Backbone-ion engineering enables MOF-derived single platinum atomic arrays for high-performance photovoltaic devices

Abstract

Metal–organic frameworks (MOFs) are attractive scaffolds for single-atom systems, yet their conventional synthesis typically offers limited control over atomic dispersion and local coordination environments. Here we introduce a ligand precursor-mediated backbone-ion engineering strategy that enables the synthesis of two-dimensional (2D) MOF-based SACs with atomically dispersed platinum. By pre-complexing Pt with tetracarboxyphenylporphyrin (TCPP) and assembling it with Cu²⁺, Ni²⁺, or Co²⁺ backbone nodes, we achieve high Pt loadings (11–12 wt%) and uniform Pt–Pt distances (1.68 nm), consistent with theoretical predictions. When employed as counter electrodes in dye-sensitized solar cells, the resulting SACs exhibit framework-dependent performance, with Co@Pt-SACs delivering the highest efficiency. This work presents a sustainable and general strategy for designing atomically precise single-atom frameworks, facilitating the rational development of atomically dispersed materials with tailored properties.