Chirality-Induced Selective Electrosynthesis Hydrogen Peroxide and Tandem Green Chemical Synthesis.

Authors

Boying Zhang, Haochuan Li, Ruijuan Zhang, Taoyang Wang, Ranye Shi, Haining Liu, Shanlin Qiao

Published in

Angewandte Chemie (International ed. in English). Pages e7494092. Aug 12, 2026. Epub Aug 12, 2026.

Abstract

Two-electron oxygen reduction reaction (2e^--ORR) toward hydrogen peroxide (H₂O₂) suffers from sluggish O─O preservation and spin-forbidden triplet O₂-to-singlet H₂O₂ transition. Herein, we resolve this pivotal challenge by leveraging the chirality-induced spin selectivity (CISS) effect in inherently chiral Salen covalent organic frameworks (C-Salen-COFs-Zn) as 2e^--ORR electrocatalysts. The CISS effect imparts uniform surface electron spin polarization to the C-Salen-COFs-Zn, whereby triplet O₂ bearing two parallel-spin electrons readily accepts opposite-spin electrons, alleviating the spin-forbidden transition to promote the generation of H₂O₂. The C-Salen-COF-Zn exhibits exceptional spin selectivity with CISS-induced spin polarization efficiency exceeding 90%, delivering superior electrocatalytic performance to its achiral counterpart. C-Salen-COF-Zn achieves 87.0% H₂O₂ selectivity, 297.7 mmol g^-1 h^-1 production rates at 0.2 V versus RHE, and Faradaic efficiencies up to 93.7% at 0.6 V versus RHE in H-type cell. Flow-cell system achieves 1169.7 and 1207.6 mmol g^-1 h^-1 H₂O₂ yield for C-Salen-COF-Zn. Comprehensive mechanistic studies reveal that C-Salen-COF-Zn preferentially adopts a Pauling-type adsorption mode, favoring •O₂ ^- formation by partially filling the π* antibonding orbitals, preserving the O─O bond. The spin-selective C-Salen-COF-Zn was integrated into a closed-loop cascade system for on-demand H₂O₂ generation and utilization, delivering 72% sodium perborate, 56% sodium peroxycarbonate, 82.7% lignin-to-benzoic acid conversions, and electro-Fenton degradation in advanced oxidation processes.

PMID:
42585028
Bibliographic data and abstract were imported from PubMed on 13 Aug 2026.

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