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化学气相沉积生长的镍封装氮掺杂碳纳米管作为一种无直接金属-氮配位的高活性氧还原反应催化剂。

Chemical Vapor Deposition-Grown Nickel-Encapsulated N-Doped Carbon Nanotubes as a Highly Active Oxygen Reduction Reaction Catalyst without Direct Metal-Nitrogen Coordination.

作者信息

Ganguly Dipsikha, Sundara Ramaprabhu, Ramanujam Kothandaraman

机构信息

Alternative Energy Nanotechnology Laboratory, Nano Functional Materials Technology Centre (NFMTC), Department of Physics, and Clean Energy Laboratory, Department of Chemistry, Indian Institute of Technology Madras, Chennai 600036, India.

出版信息

ACS Omega. 2018 Oct 19;3(10):13609-13620. doi: 10.1021/acsomega.8b01565. eCollection 2018 Oct 31.

DOI:10.1021/acsomega.8b01565
PMID:31458066
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC6644947/
Abstract

Nickel-encapsulated nitrogen-doped carbon nanotubes (Ni-TiO-NCNTs) are synthesized via chemical vapor deposition by thermal decomposition of acetylene with acetonitrile vapor at 700 °C on the Ni-TiO matrix. TiO is used as a dispersant medium for Ni nanoparticles, which assists in higher CNT growth at high temperatures. A reference catalyst is made by following the similar procedure without acetonitrile vapor, which is called a Ni-TiO-CNT. Acid treatment of these two catalysts dissolved Ni on the surface of CNTs-NCNTs, producing catalysts with enhanced surface area and defects. The transmission electron microscopy-energy-dispersive X-ray spectra analysis of acid-treated version of the catalysts confirmed the presence of encapsulated Ni. Oxygen reduction reaction (ORR) activity of these catalysts was analyzed in 0.1 N KOH solution. Among these, the acid-treated Ni-TiO-NCNT exhibited highest ORR onset potential of 0.88 V versus reversible hydrogen electrode and a current density of 3.7 mA cm at 170 μg cm of catalyst loading. The stability of the acid-treated Ni-TiO-NCNT is proved by cyclic voltammetry and chronoamperometry measurements which are done for 800 cycles and 100 h, respectively. Primarily N doping of CNTs is the reason behind the improved ORR activity.

摘要

通过化学气相沉积法,在700℃下于镍-二氧化钛基体上使乙炔与乙腈蒸汽热分解,合成了镍封装的氮掺杂碳纳米管(Ni-TiO-NCNTs)。二氧化钛用作镍纳米颗粒的分散介质,有助于在高温下实现更高的碳纳米管生长。通过遵循类似的程序但不使用乙腈蒸汽制备了一种参考催化剂,称为Ni-TiO-CNT。对这两种催化剂进行酸处理,溶解了碳纳米管-NCNTs表面的镍,从而制备出具有更大表面积和缺陷的催化剂。对催化剂的酸处理版本进行的透射电子显微镜-能量色散X射线光谱分析证实了存在封装的镍。在0.1N氢氧化钾溶液中分析了这些催化剂的氧还原反应(ORR)活性。其中,酸处理后的Ni-TiO-NCNT相对于可逆氢电极表现出最高的ORR起始电位为0.88V,在催化剂负载量为170μg/cm²时电流密度为3.7mA/cm²。通过分别进行800次循环和100小时的循环伏安法和计时电流法测量,证明了酸处理后的Ni-TiO-NCNT的稳定性。碳纳米管的主要氮掺杂是ORR活性提高的原因。

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本文引用的文献

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氮掺杂石墨烯量子点修饰的三维 MoS-石墨烯纳米杂化物对氧还原反应的协同增强电催化性能
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