A dual spin-controlled chiral two-/three-dimensional perovskite artificial leaf for efficient overall photoelectrochemical water splitting

Hyungsoo Lee, Chan Uk Lee, Juwon Yun, Chang-Seop Jeong, Wooyong Jeong, Jaehyun Son, Young Sun Park, Subin Moon, Soobin Lee, Jun Hwan Kim and Jooho Moon ()
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Hyungsoo Lee: Yonsei University
Chan Uk Lee: Yonsei University
Juwon Yun: Yonsei University
Chang-Seop Jeong: Yonsei University
Wooyong Jeong: Yonsei University
Jaehyun Son: Yonsei University
Young Sun Park: Yonsei University
Subin Moon: Yonsei University
Soobin Lee: Yonsei University
Jun Hwan Kim: Yonsei University
Jooho Moon: Yonsei University

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

Abstract: Abstract The oxygen evolution reaction, which involves high overpotential and slow charge-transport kinetics, plays a critical role in determining the efficiency of solar-driven water splitting. The chiral-induced spin selectivity phenomenon has been utilized to reduce by-product production and hinder charge recombination. To fully exploit the spin polarization effect, we herein propose a dual spin-controlled perovskite photoelectrode. The three-dimensional (3D) perovskite serves as a light absorber while the two-dimensional (2D) chiral perovskite functions as a spin polarizer to align the spin states of charge carriers. Compared to other investigated chiral organic cations, R-/S-naphthyl ethylamine enable strong spin-orbital coupling due to strengthened π–π stacking interactions. The resulting naphthyl ethylamine-based chiral 2D/3D perovskite photoelectrodes achieved a high spin polarizability of 75%. Moreover, spin relaxation was prevented by employing a chiral spin-selective L-NiFeOOH catalyst, which enables the secondary spin alignment to promote the generation of triplet oxygen. This dual spin-controlled 2D/3D perovskite photoanode achieves a 13.17% of applied-bias photon-to-current efficiency. Here, after connecting the perovskite photocathode with L-NiFeOOH/S-naphthyl ethylamine 2D/3D photoanode in series, the resulting co-planar water-splitting device exhibited a solar-to-hydrogen efficiency of 12.55%.

Date: 2024
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DOI: 10.1038/s41467-024-49216-x

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