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Hydrogen spillover bridged dual nano-islands triggered by built-in electric field for efficient and robust alkaline hydrogen evolution at ampere-level current density
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作者 Kecheng Tong Liangliang Xu +7 位作者 hanxu yao Xingkun Wang Canhui Zhang Fan Yang Lei Chu Jinwoo Lee Heqing Jiang Minghua Huang 《Nano Research》 SCIE EI CSCD 2024年第6期5050-5060,共11页
Employing the alkaline water electrolysis system to generate hydrogen holds great prospects but still poses significant challenges,particularly for the construction of hydrogen evolution reaction(HER)catalysts operati... Employing the alkaline water electrolysis system to generate hydrogen holds great prospects but still poses significant challenges,particularly for the construction of hydrogen evolution reaction(HER)catalysts operating at ampere-level current density.Herein,the unique Ru and RuP_(2)dual nano-islands are deliberately implanted on N-doped carbon substrate(denoted as Ru-RuP_(2)/NC),in which a built-in electric field(BEF)is spontaneously generated between Ru-RuP_(2)dual nano-islands driven by their work function difference.Experimental and theoretical results unveil that such constructed BEF could serve as the driving force for triggering fast hydrogen spillover process on bridged Ru-RuP_(2)dual nano-islands,which could invalidate the inhibitory effect of high hydrogen coverage at ampere-level current density,and synchronously speed up the water dissociation on Ru nano-islands and hydrogen adsorption/desorption on RuP_(2)nano-islands through hydrogen spillover process.As a result,the Ru-RuP_(2)/NC affords an ultra-low overpotential of 218 mV to achieve 1.0 A·cm^(−2)along with the superior stability over 1000 h,holding the great promising prospect in practical applications at ampere-level current density.More importantly,this work is the first to advance the scientific understanding of the relationship between the constructed BEF and hydrogen spillover process,which could be enlightening for the rational design of the cost-effective alkaline HER catalysts at ampere-level current density. 展开更多
关键词 built-in electric field hydrogen spillover dual nano-islands ampere-level current density alkaline hydrogen evolution
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近邻Ni位点对双Fe中心电子自旋态调制实现催化剂增强的催化活性和锌空气电池超长稳定性 被引量:1
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作者 张灿辉 汪兴坤 +11 位作者 马镇涛 姚涵旭 刘恒均 李铖 周健 徐仁 郑旭升 王焕磊 李强 谷猛 江河清 黄明华 《Science Bulletin》 SCIE EI CAS CSCD 2023年第18期2042-2053,M0004,共13页
在锌空气电池(ZABs)领域中,开发具有优异氧还原反应(ORR)活性和超长期稳定性的Fe基单原子催化剂是一项充满挑战的任务.为此,本文在氮掺杂空心碳球上构建了近邻NiN4单原子位点和Fe_(2)N_(5)双原子位点共存的催化剂(Fe/Ni-NHCS),作为ZABs... 在锌空气电池(ZABs)领域中,开发具有优异氧还原反应(ORR)活性和超长期稳定性的Fe基单原子催化剂是一项充满挑战的任务.为此,本文在氮掺杂空心碳球上构建了近邻NiN4单原子位点和Fe_(2)N_(5)双原子位点共存的催化剂(Fe/Ni-NHCS),作为ZABs中高效稳定的空气阴极ORR电催化剂.理论计算和磁性测试结果均表明,近邻NiN_(4)位点的引入对优化Fe2Ns位点的电子自旋态和降低含氧中间体吸附和转化能垒起到关键作用,从而使得Fe/Ni-NHCS具有出色的ORR催化活性和极低的副产物HO_(2)产率。更重要的是,由Fe/Ni-NHCS作为空气阴极驱动的ZABs展现出超过1200h的长时间可充放电循环稳定性。该工作通过调制活性位点的自旋态同时实现了对于催化活性和稳定性的双重优化,从而为能量转换技术的发展拓展了一条新路径。 展开更多
关键词 Dual-metal-atom Electron spin state Oxygen reduction reaction Rechargeable stability
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