Remarkably boosting Ru-Ni nanocatalysis via surface/interface regulation for efficient hydrolytic dehydrogenation of ammonia borane
Remarkably boosting Ru-Ni nanocatalysis via surface/interface regulation for efficient hydrolytic dehydrogenation of ammonia borane
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通过表面/界面调节显着促进Ru-Ni纳米催化，实现氨硼烷的高效水解脱氢
DOI：
10.1016/j.fuel.2021.121800
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发表时间：
2022-01
期刊：
影响因子：
7.4
通讯作者：
Fushen Lu
中科院分区：
文献类型：
--
作者：
Zier Jin;Hong Xia;Wenxin Yang;Mingen Liu;Xiaoyu Liu;Jiao Xiang;Abdul Qayum;Liangsheng Hu;Lianfeng Duan;Wenhua Gao;Zhi Liu;Fushen Lu
氨硼烷（NH3BH3，AB）被认为是化学储氢材料中最具吸引力的候选材料之一。开发低成本、高性能的AB制氢催化剂是非常有必要的，但这仍然是一个巨大的挑战。在此，通过一种简单的一步原位共还原策略在（3-氨基丙基）三乙氧基硅烷功能化的还原氧化石墨烯纳米片（APTS-rGO）上制备了Ru-Ni双金属纳米颗粒。新开发的Ru1Ni4/APTS-rGO催化剂具有亲水界面和窄粒径分布，对AB水解产氢具有显着增强的催化活性，提供1559 min−1的超高TOF值。 APTS-rGO 载体可有效减少 Ru-Ni 纳米粒子的聚集，实现超小型 Ru-Ni 纳米粒子 (2.0 nm) 在载体表面的固定。 Ru-Ni协同效应和金属-载体相互作用引起的催化剂表面局部电荷密度的变化提高了Ru1Ni4/APTS-rGO的催化性能。亲水性的含NH2界面保证了催化剂在反应溶液中的高分散性，增加了活性位点与AB分子之间的接触机会。这些因素共同促成了 Ru1Ni4/APTS-rGO 优异的催化性能。该催化体系由于其制备方法简便、亲水性好、催化性能突出等明显优点，在各个催化领域具有潜在的应用前景。
Ammonia borane (NH3BH3, AB) has been considered as one of the most attractive candidates for chemical hydrogen-storage materials. Development of low-cost and high-performance catalysts for hydrogen generation from AB is highly desirable, which is still a huge challenge. Herein, Ru-Ni bimetallic nanoparticles were fabricated on (3-aminopropyl) triethoxysilane-functionalized reduced graphene oxide nanosheet (APTS-rGO) by a facile one-step in situ co-reduction strategy. The newly developed Ru1Ni4/APTS-rGO catalyst with hydrophilic interface and narrow particle size-distribution presented a remarkably enhanced catalytic activity for hydrolytic H2generation from AB, affording an ultra-high TOF value of 1559 min−1. The APTS-rGO support was effective to minimize the aggregation of Ru-Ni nanoparticles, achieving the immobilization of ultrasmall Ru-Ni nanoparticles (2.0 nm) on support surface. The change in local charge density of catalyst surface caused by Ru-Ni synergistic effect and metals-support interaction improved the catalytic performance of Ru1Ni4/APTS-rGO. Hydrophilic NH2-containing interface ensured high dispersibility of catalysts in reaction solution, increasing the contact opportunities between active sites and AB molecules. These factors contributed together to the exceptional catalytic performance of Ru1Ni4/APTS-rGO. This catalytic system has potential applications in various catalytic fields due to its obvious advantages of the facile preparation method, good hydrophilicity, and the outstanding catalytic performance.
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