Highly efficient hydrogen evolution from the hydrolysis of ammonia borane solution with the Co–Mo–B/NF nanocatalyst
Highly efficient hydrogen evolution from the hydrolysis of ammonia borane solution with the Co–Mo–B/NF nanocatalyst
复制标题
DOI：
10.1016/j.renene.2020.03.032
复制
发表时间：
2020-07
期刊：
影响因子：
8.7
通讯作者：
Yan Wang;Kailun Zou;Dan Wang;Wei Meng;Nanchang Qi;Z. Cao;Kecheng Zhang;Hong-Hua Chen;Guode Li
中科院分区：
文献类型：
--
作者：
Yan Wang;Kailun Zou;Dan Wang;Wei Meng;Nanchang Qi;Z. Cao;Kecheng Zhang;Hong-Hua Chen;Guode Li
氨硼烷（NH_3BH_3）催化水解被认为是质子交换膜燃料电池氢源的一种安全、有效的方法。因此，需要开发廉价且高活性的催化剂。本工作通过调节沉积pH值，采用化学镀法在泡沫镍（NF）表面成功负载了一系列钴钼硼（Co-Mo-B）复合材料。采用电感耦合等离子体质谱、扫描电子显微镜、X射线衍射、透射电子显微镜和X射线光电子能谱等技术对催化剂进行了表征，并将其标记为Co-Mo-B/NF。结果表明，该催化剂对NH3 BH 3水溶液的水解具有高效的催化性能，其中在pH = 11.5条件下制备的Co-Mo-B/NF纳米催化剂在室温下的析氢速率高达6027.1 mL. min-1. g-1.动力学测试表明，Co-Mo-B/NF催化水解反应对NH3 BH 3浓度为零级反应，对催化剂浓度为一级反应。此外，计算得到Co-Mo-B/NF纳米催化剂（pH = 11.5）水解NH3 BH 3的活化能为43.6 kJ·mol− 1，低于以往大多数贵金属和非贵金属催化剂的活化能.相应的吉布斯活化自由能为43.1 kJ·mol−1，表明NH3 BH 3水解反应是非自发的。
Catalytic hydrolysis of ammonia borane (NH3BH3) is considered as a secure and effective way to supply hydrogen (H2) source for the proton exchange membrane fuel cell. Hence, cheap and high activity catalysts need to be exploited. In this work, a series of cobalt–molybdenum–boron (Co–Mo–B) composites were successfully supported on the surface of Ni foam (NF in short) via electroless plating method by tuning the depositional pH values. The as-prepared nanocatalysts were marked as Co–Mo–B/NF and characterized using the inductively coupled plasma-mass spectroscopy, scanning electron microscopy, X–ray diffraction, transmission electron microscopy and X-ray photoelectron spectroscopy technology. These catalysts showed highly efficient catalytic performance for H2evolution toward the hydrolysis of NH3BH3solution, and the optimized Co–Mo–B/NF nanocatalyst deposited at pH = 11.5 achieved a higher H2evolution rate of 6027.1 mL·min−1·g−1under ambient temperature. The kinetics tests displayed that hydrolysis reaction catalyzed by Co–Mo–B/NF was zero-order in terms of the NH3BH3concentration, while it was first-order in view of the catalyst concentration. In addition, the activation energy of NH3BH3hydrolysis was calculated to be 43.6 kJ·mol−1with the Co–Mo–B/NF nanocatalyst (pH = 11.5), which was lower than that of most of the previous precious metal and non-precious metal catalysts. The corresponding Gibbs free energy of activation was 43.1 kJ·mol−1, meaning that NH3BH3hydrolysis reaction was non-spontaneous.