Electronic structure modulation of metal based organic catalysts for photocatalytic H2O2 production

doi:10.1016/S1872-2067(25)64788-7

Chinese Journal of Catalysis ›› 2025, Vol. 77: 45-69.DOI: 10.1016/S1872-2067(25)64788-7

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Electronic structure modulation of metal based organic catalysts for photocatalytic H₂O₂ production

Wenhui Qi^a, Xiuyan Li^b, Shaonan Gu^a^,^*(), Bin Sun^a, Yinan Wang^a, Guowei Zhou^a^,^*()

^aKey Laboratory of Fine Chemicals in Universities of Shandong, Jinan Engineering Laboratory for Multi-scale Functional Materials, School of Chemistry and Chemical Engineering, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250353, Shandong, China
^bSchool of Chemical Engineering and Environment, Shandong Engineering Research Center of Green and High-value Marine Fine Chemical, Weifang University of Science and Technology, Weifang 262700, Shandong, China

Received:2025-05-18 Accepted:2025-06-14 Online:2025-10-18 Published:2025-10-05
Contact: *E-mail: sngu@qlu.edu.cn (S. Gu), gwzhou@qlu.edu.cn (G. Zhou).
About author:Shaonan Gu (School of Chemistry and Chemical Engineering, Qilu University of Technology) received his Ph.D degree in 2016 from the University of Science and Technology Beijing. He then conducted postdoctoral research at the Hong Kong University of Science and Technology and the Hong Kong Polytechnic University from 2016 to 2018, respectively. His research interests center on designing and synthesizing photocatalysts with activities for photocatalytic hydrogen peroxide production and photocatalytic water splitting, as well as developing and investigating energy conversion and storage materials such as lithium ions and lithium sulfur battery electrodes, including their structural properties through theoretical calculations. His recent progresses focused on the theory and application of materials like MOFs, rare earth single atoms, and COFs in photo- and electro-catalysis. Now he has published over 80 peer-reviewed papers.
Guowei Zhou (School of Chemistry and Chemical Engineering, Qilu University of Technology) received his B.S., M.S., and Ph.D. degrees in Chemistry at Shandong University (1986, 1989, and 2001). He carried out postdoctoral research in Prof. Young Soo Kang’s group at Pukyong National University (Korea) from 2012 to 2013 and worked as an advanced research scholar in Prof. Shihe Yang’s group at The Hong Kong University of Science and Technology from 2015 to 2016. He is currently a Professor at Qilu University of Technology. His research group focuses primarily on the design, controlled synthesis, modification, and hierarchical assembly mesostructure functional materials with specific morphology for energy applications including batteries and photocatalysis. His current research interests include the different application of functional mesoporous materials for photocatalytic hydrogen production, CO₂ reduction, environmental remediation, and energy conversion and storage. He has published more than 160 peer-reviewed papers. He was granted 54 national invention patents in China. He also serves as the editor for Acta Phys.-Chim. Sin. from 2025.
Supported by:
National Natural Science Foundation of China(22108133);National Natural Science Foundation of China(52472215);National Natural Science Foundation of China(52202102);National Natural Science Foundation of China(51972180);Science, Education and Industry Integration Innovation Pilot Project from Qilu University of Technology (Shandong Academy of Sciences)(2024ZDZX13)

Abstract

Abstract:

Photocatalytic synthesis of hydrogen peroxide (H₂O₂) has emerged as a promising approach because of its simplicity and environmental benefits. However, significant challenges remain obstacles to their advancement, such as the rapid recombination of photogenerated charge carriers and sluggish surface redox reactions on nonmetallic organic catalysts. Metal-based organic catalysts with tunable electronic structures are considered ideal for exploring the mechanisms and structure-performance relationships in H₂O₂ synthesis. This review summarizes the fundamental principles of photocatalytic H₂O₂ synthesis via oxygen reduction and water oxidation reactions. Recent advancements in electronic structure tuning strategies for metal-based organic catalysts are critically examined, focusing on their impact on light absorption range, photogenerated carrier separation, O₂ activation, and the selective generation of H₂O₂. In addition, this review comprehensively evaluates the applications of sacrificial agents in photocatalytic reaction systems and offers insights into the future development of metal-based organic catalysts for H₂O₂ photosynthesis.

Key words: Metal based organic catalysts, Electronic structure, Photocatalytic H₂O₂ synthesis, Oxygen reduction reaction, Water oxidation reaction, S-scheme photocatalysis

Wenhui Qi, Xiuyan Li, Shaonan Gu, Bin Sun, Yinan Wang, Guowei Zhou. Electronic structure modulation of metal based organic catalysts for photocatalytic H₂O₂ production[J]. Chinese Journal of Catalysis, 2025, 77: 45-69.

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Figures/Tables 17

Fig. 1. Influence of electronic structure regulation in metal based organic catalysts on H2O2 generation, and the role of sacrificial agents in catalytic systems.

Fig. 2. Illustration of photocatalytic H2O2 production and schematic of the WOR and ORR mechanism during H2O2 reduction.

Fig. 3. (a) Preparation schematics of Au/TB-COF. ISI-XPS spectra of Au 4f (b) and N 1s (c) for Au, TB-COF, and AT-1 under different condition. EIS spectra (d) and transient photocurrent curves (e) of the as-prepared samples. Reproduced with permission from Ref. [85]. Copyright 2024, Elsevier. (f) PL spectra of C3N4, CP, Pt/C3N4, and Pt/CP. (g) In-situ Pt 4f XPS spectra under dark and illumination. Reproduced with permission from Ref. [87]. Copyright 2024, Wiley. (h) The preparation route of Co-N-C/SA-PDI photocatalyst. (i) UV-vis DRS analysis of SA-PDI, Co-N-C and Co-N-C/SA-PDI. (j) PL emission spectra of SA-PDI, Co-N-C and Co-N-C/SA-PDI-70%. (k) O 1s spectra of SA-PDI, Co-N-C/SA-PDI-70% and Co-N-C. Reproduced with permission from Ref. [89]. Copyright 2023, Elsevier.

Fig. 4. (a) Charge density difference distribution of O2 molecule on Cu-NG/CN and NG/CN. (b) PL spectra of all the samples. (c) UV-vis DRS of all the samples. (d) transient photocurrent curves of all the samples. Reproduced with permission from Ref. [98]. Copyright 2023, Elsevier. (e) band structure alignments of CN and CN-KI-X. (f) Top views of the structure with different charge densities of CN and CN-KI-10. (g) PL spectra. (h) The H2O2 formation (Kf) and the decomposition (Kd) rate constant over CN and CN-KI-10. Reproduced with permission from Ref. [101]. Copyright 2023, Elsevier. (i) PL spectra of g-C3N4 in pure and K+-added solvents. (j) Time-resolved PL data and corresponding fits. (k) Schematic illustrating potential pathways of K+ adsorption in promoting H2O2 generation by g-C3N4. Reproduced with permission from Ref. [102]. Copyright 2025, Elsevier.

Fig. 5. (a) Approximate binding energies of Melem_3 and Melem_3M for the lowest-lying excited states. (b) Visualization of the LUMOs of Melem_3In3+ and Melem_3Sn4+. (c) Transition densities of Melem_3M. Reproduced with permission from Ref. [106]. Copyright 2021, Elsevier. (d) Schematic illustration for the fabrication of MLCD defects in NTU-9. (e,f) TDOS and PDOS of nondefective NTU-9 and NTU-9 with MLCD defects, respectively. (g) The relationship between spin polarization and O2 activation. Reproduced with permission from Ref. [110]. Copyright 2023, Elsevier. Illustration of the crystal structures of Hf-UiO-66-NH2 (h) and Hf-UiO-66-NH2 (i). Reproduced with permission from Ref. [113]. Copyright 2022, American Chemical Society.

Fig. 6. (a) Schematic of S-scheme heterojunction photocatalysts mechanism. Reproduced with permission from Ref. [69]. Copyright 2023, American Chemical Society. (b) Charge carrier transfer mechanism in the COF/IS S-scheme heterojunction. (c) UV-vis DRS spectra of COF, IS, and COFIS composites. Reproduced with permission from Ref. [73]. Copyright 2024, Wiley. (d) FT-EXAFS fitting curves of ZnO and ZCOF20 at the Zn K-edge using the structural model of Zn-O4 and Zn-O3N. In situ irradiated XPS spectra of Zn 2p (e) and N 1s (f) for ZCOF20 as compared with those for ZCOF20, ZnO, and COF in the dark. (g) Schematic of the interfacial electron transfer and the IEF formation upon hybridization and S-scheme charge transfer via Zn-N bonds under light irradiation. Reproduced with permission from Ref. [114]. Copyright 2025, Wiley. (h) The catalytic mechanism diagram of C3N4/NiIn2S4. Reproduced with permission from Ref. [115]. Copyright 2022, Elsevier.

Fig. 7. (a) Schematic of the synthesis of high-loading M-SAPs-PuCN. (b) Schematic diagram of Ni sites structure evolution of NiSAPs-PuCN. (c) Free energy profiles for photocatalytic H2O2 evolution reactions over BCN and NiSAPs-PuCN. Reproduced with permission from Ref. [138]. Copyright 2023, Springer Nature. (d) Schematic diagram of catalytic structures to show Li migration in plan and interlayer under light irradiation. (e) Reaction pathway of H2O2 product based on different Li-coordinated structures. (f) Free energies for different intermediates on the Li-coordinated C3N4 sample under different applied electrical fields. Reproduced with permission from Ref. [139]. Copyright 2024, American Chemical Society.

Fig. 8. (a) Schematic of the photocatalytic mechanism for HAAQ-Sb. Reproduced with permission from Ref. [162]. Copyright 2024, Elsevier. (b) Schematic illustration of the synthesis route for CN/Zn-OAc. (c) PDOS and d-band centers for Zn-N3O models. (d) Charge density difference of Zn-N4/OOH and Zn-N3O/OOH models and the corresponding charge accumulated in ?OOH intermediate. (e) Free energy diagram of 2e- O2 reduction on Zn sites within different models. Reproduced with permission from Ref. [149]. Copyright 2024, Wiley. (f) TEM image of O/K-CN. (g) The α/β-HOMO and α/β-LUMO of O2 adsorbed O/K-CN, the iso-surface value is 0.03 e ?-3. (h) Mechanism of electron migration from β-LUMO orbitals to O2 after O/K-CN excitation. The electron-hole distribution of O2 adsorbed PCN (i) and O/K-CN (j) in different excited states, the iso-surface value is 0.002 e ?-3. (k) The free energy diagrams of the as-prepared samples. Reproduced with permission from Ref. [163]. Copyright 2022, Wiley. (l) Free energy diagrams for H2O2 generation on UiO-67-B and UiO-67-B/Pt(II). (m) Plausible mechanism of H2O2 formation and decomposition over UiO-67-B and UiO-67-B/Pt(II). Reproduced with permission from Ref. [168]. Copyright 2023, Elsevier.

Fig. 9. Mechanism for photocatalytic H2O2 production under visible-light irradiation of MIL-125-NH2 (a) and MIL-125-PDI (b). Reproduced with permission from Ref. [172]. Copyright 2021, Royal Society of Chemistry. (c) HAADF-STEM image of Cu-NG/CN. (d) Schematic illustration of charge transfer route and mechanism over Cu-NG/CN. Reproduced with permission from Ref. [96]. Copyright 2023, Elsevier. (e) Open circuit photovoltage. (f) Derivative of Mott-Schottky plots within the potential range between -0.4 and 1.4 vs. Ag/AgCl. (g) Photocatalytic H2O2 production mechanism of K-CAN. Reproduced with permission from Ref. [176]. Copyright 2023, Elsevier.

Fig. 11. (a) Structures of intermediates on NiCN-4 catalyst for 2e- ORR process. (b) Free energy profiles of ORR processes for NiCN-4 catalysts. (c) Schematic demonstration of H2O2 generation for NiCN-4 catalyst. Reproduced with permission from Ref. [191]. Copyright 2022, Elsevier. (d) Schematic synthesis of CoPc-BTM-COF and CoPc-DAB-COF. (e) Free energy diagrams for ORR processes on CoPc. Reproduced with permission from Ref. [192]. Copyright 2022, American Chemical Society. (f) Different charge densities for O2 adsorption on non-defective and defective clusters. Reproduced with permission from Ref. [110]. Copyright 2023, Elsevier.

Fig. 12. (a) Simulated electron density distribution after O2 and H+ adsorption onto UiO-66 and UiO-66-B. (b)The mechanism for photocatalytic H2O2 production over UiO-66 and UiO-66-B. Reproduced with permission from Ref. [200]. Copyright 2021, Royal Society of Chemistry. (c) The structure variation of UIO-66-NH2 before and after OMe group incorporation along with lattice distortion. (d) The intermediate structures for HCOO-UIO-66-NH2 and OMe-UIO-66-NH2-LD. (e) Illustration of the lattice distortion induced by the replacement of -COO- by -OMe coordinated to UIO-66-NH2. (f) Free energy reaction profiles of the 2e- ORR reaction path towards H2O2 generation at 0 V (vs. NHE). Reproduced with permission from Ref. [201]. Copyright 2022, Elsevier.

Fig. 13. (a) Proposed reaction mechanism for photocatalytically synthesized H2O2. Reproduced with permission from Ref. [203]. Copyright 2023, Wiley. (b) Schematic illustrations of the dynamic spin-state transition for Fe(II) and the spin-related photocatalytic H2O2 synthesis overall reaction. Reproduced with permission from Ref. [204]. Copyright 2023, American Chemical Society. (c) Interlaminar charge density mapping of CN layer with Al. (d) PDOS of pristine CN layer and CN layer with Al. Reproduced with permission from Ref. [205]. Copyright 2024, American Chemical Society. (e) TDOS, PDOS and ODOS of Melem_3 Sb3+ combined with the iso-surface of LUMO. Reproduced with permission from Ref. [207]. Copyright 2021, Springer Nature.

Fig. 14. (a) Mechanism of photocatalytic H2O2 production. Reproduced with permission from Ref. [207]. Copyright 2021, Springer Nature. (b) Photocatalysts with different exposed crystalline facets. Reproduced with permission from Ref. [208]. Copyright 2020, Proceedings of the National Academy of Sciences. (c) Schematic illustration of the preparation of the Au-Co TCPP photocatalyst. (d) The mechanism for photocatalytic H2O2 production of Au-Co-TCPP. Reproduced with permission from Ref. [83]. Copyright 2022, Royal Society of Chemistry.

Table 1 Summary of representative metal based organic catalysts for photocatalytic hydrogen peroxide production.

Photocatalyst	Light source	Type of sacrifice	Hydrogen generation rate (μmol g^-1 h^-1)	Apparent quantum yield	Ref.
Au-Co-TCPP	300 W Xe lamp (λ ≥ 400 nm)	—	236	—	[83]
Au/TB-COF.	300 W Xe lamp (λ > 420 nm)	10 vol% EtOH	6067	—	[84]
Cu-NG/CN	300 W Xe lamp (AM 1.5 G)	10 vol% EtOH	2856	—	[96]
ZnO/COF	5 W LED lamp (365 nm)	8 mM IPA	10560	5.0% (365 nm)	[114]
C₃N₄-Zn-N(C)	LED (365 nm)	10 vol% EtOH	7800	26.8% (365 nm)	[133]
Ni_SAPs-PuCN	300 W Xe lamp (AM 1.5 G)	—	640	10.9% (420 nm)	[138]
CN/Zn-OAc	300 W Xe lamp (λ > 400 nm)	20 vol% EtOH	7750	—	[149]
HAAQ-Sb	300 W Xe lamp (λ > 400 nm)	10 vol% IPA	2855	20.2% (400 nm)	[162]
O/K-CN	300 W Xe lamp (λ > 420 nm)	10 vol% IPA	15472	—	[163]
UiO‐67‐B/Pt(II)	300 W Xe lamp (AM 1.5)	10 vol% IPA	27583	—	[168]
NiCN-4	300 W Xe lamp (λ ≥ 420)	10 vol% IPA	27110	8.6% (400 nm)	[191]
CoPc-BTM-COF	300 W Xe lamp (λ > 400 nm)	10 vol% EtOH	2096	7.2% (630 nm)	[192]
CoPc-DAB-COF	300 W Xe lamp (λ > 400 nm)	10 vol% EtOH	1851	5.2% (630 nm)	[192]
OMe-UIO-66-NH₂-LD	300 W Xe lamp (λ ≥ 420 nm)	10 mL acetonitrile and 2 mL BA	3129	5.1% (365 nm)	[201]
Co₁₄-(L-CH₃)₂₄	300 W Xe lamp (300-1100 nm)	—	147	—	[203]
Co₁/AQ/C₃N₄	300 W Xe lamp (AM 1.5 G)	—	124	0.05% (full spectrum)	[208]
Ru@Cu-HHTP	300 W Xe lamp (λ ≥ 400 nm)	10 vol% EtOH	571	15.3% (450 nm)	[214]
ZIF-8/C₃N₄	300 W Xe lamp (420 ≤ λ ≤ 700 nm)	—	2641	19.6% (420 nm)	[224]
Bi₃TiNbO₉@C₄N	300 W Xe lamp (AM 1.5)	—	1250	—	[226]
TT-COF/ZCS	300 W Xe lamp (λ ≥ 420 nm)	—	5171	0.4% (420 nm)	[227]
TAPT-TFPA COFs@Pd ICs	300 W Xe lamp (1.5 G)	10 vol% EtOH	2143	6.5% (400 nm)	[228]
TAPT-2KtTbPd COF	300W Xe (1.5 G)	10 vol% EtOH	3232	9.5% (420 nm)	[229]
CoO_x-BCN-FeOOH	100 mW cm (λ ≥ 420 nm)	—	340	8.4% (420 nm)	[230]
Zn-CN_2nd	300 W Xe lamp (AM 1.5)	5 vol% EtOH	1363	24.6% (350 nm)	[231]
BI-CN	5 W LED lamp (λ ≥ 420 nm)	10 vol% EtOH	706	—	[232]
MgIn₂S₄/COF	300 W Xe lamp (λ ≥ 420 nm)	—	4250	6.4% (420 nm)	[233]
TiO₂/TD COF	300 W Xe lamp	10 vol% EtOH	1703	4.1% (420 nm)	[234]
TiO₂/COF	300 W Xe lamp	10 vol% EtOH	2162	—	[235]
TiO₂/BTTA	300 W Xe lamp	2 mM FAL	1480	5.5% (365 nm)	[236]
Zn-TCPP/CN	300 W Xe lamp	10 vol% EtOH	592	7.0% (365 nm)	[237]
CdS/RF	300 W Xe lamp (λ > 420 nm)	10 vol% EtOH	2136	—	[238]
SCN/T9	300 W Xe lamp (300 ≤ λ ≤ 700)	—	2128	0.6% (365 nm)	[239]
BTC40	300 W Xe lamp	10 vol% EtOH	3749	—	[240]

Table 1 Summary of representative metal based organic catalysts for photocatalytic hydrogen peroxide production.

Photocatalyst	Light source	Type of sacrifice	Hydrogen generation rate (μmol g^-1 h^-1)	Apparent quantum yield	Ref.
Au-Co-TCPP	300 W Xe lamp (λ ≥ 400 nm)	—	236	—	[83]
Au/TB-COF.	300 W Xe lamp (λ > 420 nm)	10 vol% EtOH	6067	—	[84]
Cu-NG/CN	300 W Xe lamp (AM 1.5 G)	10 vol% EtOH	2856	—	[96]
ZnO/COF	5 W LED lamp (365 nm)	8 mM IPA	10560	5.0% (365 nm)	[114]
C₃N₄-Zn-N(C)	LED (365 nm)	10 vol% EtOH	7800	26.8% (365 nm)	[133]
Ni_SAPs-PuCN	300 W Xe lamp (AM 1.5 G)	—	640	10.9% (420 nm)	[138]
CN/Zn-OAc	300 W Xe lamp (λ > 400 nm)	20 vol% EtOH	7750	—	[149]
HAAQ-Sb	300 W Xe lamp (λ > 400 nm)	10 vol% IPA	2855	20.2% (400 nm)	[162]
O/K-CN	300 W Xe lamp (λ > 420 nm)	10 vol% IPA	15472	—	[163]
UiO‐67‐B/Pt(II)	300 W Xe lamp (AM 1.5)	10 vol% IPA	27583	—	[168]
NiCN-4	300 W Xe lamp (λ ≥ 420)	10 vol% IPA	27110	8.6% (400 nm)	[191]
CoPc-BTM-COF	300 W Xe lamp (λ > 400 nm)	10 vol% EtOH	2096	7.2% (630 nm)	[192]
CoPc-DAB-COF	300 W Xe lamp (λ > 400 nm)	10 vol% EtOH	1851	5.2% (630 nm)	[192]
OMe-UIO-66-NH₂-LD	300 W Xe lamp (λ ≥ 420 nm)	10 mL acetonitrile and 2 mL BA	3129	5.1% (365 nm)	[201]
Co₁₄-(L-CH₃)₂₄	300 W Xe lamp (300-1100 nm)	—	147	—	[203]
Co₁/AQ/C₃N₄	300 W Xe lamp (AM 1.5 G)	—	124	0.05% (full spectrum)	[208]
Ru@Cu-HHTP	300 W Xe lamp (λ ≥ 400 nm)	10 vol% EtOH	571	15.3% (450 nm)	[214]
ZIF-8/C₃N₄	300 W Xe lamp (420 ≤ λ ≤ 700 nm)	—	2641	19.6% (420 nm)	[224]
Bi₃TiNbO₉@C₄N	300 W Xe lamp (AM 1.5)	—	1250	—	[226]
TT-COF/ZCS	300 W Xe lamp (λ ≥ 420 nm)	—	5171	0.4% (420 nm)	[227]
TAPT-TFPA COFs@Pd ICs	300 W Xe lamp (1.5 G)	10 vol% EtOH	2143	6.5% (400 nm)	[228]
TAPT-2KtTbPd COF	300W Xe (1.5 G)	10 vol% EtOH	3232	9.5% (420 nm)	[229]
CoO_x-BCN-FeOOH	100 mW cm (λ ≥ 420 nm)	—	340	8.4% (420 nm)	[230]
Zn-CN_2nd	300 W Xe lamp (AM 1.5)	5 vol% EtOH	1363	24.6% (350 nm)	[231]
BI-CN	5 W LED lamp (λ ≥ 420 nm)	10 vol% EtOH	706	—	[232]
MgIn₂S₄/COF	300 W Xe lamp (λ ≥ 420 nm)	—	4250	6.4% (420 nm)	[233]
TiO₂/TD COF	300 W Xe lamp	10 vol% EtOH	1703	4.1% (420 nm)	[234]
TiO₂/COF	300 W Xe lamp	10 vol% EtOH	2162	—	[235]
TiO₂/BTTA	300 W Xe lamp	2 mM FAL	1480	5.5% (365 nm)	[236]
Zn-TCPP/CN	300 W Xe lamp	10 vol% EtOH	592	7.0% (365 nm)	[237]
CdS/RF	300 W Xe lamp (λ > 420 nm)	10 vol% EtOH	2136	—	[238]
SCN/T9	300 W Xe lamp (300 ≤ λ ≤ 700)	—	2128	0.6% (365 nm)	[239]
BTC40	300 W Xe lamp	10 vol% EtOH	3749	—	[240]

Fig. 15. (a) Schematic of the preparation process of C3N4-Zn-N(C). (b,c) Calculated 1D and 3D (inset) charge density difference distribution. Reproduced with permission from Ref. [133]. Copyright 2025, Wiley. (d) Self-assembly of [Ru(bpy)2]2 into Cu-HHTP to create the photocatalyst with bi-functional unit. Reproduced with permission from Ref. [214]. Copyright 2025, Wiley. (e) Left: two-phase systems composed of an aqueous phase and a BA phase containing MIL-125-NH2 and MIL-125-Rn. Right: photocatalytic H2O2 production utilizing the two-phase system. Reproduced with permission from Ref. [217]. Copyright 2019, Wiley.

Fig. 16. (a) Proposed mechanism for H2O2 production over hydrophobic ZIS/PCN heterojunction in pure water and in two-phase systems. Reproduced with permission from Ref. [219]. Copyright 2024, Elsevier. (b) The mechanisms for production of H2O2 over ZCN. Reproduced with permission from Ref. [224]. Copyright 2020, Elsevier. (c) Scheme illustration for the synthesis process of the Bi3TiNbO9@C4N heterojunction. Reproduced with permission from Ref. [226]. Copyright 2024, Wiley.

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Electronic structure modulation of metal based organic catalysts for photocatalytic H₂O₂ production

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