Cascade Charge-Transport-Chain Engineering in Alloy Nanocluster–Semiconductor Artificial Photosystems

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Chem. Sci., 2026, Accepted ManuscriptDOI: 10.1039/D6SC02262F, Edge Article Open Access &nbsp This article is licensed under a Creative Commons Attribution-NonCommercial 3.0 Unported Licence.Zi-Han Zheng, Qing Chen, Peng Su, Lifeng Cai, Jie Liang, Guangcan Xia…

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Cascade Charge-Transport-Chain Engineering in Alloy Nanocluster–Semiconductor Artificial Photosystems

Abstract

Atomically precise metal nanoclusters (NCs), featuring discrete electronic structure and pronounced quantum confinement effects, are emerging as promising photosensitizers for artificial photosystems; however, their practical implementation remains fundamentally constrained by rapid charge recombination and poorly controlled charge transport. Here, we introduce a conceptual cascade charge-transport-chain engineering strategy that addresses this intrinsic bottleneck by constructing directional and continuous carrier transport pathways across NC-semiconductor interfaces. By integrating alloy NCs photosensitization with atomic Ni doping of TiO2, a robust interfacial electronic coupling is established, enabling directional and accelerated extraction of photogenerated carriers. The resulting BNC/Ni-TiO2 heterostructures exhibit markedly enhanced visible-light-driven hydrogen evolution, accompanied by effective suppression of charge recombination within alloy NCs. Combined experimental and theoretical investigations reveal that the performance enhancement originates from cascade charge-transport-chain engineering rather than simple binary synergy. This work provides a general design principle for constructing tunable charge-transport pathways with alloy NCs, advancing NC-based artificial photosystems toward solar-to-hydrogen energy conversion.