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首页> 外文期刊>ACS catalysis >N-8(-) Polynitrogen Stabilized on Boron-Doped Graphene as Metal-Free Electrocatalysts for Oxygen Reduction Reaction
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N-8(-) Polynitrogen Stabilized on Boron-Doped Graphene as Metal-Free Electrocatalysts for Oxygen Reduction Reaction

机译：N-8（ - ）多氧化碳稳定在硼掺杂石墨烯上作为无金属电催化剂进行氧还原反应

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摘要

Polynitrogen (PN) chain was predicted theoretically to be stable at ambient pressure by intercalating in multiple graphene layers. In this work, polynitrogen (N-8(-)) deposited on boron-doped graphene (PN-BG) and graphene (PN-G) was synthesized experimentally by a facile cyclic voltammetry (CV) method. It was further used for oxygen reduction reaction (ORR), which showed superior activity via a four-electron pathway mechanism. BG was prepared by a one-pot hydrothermal method. Characterizations over BG substrate, including X-ray photoelectron spectroscopy, Raman specstroscopy, Brunauer-Emmett-Teller, scanning electron microscopy, and transmission electron microscopy, demonstrated that boron atoms were successfully doped into graphene matrix. The formation of polynitrogen (N-8(-)) on BG was confirmed by attenuated total reflection Fourier transform infrared spectroscopy and temperature-programmed desorption. A larger amount of N-8(-) was obtained on boron-doped graphene than that on graphene. Rotating disk electrode measurements indicated that PN-BG showed higher current density than PN-G catalyst because of the larger amount of N-8(-) on BG. Compared to commercial Pt/C catalyst, PN-B1G has much better methanol tolerance. Kinetics study was also carried out to investigate the ORR pathway. Natural bonding orbital analysis confirmed the mechanism. This work provides a facile strategy to modify graphene structure and efficiently stabilize N-8(-) on a graphene-based matrix.
机译：通过在多个石墨烯层中嵌入，从理论上预测多尼（PN）链以在环境压力下稳定。在该作品中，通过裂缝循环伏安法（CV）方法实验合成沉积在掺杂的石墨烯（PN-B）和石墨烯（PN-G）上的聚硝基（N-8（ - ））。它还用于氧还原反应（ORR），其通过四电子通路机构显示出优异的活性。 BG由单罐水热法制备。对BG衬底的特征，包括X射线光电子能谱，拉曼样品镜，Brunauer-Emmett-exers，扫描电子显微镜和透射电子显微镜，证明了硼原子被成功掺杂到石墨烯基质中。通过减弱的总反射傅里叶变换红外光谱和温度编程解吸来确认BG上的聚硝基（N-8（ - 8（））的形成。在掺硼石墨烯上获得大量的N-8（ - ），而不是石墨烯。旋转盘电极测量表明，由于BG上的较大量的N-8（）显示，PN-BG显示比PN-G催化剂更高的电流密度。与商业Pt / C催化剂相比，PN-B1G具有更好的甲醇耐受性。还进行了动力学研究以研究ORR途径。天然键合轨道分析证实了该机制。这项工作提供了一种容易策略来修改石墨烯结构，并有效地稳定基于石墨烯基质的N-8（ - ）。

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