{"title":"通过异质结工程调控电子结构增强氧还原反应","authors":"Shuaishuai Cheng, Weidong Xing, Yahui Wang, Qile Zhao, Jinfang Wu, Xuerong Zheng, Wenbo Wang","doi":"10.1063/5.0271813","DOIUrl":null,"url":null,"abstract":"Transition metal catalysts have promising applications as potential alternatives to platinum-based catalysts in oxygen reduction reactions (ORR), and fine-tuning their local electronic structure is an essential strategy to boost the intrinsic activity. Herein, a Zr–Cu heterojunction catalyst was synthesized by combining ZrO2/C and Cu2(OH)2CO3/C using a simple sol-gel synthesis method. The Zr–Cu heterojunction synergistically achieved high ORR performance with a noticeable half-wave potential of 0.827 V, comparable to commercial Pt/C, along with superior stability and methanol tolerance in alkaline solution. X-ray absorption near-edge spectroscopy (XANES) demonstrated that the interfacial electronic interaction between Zr and Cu species in Zr–Cu heterojunction was enhanced, leading to the enhanced ORR activity. Combined with density functional theory calculations, the Cu atoms located at the interface of Zr–Cu heterojunction were identified as the ORR active sites, while the Zr atoms served as an electronic regulator to induce the electron redistribution by facilitating electron transfer from Zr species and Cu active sites. Therefore, the engineering of Zr–Cu heterojunction catalyst greatly optimized the adsorption strength of O2 as well as reduced the energy barrier of *O2 → *OOH intermediate, ultimately resulting in the promoted ORR performance. The findings of this study suggest a valuable strategy for manipulating heterojunction to optimize the electronic structure of catalytic active sites and improve electrocatalytic reactions.","PeriodicalId":8094,"journal":{"name":"Applied Physics Letters","volume":"3 1","pages":""},"PeriodicalIF":3.6000,"publicationDate":"2025-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Electronic structure regulation via heterojunction engineering for enhanced oxygen reduction reaction\",\"authors\":\"Shuaishuai Cheng, Weidong Xing, Yahui Wang, Qile Zhao, Jinfang Wu, Xuerong Zheng, Wenbo Wang\",\"doi\":\"10.1063/5.0271813\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Transition metal catalysts have promising applications as potential alternatives to platinum-based catalysts in oxygen reduction reactions (ORR), and fine-tuning their local electronic structure is an essential strategy to boost the intrinsic activity. Herein, a Zr–Cu heterojunction catalyst was synthesized by combining ZrO2/C and Cu2(OH)2CO3/C using a simple sol-gel synthesis method. The Zr–Cu heterojunction synergistically achieved high ORR performance with a noticeable half-wave potential of 0.827 V, comparable to commercial Pt/C, along with superior stability and methanol tolerance in alkaline solution. X-ray absorption near-edge spectroscopy (XANES) demonstrated that the interfacial electronic interaction between Zr and Cu species in Zr–Cu heterojunction was enhanced, leading to the enhanced ORR activity. Combined with density functional theory calculations, the Cu atoms located at the interface of Zr–Cu heterojunction were identified as the ORR active sites, while the Zr atoms served as an electronic regulator to induce the electron redistribution by facilitating electron transfer from Zr species and Cu active sites. Therefore, the engineering of Zr–Cu heterojunction catalyst greatly optimized the adsorption strength of O2 as well as reduced the energy barrier of *O2 → *OOH intermediate, ultimately resulting in the promoted ORR performance. The findings of this study suggest a valuable strategy for manipulating heterojunction to optimize the electronic structure of catalytic active sites and improve electrocatalytic reactions.\",\"PeriodicalId\":8094,\"journal\":{\"name\":\"Applied Physics Letters\",\"volume\":\"3 1\",\"pages\":\"\"},\"PeriodicalIF\":3.6000,\"publicationDate\":\"2025-05-29\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Physics Letters\",\"FirstCategoryId\":\"101\",\"ListUrlMain\":\"https://doi.org/10.1063/5.0271813\",\"RegionNum\":2,\"RegionCategory\":\"物理与天体物理\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"PHYSICS, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Physics Letters","FirstCategoryId":"101","ListUrlMain":"https://doi.org/10.1063/5.0271813","RegionNum":2,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"PHYSICS, APPLIED","Score":null,"Total":0}
Electronic structure regulation via heterojunction engineering for enhanced oxygen reduction reaction
Transition metal catalysts have promising applications as potential alternatives to platinum-based catalysts in oxygen reduction reactions (ORR), and fine-tuning their local electronic structure is an essential strategy to boost the intrinsic activity. Herein, a Zr–Cu heterojunction catalyst was synthesized by combining ZrO2/C and Cu2(OH)2CO3/C using a simple sol-gel synthesis method. The Zr–Cu heterojunction synergistically achieved high ORR performance with a noticeable half-wave potential of 0.827 V, comparable to commercial Pt/C, along with superior stability and methanol tolerance in alkaline solution. X-ray absorption near-edge spectroscopy (XANES) demonstrated that the interfacial electronic interaction between Zr and Cu species in Zr–Cu heterojunction was enhanced, leading to the enhanced ORR activity. Combined with density functional theory calculations, the Cu atoms located at the interface of Zr–Cu heterojunction were identified as the ORR active sites, while the Zr atoms served as an electronic regulator to induce the electron redistribution by facilitating electron transfer from Zr species and Cu active sites. Therefore, the engineering of Zr–Cu heterojunction catalyst greatly optimized the adsorption strength of O2 as well as reduced the energy barrier of *O2 → *OOH intermediate, ultimately resulting in the promoted ORR performance. The findings of this study suggest a valuable strategy for manipulating heterojunction to optimize the electronic structure of catalytic active sites and improve electrocatalytic reactions.
期刊介绍:
Applied Physics Letters (APL) features concise, up-to-date reports on significant new findings in applied physics. Emphasizing rapid dissemination of key data and new physical insights, APL offers prompt publication of new experimental and theoretical papers reporting applications of physics phenomena to all branches of science, engineering, and modern technology.
In addition to regular articles, the journal also publishes invited Fast Track, Perspectives, and in-depth Editorials which report on cutting-edge areas in applied physics.
APL Perspectives are forward-looking invited letters which highlight recent developments or discoveries. Emphasis is placed on very recent developments, potentially disruptive technologies, open questions and possible solutions. They also include a mini-roadmap detailing where the community should direct efforts in order for the phenomena to be viable for application and the challenges associated with meeting that performance threshold. Perspectives are characterized by personal viewpoints and opinions of recognized experts in the field.
Fast Track articles are invited original research articles that report results that are particularly novel and important or provide a significant advancement in an emerging field. Because of the urgency and scientific importance of the work, the peer review process is accelerated. If, during the review process, it becomes apparent that the paper does not meet the Fast Track criterion, it is returned to a normal track.