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Orienting Active Crystal Planes of New Class Lacunaris Fe_2PO_5 Polyhedrons for Robust Water Oxidation in Alkaline and Neutral Media

机译:定向新型Lacunaris Fe_2PO_5多面体的有源晶体平面,以在碱性和中性介质中进行稳健的水氧化

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摘要

Developing efficient and stable oxygen evolution reaction (OER) electrocatalysts is essential for realizing sustainable energy conversion, such as solar fuels. Although modulating active sites and electron transfer is of great significance to boost electrocatalysis activity, it still remains a big challenge to desirably actualize this goal. Herein, engineering of active sites and electronic framework is implemented via oriented modulation of crystal planes and construction of lacunaris architecture supported by ammonification-elicited simultaneous incorporation of nitrogen and oxygen-defect strategy. The new class porous nitrogen-incorporated Fe2PO5 with oxygen-defect (N-Fe2PO5-x) polyhedron with dominantly exposed {110} reactive facets exhibits superior performance toward water oxidation, achieving current densities of 10 mA cm(-2) at quite low overpotentials of 235 and 315 mV in alkaline and neutral media, respectively. Furthermore, density functional theoretical calculations reveal the energetically favorable {110} planes of lower absorption energy of intermediates and remolding of electronic density framework arising from the ammoniated elicitation process, contributing to excellent OER performance of lacunaris N-Fe2PO5-x polyhedrons. This work may offer a feasible guideline for regulating active sites and electron transfer to develop low-cost and highly efficient OER electrocatalysts in energy conversion systems.
机译:开发有效而稳定的氧气析出反应(OER)电催化剂对于实现可持续的能源转化至关重要,例如太阳能。尽管调节活性位和电子转移对于提高电催化活性具有重要意义,但仍难以实现理想的目标。在此,通过晶面的定向调制和通过氨化引发的氮和氧缺陷策略的同时引入支持的空洞结构的构建,实现了活性位点和电子框架的工程。具有氧缺陷(N-Fe2PO5-x)多面体的新型多孔氮结合Fe2PO5,具有显着暴露的{110}反应性面,表现出优异的抗水氧化性能,在相当低的超电势下实现了10 mA cm(-2)的电流密度在碱性和中性介质中分别为235 mV和315 mV。此外,密度泛函理论计算揭示了氨化激发过程产生的较低的中间体吸收能和电子密度骨架的重塑在能量上有利的{110}面,这有助于腔隙N-Fe2PO5-x多面体的优异OER性能。这项工作可能为调节活性位点和电子转移以在能量转换系统中开发低成本和高效的OER电催化剂提供可行的指导。

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  • 来源
    《Advanced Functional Materials》 |2018年第35期|1801397.1-1801397.11|共11页
  • 作者单位

    Dalian Univ Technol, Inst Energy Sci & Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China;

    Chinese Acad Sci, Changchun Inst Appl Chem, State Key Lab Rare Earth Resource Utilizat, Changchun 130022, Jilin, Peoples R China;

    Dalian Univ Technol, Inst Energy Sci & Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China;

    Dalian Univ Technol, Inst Energy Sci & Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China;

    Dalian Univ Technol, Inst Energy Sci & Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China;

    Chinese Acad Sci, Changchun Inst Appl Chem, State Key Lab Rare Earth Resource Utilizat, Changchun 130022, Jilin, Peoples R China;

    Dalian Univ Technol, Inst Energy Sci & Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    active plane; electronic framework; Fe2PO5 polyhedrons; lacunaris structure; water oxidation;

    机译:活性平面;电子框架;Fe2PO5多面体;腔隙结构;水氧化;

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