Catalyst Self-Assembly Accelerates Bimetallic Light-Driven Electrocatalytic H2 Evolution in Water DOI Creative Commons

Isaac N. Cloward,

Tianfei Liu,

Jamie Rose

и другие.

Опубликована: Апрель 10, 2023

Hydrogen evolution is an important fuel-generating reaction that has been subject to mechanistic debate about the roles of monometallic and bimetallic pathways. In this study, molecular iridium catalysts undergo photoelectrochemical dihydrogen afford a rare opportunity systematically understand factors promote H–H coupling. Covalently tethered diiridium evolve H2 from neutral water faster than catalysts, even at lower overpotential. The origin improvement noncovalent supramolecular self-assembly into “all-catalyst” nanoscale aggregates efficiently harvest light form bonds. New containing long-chain alkane substituents leverage self-assemly close expected maximum rate for light-driven splitting with activity below 100 mV Design parameters holding multiple catalytic sites in proximity tuning catalyst microenvironment emerge work.

Язык: Английский

Enabling Internal Electric Fields to Enhance Energy and Environmental Catalysis DOI
Lei Chen, Jin‐Tao Ren, Zhong‐Yong Yuan

и другие.

Advanced Energy Materials, Год журнала: 2023, Номер 13(11)

Опубликована: Янв. 29, 2023

Abstract Recent years have witnessed an upsurge of interest in exploiting advanced photo‐/electrocatalysts for efficient energy conversion and environmental remediation. Constructing internal electric fields has been highlighted as a rising star to help facilitate various catalytic processes, with the merits promoting charge transfer/separation, optimizing redox potential creating effective active/adsorption sites. Internal are usually formed by polarization uneven distributions between different constituent layers, which widely exist piezoelectrics, polar surface terminations, heterostructure materials. Herein, groundbreaking interdisciplinary overview latest advances construction improve photo(electro)catalytic electrocatalytic activity is provided. This critical review begins encyclopedic summary classification, advantages, synthesis strategies fields. Subsequently, identification methods thoroughly discussed based on characterization techniques, experiments, theoretical calculations, can provide profound guidance in‐depth study To elaborate theory–structure–activity relationships fields, corresponding reaction mechanisms, modification strategies, performance jointly discussed, along discussion their practical applications. Finally, insightful analysis challenges future prospects field‐based catalysts discussed.

Язык: Английский

Процитировано

112

Regioisomeric effect of heteroatoms and functional groups of organic ligands: Impacts on coordination bonding and corrosion protection performance DOI Creative Commons
Chandrabhan Verma, Ambrish Singh, Prashant Singh

и другие.

Coordination Chemistry Reviews, Год журнала: 2024, Номер 515, С. 215966 - 215966

Опубликована: Май 20, 2024

The regioisomeric effect, which refers to the different positions of heteroatoms and functional groups on a molecule, significantly impacts stability, physicochemical properties, chemical reactivity, coordination bonding organic compounds. These effects are critical for their commercial applications, notably in corrosion inhibition. Regioisomeric ligands, with unique spatial configurations groups, influence ability establish stable interactions metal surfaces. Certain regioisomers may exhibit enhanced affinity adsorption capacities based structural configurations, thereby facilitating formation more durable protective layer substrate. This review explores impact regioisomerism inhibition performance A literature survey reveals that identical substituents (e.g., –OH, –NH2, –COOH, –NO2, –OR), multiple bonds >CC< –CC–), or N, O, S) at varying diverse capabilities efficiencies. detailed analysis indicates certain regioisomers, due strategic placement achieve increased stability form relatively stronger complexes. enhances effectiveness chelation mechanisms. role group has been seldom observed documented previous studies. current research also underscores significance determining ligands. thorough understanding will assist scientists engineers developing effective inhibitors.

Язык: Английский

Процитировано

37

Mechanism of Key Intermediates Regulation in Electrocatalytic Nitrate-to-Ammonia Conversion Driven by Polarized Electric Field DOI

Xiaochuan Tang,

Wei Liu,

Chenjun Lei

и другие.

Nano Energy, Год журнала: 2025, Номер unknown, С. 110708 - 110708

Опубликована: Янв. 1, 2025

Язык: Английский

Процитировано

3

Enantioselective dearomatization reactions of heteroarenes by anion-binding organocatalysis DOI Creative Commons

Martin Aleksiev,

Olga Garcı́a Mancheño

Chemical Communications, Год журнала: 2023, Номер 59(23), С. 3360 - 3372

Опубликована: Янв. 1, 2023

This feature article outlines the up-to-date implementation of anion-binding catalysis for enantioselective dearomatization hereoarenes, expanding chemical space by converting available flat building blocks into valuable chiral molecules.

Язык: Английский

Процитировано

26

Catalyst self-assembly accelerates bimetallic light-driven electrocatalytic H2 evolution in water DOI

Isaac N. Cloward,

Tianfei Liu,

Jamie Rose

и другие.

Nature Chemistry, Год журнала: 2024, Номер 16(5), С. 709 - 716

Опубликована: Март 25, 2024

Язык: Английский

Процитировано

16

Spatially Confined Microcells: A Path toward TMD Catalyst Design DOI
Shasha Guo,

Mingyu Ma,

Yuqing Wang

и другие.

Chemical Reviews, Год журнала: 2024, Номер 124(11), С. 6952 - 7006

Опубликована: Май 15, 2024

With the ability to maximize exposure of nearly all active sites reactions, two-dimensional transition metal dichalcogenide (TMD) has become a fascinating new class materials for electrocatalysis. Recently, electrochemical microcells have been developed, and their unique spatial-confined capability enables understanding catalytic behaviors at single material level, significantly promoting this field. This Review provides an overview recent progress in microcell-based TMD electrocatalyst studies. We first introduced structural characteristics discussed site engineering strategies Later, we comprehensively described two distinct types microcells: window-confined on-chip microcell (OCEM) droplet-confined scanning cell microscopy (SECCM). Their setups, working principles, instrumentation were elucidated detail, respectively. Furthermore, summarized advances OCEM SECCM obtained catalysts, such as identification imaging, monitoring, modulation charge injection transport, electrostatic field gating. Finally, current challenges provided personal perspectives on research.

Язык: Английский

Процитировано

13

Manganese(II) complexes of thiophenyl imino-ligand with synergistic behavior in biological systems, ct-DNA interactions, and catalytic oxidative performance of benzyl alcohol DOI
Mohamed Shaker S. Adam,

Zakaria S. Bakhuraisa,

M. J. A. Abualreish

и другие.

Polyhedron, Год журнала: 2025, Номер unknown, С. 117441 - 117441

Опубликована: Фев. 1, 2025

Язык: Английский

Процитировано

1

Tuning Electrode Reactivity through Organometallic Complexes DOI Creative Commons
Yi Shen, Yu Mu, Dunwei Wang

и другие.

ACS Applied Materials & Interfaces, Год журнала: 2023, Номер 15(24), С. 28851 - 28878

Опубликована: Июнь 9, 2023

The use of molecularly modified electrodes in catalysis heralds a new paradigm designing chemical transformations by allowing control catalytic activity. Herein, we provide an overview reported methods to develop functionalized with organometallic complexes and summary commonly used techniques for characterizing the electrode surface after immobilization. In addition, highlight implications functionalization emphasize key aspects that should be considered during development optimization electrodes. Particularly, surface–molecule electronic coupling electrostatic interactions within hybrid system are discussed present effective handles tuning We envision this emerging type has potential combine advantages homogeneous heterogeneous supports could applied expanded range beyond energy conversion.

Язык: Английский

Процитировано

12

Electric‐Field‐Induced Organic Transformations DOI

Shaik Kareem,

Shaik Ramjan Vali, B. V. Subba Reddy

и другие.

European Journal of Organic Chemistry, Год журнала: 2023, Номер 26(20)

Опубликована: Апрель 10, 2023

Abstract Experiments showed that the existence of electric fields in non‐redox processes may alter catalytic activity, rate enhancement, and selection organic reactions. It is expected interaction between chemical reactions will create new avenues for producing materials with desired properties several disciplines, including synthetic chemistry, catalysis, nanotechnology, membrane technology, enzyme catalysis. Specifically, this review, we discuss elegant experimental investigations carried out using scanning tunneling microscope, interfacial field, designed local fields. The results these studies are remarkable, leading to information on function controlling reactivity selectivity different offering a glimpse great potential electrostatic This article not only presents core concepts field‐induced transformations but also illustrates use field catalysis chemistry other

Язык: Английский

Процитировано

10

Charge and Solvent Effects on the Redox Behavior of Vanadyl Salen–Crown Complexes DOI
Hien M. Nguyen, Harry W. T. Morgan, Teera Chantarojsiri

и другие.

The Journal of Physical Chemistry A, Год журнала: 2023, Номер 127(25), С. 5324 - 5334

Опубликована: Июнь 14, 2023

The incorporation of charged groups proximal to a redox active transition metal center can impact the local electric field, altering behavior and enhancing catalysis. Vanadyl salen (salen = N,N'-ethylenebis(salicylideneaminato)) complexes functionalized with crown ether containing nonredox cation (V-Na, V-K, V-Ba, V-La, V-Ce, V-Nd) were synthesized. electrochemical this series was investigated by cyclic voltammetry in solvents varying polarity dielectric constant (ε) (acetonitrile, ε 37.5; N,N-dimethylformamide, 36.7; dichloromethane, 8.93). vanadium(V/IV) reduction potential shifted anodically increasing charge compared complex lacking (ΔE1/2 > 900 mV acetonitrile >700 dichloromethane). In contrast, for all vanadyl salen-crown measured N,N-dimethylformamide insensitive magnitude cationic charge, regardless electrolyte or counteranion used. Titration studies into resulted cathodic shifting concentration N,N-dimethylformamide. Binding constants (log(KDMF)) show increased binding affinity order V-La V-Ba V-K (salen)V(O), indicating an enhancement Lewis acid/base interaction charge. (salen)V(O) (salen-OMe)V(O) (salen-OMe N,N'-ethylenebis(3-methoxysalicylideneamine) also crown-containing complexes. For (salen-OMe)V(O), weak association triflate salt at vanadium(IV) oxidation state observed through titration experiments, dissociation upon vanadium(V) identified. These demonstrate noninnocent role solvent coordination cation/anion effects on and, extension, field.

Язык: Английский

Процитировано

10