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Spinless transition natural orbitals elucidate the origin of spin–orbit coupling andg-tensor anisotropy. 

Abstract Artificial photosynthesis is an emerging technology that achieves renewable fuels, such as hydrogen, from sunlight. Its realization depends on finding highly active and stable catalysts of water splitting and photoactive materials for light absorption. To be scalable, these should contain only abundant elements. Here, for the first time, Fe‐triazolate (Fe(ta)₂) and its metal substituted derivatives (Fe‐Metal(ta)₂) Metal‐organic frameworks (MOFs) are characterized as new dual‐function materials for photo‐absorption and water oxidation catalysis in acidic media. The materials were studied by a range of structural, spectroscopic, and computational density functional theory (DFT) techniques. Fe(ta)₂and Fe‐Mn(ta)₂were found to be highly active and stable in chemical and photochemical water oxidation, and in addition function as photoanodes, with photo‐electrocatalytic currents (∼2.00 x 10⁻³Acm⁻²at + 1.4 V vs. Ag/AgCl) atpH = 1. The possibility of a unique catalytic mechanism where O─O bond formation is possible from the coupling of two adjacent Fe^IV = O fragments was demonstrated by DFT analysis. Thus, Fe‐triazolate MOF has been established as a new, stable, scalable, versatile, and efficient platform for sustainable energy conversion in the realm of artificial photosynthesis.