Liang, YunchangBanjac, KarlaMartin, KevinZigon, NicolasLee, SeunghwaVanthuyne, NicolasGarces-Pineda, Felipe AndresGalan-Mascaros, Jose R.Hu, XileAvarvari, NarcisLingenfelder, Magali2022-07-042022-07-042022-07-042022-06-1010.1038/s41467-022-31096-8https://infoscience.epfl.ch/handle/20.500.14299/189025WOS:000810123400012While solar-to-fuel catalysis requires the careful transfer of electrons, there are still challenges understanding how electron spin contributes to reactivity. Here, authors employ chiral fused thiadiazole-helicenes to control spin polarization in oxygen evolution electrocatalysts.A sustainable future requires highly efficient energy conversion and storage processes, where electrocatalysis plays a crucial role. The activity of an electrocatalyst is governed by the binding energy towards the reaction intermediates, while the scaling relationships prevent the improvement of a catalytic system over its volcano-plot limits. To overcome these limitations, unconventional methods that are not fully determined by the surface binding energy can be helpful. Here, we use organic chiral molecules, i.e., hetero-helicenes such as thiadiazole-[7]helicene and bis(thiadiazole)-[8]helicene, to boost the oxygen evolution reaction (OER) by up to ca. 130 % (at the potential of 1.65 V vs. RHE) at state-of-the-art 2D Ni- and NiFe-based catalysts via a spin-polarization mechanism. Our results show that chiral molecule-functionalization is able to increase the OER activity of catalysts beyond the volcano limits. A guideline for optimizing the catalytic activity via chiral molecular functionalization of hybrid 2D electrodes is given.Multidisciplinary SciencesScience & Technology - Other Topicsspin polarizationmagnetic-fieldswater oxidationfehelicenescatalystelectrochemistryadsorptiondepositionnanosheetstext::journal::journal article::research article