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Journal article
Electrochemical Corrosion and Catalysis Dynamics of Tin Oxide during Water Oxidation
ACS catalysis, v 15, pp 18601-18611
27 Oct 2025
Featured in Collection : Research Supported by Drexel Libraries' OA Programs
Abstract
Metal oxide corrosion severely limits anodic electrocatalysis, particularly at high potentials in acidic environments, where degradation pathways remain poorly defined. This study establishes explicit connections between corrosion and electrocatalysis on tin oxide during water oxidation by examining the roles of lattice defects, reactive oxygen species, interfacial pH variations, and speciation of corroded tin in acid. We first demonstrate the presence of structural defects such as oxygen vacancies and substoichiometric Sn(II) species by integrating electron paramagnetic resonance spectroscopy, ultraviolet photoelectron spectroscopy, and Mott–Schottky analysis. Kohn–Sham density functional theory calculations reveal that explicit water structures thermodynamically stabilize reaction intermediates and lower reaction overpotentials. Moreover, we propose that water dissociation leads to hydrogen-bonding networks formed by H* and OH* intermediates, which may span the entire catalyst surface and decrease the interfacial pH to drive corrosion. In contrast, the electrochemical generation of reactive oxygen species is shown to play a minor role in catalyst corrosion during water oxidation using inductively coupled plasma mass spectrometry coupled with selective chemical scavengers. Square-wave voltammetry combined with rotating ring-disk electrodes is used to reveal that under open-circuit conditions, only Sn(IV) cations chemically dissolve from tin oxide, while both Sn(IV) and Sn(II) species electrochemically corrode during water oxidation. Our results unveil a dynamic and complicated interplay between corrosive and catalytic pathways on metal oxide electrocatalysts: a decrease in interfacial pH due to water oxidation exacerbates Sn(II)/Sn(IV) corrosion. Subsequently, the electrochemical corrosion of Sn(II)/Sn(IV) facilitates product formation from lattice oxygen, while the redeposition of corroded Sn(II) as Sn(IV) can enable oxygen exchange with water. By elucidating the roles of defects and interfacial chemistry, this work provides a roadmap for engineering improved electrocatalysts that balance activity and stability, a critical step toward scalable and durable energy technologies.
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Details
- Title
- Electrochemical Corrosion and Catalysis Dynamics of Tin Oxide during Water Oxidation
- Creators
- Rayan Alaufey - Drexel University, Chemical and Biological EngineeringLingyan Zhao - University of PittsburghChristina LentsBrianna Markunas - Drexel University, Chemical and Biological EngineeringAdam D. Walter - Drexel University, Materials Science and EngineeringQin Wu - Brookhaven National LaboratoryJohn A. Keith - University of PittsburghMaureen Tang (Corresponding Author) - Drexel University, Chemical and Biological Engineering
- Publication Details
- ACS catalysis, v 15, pp 18601-18611
- Publisher
- ACS Publications
- Number of pages
- 11
- Grant note
- Division of Chemistry: CHE-1855657 This work was supported by the National Science Foundation under grants CHE-1855657 and CHE-1856460 [Pitt]. Computational resources were provided by the Center for Functional Nanomaterials (CFN) at Brookhaven National Laboratory, a U.S. Department of Energy Office of Science User Facility, under Contract No. DE-SC0012704. Additional computational support was provided by the University of Pittsburgh Center for Research Computing (RRID:SCR_022735), specifically through the use of the H2P cluster, supported by NSF award OAC-2117681. The authors also acknowledge the Agilent Technologies University Relations SIRA Program (Grant ID #4906) for the loan of the Agilent 8900 ICP-QQQ instrument.
- Resource Type
- Journal article
- Language
- English
- Academic Unit
- Materials Science and Engineering; Chemical and Biological Engineering
- Web of Science ID
- WOS:001603084600001
- Scopus ID
- 2-s2.0-105019983153
- Other Identifier
- 991022127452504721
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- Collaboration types
- Domestic collaboration
- Web of Science research areas
- Chemistry, Physical