DOI: 10.1021/acsaem.6c02227 ISSN: 2574-0962

Leveraging Chirality-Induced Spin Selectivity to Enhance the Production of Reactive Oxygen Species

Fan He, Tytan Le Nguyen, James R. Wilkes, Jier Huang, Xingxing Wang, Chuanxiao Xiao, Yong Yan, Jing Gu

Abstract

Chirality-induced spin selectivity (CISS) enables spin-selective electron transport without ferromagnetic materials and external magnetic fields. While previous studies have demonstrated CISS-induced modulation of O2 and H2O2 formation during water oxidation, its influence on the one-electron pathway leading to •OH formation remains unexplored. Here, chiral-molecule-modified BiVO4 photoelectrodes were employed to investigate spin-dependent •OH generation during water oxidation. Quantitative fluorescence measurements reveal a 3.5–4.6-fold enhancement in •OH production on interfaces relative to racemic controls, accompanied by suppressed H2O2 formation and enhanced photoelectrochemical performance. Transient absorption spectroscopy confirms the CISS effect, which has been shown to involve a metastable, long-lived charge-trapped state at a semiconductor/chiral molecule interface. The pronounced increase in •OH generation demonstrates that spin polarization can influence not only final reaction products but also transient reactive intermediates. This insight expands the scope of CISS-enabled catalysis and highlights the potential of chiral interfacial engineering to enhance charge-transfer efficiency and photocatalytic performance.