Publication date: 26th March 2026
By virtue of its high volumetric energy density, well-defined distribution infrastructure and the possibility to obtain COx-free hydrogen (H2) from its decomposition, ammonia (NH3) is considered a key energy carrier in future neutral-carbon energy systems. Unfortunately, the use of this carrier has been limited by the absence of an efficient NH3 decomposition process. Photo-thermal catalysis, a hybrid approach that combines both thermal and non-thermal contributions of light, has showed a great potential to drive chemical reactions using sunlight as unique energy source. Among others, MOF-derived materials have recently appeared as promising candidates for applications in photo-thermal catalysis due to their broad light absorption, effective light-to-heat conversion and well-dispersed metal active sites. Here, we demonstrate the use of MOF-derived photo-thermal catalysts to perform the NH3 decomposition reaction at low temperatures and high conversion rates.
Catalysts were obtained from the controlled pyrolysis under inert atmosphere of different Fe- and Co-based MOF precursors. The photo-thermal NH3 decomposition was performed under continuous flow configuration using a commercial reaction chamber equipped with a quartz window. At high space velocities in the order of 20000 mL g-1 h-1, the catalysts reached a temperature of 250 °C and a 25 % NH3 conversion, which translated into a H2 production rate as high as 326 mmol H2 g-1 h-1. Additional blank experiments under dark conditions displayed negligible NH3 decomposition rates, thus indicating that the synergy between light and heat is crucial to enhance the catalytic activity towards NH3 conversion. In fact, mechanistic experiments including irradiance-dependent catalytic tests and photo-current measurements demonstrated the cooperative effect between thermal and non-thermal effects in the system. DFT calculations also suggested that the combination of high temperatures and photo-generated carriers under illumination prevented the formation of a thermodynamic sink, thus facilitating the reaction rate compared to dark conditions. To the best of our knowledge, this is the first example of the use of MOF-derived catalysts for the efficient photo-thermal NH3 cracking reaction under continuous flow configuration.
The authors gratefully acknowledge the financial support from King Abdullah University of Science and Technology (KAUST) and Trinity College Dublin. Particularly, K.B. and M.G.-M. acknowledge funding from the Provost's PhD Project Awards, generously funded through alumni donations and Trinity's Commercial Revenue Unit, as well as the Science Foundation Ireland (SFI-20/FFP-P/8740). The authors are also grateful to the DJEI/DES/SFI/HEA Irish Centre for High-End Computing (ICHEC) and the Supercomputing Laboratory at King Abdullah University of Science & Technology (KAUST) in Thuwal, Saudi Arabia, for the generous provision of computational resources.
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