Chirality‐Induced Spin Selectivity of Photo‐Generated Electrons in Hybrid Organic–Inorganic Perovskites for Photocatalytic Hydrogen Evolution

IF 13 2区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Small Pub Date : 2025-07-07 DOI:10.1002/smll.202503317

Yantao Yang, Jinjie Hao, Yangen Xie, Zhengwei Yang, Yufan Zhang, Ran Duan, Hua Sheng, Baipeng Yin, Chuang Zhang

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引用次数: 0

Abstract

Photocatalytic hydrogen evolution (PHE) is attractive for sustainable energy production, yet its efficiency lags photovoltaic conversion mainly due to the step of H‒H bonding for hydrogen generation on photocatalysts. Herein, the spin‐enhanced PHE using photocatalysts of chiral perovskites (MBPI) are reported, where the spin orientations of photocarriers are aligned antiparallelly for H‒H bonding via the chiral‐induced spin selectivity (CISS) effect. It is observed that the rac‐MBPI shows a 3.5‐fold enhancement in PHE activity compared with R/S‐MBPI under visible light illumination, which is related to the chiral distortions of octahedral units in perovskite structures. Structural distortions lead to the spin polarization of photogenerated carriers in chiral perovskites due to the CISS effect, as revealed by magneto‐photocurrent measurements. Compared with the parallel spins in R/S‐MBPI, the antiparallel spins in rac‐MBPI are more favorable for the coupling of H* radicals, as proven by the electron paramagnetic resonance experiments. The spin‐enhanced mechanism for PHE is universal for reduced dimensional (quasi‐2D) chiral perovskites, and the H2 yield rate is optimized up to 0.61 mmol g−1 h−1 with an excellent stability over 100 hours.

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有机-无机杂化钙钛矿中光生电子的手性诱导自旋选择性光催化析氢

光催化析氢（PHE）在可持续能源生产中具有吸引力，但其效率落后于光伏转换，主要是由于光催化剂上的氢键生成氢的步骤。本文报道了使用手性钙钛矿（MBPI）光催化剂的自旋增强PHE，其中光载流子的自旋取向通过手性诱导的自旋选择性（CISS）效应对H-H键进行反平行排列。结果表明，在可见光照射下，rac - MBPI比R/S - MBPI的PHE活性提高了3.5倍，这与钙钛矿结构中八面体单元的手性畸变有关。磁-光电流测量表明，由于CISS效应，结构畸变导致了手性钙钛矿中光生载流子的自旋极化。电子顺磁共振实验证明，与R/S‐MBPI中的平行自旋相比，rac‐MBPI中的反平行自旋更有利于H*自由基的耦合。对于降维（准2D）手性钙钛矿，PHE的自旋增强机制是通用的，H2产率达到0.61 mmol g−1 h−1，并且在100小时内具有出色的稳定性。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Small 工程技术-材料科学：综合

CiteScore

17.70

自引率

3.80%

发文量

1830

审稿时长

2.1 months

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