Chemistry for Water Treatment under Nanoconfinement

Water Research, Journal Year: 2025, Volume and Issue: 275, P. 123173 - 123173

Published: Jan. 21, 2025

Language: Английский

---

Research Progress of Coordination Materials for Electrocatalytic Nitrogen Oxides Species Conversion into High-Value Chemicals

EnergyChem, Journal Year: 2025, Volume and Issue: unknown, P. 100146 - 100146

Published: Feb. 1, 2025

Language: Английский

---

Inverse Oxide/Alloy‐Structured Nanozymes with NIR‐Triggered Enzymatic Cascade Regulation of ROS Homeostasis for Efficient Wound Healing

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 25, 2025

The precise spatiotemporal control of reactive oxygen species (ROS) generation and scavenging remains pivotal for infected wound healing. However, conventional nanozymes fail to adaptively regulate ROS dynamics across inflammatory proliferative phases. A near-infrared (NIR)-activated inverse oxide/alloy-structured nanozyme (Co7Fe3/ZnO@C) is developed, featuring enzymatic cascade activities tune homeostasis through synergistic chemodynamic (CDT), photodynamic (PDT), photothermal (PTT) therapies. orchestrates a self-regulated cascade: peroxidase (POD)-like activity initially generates bactericidal hydroxyl radicals in acidic wounds, while subsequent NIR triggers hot electron transfer from Co7Fe3 ZnO, facilitating synchronized superoxide dismutase (SOD)-like, catalase (CAT)-like radical antioxidant capacity (HORAC) scavenge residual ROS. This cascaded network dynamically balances production (POD) (NIR-driven SOD/CAT/HORAC), eradicating bacteria resolving inflammation. In vitro/vivo studies have shown that the proposed method maintaining can markedly enhance rate healing by regulation environment within injured tissue facilitation rapid re-epithelialization. work provides an intelligent platform simulates function natural enzymes constructs reaction strategy balance antibacterial anti-inflammatory demands microenvironment.

Language: Английский

---

Adjustment of Molecular Sorption Equilibrium on Catalyst Surface for Boosting Catalysis

Accounts of Chemical Research, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 15, 2025

ConspectusFor chemical reactions with complex pathways, it is extremely difficult to adjust the catalytic performance. The previous strategies on this issue mainly focused modifying fine structures of catalysts, including optimization geometric/electronic structure metal nanoparticles (NPs), regulation composition/morphology supports, and/or adjustment metal–support interactions modulate reaction kinetics catalyst surface. Although significant advances have been achieved, performance still unsatisfactory.It accepted that equilibrium a can be disturbed by changing concentration reactants or products, and will shift another side offset perturbation until new established. This known as Le Chatelier's principle. Following understanding, we show significantly modulated adjusting molecular sorption For example, enriching intermediates surface pushes forward, thus increasing conversion; removing product away from improves conversion selectivity; inhibiting enhances selectivity durability. Using these has successfully enhanced performances in many challenging reactions, such H2O2 around active sites enhance methane oxidation, olefin boost hydroformylation, selective combustion H2 improve ethane dehydrogenation, water system Fischer–Tropsch synthesis. key successes effectively shifting under working conditions.In Account, briefly summarize recent for boosting catalysis, focus desired pathway unique functions zeolites polymers silanol nests zeolite adsorption, "molecular fence" effect enrichment, MFI nanosheets diffusion, hydrophobic sheath polymer separation/diffusion. We report via intermediates, As result, high activity, excellent selectivity, outstanding durability catalysts were achieved. In addition, current challenges perspectives applying strategy more important industrial are discussed. Applications advanced characterization tools, machine learning, artificial intelligence monitoring dynamic structural changes predicting evolutions conditions anticipated continuously play roles design. believe open door development highly efficient potential applications future.

Language: Английский

---

AI unveils metal-support interaction principle to optimize catalyst design

Chem Catalysis, Journal Year: 2025, Volume and Issue: 5(1), P. 101231 - 101231

Published: Jan. 1, 2025

Language: Английский

---

Unraveling the Effects of Metal–Support Interaction on Nitrogen Reduction: A Theoretical Study in Au₁₃/BiOCl

The Journal of Physical Chemistry Letters, Journal Year: 2025, Volume and Issue: unknown, P. 924 - 931

Published: Jan. 20, 2025

Understanding the mechanism of nitrogen reduction reaction (NRR) is essential for designing highly efficient catalysts. In this study, we investigated effects metal–support interaction (MSI) on NRR using density functional theory. The simulations revealed that MSI weak in Au13/BiOCl system, with charge accumulation and depletion primarily occurring within Au13 cluster. By replacement one Au atom either a Ag or Pt atom, becomes stronger compared to system. because doping breaks symmetry cluster, leading at interface. Specifically, enhanced reduces energy barriers rate-determining step from 1.07 eV system 0.91 Au12Ag/BiOCl 0.87 Au12Pt/BiOCl, respectively. Our study uncovers critical role activity NRR, providing theoretical insights development

Language: Английский

---

Emerging Supported Metal Atomic Clusters for Electrocatalytic Renewable Conversions

ACS Catalysis, Journal Year: 2025, Volume and Issue: unknown, P. 2434 - 2458

Published: Jan. 27, 2025

Subnanometric supported metal atomic clusters (SMACs) composed of several to tens surface atoms have attracted increased research interest in electrocatalysis. SMACs been known show distinct properties compared their nanoparticles and single atom counterparts long developed for functional improvements. Tremendous advancements made the past few years, with a notable trend more precise design down an atomic/molecular level investigation transferring into practical devices, which motivates this timely review. To begin, review presents classifies classic latest synthetic strategies state-of-the-art characterization techniques SMACs. It then outlines discusses basic structure principles SMACs, highlighting importance organic ligands, size effect clusters, support-cluster interactions determining catalytic activity device stability. Thereafter, recent advances typical electrocatalysis processes from laboratory scale industrial are discussed obtain general understanding structure–activity correlations Current challenges future perspectives emerging field also discussed, aiming at practicing SMAC catalysts energy conversion devices.

Language: Английский

---

Finely Tailoring Metal–Support Interactions via Transient High-Temperature Pulses

ACS Applied Materials & Interfaces, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 13, 2025

Metal–support interactions (MSI) play a crucial role in enhancing the catalytic activity and stability of metal catalysts by establishing stable metal-oxide interface. However, precisely controlling MSI at atomic scale remains significant challenge, as how to construct an optimal is still not fully understood: Both insufficient excessive showed inferior performance. In this study, we propose finely tuning using temporal-precise transient high-temperature pulse heating. Using Pt/CeO2 model system, systematically investigate variations duration atmosphere influence reconstruction metal–support interface MSIs. This leads formation two distinct types MSI: (1) strong (SMSI, Pt@CeO2) (2) reactive (RMSI, Pt5Ce@CeO2), each with unique compositions, structures, electrochemical behaviors. Notably, Pt5Ce@CeO2 RMSI exhibits remarkable performance alkaline hydrogen evolution, showing overpotential −29 mV operation for over 300 h −10 mA·cm–2. Theoretical studies reveal that alloying Pt Ce form Pt5Ce modifies electronic structure Pt, shifting d-band center optimize adsorption dissociation intermediates, thereby reducing reaction energy barrier. Moreover, intimate interaction CeO2 further improves stability. Our strategy enables precise, stepwise, controllable regulation MSIs, providing insights development highly efficient durable heterostructured wide range applications.

Language: Английский

---

Ligand-Restricted Strategy for Synthesizing Highly Pairing Dual Atom Catalysts

Research Square (Research Square), Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 14, 2025

Dual atom catalysts (DACs), characterized by high activity and metal utilization, as well structural diversity with a large variety of catalytic sites, hold immense promise for energy conversion technologies, garnering substantial interest from both academia industry. However, achieving precise control manipulation atomic dispersion, pairing ratios, interatomic distances in DACs, which significantly affect their multifunctional properties, remains significant challenge. Herein, we developed ligand-restricted strategy the synthesis highly DACs tunable distances. This was accomplished coordinating diamine ligands dual precursors, restricting relative positions two atoms on two-dimensional graphitic carbon nitride. The ratio exceeded 82%, chain length molecules effectively regulating distance between paired atoms. As demonstration, Pt₁-Au₁ exhibited almost three times nitrate reduction to ammonia compared unpaired counterparts. Furthermore, shorter distanced DAC reveals four photothermal catalyzed hydrogenation reactions than longer ones. work not only introduces novel design atomic-scale fabrication complex but also provides valuable insights into nanoscale reaction mechanisms heterogeneous catalysis.

Language: Английский

---

Digital Descriptors in Predicting Catalysis Reaction Efficiency and Selectivity

The Journal of Physical Chemistry Letters, Journal Year: 2025, Volume and Issue: 16(9), P. 2357 - 2368

Published: Feb. 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.

Language: Английский

---