Liu Jiangchuan, Zhang Mengchen, Tang Qinke, Zhao Yingyan, Zhang Jiguang, Zhu Yunfeng, Liu Yana, Hu Xiaohui, Li Liquan
College of Materials Science and Engineering, Jiangsu Collaborative Innovation Centre for Advanced Inorganic Function Composites, Nanjing Tech University, 30 South Puzhu Road, Nanjing, 211816, P. R. China.
Adv Sci (Weinh). 2022 Jul;9(21):e2201428. doi: 10.1002/advs.202201428. Epub 2022 May 6.
Light metal hydrolysis for hydrogen supply is well suited for portable hydrogen fuel cells. The addition of catalysts can substantially aid Mg hydrolysis. However, there is a lack of clear catalytic mechanism to guide the design of efficient catalysts. In this work, the essential role of nanosized catalyst (Ni Fe/rGO) in activating micro-sized Mg with ultra-rapid hydrolysis process is investigated for the first time. Here, an unprecedented content of 0.2 wt% Ni Fe/rGO added Mg can release 812.4 mL g hydrogen in just 60 s at 30 °C. Notably, an impressive performance with a hydrogen yield of 826.4 mL g at 0 °C in only 30 s is achieved by the Mg-2 wt% Ni Fe/rGO, extending the temperature range for practical applications of hydrolysis. Moreover, the four catalysts (Ni Fe/rGO, Ni Fe, Ni/rGO, Fe/rGO) are designed to reveal the influence of composition, particle size, and dispersion on catalytic behavior. Theoretical studies corroborate that the addition of Ni Fe/rGO accelerates the electron transfer and coupling processes and further provides a lower energy barrier diffusion path for hydrogen. Thus, a mechanism concerning the catalyst as migration relay is proposed. This work offers guidelines designing high-performance catalysts especially for activating the hydrolysis of micro-sized light weight metals.
用于供氢的轻金属水解非常适合便携式氢燃料电池。催化剂的添加可以极大地促进镁的水解。然而,缺乏明确的催化机制来指导高效催化剂的设计。在这项工作中,首次研究了纳米催化剂(Ni Fe/rGO)在通过超快速水解过程活化微米级镁中的关键作用。在此,添加0.2 wt% Ni Fe/rGO的镁在30°C下仅60秒就能释放出812.4 mL g的氢气。值得注意的是,Mg-2 wt% Ni Fe/rGO在0°C下仅30秒就能实现令人印象深刻的产氢性能,产氢量为826.4 mL g,扩展了水解实际应用的温度范围。此外,设计了四种催化剂(Ni Fe/rGO、Ni Fe、Ni/rGO、Fe/rGO)以揭示组成、粒径和分散性对催化行为的影响。理论研究证实,Ni Fe/rGO的添加加速了电子转移和耦合过程,并进一步为氢提供了更低能垒的扩散路径。因此,提出了一种将催化剂作为迁移中继的机制。这项工作为设计高性能催化剂提供了指导,特别是用于活化微米级轻质金属的水解。