Solar overall water-splitting by a spin-hybrid all-organic semiconductor

Xinyu Lin, Yue Hao, Yanjun Gong, Peng Zhou, Dongge Ma, Zhonghuan Liu, Yuming Sun, Hongyang Sun, Yahui Chen, Shuhan Jia, Wanhe Li, Chengqi Guo, Yiying Zhou, Pengwei Huo, Yan Yan (), Wanhong Ma (), Shouqi Yuan () and Jincai Zhao
Additional contact information
Xinyu Lin: Jiangsu University
Yue Hao: Jiangsu University
Yanjun Gong: Chinese Academy of Sciences
Peng Zhou: University of Michigan
Dongge Ma: College of Chemistry and Materials Engineering, Beijing Technology and Business University
Zhonghuan Liu: Jiangsu University
Yuming Sun: Jiangsu University
Hongyang Sun: Jiangsu University
Yahui Chen: Jiangsu University
Shuhan Jia: Jiangsu University
Wanhe Li: Jiangsu University
Chengqi Guo: Jiangsu University
Yiying Zhou: Jiangsu University
Pengwei Huo: Jiangsu University
Yan Yan: Jiangsu University
Wanhong Ma: Chinese Academy of Sciences
Shouqi Yuan: Jiangsu University
Jincai Zhao: Chinese Academy of Sciences

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Direct solar-to-hydrogen conversion from pure water using all-organic heterogeneous catalysts remains elusive. The challenges are twofold: (i) full-band low-frequent photons in the solar spectrum cannot be harnessed into a unified S1 excited state for water-splitting based on the common Kasha-allowed S0 → S1 excitation; (ii) the H+ → H2 evolution suffers the high overpotential on pristine organic surfaces. Here, we report an organic molecular crystal nanobelt through the self-assembly of spin-one open-shell perylene diimide diradical anions (:PDI2-) and their tautomeric spin-zero closed-shell quinoid isomers (PDI2-). The self-assembled :PDI2-/PDI2- crystal nanobelt alters the spin-dependent excitation evolution, leading to spin-allowed S0S1 → 1(TT) → T1 + T1 singlet fission under visible-light (420 nm~700 nm) and a spin-forbidden S0 → T1 transition under near-infrared (700 nm~1100 nm) within spin-hybrid chromophores. With a triplet-triplet annihilation upconversion, a newly formed S1 excited state on the diradical-quinoid hybrid induces the H+ reduction through a favorable hydrophilic diradical-mediated electron transfer, which enables simultaneous H2 and O2 production from pure water with an average apparent quantum yield over 1.5% under the visible to near-infrared solar spectrum.

Date: 2024
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DOI: 10.1038/s41467-024-49511-7

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