Individual High-Quality N-Doped Carbon Nanotubes Embedded with Nonprecious Metal Nanoparticles toward Electrochemical Reaction
Individual High-Quality N-Doped Carbon Nanotubes Embedded with Nonprecious Metal Nanoparticles toward Electrochemical Reaction
复制标题
嵌入非贵金属纳米颗粒的单个高质量氮掺杂碳纳米管用于电化学反应
DOI：
10.1021/acsami.8b14536
复制
发表时间：
2018
影响因子：
9.5
通讯作者：
Wang Hua
中科院分区：
文献类型：
--
作者：
Zhang Shengbo;Wu Qilon;Tang Lei;Hu Yuge;Wang Mengyun;Zhao Jiankang;Li Mei;Han Jinyu;Liu Xiao;Wang Hua
开发用于电化学反应的高活性和稳定的非贵金属催化剂是期望的，但仍然是一个巨大的挑战。本文报道了一种新型的金属离子吸附-热解策略，通过可控的咪唑骨架8分子筛合成了高质量的氮掺杂碳纳米管，并在碳纳米管中嵌入了分散性良好的非贵金属纳米颗粒，该纳米颗粒对电化学CO2还原反应、氧气还原反应和析氧反应具有上级电催化活性和稳定性.实验分析和密度泛函理论计算表明，该材料的电催化活性主要归因于金属纳米颗粒与N掺杂碳壳之间的界面效应，以及其大的比表面积、独特的管状结构、合适的掺杂、高石墨化度和坚固的骨架结构.高反应稳定性归因于多壁石墨碳壳有效地防止金属纳米颗粒聚集、腐蚀和氧化。这种新的合成策略为合成N掺杂碳纳米管结构提供了一种简单的通用性，并将为开发低成本，高活性和稳定的电催化材料提供指导，用于可持续的能源转换。
Developing highly active and stable nonprecious metal catalysts for electrochemical reactions is desirable but remains a great challenge. Herein, we report a novel metal-ion adsorption-pyrolysis strategy for the controllable zeolitic imidazolate framework-8 derived synthesis of individual high-quality N-doped carbon nanotubes embedded with well-dispersed nonprecious metal nanoparticles, which exhibit superior electrocatalytic activity and stability for electrochemical CO2reduction reaction, oxygen reduction reaction, and oxygen evolution reaction. Experimental analysis and density functional theory calculations indicate that the remarkable electrocatalytic activities are mainly attributed to the interface effects for the efficient electron transfer from metal nanoparticles to the N-doped carbon shell, as well as the large specific areas, unique tube structures, appropriate doping, high graphitization degree, and robust frameworks. The high reaction stability is attributed to the multiwalled graphitic carbon shells efficiently preventing metal nanoparticles from aggregation, corrosion, and oxidation. This novel synthetic strategy presents a facile universality for synthesizing N-doped carbon nanotube structures and will provide a guideline for developing low-cost, highly active, and stable electrocatalytic materials for sustainable energy conversion.