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Open Access Research Article Issue
Room temperature aqueous-phase hydrogenation coupling with green hydrogen: Sustainable technologies innovating by efficient Co-CoOx@NC catalyst derived from N-induced interfacial electron rearrangement
Nano Research 2025, 18(2): 94907118
Published: 11 January 2025
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Utilization and storage are the two main themes of green hydrogen. In hydrogen-involved system, development of highly active catalysts to achieve catalytic hydrogenation under mild conditions is a prerequisite for coupling with green hydrogen, so that green hydrogen with low outlet pressure can be directly used as a hydrogen source. To achieve this aim, we developed a high active Co-CoOx@NC catalyst with metal/metal oxide induced by N-doping. The work function and Bader charge calculations reveal that N-doping can induce interfacial electrons rearrangement to form Co-CoOx interface on the surface of Co nanoparticles (NPs). The interface is the dual active sites, where Co plays a role in H2 dissociation and CoOx can enhance the adsorption and activation of aldehyde compounds. Different from traditional dissimilar metal/oxide interface, the Co-CoOx interface can effectively shorten hydrogen spillover distance and energy barrier, and thus exhibits high catalytic performance in hydrogenation of a variety of bio-derived aldehydes under aqueous-phase and mild reaction conditions that can couple with green hydrogen.

Research Article Issue
Synergistic catalysis of cluster and atomic copper induced by copper-silica interface in transfer-hydrogenation
Nano Research 2021, 14(12): 4601-4609
Published: 09 March 2021
Abstract PDF (12 MB) Collect
Downloads:39

To data, using strong metal-support interaction (SMSI) effect to improve the catalytic performance of metal catalysts is an important strategy for heterogeneous catalysis, and this effect is basically achieved by using reducible metal oxides. However, the formation of SMSI between metal and inert-support has been so little coverage and remains challenge. In this work, the SMSI effect can be effectively extended to the inert support-metal catalysis system to fabricate a Cu0/Cu-doped SiO2 catalyst with high dispersion and loading (38.5 wt.%) through the interfacial effect of inert silica. In the catalyst, subnanometric composite of Cu cluster and atomic copper (in the configuration of Cu–O–Si) can be consciously formed on the silica interface, and verified by extended X-ray absorption fine structure (EXAFS), in situ X-ray photoelectron spectroscopy (XPS), and high-angle annular dark field-scanning transmission electron microscopy (HAADF-STEM) characterization. The promoting activity in transfer-hydrogenation by the SMSI effect of Cu-silica interface and the synergistic active roles of cluster and atomic Cu have also been revealed from surface interface structure, catalytic activity, and density functional theory (DFT) theoretical calculation at an atomic level. The subnanometric composite of cluster and atomic copper species can be derived from a facile synthesis strategy of metal-inert support SMSI effect and the realistic active site of Cu-based catalyst can also been identified accurately, thus it will help to expand the application of subnanometric materials in industrial catalysis.

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