Spin-cross interface-inducing ultra-high catalytic activity in Co(OH)xPy-MXene toward alkali-free liquid hydrogen generation

• Published in: Applied catalysis. B, Environmental Environmental, 2024-10, Vol.354, p.124143, Article 124143
• Main Authors: Liu, Yanyan, Zhang, Huanhuan, Zhou, Jingjing, Guan, Shuyan, Shen, Ruofan, Zhang, Wenbo, Sheng, Xia, Wang, Lixia, Guo, Xianji, Wu, Xianli, Jiang, Jianchun, Liu, Baozhong, Wang, Yongfeng, Li, Baojun
• Format: Article
• Language: English
• Subjects: Bimolecular activation; Cobalt catalysts; MXene; P-inducing; Spin-cross interface
• ISSN: 0926-3373; 1873-3883
• DOI: 10.1016/j.apcatb.2024.124143

Proclaiming the interfacial active sites of non-noble metals on supported catalysts is a paramount topic. Herein, a spin-cross interface (Co(OH)xPy (x/y=3.2)) in the intimate region between Co(OH)2 and CoP is designed by in situ hydroxylation and P-inducing strategy. An ultra-high catalytic hydrogen generation activity with a turnover frequency of 1640 min−1 is achieved for hydrolysis of ammonia borane (NH3BH3). Both experimental observations and computational simulations reveal that the spin-cross interface dramatically reduces the energy barriers for the dissociation of reactant molecules (NH3BH3 and H2O) to expedite the catalytic activity. The coexistence of active interface and MXene create the ensembles of Co atoms coordinated by OH and P. The construction of active sites of Co(OH)xPy simultaneously boosts the adsorption and dissociation of H2O and NH3BH3 molecules. This research provides new paradigm for the rational design of spin-induced catalysts in the future energy system depending on the activation of multi-molecules. [Display omitted] •A spin-cross interface Co(OH)xPy is designed in the intimate region between Co(OH)2 and CoP.•An unprecedented turnover frequency of 1640 min−1 was obtained over the dual-active surfaces for the hydrolysis of NH3BH3.•The spin-cross interface optimizes the adsorption and dissociation of NH3BH3 and H2O.