Quantum spin regulates the catalytic cycle beyond binding energy
Abstract
Conventional catalytic descriptors evaluate symmetric, dissipative responses (π), remaining blind to the antisymmetric, non-dissipative circulation (β) associated with cyclic catalyst turnover. We address this by applying an augmented Onsager operator, π = π + β, to catalytic interfaces. Through Onsager--Casimir parity rules, we show that electron spin governs this non-dissipative circulation within the reduced state space, as antisymmetric coupling necessitates a time-reversal-odd coordinate. We map these multi-physical couplings (Thermo-Hydro-Mechanical-Chemical-Electrical-Spin) using a Hasse diagram and introduce a basis-invariant Gateway number to quantify circulation relative to dissipation, thereby expanding standard one-dimensional volcano plots into a two-dimensional activity surface. Using metal--nitrogen single-atom sites on doped carbon as a model, published electronic-structure calculations supply the static response quantities from which both operator components can be constructed. Finally, we propose an explicitly falsifiable experimental test utilising magnetic field modulation near a spin-crossover to probe the effect of quantum spin on this non-dissipative regime.
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BibTeX
@misc{regenauerlieb2026quantum,
title = {{Quantum spin regulates the catalytic cycle beyond binding energy}},
author = {K. Regenauer-Lieb and W. Li and Z. Xia and Y. Jiao and Y. Liu and Y. Chen and Q. Xie and Q. P. Sun and B. Hamblin and V. Calo},
howpublished = {arXiv},
year = {2026},
month = oct,
doi = {10.48550/arxiv.2610.02592},
eprint = {2610.02592},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2610.02592},
note = {CC BY 4.0},
}
RIS
TY - UNPB
TI - Quantum spin regulates the catalytic cycle beyond binding energy
AU - K. Regenauer-Lieb
AU - W. Li
AU - Z. Xia
AU - Y. Jiao
AU - Y. Liu
AU - Y. Chen
AU - Q. Xie
AU - Q. P. Sun
AU - B. Hamblin
AU - V. Calo
PY - 2026
DA - 2026/10/01
PB - arXiv
DO - 10.48550/arxiv.2610.02592
UR - https://arxiv.org/abs/2610.02592
AB - Conventional catalytic descriptors evaluate symmetric, dissipative responses (π), remaining blind to the antisymmetric, non-dissipative circulation (β) associated with cyclic catalyst turnover. We address this by applying an augmented Onsager operator, π = π + β, to catalytic interfaces. Through Onsager--Casimir parity rules, we show that electron spin governs this non-dissipative circulation within the reduced state space, as antisymmetric coupling necessitates a time-reversal-odd coordinate. We map these multi-physical couplings (Thermo-Hydro-Mechanical-Chemical-Electrical-Spin) using a Hasse diagram and introduce a basis-invariant Gateway number to quantify circulation relative to dissipation, thereby expanding standard one-dimensional volcano plots into a two-dimensional activity surface. Using metal--nitrogen single-atom sites on doped carbon as a model, published electronic-structure calculations supply the static response quantities from which both operator components can be constructed. Finally, we propose an explicitly falsifiable experimental test utilising magnetic field modulation near a spin-crossover to probe the effect of quantum spin on this non-dissipative regime.
ER -