Wu Fenglong, Tian Xiao, Song Jin, Zhang Ying, Li Wei
College of Physics and Electronic Information, Inner Mongolia Normal University, Hohhot 010022, China; Department of Chemical and Environmental Engineering, Hetao College, Bayan Nur 015000, China.
College of Physics and Electronic Information, Inner Mongolia Normal University, Hohhot 010022, China; Inner Mongolia Key Laboratory for Physics and Chemistry of Functional Materials, Inner Mongolia Normal University, Hohhot 010022, China; Inner Mongolia Engineering and Research Center for Rare Earth Functional and New Energy Storage Materials, Inner Mongolia Normal University, Hohhot 010022, China.
J Colloid Interface Sci. 2025 Jul 2;700(Pt 1):138322. doi: 10.1016/j.jcis.2025.138322.
The activation of the water molecule (H₂O) serves as the rate-determining step for hydrogen (H) evolution from the photo-assisted hydrolysis of ammonia borane (NH₃BH₃). Therefore, developing a low-cost efficient catalyst that can expedite the cleavage of OH bonds in H₂O is needed for improving hydrogen production efficiency in practical applications. Here, we prepared a supported non-noble metal catalyst (Co/Mo@MoO-200) with a large number of active sites, comprising ultrathin low-crystalline cobalt (Co) nanosheets grown on amorphous molybdenum oxide (MoO)-coated molybdenum (Mo) nanoparticles (Mo@MoO-200), which serves as a high-performance non-noble metal catalyst to accelerate the activation of OH bonds in HO. Notably, visible light irradiation facilitates the formation of ultrathin Co nanosheets by inducing the localized surface plasmon resonance of MoO, as verified by transmission electron microscopy (TEM) images. Moreover, X-ray absorption near-edge structure (XANES) and X-ray photoelectron spectroscopy (XPS) spectra confirm the electron transfer from Co nanosheets to O sites in Mo@MoO-200, establishing robust interfaces. Co/Mo@MoO-200 exhibits high catalytic performance with the turnover frequency (TOF) value of 110.8 min under visible light irradiation, which is greater than that of Co/Mo by 1.21 times and most of the reported Co-based catalysts. DFT calculations reveal that the Mo@MoO-200 support in the catalyst can promote the Co-adsorption of NHBH and HO, while facilitating H desorption. Particularly, the Co/Mo@MoO-200 can significantly decrease the activation energy barrier of the OH bond in HO, compared with pristine Co and Mo@MoO-200. This paper presents a flexible catalyst design strategy for NHBH hydrolysis and other HO-associated catalytic reactions.
水分子（H₂O）的活化是氨硼烷（NH₃BH₃）光辅助水解制氢（H）过程中的速率决定步骤。因此，开发一种能够加速H₂O中OH键断裂的低成本高效催化剂，对于提高实际应用中的制氢效率至关重要。在此，我们制备了一种具有大量活性位点的负载型非贵金属催化剂（Co/Mo@MoO-200），它由生长在非晶态氧化钼（MoO）包覆的钼（Mo）纳米颗粒（Mo@MoO-200）上的超薄低结晶钴（Co）纳米片组成，可作为高性能非贵金属催化剂加速H₂O中OH键的活化。值得注意的是，透射电子显微镜（TEM）图像证实，可见光照射通过诱导MoO的局域表面等离子体共振促进了超薄Co纳米片的形成。此外，X射线吸收近边结构（XANES）和X射线光电子能谱（XPS）光谱证实了电子从Co纳米片转移到Mo@MoO-200中的O位点，形成了稳定的界面。Co/Mo@MoO-200在可见光照射下表现出高催化性能，周转频率（TOF）值为110.8 min⁻¹，比Co/Mo高1.21倍，且高于大多数已报道的钴基催化剂。密度泛函理论（DFT）计算表明，催化剂中的Mo@MoO-200载体可促进NH₃BH₃和H₂O的Co吸附，同时促进H脱附。特别是，与原始Co和Mo@MoO-200相比，Co/Mo@MoO-200可显著降低H₂O中OH键的活化能垒。本文提出了一种用于NH₃BH₃水解及其他与H₂O相关催化反应的灵活催化剂设计策略。
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