Report
Quantum spin regulates the catalytic cycle beyond binding energy
| Title: | Quantum spin regulates the catalytic cycle beyond binding energy |
|---|---|
| Authors: | Regenauer-Lieb, K., Li, W., Xia, Z., Jiao, Y., Liu, Y., Chen, Y., Xie, Q., Sun, Q. P., Hamblin, B., Calo, V. |
| Publication Year: | 2026 |
| Subject Terms: | Geophysics, Chemical Physics |
| Description: | Conventional catalytic descriptors evaluate symmetric, dissipative responses ($\mathcal{D}$), remaining blind to the antisymmetric, non-dissipative circulation ($\mathcal{L}$) associated with cyclic catalyst turnover. We address this by applying an augmented Onsager operator, $\mathcal{A} = \mathcal{D} + \mathcal{L}$, 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. Communication submitted to JCP, 16 pages 2 figures |
| Document Type: | Working Paper |
| DOI: | 10.48550/arXiv.2610.02592 |
| Access URL: | https://arxiv.org/abs/2610.02592 |
| Accession Number: | edsarx.2610.02592 |
| Database: | arXiv |
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