ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(15), P. 11273 - 11285
Published: July 13, 2024
Language: Английский
The Journal of Physical Chemistry Letters, Journal Year: 2023, Volume and Issue: 14(14), P. 3491 - 3497
Published: April 3, 2023
Quantum computing has emerged as a promising platform for simulating strongly correlated systems in chemistry, which the standard quantum chemistry methods are either qualitatively inaccurate or too expensive. However, due to hardware limitations of available noisy near-term devices, their application is currently limited only small chemical systems. One way extending range applicability can be achieved within embedding approach. Herein, we employ projection-based method combining variational eigensolver (VQE) algorithm, although not to, with density functional theory (DFT). The developed VQE-in-DFT then implemented efficiently on real device and employed triple bond breaking process butyronitrile. results presented herein show that approach fragment computer.
Language: Английский
Citations
33
Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(21)
Published: March 21, 2023
This work suggests an intriguing light-driven atomic assembly proposal to orderly configure the distribution of reactive sites optimize spin-entropy-related orbital interaction and charge transfer from electrocatalysts intermediates. Herein, introduced fluorine (F) atoms acting as photo-corrosion centres in MnO1.9 F0.1 effectively soften bonding Mn-O bonds IrCl3 solution. Therefore, partial Mn can be successively replaced form atomic-hybridized catalysts with a spin-related low entropy due coexistence Ir-atomic chains clusters. The time-related elemental analysis demonstrates that dynamic dissolution/redeposition Ir clusters acidic oxygen evolution leads reintegration reaction pathway seek switchable rate-limiting step lower activation energy.
Language: Английский
Citations
30
ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(8), P. 5685 - 5695
Published: April 1, 2024
Creating highly effective electrocatalysts for the oxygen evolution reaction (OER) holds paramount importance in advancing carbon-neutral hydrogen production through water electrolysis. Recent research highlights crucial role of spin effects on OER, emphasizing that manipulation polarization is a promising strategy to augment OER kinetics. Here, we present core–shell heterostructure electrocatalyst, which leverages strong coupling interface between antiferromagnetic Co3O4 and NiFe-layered double hydroxide (NiFe-LDH) trigger spontaneous magnetic response enhancement, suggests exchange interaction at heterostructure. This electrocatalyst displays 26-fold increase intrinsic activity compared pristine NiFe-LDH an overpotential 0.25 V. Through experimental computational analyses, find within creates polarized conduction channels interface, enables efficient accumulation electrons with appropriate states, thereby lowering energy barrier generation triplet O2. Our work presents approach designing high-performance catalysts by introducing selectivity traditional metal oxide electrocatalysts.
Language: Английский
Citations
15
npj Computational Materials, Journal Year: 2024, Volume and Issue: 10(1)
Published: April 22, 2024
Abstract Green hydrogen production is crucial for a sustainable future, but current catalysts the oxygen evolution reaction (OER) suffer from slow kinetics, despite many efforts to produce optimal designs, particularly through calculation of descriptors activity. In this study, we develop dataset density functional theory calculations bulk and surface perovskite oxides, adsorption energies OER intermediates, which includes compositions up quaternary facets (555). We demonstrate that per-site properties oxides such as Bader charge or band center can be tuned element substitution faceting, machine learning model accurately predicts these directly local chemical environment. leverage identify promising perovskites with high theoretical The identified design principles materials provide roadmap closing gap between artificial biological enzymes photosystem II.
Language: Английский
Citations
13
Applied Physics Reviews, Journal Year: 2024, Volume and Issue: 11(1)
Published: March 1, 2024
To reach a long term viable green hydrogen economy, rational design of active oxygen evolution reaction (OER) catalysts is critical. An important hurdle in this originates from the fact that reactants are singlet molecules, whereas molecule has triplet ground state with parallel spin alignment, implying magnetic order catalyst essential. Accordingly, multiple experimentalists reported positive effect external fields on OER activity ferromagnetic catalysts. However, it remains challenge to investigate influence intrinsic catalytic activity. Here, we tuned epitaxial La0.67Sr0.33MnO3 thin film model ferro- paramagnetic by changing temperature situ during water electrolysis. Using strategy, show ordering below Curie enhances Moreover, slight current density enhancement upon application an field and find dependence direction correlates anisotropy film. Our work, thus, suggests both films domain alignment increase their We observe no long-range at surface, connected bulk catalyst. Combining effects found existing literature, propose unifying picture for spin-polarized oxide
Language: Английский
Citations
12
Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 361, P. 124585 - 124585
Published: Sept. 10, 2024
Language: Английский
Citations
12
Journal of Cleaner Production, Journal Year: 2024, Volume and Issue: 466, P. 142886 - 142886
Published: June 12, 2024
Language: Английский
Citations
10
Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(34)
Published: April 1, 2024
Abstract Electron spinning polarization has garnered increased attention for its potential to enhance device properties. However, application in life health, specifically anti‐infection and tissue repair, remains under‐explored. In this study, a ferromagnetic heterojunction CF (Fe 3 O 4 /TiO 2 ) is constructed with spin‐polarized electrons, demonstrating efficient antibiosis performance ultrasound (US) assistance. The antibacterial mechanism elucidated as follows: metallic states of Fe induce an asymmetric distribution the electron spin state TiO , increasing density electrons near Fermi level CF. Under US treatment, built‐in electric field synergistically suppress recombination sono‐activated carriers, promoting reactive oxygen species (ROS) production. Simultaneously, bacterial membrane influenced by micromagnetic induced causing severe disturbance respiratory chain. combined damage from ROS disturbed chain results death. Fortunately, built activates specific mechanosensitive ion channels, including TREK1, Piezo1, related pathways, enhancing osteoblast differentiation. Sonotherapy using exhibits excellent therapeutic effect treating osteomyelitis. This study provides novel insights into manipulating applications health.
Language: Английский
Citations
9
Chem Catalysis, Journal Year: 2024, Volume and Issue: 4(9), P. 101083 - 101083
Published: Aug. 20, 2024
Language: Английский
Citations
9
Nano Letters, Journal Year: 2023, Volume and Issue: 23(19), P. 9042 - 9049
Published: Sept. 22, 2023
Electron spin polarization is identified as a promising avenue for enhancing the oxygen evolution reaction (OER), which bottleneck that limits energy efficiency of water-splitting. Here, we report both ferrimagnetic (f-Fe3O4) and superparamagnetic iron oxide (s-Fe3O4) catalysts can exhibit external magnetic field (Hext)-induced OER enhancement, activity proportional to their intrinsic moment. Additionally, chirality-induced selectivity (CISS) effect was utilized in synergy with Hext get maximum enhancement up 89% improvement current density (at 1.8 V vs RHE) low onset potential 270 mV s-Fe3O4 catalysts. Spin resultant suppress production H2O2 promote formation ground state triplet O2 during OER. Furthermore, design chiral synergistic demonstrates high ∼42%, measured using conductive atomic force microscopy (c-AFM).
Language: Английский
Citations
20