marked by the circles, scale bar: 2 nm. (c) HER performance of Pt SAs/TiO2 in 2 h under UV/Vis light; sacrificial electron donor: CH3OH. (a-c) Adapted with permission from Ref. [79], Copyright 2020, Wiley-VCH. (d) Selective photo-deposition of Pt SAs on (101) facet of TiO2 for HER. (e) Size distribution of Pt SAs on TiO2 single-crystal (TiO2-A) and Pt NPs on commercial TiO2 (TiO2-0); and (f) photocatalytic HER with TiO2-A, Pt1/TiO2-A, and Pt/TiO2-0. (d-f) Adapted with permission from Ref. [81]. Copyright 2017, Elsevier. (g) Photocatalytic HER performance comparison over Pt SAs, Pt NPs loaded CdS, and pristine CdS. Adapted with permission from Ref. [22]. Copyright 2018, Elsevier.

Fig. 4. (a) Photos of Cu SAs/TiO2 film in different states of a photoactivation cycle. (b) Related photoactivation cycle. (c) Photocatalytic HER rates of different types of SAs on TiO2 with same loading 0.75 wt%. (a-c) Adapted with permission from Ref. [96], Copyright 2019, Springer Nature. (d) Molten-salt-mediated anchoring of Ni SAs on TiO2. (e) Free energy versus the H* of different active sites; HER performance of Ni-SAs/TiO2 (f) and its comparison with Ni-NP/TiO2, and Pt/TiO2 (g) with the same loading amount (ca. 0.5 wt%). (d-f) Adapted with permission from Ref. [90], Copyright 2020, Wiley-VCH.

Fig. 5. (a,b) TEM and illustration of single Ag chain in the lattice channel of MnO2 (Ag-HMO). (c) Photocatalytic CRR comparison of HMO, Ag/HMO and Ag-HMO. (a-c) Adapted with permission from Ref. [62,106]. Copyright 2019, Elsevier. (d) TEM image of Pd7Cu1-TiO2. (e) Average production rates of CH4 and CO in photocatalytic CRR with H2O by bare TiO2, Pd, and PdxCu1 with different ratios. (d,e) Adapted with permission from Ref. [50]. Copyright 2019, American Chemical Society. (f) Proposed reaction pathways for photocatalytic CRR over Cu SAs-mTiO2. (g) Photocatalytic CRR results of mTiO2 and 1Cu SAs-mTiO2. (f,g) Adapted with permission from Ref. [107]. Copyright 2019, American Chemical Society. (h) Energy band positions for CdS QDs and Ni:CdS QDs for the CO2 reduction potentials (pH = 7); Illustration (i) and photocatalytic CRR comparison (j) of Ni2+ species on QDs with the different anchoring modes. (k) Cycling production of CH4 and CO using Ni (0.26%):CdS QDs. (h-k) Adapted with permission from Ref. [47]. Copyright 2018, Wiley-VCH.

Fig. 6. (a,b) HAADF-STEM images of Ru-SAs/Def-TiO2; Photoexcited electron transfer involved in Ru-SAs/Def-TNs (c), and Ru-NPs/Def-TNs (d). (a-d) Adapted with permission from Ref. [123]. Copyright 2020, American Chemical Society. (e) STEM images of Fe-T-S with 2% loading amount; Photocatalytic H2 and O2 evolution (f), and NRR (g) of different samples under 300 W Xe lamp irradiation. (e-g) Adapted with permission from Ref. [124]. Copyright 2020, American Chemical Society. (h) Illustration for the synthesis of Mo-doped W18O49 ultrathin nanowires. (i) Photocatalytic NH3 production rates by different samples, using Na2SO3 as a sacrificial agent and under full-spectrum or visible-NIR light (λ > 400 nm) irradiation. (h,i) Adapted with permission from Ref. [125]. Copyright 2018, American Chemical Society.

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