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首页> 外文期刊>Advanced Functional Materials >All-pH Stable Sandwich-Structured MoO_2/MoS_2/C Hollow Nanoreactors for Enhanced Electrochemical Hydrogen Evolution
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All-pH Stable Sandwich-Structured MoO_2/MoS_2/C Hollow Nanoreactors for Enhanced Electrochemical Hydrogen Evolution

机译：全pH稳定夹层结构MOO_2 / MOS_2 / C中空纳米反应器，用于增强电化学氢气进化

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摘要

Molybdenum sulfide has great potential for the electrocatalytic hydrogen evolution, but its structural instability in acidic media and high barriers in alkaline/neutral media limits its practical applications. Herein, the design of monodispersed sandwich-structured MoO2/MoS2/C hollow nanoreactors is reported with a triple layer "conductor/catalyst/protector" configuration for efficient electrochemical hydrogen evolution over all pH values. Metallic MoO2 substrates with ultrahigh pristine electroconductivity can promote the charge transfer while sulfur vacancies are introduced to activate the highly exposed (002) facets of MoS2. The optimized MoO2/MoS2/C nanoreactor exhibits overpotentials of 77, 91, and 97 mV (10 mA cm(-2)) and Tafel slopes of 41, 49, and 53 mV dec(-1) in acidic, alkaline, and neutral media, respectively, which are much better than most of the MoS2-based electrocatalysts. Moreover, defective carbon shells are in situ generated, preventing the electrocatalysts from corrosion in acidic and alkaline media; the structural stability is verified via in situ Raman and XRD characterizations. Based on the density functional theory calculations, vacancy engineering can regulate the band structures, electron density differences, total density of states, and the H* and H2O adsorption-dissociation ability over the entire pH range. The findings may shed light on the rational development of practical pH-universal electrocatalysts for durable hydrogen evolution.
机译：硫化钼对电催化氢进化具有很大的潜力，但其在酸性介质和碱性/中性介质中的高屏障中的结构不稳定限制了其实际应用。这里，用三层“导体/催化剂/保护器”构造报告了单分散的夹层结构MOO2 / MOO2 / C中空纳米反应器的设计，用于所有pH值上有效电化学氢气进化。具有超高原始导电性的金属MOO2基材可以促进电荷转移，而引入硫空位以激活MOS2的高曝光（002）刻面。优化的MOO2 / MOS2 / C纳米反应器表现出77,91和97mV（10 mA cm（-2））和41,49和53mV（-1）的Tafel斜率在酸性，碱性和中性中的过电分别比大多数基于MOS2的电催化剂更好的媒体。此外，有缺陷的碳壳原位产生，防止电催化剂免受酸性和碱性介质的腐蚀;通过原位拉曼和XRD表征验证了结构稳定性。基于密度函数理论计算，空缺工程可以调节带结构，电子密度差，状态的总密度，以及在整个pH范围内的H *和H2O吸附 - 解离能力。该研究结果可能阐明了实际pH-通用电催化剂的合理发育，用于耐用的氢气进化。

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  • 来源
    《Advanced Functional Materials》 |2021年第27期|2101715.1-2101715.10|共10页
  • 作者

    Gong Feilong; Liu Mengmeng; Ye Sheng; Gong Lihua; Zeng Guang; Xu Lin; Zhang Xiaoli; Zhang Yonghui; Zhou Liming; Fang Shaoming; Liu Jian;

  • 作者单位

    Zhengzhou Univ Light Ind Coll Mat & Chem Engn Key Lab Surface & Interface Sci & Technol Henan P Zhengzhou 450002 Henan Peoples R China;

    Zhengzhou Univ Light Ind Coll Mat & Chem Engn Key Lab Surface & Interface Sci & Technol Henan P Zhengzhou 450002 Henan Peoples R China;

    Chinese Acad Sci Dalian Inst Chem Phys State Key Lab Catalysis Dalian 116023 Liaoning Peoples R China;

    Zhengzhou Univ Light Ind Coll Mat & Chem Engn Key Lab Surface & Interface Sci & Technol Henan P Zhengzhou 450002 Henan Peoples R China;

    Chinese Acad Sci Dalian Inst Chem Phys State Key Lab Catalysis Dalian 116023 Liaoning Peoples R China;

    Sch Mat Sci & Engn Wuhan 430070 Hubei Peoples R China|State Key Lab Adv Technol Mat Synth & Proc Wuhan 430070 Hubei Peoples R China;

    Zhengzhou Univ Sch Mat Sci & Engn Zhengzhou 450001 Henan Peoples R China|Zhengzhou Univ State Ctr Int Cooperat Designer Low Carbon & Envi Zhengzhou 450001 Henan Peoples R China;

    Zhengzhou Univ Light Ind Coll Mat & Chem Engn Key Lab Surface & Interface Sci & Technol Henan P Zhengzhou 450002 Henan Peoples R China;

    Zhengzhou Univ Light Ind Coll Mat & Chem Engn Key Lab Surface & Interface Sci & Technol Henan P Zhengzhou 450002 Henan Peoples R China;

    Zhengzhou Univ Light Ind Coll Mat & Chem Engn Key Lab Surface & Interface Sci & Technol Henan P Zhengzhou 450002 Henan Peoples R China;

    Chinese Acad Sci Dalian Inst Chem Phys State Key Lab Catalysis Dalian 116023 Liaoning Peoples R China|Univ Surrey DICP Surrey Joint Ctr Future Mat Dept Chem & Proc Engn Guildford GU2 7XH Surrey England|Univ Surrey Adv Technol Inst Guildford GU2 7XH Surrey England;

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  • 正文语种 eng
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  • 关键词

    all-pH stability; electrocatalytic hydrogen evolution; MoS; (2); nanoreactors; vacancies;

    机译：全pH稳定性;电催化氢进化;MOS;（2）;纳米反应器;职位空缺;

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