{"title":"氧驱动重建激活锌-空气和燃料电池中空心PdAg纳米管准单钯位。","authors":"Zongge Li, Wenjie Tian, Kunsheng Hu, Yajie Guo, Xiaotan Tian, Wenjun Kang, Rui Li, Konggang Qu, Lei Wang, Fanpeng Meng, Huayang Zhang, Haibo Li","doi":"10.1002/advs.202509329","DOIUrl":null,"url":null,"abstract":"<p><p>Here, a template-engaged galvanic replacement strategy is developed to construct hollow PdAg alloy nanotubes, where interfacial oxygen drives surface reconstruction and stabilizes quasi-single Pd active sites. The interplay of atomic-scale characterizations and theoretical calculations reveals that the oxygen-induced atomic rearrangement downshifts the Pd d-band center, optimizes the adsorption-desorption energetics of ORR intermediates, and lowers the energy barrier for <sup>*</sup>OH desorption. The optimized Pd<sub>0.30</sub>@Ag catalyst achieves an onset potential of 0.951 V and a half-wave potential of 0.868 V in alkaline media, surpassing commercial Pt/C even at an ultra-low Pd loading (3 wt.%). Furthermore, Pd<sub>0.30</sub>@Ag-based electrodes deliver outstanding performance in both zinc-air batteries (ZABs) and anion-exchange membrane fuel cells (AEMFCs), demonstrating high power densities, excellent cycling stability, and strong potential for scalable platinum-free energy conversion devices. This work provides a general strategy for engineering interface-confined active sites through surface reconstruction, offering new insights into the rational design of next-generation electrocatalysts.</p>","PeriodicalId":117,"journal":{"name":"Advanced Science","volume":" ","pages":"e09329"},"PeriodicalIF":14.1000,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Oxygen-Driven Reconstruction Activates Quasi-Single Pd Sites in Hollow PdAg Nanotubes for Zinc-Air and Fuel Cells.\",\"authors\":\"Zongge Li, Wenjie Tian, Kunsheng Hu, Yajie Guo, Xiaotan Tian, Wenjun Kang, Rui Li, Konggang Qu, Lei Wang, Fanpeng Meng, Huayang Zhang, Haibo Li\",\"doi\":\"10.1002/advs.202509329\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Here, a template-engaged galvanic replacement strategy is developed to construct hollow PdAg alloy nanotubes, where interfacial oxygen drives surface reconstruction and stabilizes quasi-single Pd active sites. The interplay of atomic-scale characterizations and theoretical calculations reveals that the oxygen-induced atomic rearrangement downshifts the Pd d-band center, optimizes the adsorption-desorption energetics of ORR intermediates, and lowers the energy barrier for <sup>*</sup>OH desorption. The optimized Pd<sub>0.30</sub>@Ag catalyst achieves an onset potential of 0.951 V and a half-wave potential of 0.868 V in alkaline media, surpassing commercial Pt/C even at an ultra-low Pd loading (3 wt.%). Furthermore, Pd<sub>0.30</sub>@Ag-based electrodes deliver outstanding performance in both zinc-air batteries (ZABs) and anion-exchange membrane fuel cells (AEMFCs), demonstrating high power densities, excellent cycling stability, and strong potential for scalable platinum-free energy conversion devices. This work provides a general strategy for engineering interface-confined active sites through surface reconstruction, offering new insights into the rational design of next-generation electrocatalysts.</p>\",\"PeriodicalId\":117,\"journal\":{\"name\":\"Advanced Science\",\"volume\":\" \",\"pages\":\"e09329\"},\"PeriodicalIF\":14.1000,\"publicationDate\":\"2025-07-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Advanced Science\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1002/advs.202509329\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Science","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/advs.202509329","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Oxygen-Driven Reconstruction Activates Quasi-Single Pd Sites in Hollow PdAg Nanotubes for Zinc-Air and Fuel Cells.
Here, a template-engaged galvanic replacement strategy is developed to construct hollow PdAg alloy nanotubes, where interfacial oxygen drives surface reconstruction and stabilizes quasi-single Pd active sites. The interplay of atomic-scale characterizations and theoretical calculations reveals that the oxygen-induced atomic rearrangement downshifts the Pd d-band center, optimizes the adsorption-desorption energetics of ORR intermediates, and lowers the energy barrier for *OH desorption. The optimized Pd0.30@Ag catalyst achieves an onset potential of 0.951 V and a half-wave potential of 0.868 V in alkaline media, surpassing commercial Pt/C even at an ultra-low Pd loading (3 wt.%). Furthermore, Pd0.30@Ag-based electrodes deliver outstanding performance in both zinc-air batteries (ZABs) and anion-exchange membrane fuel cells (AEMFCs), demonstrating high power densities, excellent cycling stability, and strong potential for scalable platinum-free energy conversion devices. This work provides a general strategy for engineering interface-confined active sites through surface reconstruction, offering new insights into the rational design of next-generation electrocatalysts.
期刊介绍:
Advanced Science is a prestigious open access journal that focuses on interdisciplinary research in materials science, physics, chemistry, medical and life sciences, and engineering. The journal aims to promote cutting-edge research by employing a rigorous and impartial review process. It is committed to presenting research articles with the highest quality production standards, ensuring maximum accessibility of top scientific findings. With its vibrant and innovative publication platform, Advanced Science seeks to revolutionize the dissemination and organization of scientific knowledge.