IF 11.3 1区 化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2024-12-16 DOI:10.1021/acscatal.4c05857
Jaeyoung Yoo, Jungwoo Choi, Suyeon Choi, Changsoo Lee, Hyuck Mo Lee
{"title":"Facet-Controlled Pt3M Alloys as Enhanced Catalysts for Ammonia Oxidation Reaction: A Combined Theoretical and Experimental Study","authors":"Jaeyoung Yoo, Jungwoo Choi, Suyeon Choi, Changsoo Lee, Hyuck Mo Lee","doi":"10.1021/acscatal.4c05857","DOIUrl":null,"url":null,"abstract":"Ammonia (NH<sub>3</sub>) is emerging as a promising carbon-free chemical energy source, offering higher storage capacity per unit volume compared to hydrogen and enhanced ease of liquefaction. This makes NH<sub>3</sub> suitable for long-distance transportation and various industrial applications. The ammonia oxidation reaction (AOR) is crucial for electrochemically converting NH<sub>3</sub> into H<sub>2</sub>, but current AOR catalysts face commercialization challenges due to cost and efficiency issues. This study explores ways to enhance AOR catalysts through a combined theoretical and experimental approach, focusing on Pt<sub>3</sub>X (where X represents screening elements) alloys. Density functional theory calculations were employed to analyze the AOR mechanism on Pt(111), (110), and (100) surfaces, identifying descriptors that facilitated the high-throughput screening of Pt<sub>3</sub>X alloys with (111), (110), and (100) facets for the highest AOR activity. The selected Pt<sub>3</sub>M (M = Fe, Co, and Ni) alloys were synthesized and characterized, revealing well-defined cubic shapes and superior AOR properties compared to pure Pt. Experimental results confirmed that Pt<sub>3</sub>Fe and Pt<sub>3</sub>Co nanocubes exhibit enhanced AOR activity and stability, aligning with theoretical predictions. This integrated approach highlights the potential of Pt<sub>3</sub>M alloys as cost-effective and efficient AOR catalysts, advancing ammonia electrolysis technologies for hydrogen production.","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"22 1","pages":""},"PeriodicalIF":11.3000,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Catalysis ","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acscatal.4c05857","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0

摘要

氨气(NH3)是一种前景广阔的无碳化学能源,与氢气相比,它的单位体积储存能力更高,而且更易于液化。这使得 NH3 适合长途运输和各种工业应用。氨氧化反应(AOR)是电化学将 NH3 转化为 H2 的关键,但由于成本和效率问题,目前的 AOR 催化剂面临商业化挑战。本研究通过理论与实验相结合的方法,以 Pt3X(其中 X 代表筛选元素)合金为重点,探索增强 AOR 催化剂的方法。采用密度泛函理论计算分析了 Pt(111)、(110)和(100)表面的 AOR 机理,确定了有助于高通量筛选具有 (111)、(110) 和 (100) 面的 Pt3X 合金的描述符,以获得最高的 AOR 活性。对筛选出的 Pt3M(M = 铁、钴和镍)合金进行了合成和表征,结果表明与纯铂相比,这些合金具有明确的立方体形状和优异的 AOR 性能。实验结果证实,Pt3Fe 和 Pt3Co 纳米立方体表现出更强的 AOR 活性和稳定性,与理论预测一致。这种综合方法凸显了 Pt3M 合金作为具有成本效益的高效 AOR 催化剂的潜力,从而推动了氨电解制氢技术的发展。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

摘要图片

查看原文
分享 分享
微信好友 朋友圈 QQ好友 复制链接
本刊更多论文
Facet-Controlled Pt3M Alloys as Enhanced Catalysts for Ammonia Oxidation Reaction: A Combined Theoretical and Experimental Study
Ammonia (NH3) is emerging as a promising carbon-free chemical energy source, offering higher storage capacity per unit volume compared to hydrogen and enhanced ease of liquefaction. This makes NH3 suitable for long-distance transportation and various industrial applications. The ammonia oxidation reaction (AOR) is crucial for electrochemically converting NH3 into H2, but current AOR catalysts face commercialization challenges due to cost and efficiency issues. This study explores ways to enhance AOR catalysts through a combined theoretical and experimental approach, focusing on Pt3X (where X represents screening elements) alloys. Density functional theory calculations were employed to analyze the AOR mechanism on Pt(111), (110), and (100) surfaces, identifying descriptors that facilitated the high-throughput screening of Pt3X alloys with (111), (110), and (100) facets for the highest AOR activity. The selected Pt3M (M = Fe, Co, and Ni) alloys were synthesized and characterized, revealing well-defined cubic shapes and superior AOR properties compared to pure Pt. Experimental results confirmed that Pt3Fe and Pt3Co nanocubes exhibit enhanced AOR activity and stability, aligning with theoretical predictions. This integrated approach highlights the potential of Pt3M alloys as cost-effective and efficient AOR catalysts, advancing ammonia electrolysis technologies for hydrogen production.
求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
期刊最新文献
Highly Active and Stable Al-Doped NiFe Self-Supported Oxygen Evolution Reaction Electrode for Alkaline Water Electrolysis Bioinspired Molecular Catalyst for Photocatalytic Semihydrogenation of Acetylene with Water as a Proton Source Construction of Highly Active Fe5C2–FeCo Interfacial Sites for Oriented Synthesis of Light Olefins from CO2 Hydrogenation Dynamic Kinetic Reductive Grignard-Type Addition for the Construction of Axial and Central Chirality Hydrogen Evolution and Oxygen Reduction on OH/F-Terminated Titanium Nitride MXene Reveal the Role of the Surface Termination Group in Electrocatalysis
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
已复制链接
已复制链接
快去分享给好友吧!
我知道了
×
扫码分享
扫码分享
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1