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251004s2025 xx |||||o 00| ||eng c |
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|a 10.1021/acs.langmuir.5c03848
|2 doi
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|a eng
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| 100 |
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|a Wang, Yu-Le
|e verfasserin
|4 aut
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|a Spontaneous H2O2 Accumulation under O2 Driven by Sacrificial Oxidation of NiS2 without External Electrical/Photonic Input
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|c 2025
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|a Text
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|a ƒaComputermedien
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|a Date Revised 14.10.2025
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|a published: Print-Electronic
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|a Citation Status PubMed-not-MEDLINE
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|a Although spontaneous H2O2 accumulation by sacrificial oxidation of metal disulfides (FeS2, NiS2, etc.) under oxic conditions without external electrical/photonic input has been observed, the mechanistic understanding of HCO3- on the production of H2O2 is still not clear. In this study, HCO3- apparently accelerates the production of H2O2 on NiS2, and the produced H2O2 increases from 53.85 to 90.12 μM with increasing concentrations of HCO3- from 0 to 0.5 M at pH 9.0. Electrochemical analyses indicate that HCO3- effectively mediates the 2e reduction of O2 to H2O2 on the surface of NiS2. EPR and Raman analyses rule out the primary contributions of soluble •OH and O2•- to the production of H2O2 and reveal the presence of both ≡Ni-OO• superoxo and ≡Ni-OOH peroxo on NiS2, which are important precursors for H2O2. The presence of CO3•- also indicates that HCO3- is an important H-donor during the reduction of O2 to H2O2. DFT calculations further reveal that it is thermodynamically more favorable for ≡Ni-OO• and ≡Ni-OOH to abstract H from HCO3- than from H2O to produce H2O2, confirming that HCO3- is a better H-donor than H2O to produce H2O2 via the H-abstraction pathway. This study provides insight into the importance of HCO3- on spontaneous H2O2 accumulation by sacrificial oxidation of NiS2 under oxic conditions without external electrical/photonic input
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|a Journal Article
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1 |
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|a Wang, Cong
|e verfasserin
|4 aut
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| 700 |
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|a Wu, Song-Hai
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Liu, Yong
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Han, Xu
|e verfasserin
|4 aut
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| 773 |
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|i Enthalten in
|t Langmuir : the ACS journal of surfaces and colloids
|d 1985
|g 41(2025), 40 vom: 14. Okt., Seite 27492-27501
|w (DE-627)NLM098181009
|x 1520-5827
|7 nnas
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| 773 |
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|g volume:41
|g year:2025
|g number:40
|g day:14
|g month:10
|g pages:27492-27501
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| 856 |
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|u http://dx.doi.org/10.1021/acs.langmuir.5c03848
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