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

• Published in: Nature communications 2024-06, Vol.15 (1), p.4672-15
• Main Authors: Lee, Hyungsoo, Lee, Chan Uk, Yun, Juwon, Jeong, Chang-Seop, Jeong, Wooyong, Son, Jaehyun, Park, Young Sun, Moon, Subin, Lee, Soobin, Kim, Jun Hwan, Moon, Jooho
• Format: Article
• Language: English
• Subjects: 147/135; 147/3; 639/166/898; 639/301/299/890; 639/4077/4072/4062; 639/638/77/890; Catalysts; Cations; Current carriers; Current efficiency; Efficiency; Humanities and Social Sciences; multidisciplinary; Oxygen evolution reactions; Perovskites; Photoanodes; Photocathodes; Polarizability; Polarization (spin alignment); Science; Science (multidisciplinary); Selectivity; Splitting; Water splitting
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-024-49216-x

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%. Enhancing the efficiency of solar-driven water splitting is challenging but highly interesting. Here the authors report a dual spin-controlled 2D/3D perovskite photoelectrode that achieves 12.55% efficiency by utilizing the chiral-induced spin selectivity phenomenon.