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The chiral-induced spin selectivity (CISS) effect holds transformative potential for spin-controlled electrocatalysis, yet its implementation in metal-organic frameworks (MOFs) remains constrained by the reliance on chiral ligands or crystallographic asymmetry. Herein, we challenge this paradigm by demonstrating morphological chirality engineering in achiral CoNi-MOFs (C2/m symmetry) as a new route to CISS-enhanced oxygen evolution reaction (OER). Through amino acid-mediated growth control, these MOFs adopt left-/right-handed distorted morphologies despite their achiral space group and linkers, achieving 42% spin polarization and 30–50 mV lower OER overpotentials at 100 mA·cm−2 compared to the achiral counterparts. This work establishes nanoscale morphological chirality control as a generalizable strategy to design spin-selective MOF electrocatalysts, potentially unlocking over 90% of the MOF family previously excluded from CISS applications.

This is an open access article under the terms of the Creative Commons Attribution 4.0 International License (CC BY 4.0, https://creativecommons.org/licenses/by/4.0/).
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