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Carbon-Shielded Single-Atom Alloy Material Family for Multi-Functional Electrocatalysis

机译:Carbon-Shielded Single-Atom Alloy Material Family for Multi-Functional Electrocatalysis

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摘要

Encapsulating metal-based catalysts inside carbon sheaths is a frequentlyadoptedstrategy to enhance their durability under various harsh situationsand improve their catalytic activity simultaneously. Such carbon encapsulation,however, imposes significant complications for directly modifying materials’surface atomic/electronic configurations, fundamentally impeding theaccurate tuning of their catalytic capabilities. Herein, a universal single-atomalloy (SAA) strategy is reported to indirectly yet precisely manipulate the surfaceelectronic structure of carbon-encapsulated electrocatalysts. By versatilelyconstructing a SAA core inside an N-doped carbon sheath, material’s electrocatalyticcapability can be flexibly tuned. The one with Ru-SAA cores servesas an excellent bifunctional electrocatalyst for oxygen/hydrogen evolution,exhibiting minimal cell voltage of 1.55 V (10 mA cm~(?2)) and outstanding massactivity of 1251 mA mg_(Ru)~(?1) for overall water splitting, while the one with Ir-SAAcores possesses superior oxygen reduction activity with a half-wave potentialof 919 mV. Density functional theory calculations reveal that the doped atomscan simultaneously optimize the adsorption of protons (H*) and oxygenatedintermediates (OH*, O*, and OOH*) to achieve the remarkable thermoneutralhydrogen evolution and enhanced oxygen evolution. This work thusdemonstrates a versatile strategy to precisely modify the surface electronicproperties of carbon-shielded materials for optimized performances.

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  • 来源
    《Advanced functional materials》 |2022年第43期|2205654.1-2205654.11|共11页
  • 作者单位

    Key Laboratory for Advanced Ceramics and Machining Technology ofMinistry of EducationSchool of Materials Science and EngineeringTianjin UniversityTianjin 300350, P. R. China Institute for Superconducting & Electronic MaterialsAustralian Institute of Innov;

    Key Laboratory for Advanced Ceramics and Machining Technology ofMinistry of EducationSchool of Materials Science and EngineeringTianjin UniversityTianjin 300350, P. R. China;

    Applied Physics DepartmentCollege of Physics and Materials ScienceTianjin Normal UniversityTianjin 300387, P. R. ChinaDepartment of ElectrophysicsNational Chiao Tung UniversityHsinchu, Taiwan 30076, P. R. ChinaSchool of Chemical EngineeringThe University of New South WalesSydney, NSW 2052, AustraliaShenyang National Laboratory for Materials ScienceInstitute of Metal ResearchChinese Academy of SciencesShenyang, Liaoning 110016, P. R. ChinaInstitute for Superconducting & Electronic MaterialsAustralian Institute of Innovative MaterialsUniversity of WollongongInnovation Campus, Squires Way, North Wollongong, NSW 2500, AustraliaDICP-Surrey Joint Centre for Future MaterialsDepartment of Chemical and Process Engineeringand Advanced Technology InstituteUniversity of SurreyGuildford, Surrey GU2 7XH, UK;

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

    multifunctional electrocatalysts; oxygen reduction reactions; remote manipulations; single atom alloys; water splitting;

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