College of Chemistry and Materials Science, Sichuan Normal University, Chengdu 610068, China.
College of Chemistry and Materials Science, Sichuan Normal University, Chengdu 610068, China.
J Colloid Interface Sci. 2022 Apr 15;612:57-65. doi: 10.1016/j.jcis.2021.12.127. Epub 2021 Dec 22.
Developing efficient catalytic systems to boost hydrogen evolution from hydrolytic dehydrogenation of ammonia borane (AB) is of broad interest but remains a formidable challenge since the widespread usages of hydrogen have been considered as sustainable solutions to ensure future energy security. Herein, we developed an alkaline ultrasonic irradiation-mediated catalytic system with O/N-rich porous carbon supported Ru nanoclusters (NCs) (Ru/ONPC) to considerably boost the catalytic activity for hydrogen production from the hydrolytic dehydrogenation of AB. The uniformly distributed sub-2.0 nm Ru NCs on the ONPC were demonstrated to be efficient catalysts to boost hydrogen generation from the hydrolytic dehydrogenation of AB with the synergistic effect between ultrasonic irradiation and alkaline additive without any additional heating. An ultrahigh turnover frequency (TOF) of 4004 min was achieved in the developed catalytic system, which was significantly higher than that of ultrasound-mediated AB hydrolysis without alkali (TOF: 485 min) and alkaline AB hydrolysis (TOF: 1747 min) without ultrasound mixing. The alkaline ultrasonic irradiation was beneficial for the cleavage of the OH bonds in the attacked HO molecules catalyzed by the Ru/ONPC and thus considerably boost the catalytic hydrogen generation from AB. This study provides a tractable and ecofriendly pathway to promote the activity toward AB hydrolysis to release hydrogen.
开发高效的催化体系以促进氨硼烷(AB)水解脱氢析氢反应是一项具有广泛意义的挑战,因为人们普遍认为氢气的广泛应用是确保未来能源安全的可持续解决方案。在此,我们开发了一种碱性超声辐射介导的催化体系,其中负载 Ru 纳米团簇(NCs)的富 O/N 多孔碳(Ru/ONPC)可显著提高 AB 水解脱氢析氢反应的催化活性。ONPC 上分布均匀的亚 2.0nm Ru NCs 被证明是高效的催化剂,可在超声辐射和碱性添加剂的协同作用下促进 AB 水解制氢,而无需额外加热。在开发的催化体系中,实现了超高的周转频率(TOF)为 4004min,明显高于没有碱的超声介导 AB 水解(TOF:485min)和没有超声混合的碱性 AB 水解(TOF:1747min)。碱性超声辐射有利于 Ru/ONPC 催化的被攻击 HO 分子中 OH 键的断裂,从而显著提高了 AB 催化制氢的活性。本研究为促进 AB 水解释放氢气的活性提供了一种可行且环保的途径。