studies of the relationship between surface spin configurations and spin-related electrocatalytic reactions are crucial for understanding how magnetic catalysts enhance oxygen evolution reaction (OER) performance under magnetic fields. In this work, 2D FeSe nanosheets with rich surface spin configurations are synthesized via chemical vapor deposition. magnetic force microscopy and Raman spectroscopy reveal that a 200 mT magnetic field eliminates spin-disordered domain walls, forming a spin-ordered single-domain structure, which lowers the OER energy barrier, as confirmed by theoretical calculations. Electrochemical tests show that under a 200 mT magnetic field, the OER overpotential of multidomain FeSe nanosheets at 10 mA cm decreases from 346 mV to 259 mV, while the magnetic field has minimal effect on single-domain nanosheets. These findings highlight the critical role of spin configurations in enhancing electrocatalytic performance, offering new insights into the design of magnetic catalysts for industrial applications.
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http://dx.doi.org/10.1021/acs.nanolett.4c05609 | DOI Listing |
Magn Reson Med
January 2025
Department 8.1 - Biomedical Magnetic Resonance, Physikalisch-Technische Bundesanstalt (PTB), Braunschweig and Berlin, Germany.
Purpose: To develop a low-cost, high-performance, versatile, open-source console for low-field MRI applications that can integrate a multitude of different auxiliary sensors.
Methods: A new MR console was realized with four transmission and eight reception channels. The interface cards for signal transmission and reception are installed in PCI Express slots, allowing console integration in a commercial PC rack.
J Phys Chem A
January 2025
Department of Chemistry and Supercomputing Institute, University of Minnesota, Minneapolis, Minnesota 55455-0431, United States.
The energy gaps, spin-orbit coupling (SOC), and admixture coefficients over a series of the configurations are evaluated by the SA-CASSCF/6-31G, SA-CASSCF/6-31G*, SA-CASSCF/ANO-RCC-VDZP, and MS-CASPT2/ANO-RCC-VDZP to reveal the extent of the inaccuracy of the SA-CASSCF. By comparing the mean absolute errors for the energy gaps and the admixture coefficient magnitudes (ACMs) measured between the SA-CASSCF/6-31G, SA-CASSCF/6-31G*, or SA-CASSCF/ANO-RCC-VDZP and the MS-CASPT2/ANO-RCC-VDZP, the SA-CASSCF/6-31G is selected as the electronic structure method in the nonadiabatic molecular dynamics simulation. The major components of the ACMs of the SA-CASSCF/6-31G and MS-CASPT2/ANO-RCC-VDZP are identified and compared; we find that the ACMs are underestimated by the SA-CASSCF/6-31G, which is verified by the reasonable triplet quantum yield simulated by the trajectory surface hopping and the calibrated SA-CASSCF/6-31G.
View Article and Find Full Text PDFJ Am Chem Soc
January 2025
Department of Chemistry, Southern University of Science and Technology, Shenzhen 518055, China.
A small but growing set of radical SAM (-adenosyl-l-methionine) enzymes catalyze the radical mediated dehydration or dehydrogenation of 1,2-diol substrates. In some cases, these activities can be interchanged via minor structural perturbations to the reacting components raising questions regarding the relative importance of hyperconjugation, proton circulation and leaving group stability in determining the reaction outcome. The present work describes trapping and electron paramagnetic resonance (EPR) characterization of an α-hydroxyalkyl radical intermediate during dehydration and dehydrogenation of cytosylglucuronic acid and its derivatives catalyzed by the radical SAM enzyme BlsE and its Glu189Ala mutant from the blasticidin S biosynthetic pathway.
View Article and Find Full Text PDFJ Med Chem
January 2025
College of Chemistry and Environmental Engineering, Shenzhen University, Shenzhen 518060, China.
The hypoxic environment of solid tumors significantly diminishes the therapeutic efficacy of oxygen-dependent photodynamic therapy. Developing efficient photosensitizers that operate photoredox catalysis presents a promising strategy to overcome this challenge. Herein, we report the rational design of two rhenium(I) tricarbonyl complexes ( and ) with electron donor-acceptor-donor configuration.
View Article and Find Full Text PDFJ Comput Chem
January 2025
Department of Chemistry, Gottwald Center for the Sciences, University of Richmond, Richmond, Virginia, USA.
The energies and geometries of the lowest lying singlet and triplet states of the four diradicals formed by removing two H atoms from thiophene have been characterized. We utilized the highly correlated, multireference methods configuration interaction with single and double excitations with and without the Pople correction for size-extensivity (MR-CISD+Q and MR-CISD) and averaged quadratic coupled cluster theory (MR-AQCC). CAS (8,7) and CAS (10,8) active spaces involving σ, σ*, π, and π* orbitals were employed along with the cc-pVDZ and cc-pVTZ basis sets.
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