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Hierarchical Porous g-C3N4 Coupled Ultrafine RuNi Alloys as Extremely Active Catalysts for the Hydrolytic Dehydrogenation of Ammonia Borane
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2020-05-15 , DOI: 10.1021/acssuschemeng.0c03009 Yong-Ting Li 1 , Xiao-Li Zhang 1 , Zhi-Kun Peng 2 , Pu Liu 1 , Xiu-Cheng Zheng 1, 3
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2020-05-15 , DOI: 10.1021/acssuschemeng.0c03009 Yong-Ting Li 1 , Xiao-Li Zhang 1 , Zhi-Kun Peng 2 , Pu Liu 1 , Xiu-Cheng Zheng 1, 3
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It is a crucial and urgent task to develop high performance catalysts for the hydrolysis of ammonia borane (NH3BH3, AB), which is presently thought to be an effective strategy for hydrogen generation. In this work, we immobilize the ultrafine RuNi alloy nanoparticles in the network of hierarchical porous g-C3N4 thin sheets with a facile adsorption–in situ reduction method. The structural and physicochemical properties of the as-prepared catalysts are studied using various techniques. The influence of different molar ratios of Ru to Ni in the catalysts on the hydrolytic dehydrogenation rate of AB is investigated to optimize the best one. The detailed reaction kinetics and the enhancing effect of NaOH with different dosages on the hydrolysis rate are studied through a series of experiments. Catalyzed by the optimal catalysts (denoted as Ru0.5Ni0.5/p-g-C3N4), the hydrolysis reaction is first-order and near zero-order relative to the Ru and AB concentrations, respectively. The corresponding turnover frequency reaches 840.3 min–1, and the apparent activation energy is as low as 14.1 kJ mol–1, which are greatly superior to many similar or counterpart catalysts previously reported. The results indicate the potential of the bimetallic alloy catalysts for the hydrolytic dehydrogenation of hydrogen storage materials.
中文翻译：
分层多孔gC 3 N 4偶联超细RuNi合金作为氨硼烷水解脱氢的极活泼催化剂
开发用于氨硼烷（NH 3 BH 3，AB）水解的高性能催化剂是一项紧迫而紧迫的任务，目前认为这是一种有效的制氢策略。在这项工作中，我们将超细RuNi合金纳米颗粒固定在分层多孔gC 3 N 4薄板网络中，并易于吸附–原位还原法。使用各种技术研究了所制备催化剂的结构和物理化学性质。研究了催化剂中Ru与Ni的摩尔比不同对AB水解脱氢速率的影响，以求得最佳的脱氢速率。通过一系列实验研究了不同剂量NaOH的详细反应动力学和增强作用。由最佳催化剂催化（表示为钌0.5镍0.5 /对-克-C 3 Ñ 4），水解反应是分别在第一阶和相对零级靠近Ru和AB的浓度。相应的周转频率达到840.3 min –1，表观活化能低至14.1 kJ mol –1，大大优于以前报道的许多相似或对应的催化剂。结果表明双金属合金催化剂在储氢材料的水解脱氢方面的潜力。
更新日期：2020-05-15
中文翻译：
分层多孔gC 3 N 4偶联超细RuNi合金作为氨硼烷水解脱氢的极活泼催化剂
开发用于氨硼烷（NH 3 BH 3，AB）水解的高性能催化剂是一项紧迫而紧迫的任务，目前认为这是一种有效的制氢策略。在这项工作中，我们将超细RuNi合金纳米颗粒固定在分层多孔gC 3 N 4薄板网络中，并易于吸附–原位还原法。使用各种技术研究了所制备催化剂的结构和物理化学性质。研究了催化剂中Ru与Ni的摩尔比不同对AB水解脱氢速率的影响，以求得最佳的脱氢速率。通过一系列实验研究了不同剂量NaOH的详细反应动力学和增强作用。由最佳催化剂催化（表示为钌0.5镍0.5 /对-克-C 3 Ñ 4），水解反应是分别在第一阶和相对零级靠近Ru和AB的浓度。相应的周转频率达到840.3 min –1，表观活化能低至14.1 kJ mol –1，大大优于以前报道的许多相似或对应的催化剂。结果表明双金属合金催化剂在储氢材料的水解脱氢方面的潜力。
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