{"title":"具有相依赖电子结构的焦耳加热PdFe合金用于高效氧还原","authors":"Dandan Jiang, Danyang Wu, Yu Wang, Yongze Cao, Xizhen Zhang, Baojiu Chen","doi":"10.1016/j.ijhydene.2025.05.400","DOIUrl":null,"url":null,"abstract":"<div><div>The design of Pd-based alloys with tailored electronic structures and stable architectures is crucial for enhancing catalytic properties. Here, we present a rapid Joule heating strategy for fabricating a palladium-iron (PdFe) alloy anchored on nitrogen-doped carbon (NC–FePd) featuring exceptional performance and durability. By combining ultrafast phase formation and quenching, the NC-FePd system achieves uniform dispersion of cubic-phase FePd<sub>3</sub> nanoparticles with minimized agglomeration. X-ray diffraction and XPS analyses reveal lattice expansion planes and electron transfer between Pd and Fe, which lowers the d-band center of Pd, thereby weakening the Pd–O binding energy. In alkaline media, NC-FePd achieves an exceptional half-wave potential (0.84 V vs. RHE), showing a clear advantage over commercial Pt/C (0.82 V vs. RHE), coupled with elevated limiting current density (6.01 mA cm<sup>−2</sup>) and the diminished Tafel slope (53.73 mV dec<sup>−1</sup>). This work sheds light on the synergy between rapid Joule-heating synthesis and Fe–Pd electronic modulation for designing durable alloy catalysts.</div></div>","PeriodicalId":337,"journal":{"name":"International Journal of Hydrogen Energy","volume":"148 ","pages":"Article 149770"},"PeriodicalIF":8.3000,"publicationDate":"2025-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Joule-heated PdFe alloys with phase-dependent electronic structures for high-efficiency oxygen reduction\",\"authors\":\"Dandan Jiang, Danyang Wu, Yu Wang, Yongze Cao, Xizhen Zhang, Baojiu Chen\",\"doi\":\"10.1016/j.ijhydene.2025.05.400\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The design of Pd-based alloys with tailored electronic structures and stable architectures is crucial for enhancing catalytic properties. Here, we present a rapid Joule heating strategy for fabricating a palladium-iron (PdFe) alloy anchored on nitrogen-doped carbon (NC–FePd) featuring exceptional performance and durability. By combining ultrafast phase formation and quenching, the NC-FePd system achieves uniform dispersion of cubic-phase FePd<sub>3</sub> nanoparticles with minimized agglomeration. X-ray diffraction and XPS analyses reveal lattice expansion planes and electron transfer between Pd and Fe, which lowers the d-band center of Pd, thereby weakening the Pd–O binding energy. In alkaline media, NC-FePd achieves an exceptional half-wave potential (0.84 V vs. RHE), showing a clear advantage over commercial Pt/C (0.82 V vs. RHE), coupled with elevated limiting current density (6.01 mA cm<sup>−2</sup>) and the diminished Tafel slope (53.73 mV dec<sup>−1</sup>). This work sheds light on the synergy between rapid Joule-heating synthesis and Fe–Pd electronic modulation for designing durable alloy catalysts.</div></div>\",\"PeriodicalId\":337,\"journal\":{\"name\":\"International Journal of Hydrogen Energy\",\"volume\":\"148 \",\"pages\":\"Article 149770\"},\"PeriodicalIF\":8.3000,\"publicationDate\":\"2025-06-18\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"International Journal of Hydrogen Energy\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0360319925027168\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"International Journal of Hydrogen Energy","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0360319925027168","RegionNum":2,"RegionCategory":"工程技术","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
设计具有定制电子结构和稳定结构的pd基合金对于提高催化性能至关重要。在这里,我们提出了一种快速焦耳加热策略,用于制造锚定在氮掺杂碳(NC-FePd)上的钯铁(PdFe)合金,具有卓越的性能和耐用性。NC-FePd体系通过超快相形成和淬灭相结合,实现了三相FePd3纳米颗粒的均匀分散和最小团聚。x射线衍射和XPS分析表明,Pd和Fe之间的晶格扩展面和电子转移降低了Pd的d带中心,从而减弱了Pd - o的结合能。在碱性介质中,NC-FePd实现了特殊的半波电位(0.84 V vs. RHE),与商用Pt/C (0.82 V vs. RHE)相比,具有明显的优势,同时具有更高的极限电流密度(6.01 mA cm−2)和降低的塔菲尔斜率(53.73 mV dec−1)。这项工作揭示了快速焦耳加热合成和Fe-Pd电子调制之间的协同作用,用于设计耐用的合金催化剂。
Joule-heated PdFe alloys with phase-dependent electronic structures for high-efficiency oxygen reduction
The design of Pd-based alloys with tailored electronic structures and stable architectures is crucial for enhancing catalytic properties. Here, we present a rapid Joule heating strategy for fabricating a palladium-iron (PdFe) alloy anchored on nitrogen-doped carbon (NC–FePd) featuring exceptional performance and durability. By combining ultrafast phase formation and quenching, the NC-FePd system achieves uniform dispersion of cubic-phase FePd3 nanoparticles with minimized agglomeration. X-ray diffraction and XPS analyses reveal lattice expansion planes and electron transfer between Pd and Fe, which lowers the d-band center of Pd, thereby weakening the Pd–O binding energy. In alkaline media, NC-FePd achieves an exceptional half-wave potential (0.84 V vs. RHE), showing a clear advantage over commercial Pt/C (0.82 V vs. RHE), coupled with elevated limiting current density (6.01 mA cm−2) and the diminished Tafel slope (53.73 mV dec−1). This work sheds light on the synergy between rapid Joule-heating synthesis and Fe–Pd electronic modulation for designing durable alloy catalysts.
期刊介绍:
The objective of the International Journal of Hydrogen Energy is to facilitate the exchange of new ideas, technological advancements, and research findings in the field of Hydrogen Energy among scientists and engineers worldwide. This journal showcases original research, both analytical and experimental, covering various aspects of Hydrogen Energy. These include production, storage, transmission, utilization, enabling technologies, environmental impact, economic considerations, and global perspectives on hydrogen and its carriers such as NH3, CH4, alcohols, etc.
The utilization aspect encompasses various methods such as thermochemical (combustion), photochemical, electrochemical (fuel cells), and nuclear conversion of hydrogen, hydrogen isotopes, and hydrogen carriers into thermal, mechanical, and electrical energies. The applications of these energies can be found in transportation (including aerospace), industrial, commercial, and residential sectors.