Article(id=1319726169763721394, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1319726164160139662, articleNumber=null, orderNo=null, doi=10.14062/j.issn.0454-5648.20240822, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1735142400000, receivedDateStr=2024-12-26, revisedDate=1737216000000, revisedDateStr=2025-01-19, acceptedDate=null, acceptedDateStr=null, onlineDate=1792576838198, onlineDateStr=2026-10-21, pubDate=1752940800000, pubDateStr=2025-07-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1792576838198, onlineIssueDateStr=2026-10-21, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1792576838198, creator=13701087609, updateTime=1792576838198, updator=13701087609, issue=Issue{id=1319726164160139662, tenantId=1146029695717560320, journalId=1263187385517883426, year='2025', volume='53', issue='7', pageStart='1777', pageEnd='2078', issueExtLink='null', onlineDate='null', pubDate='1752940800000', pubDateStr='2025-07-20', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1792576836862, creator='13701087609', updateTime=1792577335628, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext={EN=IssueExt(id=1319728256174117458, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1319726164160139662, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1319728256174117459, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1319726164160139662, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null, downloadFileDto=null}, startPage=1816, endPage=1821, ext={EN=ArticleExt(id=1319726169973436595, articleId=1319726169763721394, tenantId=1146029695717560320, journalId=1263187385517883426, language=EN, title=Theoretical Design of Catalysts for Neutral Zinc-Air Batteries, columnId=1322569937034527403, journalTitle=Journal of the Chinese Ceramic Society, columnName=Special Issue on Computation and Design of Electrochemical Energy Storage Materials—Research Article, runingTitle=null, highlight=null, articleAbstract=
Introduction Zinc-air batteries have a significant promise for next-generation energy storage due to their low cost, high safety, high theoretical capacity, and abundant availability. Recently, we reported a new rechargeable zinc-air battery based on zinc peroxide chemistry. Compared to conventional zinc-air batteries, this neutral zinc-air battery exhibits higher reversibility and stability, making it a more promising candidate for secondary zinc-air batteries. However, the low energy efficiency of neutral zinc-air batteries remains a challenge. And the mechanism of these neutral zinc-air battery reactions is still unclear. In this work, we systematically investigated the reaction pathways of neutral zinc-air reaction by first-principles calculations.
Methods Density Functional Theory calculations based on a software package named VASP was employed with PAW potentials and the PBE functional. The vdW interactions were corrected by the Grimme's D3 method. The k-point mesh was generated by the Monkhorst-Pack scheme via Pymatgen with MPRelaxSet settings. A cutoff energy of 520 eV was utilized within a convergence criterion of 10-5 eV for self-consistent calculations. The convergence criterion for ionic relaxation was set to be 0.02 eV/Å. The calculations were performed by a slab model with a thickness of approximately 10 Å and a vacuum layer of greater than 15 Å.
Results and discussion There is a clear linear scaling relationship among the adsorption strengths of O*, ZnO2*, and ZnO4* in neutral zinc-air reactions. This relationship constrains the freedom in catalyst design, making it difficult to optimize all intermediate adsorption strengths simultaneously. Breaking this linear scaling relationship will be a focus of future research. The rate-determined step for both the four-electron and two-electron reactions in Ag (111) is the first electron transfer. A weaker ZnO4* adsorption makes the first reaction barrier as high as 0.78 eV at 1.2 V (vs. Zn/Zn2+). This result indicates that even with this metal catalyst, the discharge voltage of neutral zinc-air batteries remains smaller than that of alkaline batteries due to the limitation of linear scaling relationships.
Among various catalysts, Pt (111) exhibits a lowest reaction barrier, indicating that Pt maintains a high catalytic activity in Zn2+-involved ORR processes. Conversely, the surface reactivity of Ru (111) and Co (001) catalyst surfaces is significantly greater than that of Ag (111), where over-strong ZnO4* adsorption makes the second electron transfer the rate-determined step. Meanwhile, the energy barrier of four-electron pathway is notably lower than that of two-electron transfer pathway, showing that the Ru (111) and Co (001) catalyst can favor a four-electron transfer reaction and form ZnO discharge products.
The optimal O* adsorption free energy is found to be around -6 eV based on the linear scaling relationships. And Ag (111) and Pt (111) have relatively appropriate O* adsorption strengths. The neutral zinc-air catalytic activity of Ag and Pt can be further improved via increasing the d-band center. In addition, the calculations also reveal that catalysts with a strong reactivity favor a four-electron transfer pathway.
Conclusions The theoretical calculation results showed that linear scaling relationships still had true among various adsorption intermediates in neutral zinc-air reactions. Oxygen adsorption strength and overpotential followed the Sabatier principle, indicating that a moderate strength (i.e., ΔGO* ~ -6 eV) yielded an optimal catalytic activity. Among numerous catalysts, Ag and Pt exhibited an optimal surface reactivity with a high theoretical catalytic activity. Furthermore, employing catalysts with a strong surface reactivity, such as Co and Ru, represented a potential approach to achieve non-protonic four-electron zinc-air batteries.
, authors=Zhongxian SUN, Bao ZHANG, Wei SUN, authorsList=Zhongxian SUN, Bao ZHANG, Wei SUN, authorCompany=null, correspAuthors=Bao ZHANG, Wei SUN, authorNote=
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中性锌空气电池因其高比能、高安全性和长寿命受到广泛关注，但其空气正极动力学迟滞问题限制了其实际应用。通过第一性原理计算方法，研究了中性锌空气电池的催化路径，并提出了其催化剂设计的描述符。结果表明：4电子路径倾向于发生在氧吸附强度较强的催化剂上，而2电子路径更易出现在吸附强度较弱的催化剂表面。此外，吸附强度与过电势遵循Sabatier原理，适中吸附强度具有最佳性能。研究发现Pt和Ag表现出适中的氧吸附特性，是中性锌空气电池正极催化剂的潜在候选材料。
, authors=孙中贤, 张宝, 孙威, authorsList=孙中贤, 张宝, 孙威, authorCompany=null, correspAuthors=张宝, 孙威, authorNote=
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张宝（1993—），男，博士，特聘研究员；
孙威（1989—），男，博士，教授。
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SUN Zhongxian (2002-), male, Master candidate. E-mail: szx1341119206@163.com
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SUN Zhongxian (2002-), male, Master candidate. E-mail: szx1341119206@163.com
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孙中贤（2002—），男，硕士研究生。
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孙中贤（2002—），男，硕士研究生。
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