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钼促进对以二氧化碳为碳源合成高质量碳纳米管的镍基催化剂的影响。

Impacts of Mo Promotion on Nickel-Based Catalysts for the Synthesis of High Quality Carbon Nanotubes Using CO₂ as the Carbon Source.

作者信息

Li Shiyan, Sun Shuxiong, Chu Wei, Li Jing, Wang Jiajie, Hu Jiaquan, Jiang Chengfa

机构信息

School of Chemical Engineering, Sichuan University, Chengdu 610065, Sichuan, China.

出版信息

J Nanosci Nanotechnol. 2020 Feb 1;20(2):1109-1117. doi: 10.1166/jnn.2020.16966.

Abstract

In recent years, the primary greenhouse gas (carbon dioxide) has caused a series of severe issues, such as global warming, climate change, etc. Therefore, CCU, CCS and CCUS technologies have been employed to reduce CO₂ emissions. Through our developed "chemical vapor deposition integrated process (CVD-IP)" using carbon dioxide as the carbon source, CO₂ could be catalytically activated and converted to high-value carbon nanotubes. In this work, methane and carbon dioxide has been applied to synthesize CNTs respectively to compare the difference between conventional CH4 CVD and CO₂ CVD-IP technology using Ni-Mo bimetallic catalysts. In the conventional CH4 CVD technology, the carbon productivity and the thermal stability of CNTs could be improved by changing the Mo content of the catalyst, the better catalytic performance 4% Mo catalyst is selected as model catalyst to apply to CO₂ CVD-IP technology. Moreover, when the weak oxidant CO₂ is the only carbon source in the CVD-IP technology, the carbon yield is 22% and the carbon productivity is 1.98 g/gcat. TG curves and Raman spectroscopy display that the CNTs with better thermal stability and higher degree of graphitization are achieved. TEM confirms that the fewer wall numbers and defects of CNTs are obtained. These characterizations suggest that the high quality CNTs could be achieved by CO₂ CVD-IP technology.

摘要

近年来,主要温室气体(二氧化碳)引发了一系列严重问题,如全球变暖、气候变化等。因此,已采用碳捕集、碳封存及碳捕集利用与封存技术来减少二氧化碳排放。通过我们开发的以二氧化碳为碳源的“化学气相沉积集成工艺(CVD - IP)”,二氧化碳能够被催化活化并转化为高价值的碳纳米管。在这项工作中,分别应用甲烷和二氧化碳来合成碳纳米管,以比较使用镍 - 钼双金属催化剂的传统甲烷化学气相沉积与二氧化碳化学气相沉积集成工艺之间的差异。在传统甲烷化学气相沉积技术中,通过改变催化剂的钼含量可以提高碳纳米管的碳生产率和热稳定性,选择催化性能较好的4%钼催化剂作为模型催化剂应用于二氧化碳化学气相沉积集成工艺。此外,当在化学气相沉积集成工艺中弱氧化剂二氧化碳作为唯一碳源时,碳产率为22%,碳生产率为1.98克/克催化剂。热重曲线和拉曼光谱表明获得了热稳定性更好、石墨化程度更高的碳纳米管。透射电子显微镜证实获得的碳纳米管管壁数量更少且缺陷更少。这些表征表明通过二氧化碳化学气相沉积集成工艺可以获得高质量的碳纳米管。

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