NH3 is a crucial feedstock for fertilizer production and an ideal hydrogen carrier for carbon-free energy storage. Nevertheless, traditional Haber-Bosch process requires harsh conditions and heavy fossil fuels consumption, eventually exacerbating global warming. Australia’s abundant solar and ocean resources, regarded as key low-carbon renewable sources in achieving sustainable development offers a promising opportunity to develop an emission-free technology for green NH3 production, but most novel NH3 technologies are still in the lab stage. Thus, it is essential to design better catalysts to fix nearly unlimited N2 from the atmosphere into value-added NH3 via ambient-condition catalysis and unveil reaction mechanism as well as preactical application. Owing to remarkable physicochemical property, layer-structured material has been considered as a promising candidate recently, especally for their advatages of inhibiting possibility of charge carrier recombination, shortening the migration distances between charge carriers and reaction interface, and richening active sites and low-coordinated surface atoms. Furthermore, most of them are defined as p-block materials, capable of outstanding hydrophobicity and excellent interaction with N2 molecules. It can suppress hydrogen evolution better.
In the thesis, focused on recently reported nitrogen reduction reaction strategies of typical layer structured materials, we start with a brief summary of the structural characteristics, unraveling their structure–performance relationship and related application. Then, my recent nitrogen-fixation research progress from electrocatalysis to piezocatalysis including transition metal aluminum boride, p-metal based metal-organic frameworks, and perovskite materials is presented. Finally, future challenges and directions for the development tendency of layered materials in nitrogen fixation at ambient conditions are outlined.