Improved Oxygen Reduction Reaction Performance of Co Confined in Ordered N-Doped Porous Carbon Derived from ZIF-67@PILs

Improved Oxygen Reduction Reaction Performance of Co Confined in Ordered N-Doped Porous Carbon Derived from ZIF-67@PILs
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ZIF-67@PILs 衍生的有序 N 掺杂多孔碳中限制 Co 的氧还原反应性能得到改善

DOI:
10.1021/acs.iecr.7b03417
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发表时间:
2017-09
影响因子:
4.2
通讯作者:
Wang Jian-guo
Wang Jian-guo
中科院分区:
工程技术3区
文献类型:
--
作者:
Zhou Xiang;Gao Yi-jing;Deng Sheng-wei;Cheng Shan;Zhang Shao-hua;Hu Hui;Zhuang Gui-lin;Zhong Xing;Wang Jian-guo

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反应物种的扩散和活化是氧还原反应(ORR)的两个关键因素。扩散特性本质上是由反应物质在催化剂通道中的传输决定的。在此,我们报告了一种制备有序碳涂层钴纳米颗粒(Co@O-NPC)的简便方法。具体来说,我们将 ZIF-67 MOF 微晶混合到离子液体单体中,形成 ZIF-67@PILs 复合材料。随后,通过ZIF-67@PILs的高温热解得到Co@O-NPC。电化学测量表明,与商业 Pt/C 相比,它具有优异的 ORR 性能。分子动力学(MD)计算和对比实验结果相结合表明,有序多孔碳结构比无序碳更有效地提高反应物种的扩散性,从而增强ORR性能。此外,DFT计算结果表明催化活性位点位于Co@O-NPC的空腔底部,揭示了系统...
Diffusion and activation of reaction species are two critical factors of oxygen reduction reaction (ORR). Diffusion property is essentially dominated by transmission of reaction species in the channel of catalysts. Herein, we report a facile method to prepare ordered-carbon coated Co nanoparticle (Co@O-NPC). Specifically, we mixed ZIF-67 MOF microcrystal into an ionic liquid monomer which resulted in ZIF-67@PILs composites. Subsequently, Co@O-NPC was obtained by the high-temperature pyrolysis of ZIF-67@PILs. Electrochemical measurements show that it possesses superior ORR property compared to commercial Pt/C. A combination of molecular dynamics (MD) calculations and contrast experimental results reveals that the ordered porous carbon structure can improve the diffusivity of reaction species more effectively than disordered carbon, thereby enhancing ORR property. Moreover, DFT calculation results demonstrate that the catalytically active sites are located on the cavity bottom of Co@O-NPC and uncover the sy...
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