孙长航,陈鑫,李鑫,匡波,邓黎丹,马宏卿,任婷艳,姜兴茂.处理方法对多壁碳纳米管结构及负载Ru催化剂氨分解反应活性的影响[J].分子催化编辑部,2019,33(5):453-460
处理方法对多壁碳纳米管结构及负载Ru催化剂氨分解反应活性的影响
Effects of Treatment Methods on Structure of Multi-walled Carbon Nanotubes and Activity of Supported Ru Catalyst for Ammonia Decomposition
投稿时间:2019-08-16  修订日期:2019-09-23
DOI:
中文关键词:  碳纳米管  氨分解  表面化学基团
英文关键词:CNTs  ammonia decomposition  surface functional groups
基金项目:武汉工程大学校长基金(2018114);山东省自然科学基金博士基金(ZR2016EEB33)
作者单位E-mail
孙长航 武汉工程大学 化学与环境工程学院, 湖北 武汉 430205  
陈鑫 武汉工程大学 化学与环境工程学院, 湖北 武汉 430205  
李鑫 武汉工程大学 化学与环境工程学院, 湖北 武汉 430205  
匡波 武汉工程大学 化学与环境工程学院, 湖北 武汉 430205  
邓黎丹 武汉工程大学 化工与制药学院, 湖北 武汉 430205  
马宏卿 临沂大学 资源环境学院, 山东 临沂 27600  
任婷艳 生态环境部华南环境科学研究所, 广东 广州 510655  
姜兴茂 武汉工程大学 化工与制药学院, 湖北 武汉 430205 dan.213@163.com 
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中文摘要:
      分别用H2O2、强碱(NaOH、KOH)和强酸HNO3处理CNTs.以处理后的CNTs为载体、通过浸渍RuCl3水溶液结合高温H2还原制备Ru/CNTs催化剂,并将其应用在氨分解催化反应中.利用XRD、TPR、TPD-MS表征手段研究了Ru在CNTs表面的分散、还原性能及CNTs表面化学基团,探究催化剂结构-性能间构效关系.结果表明,强碱及双氧水处理CNTs,为其表面引入了数量适宜的羧基、酸酐、酚等官能团,而传统硝酸处理则引入了大量的羧基、酸酐、酯、内酯、酚、醌和羰基等官能团,对CNTs本征结构性质影响很大.经强碱及双氧水处理CNTs上负载Ru后所得催化剂的效果明显优于传统硝酸处理CNTs上负载Ru催化剂.我们发展的CNTs的新型处理方法为研制高活性Ru/CNTs催化分解氨催化剂提供了新的思路.
英文摘要:
      H2O2, strong base (NaOH, KOH) and nitric acid HNO3 were respectively used to treat CNTs. With the modified CNTs as the support, Ru/CNTs catalysts were prepared by impregnating the support with the aqueous solution of RuCl3 and reducing by H2 at high temperature, then the prepared catalysts were applied in the decomposition of ammounia. The dispersion and reduction properties of Ru on CNTs, as well as the chemical groups on CNTs surface were studied by XRD, TPR and TPD-MS characterization techniques. The structure-activity relationship between the structure and performance of the catalyst were explored. The results showed that the treatment of CNTs with strong alkali and hydrogen peroxide introduced a suitable number of functional groups such as carboxyl, anhydride and phenol on the surface, while the traditional nitric acid treatment introduced a large number of functional groups such as carboxyl, anhydride, ester, lactone, phenol, quinone and carbonyl, which greatly affected the intrinsic structure and properties of CNTs. The catalytic activities of Ru supported on CNTs treated with strong alkali and hydrogen peroxide are better than that of Ru supported on CNTs treated with nitric acid. This study provides a new idea for the new treatment method of CNTs, the analysis method of surface chemical functional groups on CNTs and the improvement of the catalytic activity of Ru/CNTs for ammonia decomposition.
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