Abstract
Achieving sustainable ammonia synthesis strategies to replace traditional Haber-Bosch process remains a significant challenge; however, photo-driven catalysis system based on natural nano-minerals promises a great potential to meet the challenge. In our work, an acid-treated natural one-dimensional clay palygorskite (Pal) is substituted with iron ion to realize lattice reconstruction via a microwave-hydrothermal process. The modified Pal with Fe substitution (Fe-Pal) has the original crystal structure with a narrowed band gap. As the mass ratio of Fe is beyond 30 wt%, extra Fe2O3 precipitates on the Pal surface and the nanocomposite resembles a dendritic heterostructure, which effectively enhances visible light absorption and exposes abundant active sites for synergistic adsorption and photo-activation of nitrogen. The 60 wt% Fe-Pal nanocomposite exhibits a remarkable photocatalytic fixation capability for nitrogen under the visible light. Density function theory calculation is employed to help elucidate the photocatalytic mechanism. Our findings potentially provide a green and cost-effective way to synthase nitrogen.
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