Li Minghui, Sun Yuhan, Tang Yuqiong, Sun Jingya, Xu Zhaoyi, Zheng Shourong
State Key Laboratory of Pollution Control and Resource Reuse, State Experimental Teaching Demonstration Center for Environmental Science and Engineering, School of the Environment, Nanjing University, Nanjing 210023, PR China.
State Key Laboratory of Pollution Control and Resource Reuse, State Experimental Teaching Demonstration Center for Environmental Science and Engineering, School of the Environment, Nanjing University, Nanjing 210023, PR China.
J Hazard Mater. 2020 Apr 15;388:121745. doi: 10.1016/j.jhazmat.2019.121745. Epub 2019 Nov 22.
In this work, we coated carbon nanotubes (CNT) supported Pt catalyst by conductive carbon layers (labelled as Pt/CNT@C) and the catalyst was further functionalized by surface oxidation (denoted as Pt/CNT@Oxi-C). The textural properties of the catalysts were extensively characterized and liquid phase catalytic hydrogenation reduction of Cu was conducted. Results showed that Pt particles of Pt/CNT@C and Pt/CNT@Oxi-C were completely embedded beneath carbon overcoatings. Furthermore, contrary to Pt/CNT no CO chemisorption was observed on both Pt/CNT@C and Pt/CNT@Oxi-C, indicative of the absence of exposed Pt particles in carbon-coated Pt/CNT. Effective Cu reduction and metallic Cu deposition by catalytic hydrogenation were achieved on catalyst surface. Surface oxidation of Pt/CNT@C resulted in increased surface wetting and functionality content, leading to noticeable enhancement in catalytic activity for Cu reduction. Additionally, Cu reduction on Pt/CNT@Oxi-C proceeded through the Langmuir-Hinshelwood model, suggesting that the reduction of Cu adsorbed on catalyst surface was the rate-determining step. Carbonization of overcoatings exhibited a volcano-type relationship between carbonization temperature and catalytic activity of Pt/CNT@C for Cu reduction. As for catalyst reuse, Pt/CNT lost 92 % of initial activity after five consecutive reaction cycles, whereas Pt/CNT@Oxi-C maintained a high catalytic activity without remarkable deactivation.
在本工作中,我们用导电碳层包覆了碳纳米管(CNT)负载的Pt催化剂(标记为Pt/CNT@C),并通过表面氧化对该催化剂进行了进一步功能化(记为Pt/CNT@Oxi-C)。对催化剂的织构性质进行了广泛表征,并进行了Cu的液相催化加氢还原。结果表明,Pt/CNT@C和Pt/CNT@Oxi-C的Pt颗粒完全嵌入碳包覆层之下。此外,与Pt/CNT不同,在Pt/CNT@C和Pt/CNT@Oxi-C上均未观察到CO化学吸附,这表明碳包覆的Pt/CNT中不存在暴露的Pt颗粒。通过催化加氢在催化剂表面实现了有效的Cu还原和金属Cu沉积。Pt/CNT@C的表面氧化导致表面润湿性和官能团含量增加,从而使Cu还原的催化活性显著提高。此外,Pt/CNT@Oxi-C上的Cu还原通过Langmuir-Hinshelwood模型进行,这表明吸附在催化剂表面的Cu的还原是速率决定步骤。包覆层的碳化在碳化温度与Pt/CNT@C对Cu还原的催化活性之间呈现出火山型关系。至于催化剂的重复使用,Pt/CNT在连续五个反应循环后失去了92%的初始活性,而Pt/CNT@Oxi-C保持了高催化活性,没有明显失活。