A Molecular Catalyst‐Driven Sustainable Zinc‐Air Battery Assembly DOI Open Access
Sukanta Saha, Sampurna Mitra, Yashwant Pratap Kharwar

et al.

Small, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 5, 2024

Bidirectional oxygen reduction reaction (ORR) and evolution (OER) electrocatalysts are key for molecular oxygen-centric renewable energy transduction via metal-air batteries. Here, a cobalt complex is covalently tethered on strategically functionalized silica surface that displayed both ORR OER in alkaline media. The detailed X-ray absorbance spectroscopy (XAS) studies indicate this catalyst retains its intrinsic features while playing central role during bidirectional electrocatalysis demonstrating relatively lower gap between O

Language: Английский

Highly efficient 2D/2D NiCo-LDH/CuInS2 nanocomposites for electrocatalytic hydrogen and oxygen evolution reactions DOI
Kotesh Kumar Mandari, Younghwan Im, Youngae Lee

et al.

Fuel, Journal Year: 2025, Volume and Issue: 388, P. 134505 - 134505

Published: Jan. 30, 2025

Language: Английский

Citations

4
Impact of the Surface Microenvironment on the Redox Properties of a Co-Based Molecular Cathode for Selective Aqueous Electrochemical CO2-to-CO Reduction DOI

Matthieu Haake,

Dmitry Aldakov, Julien Pérard

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(22), P. 15345 - 15355

Published: May 20, 2024

Electrode-confined molecular catalysts are promising systems to enable the efficient conversion of CO2 useful products. Here, we describe development an original cathode for reduction CO based on noncovalent integration a tetraazamacrocyclic Co complex carbon nanotube-based matrix. Aqueous electrochemical characterization modified electrode allowed clear observation change redox behavior center as surface concentration was tuned, highlighting impact catalyst microenvironment its properties. The enabled CO2-to-CO in fully aqueous conditions, giving rise turnover number (TONCO) up 20 × 103 after 2 h constant electrolysis at mild overpotential (η = 450 mV) and with faradaic efficiency about 95%. Post operando measurements using techniques, inductively coupled plasma, X-ray photoelectron spectroscopy absorption films demonstrated that catalysis remained nature, making this Co-based new alternative electrocatalytic media.

Language: Английский

Citations

12
Polymer Binder Blends Stabilize Alkaline Hydrogen Evolution by Heterogenized Molecular Phen-Based Cobalt Electrocatalysts through Coordination and Environmental Control DOI Creative Commons
Elizabeth Johnson, Daniel P. Musikanth, Christopher Webber

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: March 11, 2025

With the increase in greenhouse gas emissions and their detrimental effect on environment, there is a push to develop renewable way produce H2, fuel source that has nonharmful byproducts, unlike traditional methods of energy production. Alkaline water electrolysis seen increasing focus as viable but efficient stable electrocatalysts are required facilitate this process. Here, heterogenized Co(II) phenanthroline-based complex for production H2 from alkaline disclosed. Activity was improved by considering role axial Co ligation reaction environment created polymer binder catalyst inks using variable ratios Nafion poly-4-vinylpyridine (P4VP). A ratio 1:1 Nafion:P4VP found have highest stability, nanoparticle formation not observed when P4VP included part mixture. The activity stability enhancement could be replicated addition molecular pyridine or use poly-2-vinylpyridine, which sterically prevented coordinating Co. increased electrochemical performance caused inclusion attributed mass transfer active site during catalysis, complementing stabilizing site.

Language: Английский

Citations

1
From structure to function: MOF-based and COF-based catalysts for efficient electrocatalytic H2O2 production via 2e− ORR DOI
Yanchao Xu,

Zeyu Sun,

Shuyan Fan

et al.

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(40), P. 27180 - 27205

Published: Jan. 1, 2024

Overview of the structure and performance organic framework materials applied in 2e − ORR electrocatalysis.

Language: Английский

Citations

5
Mechanism of Electrochemical Proton Reduction Catalyzed by a Cobalt Tetraaza Schiff Base Macrocyclic Complex: Ligand Protonation and/or Influence of the Chloro Ligand DOI

Margaux Willery,

Paul‐Gabriel Julliard, Florian Molton

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(15), P. 11352 - 11365

Published: July 19, 2024

Cobalt complexes with tetra- and pentaaza-macrocyclic ligands, including the pyridyldiimine motif isolated by Busch as early 1970s, is a very promising family of catalysts that were only quite recently exploited for both electro- photocatalytic HER CO2RR. In particular, tetraaza [CoIII(CR14)Cl2]+ (CR14 = 2,12-dimethyl-3,7,11,17-tetraazabicyclo[11.3.1]heptadeca-1(17),2,11,13,15-pentaene) appears to be one most efficient stable Co in pure aqueous solution HER. this work, we reinvestigated H2-evolving mechanism catalyzed complex an organic solvent (CH3CN) acid p-cyanoanilinium tetrafluoroborate proton source. By comparison [CoIII(CR14)(CH3CN)2]3+ electrochemical behavior without addition chloride, first characterized thermodynamical coordination decoordination properties chloro ligands at CoIII, CoII, CoI formal redox states. Then, showed (through echem, UV–visible absorption, EPR) facilitates ligand CoII state rather than protonation nitrogen ligand. The electroreduction then kinetically thorough cyclic voltammetry analysis. resting bulk course constant potential electrolysis reduction was identified nonprotonated [CoII(CR14)(CH3CN)x]2+ (x 1 or 2) species, whereas it proposed hydride diffusion-reaction layer.

Language: Английский

Citations

3
The Hydrogen Evolution Reaction: Using Molecular Design in Transition Metal Complexes to Control Catalytic Microenvironments on Electrode Surfaces” DOI

Logan Trowbridge,

Peter E. Sues

ChemCatChem, Journal Year: 2024, Volume and Issue: unknown

Published: June 13, 2024

Abstract Hydrogen gas and its production from renewable power sources will be an important part of decreasing global reliance on fossil fuels developing a sustainable energy economy. Efficient electrocatalysis, however, relies the delivery both protons electrons; ideally in concerted fashion to avoid high intermediates, prevent charge build‐up, circumvent large kinetic barriers. While this can achieved using ligand design homogenous molecular transition metal catalysts (specifically incorporating proton shuttles secondary coordination sphere), heterogeneous systems are more desirable industrial perspective due their ease use enhanced durability. Supporting electrode surfaces is therefore promising approach for next generation electrocatalysts that retain level control interfacial environments. This review first cover key principles natural systems, such as hydrogenase enzymes, then survey some representative examples synthetic homogeneous hydrogen evolution incorporate these features. We discuss species have been supported materials, with focus recent advances field, major challenges remain.

Language: Английский

Citations

1
Crowding for Confinement: Reversible Isomerization of First-Generation Donor-Acceptor Stenhouse Adduct Derivatives in Water Modulated by Thermoresponsive Dendritic Macromolecules DOI Creative Commons
Jiaxing Zhang,

Qinqin Ma,

Huan Wang

et al.

Molecules, Journal Year: 2024, Volume and Issue: 29(21), P. 5055 - 5055

Published: Oct. 26, 2024

Mimicking nature, the reversible isomerization of hydrophobic dyes in aqueous solutions is appealing for bio-applications. Here, we report on first-generation solvatochromic donor-acceptor Stenhouse adducts (DASAs) water within dendritic matrices, realized either through dendronization DASAs or incorporation DASA pendants into dendronized copolymers. These macromolecules contain three-fold oligoethylene glycols (OEGs), which afford water-solubility and unprecedented thermoresponsive behavior. The behavior both copolymers dominated by peripherals OEGs. However, hydrophilicity acceptor from moieties also play a role mediating their thermal phase transitions, more importantly, tailor interactions between OEGs moieties. Intriguingly, topologies contribute confinement to encapsulate crowding effects, cooperative crowded modulate with different media. thermally induced collapse OEGs, accompanied aggregation macromolecules, leads formation domains, exert enhanced effects efficiently Compared low molar mass DASAs, collapsed can retard hydration cooperation neighboring better confined microenvironments mediate recovery up 90% cyclic charged (hydrophilic) state noncharged (hydrophobic) linear water. This exhibits excellent fatigue resistance after several cycles alternating photo-irradiation annealing at elevated temperatures.

Language: Английский

Citations

1
Electrocatalytic hydrogen evolution reaction with a Cu porphyrin bearing meso-CF3 substituents DOI

Wenzi Li,

Xinyang Peng,

Haonan Qin

et al.

Dalton Transactions, Journal Year: 2024, Volume and Issue: 53(48), P. 19121 - 19125

Published: Jan. 1, 2024

A Cu porphyrin bearing four meso -CF 3 substituents is synthesized and displays higher activity than reported porphyrins for the electrocatalytic hydrogen evolution reaction.

Language: Английский

Citations

1
A Molecular Catalyst‐Driven Sustainable Zinc‐Air Battery Assembly DOI Open Access
Sukanta Saha, Sampurna Mitra, Yashwant Pratap Kharwar

et al.

Small, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 5, 2024

Bidirectional oxygen reduction reaction (ORR) and evolution (OER) electrocatalysts are key for molecular oxygen-centric renewable energy transduction via metal-air batteries. Here, a cobalt complex is covalently tethered on strategically functionalized silica surface that displayed both ORR OER in alkaline media. The detailed X-ray absorbance spectroscopy (XAS) studies indicate this catalyst retains its intrinsic features while playing central role during bidirectional electrocatalysis demonstrating relatively lower gap between O

Language: Английский

Citations

0