Heterogeneous N-coordinated single-atom photocatalysts and electrocatalysts

doi:10.1016/S1872-2067(22)64104-4

Chinese Journal of Catalysis ›› 2022, Vol. 43 ›› Issue (10): 2453-2483.DOI: 10.1016/S1872-2067(22)64104-4

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Heterogeneous N-coordinated single-atom photocatalysts and electrocatalysts

Rongchen Shen^a, Lei Hao^a, Yun Hau Ng^b^,^c^,^#(), Peng Zhang^d, Arramel Arramel^e^,^f, Youji Li^g, Xin Li^a^,^*()

^aInstitute of Biomass Engineering, Key Laboratory of Energy Plants Resource and Utilization Ministry of Agriculture, South China Agricultural University, Guangzhou 511443, Guangdong, China
^bSchool of Energy and Environment, City University of Hong Kong, Hong Kong, China
^cShenzhen Research Institute, City University of Hong Kong, Shenzhen Hi-Tech Industrial Park, Shenzhen 518057, Guangdong, China
^dState Centre for International Cooperation on Designer Low-Carbon & Environmental Materials (CDLCEM), School of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450001, Henan, China
^eDepartment of Physics, National University of Singapore, Singapore 117551, Singapore
^fNano Center Indonesia, Jl. PUSPIPTEK South Tangerang, Banten 15314, Indonesia
^gCollege of Chemistry and Chemical Engineering, Jishou University, Jishou 416000, Hunan, China

Received:2022-01-26 Accepted:2022-02-09 Online:2022-10-18 Published:2022-09-30
Contact: Yun Hau Ng, Xin Li
About author:Yun Hau Ng is an associate professor in the School of Energy and Environment, City University of Hong Kong. He received his PhD from Osaka University in 2009. Before joining City University of Hong Kong, he was a lecturer (2014) and senior lecturer (2016) in the School of Chemical Engineering, University of New South Wales. His research is focused on the development of novel photoactive semiconductors for sunlight energy conversion. He received the 2021 Kataoka Lectureship Award for Asian and Oceanian Photochemist, the APEC ASPIRE Prize in 2019, Distinguished Lectureship Award from the Chemical Society of Japan in 2018, and Honda-Fujishima Prize by the Electrochemical Society of Japan in 2013.
Xin Li received his B.S. and PhD degrees in Chemical Engineering from Zhengzhou University in 2002 and South China University of Technology in 2007, respectively. Then, he joined South China Agricultural University as a faculty staff member, and became a professor in 2017. During 2012 and 2019, he worked as a visiting scholar at the Electrochemistry Center, the University of Texas at Austin, and Department of Chemistry, the University of Utah, respectively. His research interests include photocatalysis, photoelectrochemistry, adsorption, biomass engineering and the related materials and devices development (see http://www.researcherid.com/rid/A-2698-2011).
Supported by:
National Natural Science Foundation of China(21975084);National Natural Science Foundation of China(51672089);National Natural Science Foundation of China(51972287);National Natural Science Foundation of China(U2004172);National Natural Science Foundation of China(51502269);Natural Science Foundation of Guangdong Province(2021A1515010075);General Program of Science and Technology Innovation Committee of Shenzhen Municipality(JCYJ20190808181805621);Hong Kong Research Grant Council (RGC) General Research Fund(GRF 11305419)

Abstract

Abstract:

Single-atom catalysts (SACs) have been widely used in heterogeneous catalysis owing to the maximum utilization of metal-active sites with controlled structures and well-defined locations. Upon tailored coordination with nitrogen atom, the metal-nitrogen (M-N)-based SACs have demonstrated interesting physical, optical and electronic properties and have become intense in photocatalysis and electrocatalysis in the past decade. Despite substantial efforts in constructing various M-N-based SACs, the principles for modulating the intrinsic photocatalytic and electrocatalytic performance of their active sites and catalytic mechanism have not been sufficiently studied. Herein, the present review intends to shed some light on recent research made in studying the correlation between intrinsic electronic structure, catalytic mechanism, single-metal atom (SMA) confinement and their photocatalytic and electrocatalytic activities (conversion, selectivity, stability and etc). Based on the analysis of fundamentals of M-N-based SACs, theoretical calculations and experimental investigations, including synthetic methods and characterization techniques, are both included to provide an integral understanding of the underlying mechanisms behind improved coordination structure and observed activity. Finally, the challenges and perspectives for constructing highly active M-N based photocatalysis and electrocatalysis SACs are provided. In particular, extensive technical and mechanism aspects are thoroughly discussed, summarized and analyzed for promoting further advancement of M-N-based SACs in photocatalysis and electrocatalysis.

Key words: N-coordinated single-atom catalyst, Photocatalysis, Electrocatalysis, Electronic structure, Active site

Rongchen Shen, Lei Hao, Yun Hau Ng, Peng Zhang, Arramel Arramel, Youji Li, Xin Li. Heterogeneous N-coordinated single-atom photocatalysts and electrocatalysts[J]. Chinese Journal of Catalysis, 2022, 43(10): 2453-2483.

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Figures/Tables 33

Fig. 1. (a) Number of publications since 2010 on SAC-based photocatalysts involving the use of “photocatalytic*” and “single-atom catalysts*” as the two topical keywords. (b) Number of publications since 2010 on SAC-based electrocatalysts involving the use of “*electrocatalytic*” and “SMAs*” as the two topical keywords. (Adapted from ISI Web of Science Core Collection, date of search: March 15, 2022).

Fig. 2. Schematic illustrations of approaches for dispersing single atoms on supports.

Fig. 3. Advantages of M-N-based photo(electro)catalysis.

Fig. 4. The involved supports in M-N-based SACs.

Fig. 5. Advantages and necessary conditions for different synthesis methods of N-M-based SACs.

Fig. 6. Schematic illustration of the synthetic process for the (a) FeN4 catalyst. Reprinted with permission from Ref. [117]. Copyright 2017, American Chemical Society. (b) Co-Nx catalyst sand. Reprinted with permission from Ref. [118]. Copyright 2016, John Wiley and Sons. (c) Ru3/CN catalysts. Reprinted with permission from Ref. [119]. Copyright 2017, American Chemical Society.

Fig. 7. Schematic illustration of the synthetic procedure of SMAs@N-doped graphene (a), Fe-, N-, and B-doped FeBNC catalysts (b), and Fe-ISA/SNC (c). Reprinted with permission from Ref. [132]. Copyright 2018, American Chemical Society.

Fig. 9. (a) Synthesis process of Al‐TCPP‐Pt. Reprinted with permission from Ref. [140]. Copyright 2018, John Wiley and Sons. (b) Synthesis process of the Fe-N4 SACs/NPC. Reprinted with permission from Ref. [92]. Copyright 2018, John Wiley and Sons. (c) Synthesis process of metal-5,10,15,20-tetra(4-pyridyl)21H,23H-porp M1-TPyP. Reprinted with permission from Ref. [56]. American Chemical Society. (d) Synthesis process of Co-N5/HNPCSs with N in N-doped carbon as a coordination site. Reprinted with permission from Ref. [88]. Copyright 2018, American Chemical Society.

Fig. 10. (a) Formation of the MCM-2. Reprinted with permission from Ref. [57]. Copyright 2017, Springer Nature. (b) View of the 3D network of MOF‐525‐Co featuring a highly porous framework and incorporated active sites. Reprinted with permission from Ref. [89]. Copyright 2016, John Wiley and Sons. (c) Synthesis processes of HNTM and HNTM-M, respectively. Reprinted with permission from Ref. [58]. Copyright 2018, John Wiley and Sons.

Fig. 11. (a) HAADF-STEM image of Pt-CN. Reprinted with permission from Ref. [143]. Copyright 2016, John Wiley and Sons. (b) HR-STEM images of Ni-LixWSy and the pixel grid where EELS mapping was obtained. Reprinted with permission from Ref. [164]. Copyright 2020, American Chemical Society.

Fig. 12. (a) XANES result of the Co1-G sample. (b) k3-weighted Fourier-transform Co K-edge EXAFS result. Reprinted with permission from Ref. [90]. Copyright 2018, John Wiley and Sons. Low temperature (c) and simulated (d) STM images of FeN4/G. (e) dI/dV spectra acquired along the white line in the inset image. Reprinted with permission from Ref. [167]. Copyright 2015, Science.

Fig. 13. (a) Fourier-transform fitting result for PtSA/CN. (b) The calculated density of state for the surface of Pt-clusters/CN; time-resolved fluorescence spectra (c) and turnover frequency (d) of as-prepared samples. Reprinted with permission from Ref. [144]. Copyright 2018, American Chemical Society.

Fig. 14. (a) Structural illustration of gCN-Pt2. UV-vis absorption spectra (b) and average hydrogen-evolution rate (c) of gCN-Pt2+. (d) Photoexcited charge density transition from the Pt2+-induced hybrid HOMO states. (e) Schematic illustration of the working mechanism. Reprinted with permission from Ref. [184]. Copyright 2016, John Wiley and Sons.

Fig. 15. Synchronous illumination of high-resolution XPS spectrum of C 1s (a), N 1s (b), and Pt 4f (c) for Pt-gCN; VB XPS spectra of Pt-C3N4 (SACs) (d) and M-Pt-C3N4 (NPs) (e) under light and dark conditions. (f) Illustration of the charge transfer and bond variation in gCN. Reprinted with permission from Ref. [6]. Copyright 2020, John Wiley and Sons.

Fig. 16. (a) Structural illustration of Co1-N4. (b) Proposed photocatalytic H2 evolution mechanism. (c) Average exciton lifetime of prepared samples. Reprinted with permission from Ref. [185]. Copyright 2017, John Wiley and Sons.

Fig. 17. (a) Structural illustration of CN-0.2Ni-HO. Ni K-edge XANES profiles (b), fitting results (c)-(f) of FT-EXAFS of as-prepared samples. DOS (g) and UV-vis spectrum (h) of CN and CN-0.2Ni-HO. (i) Average hydrogen-evolution rate of as-prepared samples. Reprinted with permission from Ref. [186]. Copyright 2020, John Wiley and Sons.

Fig. 18. (a) The EXAFS fitting curve of Au-gCN. (b) CO2 temperature-programmed desorption of as-prepared samples. (c) The proposed illustration of electron distribution and the CO2 reduction process of Au-gCN under visible-light irradiation. (d) The generated CO and CH4 amount over as-prepared samples. Reprinted with permission from Ref. [199]. Copyright 2020, John Wiley and Sons.

Fig. 19. (a) The R space of LD-Er1/CN-NT, Er (yellow), N (blue), and C (green). (b) XANES spectra of the as-prepared samples. (c) Er L3-edge XANES spectra of as-prepared photocatalysts during photocatalytic CO2 reduction reaction. (d) improvement of CO and CH4 evolution over the as-prepared samples. Reprinted with permission from Ref. [159]. Copyright 2020, John Wiley and Sons.

Fig. 20. (a) XANES spectra of samples. (b) EXAFS fitting curves of samples. (c) CO2 photoreduction activities of samples. (d) Charge density difference of CO adsorbed on the N4-C and Fe-N4-C surfaces. (e) Free-energy diagram for CRR. (f) Free-energy diagram for HER. Reprinted with permission from Ref. [201]. Copyright 2020, American Chemical Society.

Fig. 21. (a) Proposed configuration of Cu-gCN. (b) In situ FTIR spectra of Cu-gCN. ESR spectrum of samples before (c) and during (d) light irradiation. Top view (e) and side view (f) of the electron density distribution. Reprinted with permission from Ref. [204]. Copyright 2018, Springer Nature.

Fig. 22. (a) Structural illustration of Pt-SACs/CTF. (b) Band diagram of as-prepared samples. (c) Schematic of the band level for Pt-SACs/CTF. (d) Free-energy profiles of the nitrogen reduction process. Reprinted with permission from Ref. [205]. Copyright 2020, American Chemical Society.

Fig. 23. (a) FT-EXAFS curves of Mo-PCN. (b) Structural model of Mo-PCN. (c) Optimized N2 adsorption model on pure PCN and Mo-PCN. (d) photocatalytic performance of samples. (e) Time-resolved fluorescence kinetics. Reprinted with permission from Ref. [206]. Copyright 2019, Royal Society of Chemistry.

Fig. 24. (a) HAADF-STEM image of the samples. Scale bar, 1 nm. (b) Tafel plots of the polarization curves. (c) Polarization curves of the samples. (d) LSV of the samples in 0.5 mol L?1 H2SO4. Reprinted with permission from Ref. [212]. Copyright 2015, Springer Nature. Licensed under Creative commons attribution 3.0 Unported License (http://creativecommons.org/licenses/by/4.0/).

Fig. 25. (a) Structural model of sample. (b) k3-weighted FTEXAFS curves of samples. (c) Co K-edge XANES spectra of samples at different potentials for HER catalysis. (d) k FT-EXAFS at different potentials. (e) ΔGH* of H adsorption on the surface of samples. (f) Electronic structure of Co1P1N3 conﬁguration. (g) HER polarization curves of samples. (H) Overpotentials of samples. (i) Tafel plots of samples. Reprinted with permission from Ref. [214]. Copyright 2020, American Chemical Society.

Fig. 26. (a) Structural model of Cu/Ru@GN. (b) FT-EXAFS Cu K-edge signals for samples. (c) Steady-state polarization curves in 0.5 mol L?1 H2SO4. (d) Electrocatalytic OER. The corresponding FT-EXAFS spectra of Cu/Ru@GN (d) and Ru@GN (e). (f) H adsorption free energies (ΔGH*) on Ru (0001) regarding H* coverage (ML). Reprinted with permission from Ref. [215]. Copyright 2020, Elsevier.

Fig. 27. (a) Free-energy diagram of OER on Co-gCN. (b) OER polarization curves of prepared samples. (c) Electron density differences on Co-gCN. (d) D-band DOS of different transition metal-embedded gCN models. EF indicates the Fermi level. (e) Side and top views of the electron density distribution. Reprinted with permission from Ref. [95]. Copyright 2017, American Chemical Society.

Fig. 28. LSVs (a), Tafel slope (b), and ECSA-normalized activity (c) of samples in different solutions. (d) Proposed model for the samples. Reprinted with permission from Ref. [120]. Copyright 2019, American Chemical Society.

Fig. 29. (a) Formation of the MCM-2 of the samples. (b) the calculated PDOS of the samples. (c) ORR performance of as-prepared samples. Reprinted with permission from Ref. [217]. Copyright 2019, American Chemical Society.

Fig. 30. (a) Structure of the as-prepared samples. (b) OER polarization curves of the as-prepared samples. Free-energy diagram of the OER process on Co-C3N4@CS (c) and Co-O-C3N4@CS (d) surfaces. Reprinted with permission from Ref. [218]. Copyright 2020, American Chemical Society.

Fig. 31. (a) Schematic illustration of the formation of O single-atom Ni catalysts. Faradaic efficiency (b), turnover frequency (c), and Free-energy diagram (d) of CO2 reduction to CO over NiSA-Nx-C. Reprinted with permission from Ref. [233]. Copyright 2019, John Wiley and Sons.

Fig. 32. Ni K-edge XANES spectra of samples under Ar (a) and CO2 (b). Raman spectra of Ni-TAPc under Ar (c) and CO2 (d). (e) Proposed CO2 reduction pathway. Reprinted with permission from Ref. [234]. Copyright 2019, John Wiley and Sons.

Fig. 33. The involved support M-N-based SACs.

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Heterogeneous N-coordinated single-atom photocatalysts and electrocatalysts

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