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Strategic metal substitution for enhanced visible-light-driven oxygen evolution in heterometallic MOFs
Cui Luo, Peng-Hui Li, Wei-Ming Liao*, Qia-Chun Lin, Xiao-Xiang Zhou, Jun He*
https://doi.org/10.1016/j.cjsc.2025.100621
ABSTRACT
Oxygen evolution reaction (OER), a critical half-reaction in photocatalytic overall water splitting for producing hydrogen, is a key step toward sustainable energy conversion. Conventional photocatalysts often suffer from limited light absorption and rapid charge recombination, hindering their further applications. To address these challenges, we have designed and synthesized a novel series of self-sensitized metal–organic frameworks (MOFs), Fe2MCDDB (M = Ni, Mn, or Co). By incorporating photosensitive ligands, we have achieved efficient charge separation and promoted the transfer of photogenerated electrons to the active metal sites for water oxidation. Among the series, Fe2NiCDDB exhibits exceptional OER activity, achieving an oxygen evolution rate of 125.3 μmol·g−1·h−1 under visible light irradiation. Experimental and theoretical results reveal that the optimized electronic structure and prolonged excited-state lifetime of Fe2NiCDDB contribute to its enhanced catalytic performance. This work provides a promising strategy for designing two-in-one MOF photocatalysts for water oxidation.
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