Single-atom catalysts for the photocatalytic and electrocatalytic synthesis of hydrogen peroxide

doi:10.1016/S1872-2067(23)64498-5

Chinese Journal of Catalysis ›› 2023, Vol. 52: 79-98.DOI: 10.1016/S1872-2067(23)64498-5

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Single-atom catalysts for the photocatalytic and electrocatalytic synthesis of hydrogen peroxide

Xiaolong Tang^a^,^b, Feng Li^a^,^b, Fang Li^a, Yanbin Jiang^a^,^b^,^*(), Changlin Yu^a^,^*()

^aSchool of Chemical Engineering, Guangdong University of Petrochemical Technology, Maoming 525000, Guangdong, China
^bSchool of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510000, Guangdong, China

Received:2023-06-27 Accepted:2023-08-25 Online:2023-09-18 Published:2023-09-25
Contact: *E-mail: cebjiang@scut.edu.cn (Y. Jiang),yuchanglinjx@163.com (C. Yu).
About author:Yanbin Jiang (School of Chemistry and Chemical Engineering, South China University of Technology) was elected as a member of 2^th supercritical fluid technology committee, CIESC (2023‒2028). He received his B.A. degree from Beijing University of Chemical Technology (China) in 1992, and Ph.D. degree from South China University of Technology in 2000. He carried out postdoctoral research at Department of Chemical Engineering in Kyoto University (Japan) from 2003 to 2005. Since July 1995, he has been working in School of Chemistry and Chemical Engineering, South China University of Technology. He won the Science and Technology Award of Guangdong Province five times as a major completer (2000‒2015). His research interests mainly focus on chemical product engineering, especially separation engineering, process and particle technology. He has published more than 160 peer-reviewed papers.
Changlin Yu (School of Chemical Engineering, Guangdong University of Petrochemical Technology Maoming) received his B.S. in 2004 and Ph.D degree in 2007 from Hunan University Science and Technology and the Dalian Institute of Chemical Physics, Chinese Academy of Sciences, respectively. From 2007 to 2008, he did postdoctoral research at The Chinese University of Hongkong. At the end of 2008, he joined the Department School of Chemistry and Chemical Engineering, Jiangxi University of Science and Technology, Ganzhou. From 2012 to 2013, he worked as visiting scholar at Carnegie Mellon University. In 2019, He joined the Guangdong University of Petrochemical Technology and received the Guangdong Pearl River Scholar in 2019. His research interests currently focus on new materials and energy photocatalysis, electrocatalysis with emphasis on design of new catalysts and control of morphology, microstructure and reaction mechanism for hydrogen production, environmental pollutants degradation, etc. He is author or co-author of more than 220 peer-reviewed papers with over 10000 citations with an H-index of 52. He was invited as a member of the editorial board of Chin. J. Catal. Since 2021.
Supported by:
National Natural Science Foundation of China(22272034);National Natural Science Foundation of China(22102034);Guangdong Basic and Applied Basic Research Foundation(2022A1515011900);Guangdong Basic and Applied Basic Research Foundation(2023A1515012948);Guangdong Province Universities and Colleges Pearl River Scholar Funded Scheme(2019);Environment and Energy Green Catalysis Innovation Team of Colleges and Universities of Guangdong Province(2022KCXTD019);Yangfan Applied Innovation Project of Maoming Green Chemical Industry Research Institute(MMGCIRI-2022YFJH-Y-002);Science and Technology Project of Maoming(2020KJZX035)

Abstract

Abstract:

Hydrogen peroxide (H₂O₂) is widely used as an environmentally friendly oxidant and plays an important role in a range of applications, including chemical synthesis, wastewater treatment, medical disinfection, and papermaking. Compared to the conventional anthraquinone process for the preparation of H₂O₂, the photocatalytic and electrocatalytic production of H₂O₂ has the advantages of simple and controllable operating conditions and non-polluting reaction products, which is one of the most essential ideal means for H₂O₂ production. Among them, single-atom catalysts (SACs) with maximal atom utilization and special unsaturated coordination environments have attracted considerable attention because of their excellent catalytic performance in the photocatalytic and electrocatalytic production of H₂O₂. Subsequently, recent progress in H₂O₂ production based on photocatalytic and electrocatalytic activity is presented in this review. First, the working mechanisms and advantages of SACs for the photocatalytic and electrocatalytic production of H₂O₂ were presented. Second, we combined density functional theory calculations and advanced characterization techniques to introduce SAC systems for H₂O₂ production. Finally, the future directions of SACs for photocatalytic and electrocatalytic H₂O₂ production are discussed.

Key words: Single-atom catalyst, Photocatalysis, Electrocatalysis, Hydrogen peroxide, Performance enhancement

Xiaolong Tang, Feng Li, Fang Li, Yanbin Jiang, Changlin Yu. Single-atom catalysts for the photocatalytic and electrocatalytic synthesis of hydrogen peroxide[J]. Chinese Journal of Catalysis, 2023, 52: 79-98.

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Figures/Tables 20

Fig. 2. (a) Three forms of oxygen adsorption on metal surfaces. (b) Different ORR processes for oxygen on ensemble metal sites and the isolation of atomic sites.

Fig. 3. A schematic reaction mechanism of the photocatalytic production of H2O2.

Fig. 4. (a) Adsorption energies of CN and NiCN-4 catalysts. Reprinted with permission from Ref. [55]. Copyright 2022, Elsevier. (b) Band structure diagrams of PCN, PCN_Na15, and Sb-SAPC15. Reprinted with permission from Ref. [26]. Copyright 2021, Nature Publishing Group. (c) The distance between the hole and electron center of mass and (d) Coulomb attraction between hole and electron of Melem_3 and Melem_3M. Reprinted with permission from Ref. [58]. Copyright 2021, Elsevier.

Fig. 5. (a) Metal single-atom species involved in screening (left) and the schematic illustration of different carriers loaded with single-atoms (right). (b) The volcano relationship between the Gibbs free energy of OOH* and ultimate potential for single-atom catalysts (SACs). Reprinted with permission from Ref. [61]. Copyright 2019, American Chemical Society. (c) Screening of high-performance SACs with graphene as the substrate. (d) Free energy profiles of 2e- and 4e- ORR processes for Ni@V-c-GY catalysts. Reprinted with permission from Ref. [62]. Copyright 2021, Elsevier.

Fig. 6. Top and side views of the charge density difference in the (a) UCN and (b) carbon nitride photocatalyst (FeSA/CN) models. Yellow and cyan regions indicate electron accumulation and electron depletion, respectively. (c) The possible photodegradation mechanism of the OTC by a FeSA/CN. Reprinted with permission from Ref. [63]. Copyright 2023, Wiley-VCH.

Fig. 7. (a) A schematic diagram of the Al-C3N4 photocatalytic mechanism. Reprinted with permission from Ref. [64]. Copyright 2023, Elsevier. (b) Electrochemical in-situ Raman spectra of NbN4/NC and NbN3-(O)C3N4/carboxyl-functionalized multi-walled carbon nanotubes (OCNT). (c) Free energy diagrams for the 2e? ORR pathway on NbN3-(O)C3N4/OCNT and NbN4/NC. (d) Charge density differences of NbN3-(O)C3N4/OCNT and NbN4/NC. Reprinted with permission from Ref. [65]. Copyright 2023, American Chemical Society.

Fig. 8. Migration of metal single-atoms into metal clusters or nanoparticles.

Fig. 9. (a) A schematic diagram of the synthesis process of h-Pt1-CuSx, where the blue, white, and purple spheres represent Cu, S, and Pt atoms, respectively. (b) A TEM image of Pt1-CuSx, wherein cavities are pointed out by arrows. Reprinted with permission from Ref. [71]. Copyright 2019, Elsevier. (c) Free energy diagrams for the ORR pathways on Pt-S4, Pt-N4, and Pt-C4. The red and black lines represent the 2e? and 4e? ORR, respectively. Reprinted with permission from Ref. [72]. Copyright 2022, Nature Publishing Group.

Fig. 10. (a) In-situ XAS analysis of xPt/SZTC with different metal loadings. (b) A schematic representation of the structural changes of inert and labile Pt-S4 sites in contact with water, where the brown, yellow, gray, red, and white spheres represent C, S, Pt, O and H atoms, respectively. Reprinted with permission from Ref. [73]. Copyright 2023, Elsevier.

Fig. 11. (a) In-situ X-ray diffraction of PdClx/C at different temperatures. Reprinted with permission from Ref. [74]. Copyright 2020, American Chemical Society. (b) Single Pd atoms loaded on different two-dimensional materials. (c) The relationship between the H2O2/water generation activity and stability (Eb?Ec) of SACs. Reprinted with permission from Ref. [75]. Copyright 2022, Elsevier. High-resolution XPS spectra of (d) Mo 3d and (e) S 2p for MoS2 and Au(X)@MoS2 samples. Reprinted with permission from Ref. [76]. Copyright 2019, Elsevier. (f) The catalytic performance of Ru/P-CN prepared under different synthesis conditions and P-CN. Reprinted with permission from Ref. [77]. Copyright 2022, Wiley-VCH.

Table 1 Electrocatalytic and photocatalytic generation of H2O2 from noble metal-based single-atom catalysts.

Catalyst		(1) Electrolyte (2) Light source	Selective (H₂O₂%)	H₂O₂ generation rate	Ref.
Electrocatalyst	Pt/HSC	(1) 0.1 mol L^‒1 HClO₄	96	97.5 μmol h^‒1 cm^‒2	[78]
	Pt/TiN	(1) 0.1 mol L^‒1 HClO₄	65	—	[79]
	Pt/TiC	(1) 0.1 mol L^‒1 HClO₄	> 70	—	[80]
	h-Pt1-CuS_x	(1) 0.1 mol L^‒1 HClO₄	92‒96	546±30 mol kg^‒1 h^‒1	[71]
	Pt-SA/rGO	(1) 0.1 mol L^‒1 KOH	95	—	[81]
	Pt₁Ag₁/C	(1) 0.05 mol L^‒1 Na₂SO₄	>90	236.25 mol kg^‒1 h^‒1	[82]
	C@C₃N₄-Pd₁	(1) 0.1 mol L^‒1 HClO₄	94	—	[83]
	PdCl_x/C	(1) 0.1 mol L^‒1 HClO₄	90	—	[74]
	Pt₁-meso-S-C	(1) 0.1 mol L^‒1 HClO₄	—	28.25 mmol (2 h)	[84]
	Pt-S-CNT	(1) 0.1 mol L^‒1 HClO₄	81.4	—	[72]
	Ru_0.08Ti_0.92O₂	(1) 2 mol L^‒1 KHCO₃	62.8	24.2 μmol min^‒1 cm^‒2	[85]
Photocatalysis	Au@MoS₂	(2) 300 W Xe lamp	—	696.09 μmol (3 h)	[76]
Photocatalysis	Ru/P-CN	(2) 300 W Xe lamp, λ > 420 nm	—	385.8 mmol g^‒1 h^‒1	[77]

Fig. 12. (a) The OOH* adsorption energy and relative charge state of a Co atom when 4H*, 2H*, O*, or 2O* is adsorbed near it. (b) A schematic illustration of the structural changes during the synthesis of Co1-NG(O). (c) The H2O2 current for NG(O), Co1-NG(O), and Co1-NG(R). Reprinted with permission from Ref. [86]. Copyright 2020, Nature Publishing Group. (d) A schematic illustration of the structural changes during the synthesis of Co/NC. (e) Catalytic activity volcano diagrams for the 2e? (red) and 4e? ORR (grey) pathways on C-N4 and O-Co-N2C2. Reprinted with permission from Ref. [89]. Copyright 2022, Wiley-VCH.

Fig. 13. (a) Co single-atom (oxidation center)- and anthraquinone (reduction center)-assisted catalysts for the spatial separation of two-dimensional C3N4 nanosheets. Reprinted with permission from Ref. [90]. Copyright 2020, National Academy of Sciences. (b) Free energy diagrams for oxygen evolution (black) and H2O2 generation reactions over CoSAC@PCN (red) and C@PCN (blue). Reprinted with permission from Ref. [91]. Copyright 2022, American Chemical Society. (c) The FT k3-weighted χ(k)-function of the EXAFS spectra at a Co K-edge. The free energy diagram for H2O2 formation via the (d) O2 reduction pathway and (e) water oxidization route on Co-CN@G, CN@G, and Co-CN. Reprinted with permission from Ref. [92]. Copyright 2023, Nature Publishing Group.

Fig. 14. (a) A schematic diagram of the preparation process of N4Ni1O2/OCNTs and plausible reaction processes of N4Ni1O2, N4Ni1O1, and N4Ni1 for H2O2 electrosynthesis. (b) Free energy diagrams of the 2e- and 4e- ORR processes on N4Ni1O2, N4Ni1O1, N4Ni1C, N4Ni1, and bare OCNT structures. Reprinted with permission from Ref. [93]. Copyright 2022, Wiley-VCH.

Fig. 15. (a) Steady-state photoluminescence spectra. (b) Free energy diagrams of the 2e- and 4e- ORR processes of NiCN-4 catalysts. Reprinted with permission from Ref. [55]. Copyright 2022, Elsevier. (c) A proposed mechanism of photocatalytic H2O2 production from oxygen and water over Ni/Hf-0.5. (d) A comparison of the H2O2 production rates from Ni/Hf under visible light irradiation. Reprinted with permission from Ref. [94]. Copyright 2022, American Chemical Society.

Fig. 16. (a) Photocatalytic H2O2 production rates of PCNs and Sb-SAPCs with different metal loadings. (b) A reaction mechanism diagram of H2O2 generation from Sb/CN photocatalysts via the 2e- ORR pathway. Reprinted with permission from Ref. [26]. Copyright 2021, Nature Publishing Group. (c) The photoluminescence spectra of PCN and the M-SAPCs. (d) Photocatalytic rates of H2O2 production by PCN and M-SAPCs. Reprinted with permission from Ref. [58]. Copyright 2021, Elsevier.

Fig. 17. (a) A schematic of the synthesis process of Fe-F-C, Co-F-C, Ni-F-C, Mn-F-C, and Mn-F-C. Reprinted with permission from Ref. [95]. Copyright 2023, Elsevier. (b) A schematic of the synthesis of In SAs/NSBC. Reprinted with permission from Ref. [96]. Copyright 2022, Wiley-VCH.

Table 2 Electrocatalytic and photocatalytic generation of H2O2 from non-noble metal-based single-atom catalysts.

Catalyst		(1) Electrolyte (2) Light source	Selectivity (H₂O₂%) (H₂O₂%)	H₂O₂ generation rate	Ref.
Electrocatalyst	Co-NC	(1) 0.1 mol L^-1 HClO₄	> 90	275 mmol g⁻¹ h⁻¹	[97]
	EA-CoN@CNTs	(1) 0.1 mol L^-1 HClO₄	90	—	[98]
	HE-CoN@CNTs	(1) 0.1 mol L^-1 HClO₄	100	5525 ppm (12 h)	[98]
	Co₁/NG(O)	(1) 0.1 mol L^-1 KOH	82	418±19 mmol g⁻¹ h⁻¹	[86]
	Co-SA/V-C	(1) 0.1 mol L^-1 KOH	90	—	[99]
	Co-N₂-C/HO	(1) 0.1 mol L^-1 KOH	91.3	1000 mg L⁻¹ (1 h)	[100]
	Co-N-C	(1) 0.5 mol L^-1 NaCl	95.6	4.5 mol g⁻¹ h⁻¹	[101]
	Co-SAs/NC	(1) 0.1 mol L^-1 KOH	76	380.9±14.85 μmol (10 h)	[102]
	CoNOC	(1) 0.1 mol L^-1 HClO₄	>95	590 mmol g⁻¹ h⁻¹	[103]
	Co/NC	(1) 0.1 mol L^-1 PBS	>90	20.4 mmol (10 h)	[89]
	Co-F-CNT	(1) 0.1 mol L^-1 KOH	90	18.6 mol g⁻¹h⁻¹	[104]
	CoPc/CNT	(1) 0.1 mol L^-1 H₂SO₄	92	3.71 mol g⁻¹ h⁻¹	[105]
	CoNOC	(1) 0.1 mol L^-1 HClO₄	>98	760 mmol g⁻¹ h⁻¹	[106]
	Ni-SA/G	(1) 0.1 mol L^-1 KOH	>94	—	[107]
	Ni-N₂O₂/C	(1) 0.1 mol L^-1 KOH	96	5.9 mol g^-1 h^-1	[108]
	Ni SAC/Ni-NiO/NC	(1) 0.1 mol L^-1 KOH	95	325 mmol g⁻¹ h⁻¹	[109]
	NiN_x/C-AQNH₂	(1) 0.1 mol L^-1 KOH	>80	—	[110]
	N₄Ni₁O₂/OCNTs	(1) 0.1 mol L^-1 KOH	>90	5.7 mmol cm^-2 h^-1	[93]
	Fe-CNT	(1) 0.1 mol L^-1 KOH	>95	1.6 mol g⁻¹ h⁻¹	[111]
	Mo₁/OSG-H	(1) 0.1 mol L^-1 KOH	>95	—	[112]
	Mo-F-C	(1) 0.1 mol L^-1 KOH	90	27 mol g⁻¹ h⁻¹	[95]
	W₁/NO-C	(1) 0.1 mol L^-1 KOH	90-98	1.23 mol g⁻¹ h⁻¹	[113]
	In SAs/NSBC	(1) 0.1 mol L^-1 KOH	>95	6.49 mol g⁻¹ h⁻¹	[96]
	ATO	(1) 0.1 mol L^-1 NaClO₄	80	5.4 μmol h⁻¹ cm⁻²	[114]
	NbN₃-(O)C₃N₄/OCNT	(1) 0.1 mol L^-1 KOH	>95	1020.4 mmol g⁻¹ h⁻¹	[65]
	Sb-NSCF	(1) 0.1 mol L^-1 KOH	97.2	7.46 mol g⁻¹ h⁻¹	[115]
Photocatalysis	Co₁/AQ/C₃N₄	(2) 100 mW cm⁻², AM 1.5G	—	230 μmol (8 h)	[90]
	CoSAC@PCN	(2) violet LED lamp (410 nm)	—	62 μmol g^-1 h^-1	[91]
	In/CN	(2) 500 W Xe lamp, λ > 420 nm	—	7.5 mg L⁻¹ (1 h)	[58]
	Sb-SAPC	(2) 300 W Xe lamp, λ > 420 nm	—	12.4 mg L⁻¹ (2 h)	[26]
	NiCN	(2) 300 W Xe lamp, λ > 420 nm	87.3	27.11 mmol g^-1 h^-1	[55]
	Hf-UiO-66-NH₂	(2) 500 W Xe lamp, λ > 420 nm	—	222 μmol L⁻¹ (3 h)	[94]
	Al-C₃N₄	(2) 300 W Xe lamp, AM 1.5G	—	27.5 mmol g^-1 h^-1	[64]
	Cu-NG/CN	(2) 300 W Xe lamp, AM 1.5G	—	2856 μmol g^-1 h^-1	[116]

Table 2 Electrocatalytic and photocatalytic generation of H2O2 from non-noble metal-based single-atom catalysts.

Catalyst		(1) Electrolyte (2) Light source	Selectivity (H₂O₂%) (H₂O₂%)	H₂O₂ generation rate	Ref.
Electrocatalyst	Co-NC	(1) 0.1 mol L^-1 HClO₄	> 90	275 mmol g⁻¹ h⁻¹	[97]
	EA-CoN@CNTs	(1) 0.1 mol L^-1 HClO₄	90	—	[98]
	HE-CoN@CNTs	(1) 0.1 mol L^-1 HClO₄	100	5525 ppm (12 h)	[98]
	Co₁/NG(O)	(1) 0.1 mol L^-1 KOH	82	418±19 mmol g⁻¹ h⁻¹	[86]
	Co-SA/V-C	(1) 0.1 mol L^-1 KOH	90	—	[99]
	Co-N₂-C/HO	(1) 0.1 mol L^-1 KOH	91.3	1000 mg L⁻¹ (1 h)	[100]
	Co-N-C	(1) 0.5 mol L^-1 NaCl	95.6	4.5 mol g⁻¹ h⁻¹	[101]
	Co-SAs/NC	(1) 0.1 mol L^-1 KOH	76	380.9±14.85 μmol (10 h)	[102]
	CoNOC	(1) 0.1 mol L^-1 HClO₄	>95	590 mmol g⁻¹ h⁻¹	[103]
	Co/NC	(1) 0.1 mol L^-1 PBS	>90	20.4 mmol (10 h)	[89]
	Co-F-CNT	(1) 0.1 mol L^-1 KOH	90	18.6 mol g⁻¹h⁻¹	[104]
	CoPc/CNT	(1) 0.1 mol L^-1 H₂SO₄	92	3.71 mol g⁻¹ h⁻¹	[105]
	CoNOC	(1) 0.1 mol L^-1 HClO₄	>98	760 mmol g⁻¹ h⁻¹	[106]
	Ni-SA/G	(1) 0.1 mol L^-1 KOH	>94	—	[107]
	Ni-N₂O₂/C	(1) 0.1 mol L^-1 KOH	96	5.9 mol g^-1 h^-1	[108]
	Ni SAC/Ni-NiO/NC	(1) 0.1 mol L^-1 KOH	95	325 mmol g⁻¹ h⁻¹	[109]
	NiN_x/C-AQNH₂	(1) 0.1 mol L^-1 KOH	>80	—	[110]
	N₄Ni₁O₂/OCNTs	(1) 0.1 mol L^-1 KOH	>90	5.7 mmol cm^-2 h^-1	[93]
	Fe-CNT	(1) 0.1 mol L^-1 KOH	>95	1.6 mol g⁻¹ h⁻¹	[111]
	Mo₁/OSG-H	(1) 0.1 mol L^-1 KOH	>95	—	[112]
	Mo-F-C	(1) 0.1 mol L^-1 KOH	90	27 mol g⁻¹ h⁻¹	[95]
	W₁/NO-C	(1) 0.1 mol L^-1 KOH	90-98	1.23 mol g⁻¹ h⁻¹	[113]
	In SAs/NSBC	(1) 0.1 mol L^-1 KOH	>95	6.49 mol g⁻¹ h⁻¹	[96]
	ATO	(1) 0.1 mol L^-1 NaClO₄	80	5.4 μmol h⁻¹ cm⁻²	[114]
	NbN₃-(O)C₃N₄/OCNT	(1) 0.1 mol L^-1 KOH	>95	1020.4 mmol g⁻¹ h⁻¹	[65]
	Sb-NSCF	(1) 0.1 mol L^-1 KOH	97.2	7.46 mol g⁻¹ h⁻¹	[115]
Photocatalysis	Co₁/AQ/C₃N₄	(2) 100 mW cm⁻², AM 1.5G	—	230 μmol (8 h)	[90]
	CoSAC@PCN	(2) violet LED lamp (410 nm)	—	62 μmol g^-1 h^-1	[91]
	In/CN	(2) 500 W Xe lamp, λ > 420 nm	—	7.5 mg L⁻¹ (1 h)	[58]
	Sb-SAPC	(2) 300 W Xe lamp, λ > 420 nm	—	12.4 mg L⁻¹ (2 h)	[26]
	NiCN	(2) 300 W Xe lamp, λ > 420 nm	87.3	27.11 mmol g^-1 h^-1	[55]
	Hf-UiO-66-NH₂	(2) 500 W Xe lamp, λ > 420 nm	—	222 μmol L⁻¹ (3 h)	[94]
	Al-C₃N₄	(2) 300 W Xe lamp, AM 1.5G	—	27.5 mmol g^-1 h^-1	[64]
	Cu-NG/CN	(2) 300 W Xe lamp, AM 1.5G	—	2856 μmol g^-1 h^-1	[116]

Fig. 18. Challenges and prospects in the field of photocatalytic and electrocatalytic H2O2 production from single-atom catalysts.

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Single-atom catalysts for the photocatalytic and electrocatalytic synthesis of hydrogen peroxide

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