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Rational Design of Holey 2D Nonlayered Transition Metal Carbide/Nitride Heterostructure Nanosheets for Highly Efficient Water Oxidation

机译:用于高效水氧化的多孔2D非分层过渡金属碳化物/氮化物异质结构纳米片的合理设计

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摘要

Due to integrated advantages in electrochemical functionalities for energy conversion, 2D nonlayered heterostructure nanosheets offer new and fascinating opportunities for electrocatalysis but their fabrication is challenging when compared with the widely studied 2D layered heterostructure. Herein, a bottom-up approach is established for facile synthesis of holey 2D transition metal carbideitride heterostructure nanosheets (h-TMCN) with regulated hole sizes by controlled thermal annealing of the Mo/Zn bimetallic imidazolate frameworks (Mo/Zn BIFs). Ex situ phase and structural identifications disclose that the Mo/Zn BIFs precursor experiences interconnected three steps of transformation to produce h-TMCN. Especially, the slow successive solid-state diffusion of nitrogen and carbon into immediate noncrystalline molybdenum oxides allows the intergrowth of Mo2C and Mo2N into the 2D nonlayered heterostructure. X-ray fine structure analysis coupled with high resolution X-ray photoelectron spectroscopy demonstrate that Mo2C and Mo2N in the microdomains can chemically bond with each other, producing the abundant active N-Mo-C interfaces toward water splitting. Consequently, h-TMCN affords low overpotentials, high turnover frequencies, rapid charge transfer, and superior long-term stability toward electrocatalytic water oxidation. The present work demonstrates the feasibility of developing a broad range of 2D nonlayered heterostructures for high efficiency chemical energy conversion.
机译:由于用于能量转换的电化学功能方面的综合优势,二维非层状异质结构纳米片为电催化提供了新的且令人着迷的机会,但与广泛研究的二维层状异质结构相比,其制造具有挑战性。本文中,建立了一种自下而上的方法,用于通过受控的Mo / Zn双金属咪唑化物骨架(Mo / Zn BIFs)的热退火,轻松合成具有受控孔尺寸的多孔2D过渡金属碳化物/氮化物异质结构纳米片(h-TMCN)。异位相和结构鉴定表明,Mo / Zn BIFs前体经历了相互转化的三个步骤,以生成h-TMCN。尤其是,氮和碳缓慢连续的固态扩散到直接的非晶态氧化钼中,使Mo2C和Mo2N互生到2D非层状异质结构中。 X射线精细结构分析和高分辨率X射线光电子能谱表明,微区中的Mo2C和Mo2N可以彼此化学键合,从而产生了丰富的活性N-Mo-C界面,可以分解水。因此,h-TMCN具有较低的过电势,较高的周转频率,快速的电荷转移以及对电催化水氧化的优异长期稳定性。本工作证明了开发用于高效化学能转化的各种2D非分层异质结构的可行性。

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  • 来源
    《Advanced energy materials》 |2019年第16期|1803768.1-1803768.10|共10页
  • 作者单位

    Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117574, Singapore;

    Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Hubei, Peoples R China;

    Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117574, Singapore;

    Wuhan Univ Technol, State Key Lab Silicate Mat Architectures, Wuhan 430070, Hubei, Peoples R China;

    Chinese Acad Sci, Beijing Synchrotron Radiat Facil, Inst High Energy Phys, Beijing 100049, Peoples R China;

    Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117574, Singapore;

    Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117574, Singapore;

    Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117574, Singapore;

    Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Hubei, Peoples R China|Natl Res Tomsk Polytech Univ, Lenin Ave 30, Tomsk 634050, Russia;

    Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117574, Singapore;

    Wuhan Univ Technol, State Key Lab Adv Technol Mat Synth & Proc, Wuhan 430070, Hubei, Peoples R China;

    Natl Univ Singapore, Dept Mat Sci & Engn, Singapore 117574, Singapore;

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  • 正文语种 eng
  • 中图分类
  • 关键词

    2D nonlayered structure; carbide; heterostructure; nitride; water splitting;

    机译:二维非层状结构;碳化物;异质结构;氮化物;水分解;

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