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Effects of Support Types and Their Porosity Characteristics on the Catalytic Performance of Ni-Based Catalysts in Nitrobenzene Hydrogenation to Aniline
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2023-08-19 , DOI: 10.1021/acs.iecr.3c01327
Hexin Jiang 1, 2 , Guanming Yuan 1, 2 , Zhengwei Cui 2 , Zhepeng Zhao 2 , Zhijun Dong 2 , Jiang Zhang 2 , Ye Cong 2 , Xuanke Li 2
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2023-08-19 , DOI: 10.1021/acs.iecr.3c01327
Hexin Jiang 1, 2 , Guanming Yuan 1, 2 , Zhengwei Cui 2 , Zhepeng Zhao 2 , Zhijun Dong 2 , Jiang Zhang 2 , Ye Cong 2 , Xuanke Li 2
Affiliation
Ni-based catalysts are increasingly being used in nitrobenzene hydrogenation. How to select suitable catalyst supports is crucial for upgrading the catalytic performance. Herein, three Ni-based catalysts supported on activated carbon fiber (ACF), mesoporous carbon black (CB), and γ-Al2O3 were tested for nitrobenzene hydrogenation. The influence of catalyst supports, their porosity characteristics, and reaction conditions on the catalytic performance was investigated. The results show that 10 wt % Ni/CB catalyst owns an ultrafine active Ni nanoparticles (∼10 nm) with a uniform dispersion and thus exhibits the optimal catalytic activity. The conversion of nitrobenzene and the selectivity to aniline could reach nearly 100% at 120 °C for 1 h. By contrast, it takes 2 h to achieve the same conversion for 10 wt % Ni/ACF at 120 °C, whereas 10 wt % Ni/Al2O3 needs a severe reaction at 150 °C for 2 h. The turnover frequency of 10 wt % Ni/CB approaches 38 h–1, which is higher than those of other catalysts. Nitrobenzene hydrogenation over different catalysts conforms to a first-order reaction, and the apparent activation energy of 10 wt % Ni/CB (42.6 kJ/mol) is significantly lower than that of 10 wt % Ni/Al2O3 (66.0 kJ/mol). Moreover, 10 wt % Ni/CB catalyst exhibits a good recyclability and structural stability owing to the existence of abundant mesopores in CB, in comparison with 10 wt % Ni/ACF and Ni/Al2O3. It is the mesopores rather than the micropores in carbon supports to postpone the deactivation of Ni-based catalysts. This work demonstrates the superiority of porous carbons as catalyst supports over Al2O3 in nitrobenzene hydrogenation.
中文翻译:
载体类型及其孔隙率特征对镍基催化剂硝基苯加氢制苯胺催化性能的影响
镍基催化剂越来越多地用于硝基苯加氢。如何选择合适的催化剂载体对于提高催化性能至关重要。本文中,三种镍基催化剂负载在活性碳纤维(ACF)、介孔炭黑(CB)和γ-Al 2 O 3上进行了硝基苯加氢试验。研究了催化剂载体、其孔隙率特征和反应条件对催化性能的影响。结果表明,10 wt% Ni/CB 催化剂具有分散均匀的超细活性 Ni 纳米粒子(~10 nm),因此表现出最佳的催化活性。在120℃、1h下硝基苯的转化率和对苯胺的选择性可达到近100%。相比之下,10 wt% Ni/ACF 在 120 °C 下需要 2 h 才能达到相同的转化率,而 10 wt% Ni/Al 2 O 3需要在 150 °C 下剧烈反应 2 h。10 wt% Ni/CB 的周转频率接近 38 h –1,高于其他催化剂。不同催化剂上硝基苯加氢均符合一级反应,10 wt% Ni/CB (42.6 kJ/mol) 的表观活化能显着低于 10 wt% Ni/Al 2 O 3 (66.0 kJ / mol )。摩尔)。此外,与10wt%Ni/ACF和Ni/Al 2 O 3相比,由于CB中存在丰富的介孔,10wt%Ni/CB催化剂表现出良好的可回收性和结构稳定性。正是碳载体中的介孔而不是微孔延缓了镍基催化剂的失活。这项工作证明了多孔碳作为催化剂载体相对于 Al 2 O 3的优越性硝基苯加氢。
更新日期:2023-08-19
中文翻译:
载体类型及其孔隙率特征对镍基催化剂硝基苯加氢制苯胺催化性能的影响
镍基催化剂越来越多地用于硝基苯加氢。如何选择合适的催化剂载体对于提高催化性能至关重要。本文中,三种镍基催化剂负载在活性碳纤维(ACF)、介孔炭黑(CB)和γ-Al 2 O 3上进行了硝基苯加氢试验。研究了催化剂载体、其孔隙率特征和反应条件对催化性能的影响。结果表明,10 wt% Ni/CB 催化剂具有分散均匀的超细活性 Ni 纳米粒子(~10 nm),因此表现出最佳的催化活性。在120℃、1h下硝基苯的转化率和对苯胺的选择性可达到近100%。相比之下,10 wt% Ni/ACF 在 120 °C 下需要 2 h 才能达到相同的转化率,而 10 wt% Ni/Al 2 O 3需要在 150 °C 下剧烈反应 2 h。10 wt% Ni/CB 的周转频率接近 38 h –1,高于其他催化剂。不同催化剂上硝基苯加氢均符合一级反应,10 wt% Ni/CB (42.6 kJ/mol) 的表观活化能显着低于 10 wt% Ni/Al 2 O 3 (66.0 kJ / mol )。摩尔)。此外,与10wt%Ni/ACF和Ni/Al 2 O 3相比,由于CB中存在丰富的介孔,10wt%Ni/CB催化剂表现出良好的可回收性和结构稳定性。正是碳载体中的介孔而不是微孔延缓了镍基催化剂的失活。这项工作证明了多孔碳作为催化剂载体相对于 Al 2 O 3的优越性硝基苯加氢。