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A General Synthetic Strategy toward Highly Doped Pyridinic Nitrogen-Rich Carbons

机译:高掺杂吡啶富含富含碳碳的一般合成策略

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摘要

Doping carbon materials with p-block elements such as nitrogen is an effective approach to tune electronic properties of the framework and can endow the host's new characters. To date, highly doped carbons with tunable nitrogen speciation are still less explored due to the grand challenge in fabrication; for example, the typical synthesis based on the pyrolysis of nitrogen-containing precursors shows a trade-off between the total nitrogen content and the carbonization temperature, limiting the value to approximate to 12 wt% at 1073 K. Herein, intensifying ring opening of cross-linked polymers through controlled pre-oxidation followed by conventional pyrolysis is demonstrated as an elegant method to circumvent this challenge. In addition to fine tunability at different nitrogen speciation, this strategy can increase the nitrogen content by two- to threefold (maximum approximate to 22 wt%) and shows general viability in six different N-bearing (co)polymers. The highly doped pyridinic nitrogen-rich carbons show i) a remarkable capacity of 879 mAh g(-1)at 0.1 A g(-1)and excellent cycling performance in lithium ion batteries, and ii) significantly boosted catalytic performance in the selective oxidation of diverse substrates. Therefore, this facile synthetic strategy and the tunability at nitrogen functionalities will greatly broaden the applications of this new class of functional materials.
机译:掺杂碳材料具有诸如氮的P嵌段元件是调整框架电子特性的有效方法,可以赋予主机的新字符。迄今为止,由于制造的大挑战,具有可调谐氮形式的高度掺杂的碳仍然减少;例如,基于含氮前体热解的典型合成显示了总氮含量和碳化温度之间的折衷,限制了1073k的12wt%的值。这里,交叉的强化环开口 - 通过受控预氧化随后进行常规热解的链接聚合物被证明是避免这种攻击的优雅方法。除了在不同氮形状的微调性之外,该策略可以通过两个至三倍(最大近似为22wt%),并在六种不同的N轴承(CO)聚合物中显示一般可活力的氮含量。高掺杂的吡啶氢碳碳碳显示I)在0.1Ag(-1)和锂离子电池中的优异循环性能下具有879mAhg(-1)的显着容量,II)在选择性氧化中显着提高催化性能不同的基材。因此,这种容易合成策略和氮功能的可调性将大大拓宽这类新型功能材料的应用。

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  • 来源
    《Advanced Functional Materials》 |2021年第3期|2006076.1-2006076.10|共10页
  • 作者单位

    Zhejiang Normal Univ Hangzhou Inst Adv Studies Gengwen Rd 1108 Hangzhou 311231 Peoples R China;

    Chinese Acad Sci Dalian Inst Chem Phys State Key Lab Catalysis Zhongshan Rd 457 Dalian 116023 Peoples R China|Univ Chinese Acad Sci Yuquan Rd 19A Beijing 100049 Peoples R China;

    Chinese Acad Sci Dalian Inst Chem Phys State Key Lab Catalysis Zhongshan Rd 457 Dalian 116023 Peoples R China|Chinese Acad Sci Dalian Inst Chem Phys Dalian Natl Lab Clean Energy Zhongshan Rd 457 Dalian 116023 Peoples R China;

    Zhejiang Normal Univ Hangzhou Inst Adv Studies Gengwen Rd 1108 Hangzhou 311231 Peoples R China;

    Swiss Fed Inst Technol Dept Chem & Appl Biosci Inst Chem & Bioengn Vladimir Prelog Weg 1 CH-8093 Zurich Switzerland;

    Empa Swiss Fed Labs Mat Sci & Technol Uberlandstr 129 CH-8600 Dubendorf Switzerland;

    Zhejiang Normal Univ Hangzhou Inst Adv Studies Gengwen Rd 1108 Hangzhou 311231 Peoples R China;

    Chinese Acad Sci Dalian Inst Chem Phys State Key Lab Catalysis Zhongshan Rd 457 Dalian 116023 Peoples R China|Chinese Acad Sci Dalian Inst Chem Phys Dalian Natl Lab Clean Energy Zhongshan Rd 457 Dalian 116023 Peoples R China;

    Zhejiang Normal Univ Hangzhou Inst Adv Studies Gengwen Rd 1108 Hangzhou 311231 Peoples R China|Chinese Acad Sci Dalian Inst Chem Phys State Key Lab Catalysis Zhongshan Rd 457 Dalian 116023 Peoples R China|Chinese Acad Sci Dalian Inst Chem Phys Dalian Natl Lab Clean Energy Zhongshan Rd 457 Dalian 116023 Peoples R China;

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

    catalysis; lithium ion battery; nitrogen-doped carbon; polymers; synthetic strategy;

    机译:催化;锂离子电池;氮掺杂碳;聚合物;合成策略;

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