Digital Descriptors in Predicting Catalysis Reaction Efficiency and Selectivity

The Journal of Physical Chemistry Letters, Год журнала: 2025, Номер 16(9), С. 2357 - 2368

Опубликована: Фев. 26, 2025

Accurately controlling the interactions and dynamic changes between multiple active sites (e.g., metals, vacancies, lone pairs of heteroatoms) to achieve efficient catalytic performance is a key issue challenge in design complex reactions involving 2D metal-supported catalysts, metal-zeolites, metal–organic metalloenzymes. With aid machine learning (ML), descriptors play central role optimizing electrochemical elucidating essence activity, predicting more thereby avoiding time-consuming trial-and-error processes. Three kinds descriptors─active center descriptors, interfacial reaction pathway descriptors─are crucial for understanding designing catalysts. Specifically, as sites, synergize with metals significantly promote reduction energy-relevant small molecules. By combining some physical interpretable can be constructed evaluate performance. Future development ML models faces constructing vacancies multicatalysis systems rationally selectivity, stability Utilization generative artificial intelligence multimodal automatically extract would accelerate exploration mechanisms. The transferable from catalysts metalloenzymes provide innovative solutions energy conversion environmental protection.

Язык: Английский

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Silver Induced In-Phase Electronic Interaction and Chloride Ion Repelling for Efficient Electrocatalytic Oxygen Evolution in Seawater Electrolysis

ACS Applied Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 2, 2025

Seawater electrolysis for hydrogen production has emerged as a focal point in energy utilization technology due to its low carbon emissions and the abundance of seawater resources. However, high chlorine content an electrolyte negatively impacts stability performance anodic catalysts. Herein, we design silver integration strategy repel surface Cl– adsorption modulate electronic structure metal active center NiCo bimetallic organic framework (MOF). The obtained Ag@NiCo MOF achieves overpotential 269 mV at current density 10 mA cm–2 toward oxygen evolution reaction (OER) maintains this over 500 h simulated alkaline without obvious degradation. superior is because in-phase interaction induced by deposited Ag optimizes electron state sites. Moreover, situ transforms into AgCl during OER further triggering repulsion on electrode surface. This not only facilitates kinetic but also helps chloride ions enhances selectivity OER. electrochemical render them highly competitive among various catalysts spitting.

Язык: Английский

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Activating Inert Palmeirite Through Co Local‐Environment Modulation and Spin Electrons Rearrangement for Superior Oxygen Evolution

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 5, 2025

Abstract Mo‐based palmeirite oxide A 2 Mo 3 O 8 is an emerging electrocatalyst, exhibiting a bipartite honeycomb lattice consisting of tetrahedral and octahedral sites with good conductivity. However, as promising catalyst in electrocatalytic remains rarely touched. The rational design clarification the correlation between geometrical configuration modulation properties are challenging. Herein, innovative strategy reported to anchor thiospinel Co S 4 nanoparticles onto surface nanosheet, which can trigger spin electrons rearrangement, thus activating inert sites. According X‐ray absorption spectroscopy, 2+ ─O─Co 3+ bimetallic bridging asymmetric bond polarization constructed interface, triggers favorable transition from low intermediate spin. Interestingly, /Co exhibits remarkable oxygen evolution reaction performance overpotential 227 mV at 10 mA cm −2 . At industrial process temperature, it takes only 2.37 V for overall water splitting obtain large current density 1 theoretical calculation results confirm that distortion‐related optimizes energy, enhancing adsorption * OOH. This work highlights potential achieving seawater by rearrangement.

Язык: Английский

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Tuning Transition Metal 3d Spin state on Single‐atom Catalysts for Selective Electrochemical CO₂ Reduction

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 13, 2025

Abstract Tuning transition metal spin states potentially offers a powerful means to control electrocatalyst activity. However, implementing such strategy in electrochemical CO 2 reduction (CO R) is challenging since rational design rules have yet be elucidated. Here we show how the addition of P dopants ferromagnetic element (Fe, Co, and Ni) single‐atom catalyst (SAC) can shift its state. For instance, with Fe SAC, enable switch from low state ( d x2‐ y2 0 , z2 xz yz 1 xy ) Fe‐N 4 high x2‐y2 3 ‐P. This studied using suite characterization efforts, including X‐ray absorption spectroscopy (XAS), electron resonance (ESR) spectroscopy, superconducting quantum interference device (SQUID) measurements. When used for R, SAC ‐P active sites yields > 90% Faradaic efficiency over wide potential window ≈530 mV maximum partial current density ≈600 mA cm −2 . Density functional theory calculations reveal that 3+ exhibits enhanced back donation via / ‐π* bond, which enhances * COOH adsorption promotes formation. Taken together, results intentionally tuned boost R performance.

Язык: Английский

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Advances in the synthesis of Fe-based bimetallic electrocatalysts for CO₂ reduction

RSC Advances, Год журнала: 2025, Номер 15(11), С. 8367 - 8384

Опубликована: Янв. 1, 2025

Achieving carbon neutrality and mitigating global warming through efficient CO 2 reduction, by utilizing synergistic bimetallic Fe-based catalysts for enhanced electrochemical performance selectivity.

Язык: Английский

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Manipulating the Intrinsic Magnetism of Spinel Catalyst toward Magnetic Field-Enhanced OER

ACS Catalysis, Год журнала: 2025, Номер unknown, С. 5640 - 5650

Опубликована: Март 21, 2025

Язык: Английский

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The Improved Covalent Coupling Induced by Bi Cations in CoBiSe_x Nanosheet Arrays for Stable Water Electrolysis

Inorganic Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Март 25, 2025

Transition metal selenides (TMSes) with high electrical conductivity, easily regulated morphological structure, and unique electronic structure have been explored as promising electrocatalysts for electrolytic water, while the lower intrinsic electrocatalytic capability has limited their wide application. Herein, we obtained CoSe nanosheet arrays Bi cations incorporation (CoBiSex arrays) driven by spinel oxides. Compared oxides, low electronegativity of Se in CoBiSex leads to a portion Co2+ spin states (t2g6eg1) due covalent interaction between Co Se, which can facilitate charge transfer. Density functional theory (DFT) calculation results further identify redistribution electron density from Co, intensifying adsorption OOH* during water process 140 h robust catalytic performance. This work offers strategy exploring TMSe materials potential applications process.

Язык: Английский

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Electrochemistry assisted chlorine corrosion strategy: The minute-level fabrication of lattice Cl– functioned high spin-polarized Ni/Fe-LDH array for enhanced anti-Cl– OER performance

CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Год журнала: 2025, Номер 70, С. 388 - 398

Опубликована: Март 1, 2025

Язык: Английский

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How to Achieve Hydrogenation/Hydrofunctionalization via Metal Hydride Complexes

Accounts of Chemical Research, Год журнала: 2025, Номер unknown

Опубликована: Апрель 20, 2025

ConspectusMetal hydride (M-H) complexes have garnered widespread attention in the synthesis of fine chemicals, materials, agrochemicals, and pharmaceuticals owing to remarkable reactivity M-H bonds. Specifically, are active intermediates that catalyze hydrogen-transfer reactions, leading efficient hydrogenation hydrofunctionalization C═C/C═X (X = O or N) bonds unsaturated organic substrates for formation new carbon-hydrogen, carbon-carbon, carbon-heteroatom bonds.Our research group has long studied transformation mechanisms, with significant advancements over past decade. For this Account, we drawn on our extensive expertise investigate mechanisms governing numerous transformation-driven including inert C═X compounds, bonds, dehydrogenative coupling, C-H functionalizations. On basis these mechanistic investigations, developed a series representative models, which offer robust theoretical guidance modulating selectivity hydrofunctionalization.Our Account begins structures properties complexes, lead homolytic heterolytic cleavage reactions different conditions, showcasing versatility metal reactivity. Based principles, three modes discussed. First, transfer low-oxidation-state is chiefly engaged because hydrogen atom attached high electron density strongly nucleophilic. In case, serves as from center electropositive substrate through following pathways: (a) insertion an bond into bond; (b) direct electrophilic site (c) σ-bond metathesis; (d) oxidative migration. Reductive elimination might also occur when oxidation state increases becomes electron-deficient. This usually regenerates catalytic species while producing C/X'-H Notably, (MHAT) advanced approach radical-type hydrofunctionalizations. MHAT induced by one-electron redox process enabled paramagnetic low dissociation energy (BDE) values. Two possible types (i.e., spontaneous passive), regioselectivities, proposed. article provides detailed account strategies related transformations, thus offering valuable rational design novel reaction systems.

Язык: Английский

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Constructing Molecular Junctions with High-Spin Metal Sites in POMOFs to Trigger Heteropoly Blue States for Photocatalytic H₂ Production

ACS Catalysis, Год журнала: 2025, Номер unknown, С. 7601 - 7612

Опубликована: Апрель 23, 2025

Язык: Английский

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