Tailoring charge dynamics: The multifunctional role of MOFs and their derivatives in next-generation photovoltaics

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The advancement of photovoltaic technologies is constrained by charge-dynamic losses instead of insufficient light absorption. Across perovskite, dye-sensitized, organic, quantum-dot, and emerging hybrid solar cells, the challenge of recombination losses, interfacial trapping, energy-level mismatch, carrier extraction limitation and ionic instability are barriers to achieve their theoretical performance limits. To address this issue, metal-organic frameworks (MOFs) and their derivatives have emerged as viable materials for regulating charge-dynamic processes due to their tunable structural and electronic characteristics. This review presents a comprehensive discussion and focused on how pristine MOFs, conductive frameworks, defect-engineered architectures, and MOF-derived materials influence the photophysical lifecycle of charge carriers including charge generation, exciton dissociation, charge separation, carrier transport, extraction kinetics, and long-term stability in emerging photovoltaic systems. The fundamental principles governing charge dynamics in solar energy conversion were discussed, the quantitative structure-property-transport relationships across 2D MOFs, conductive frameworks, defect-engineered architectures, and MOF-derived materials were established. The roles of MOFs as charge-extraction layers, interfacial passivation agents, energy-level modulators, trap-assisted non-radiative recombination suppression, and (v) ionic transport mitigation were emphasized. The contributions of MOF-derived metal oxides, carbon frameworks, chalcogenides, heteroatom-doped materials, and hierarchical nanostructures are evaluated and their integration into perovskite, dye-sensitized, organic, quantum-dot, silicon-hybrid, tandem, indoor, and flexible photovoltaic systems. This review also covers advances in operando characterization, ultrafast spectroscopy, density functional theory (DFT), machine learning (ML), and multiscale modeling are discussed as essential tools for charge-dynamic mechanisms and materials discovery. The transition from empirical material optimization toward predictive and intelligent charge-dynamic engineering are highlighted. Finally, this review establishes a conceptual framework for the rational design of MOF-assisted photovoltaic systems with improved efficiency and stability.