Water electrolysis

Nature Reviews Methods Primers, Journal Year: 2022, Volume and Issue: 2(1)

Published: Oct. 27, 2022

Language: Английский

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Theoretical Advances in Understanding and Designing the Active Sites for Hydrogen Evolution Reaction

ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(14), P. 8404 - 8433

Published: June 30, 2022

As a fundamental step of water splitting and stepping stone toward exploring other multielectron transfer processes, the electrocatalytic hydrogen evolution reaction (HER) is an ideal model for both understanding electrocatalyst design. Here, we review fundamentals recent developments theoretical insights into HER, covering mechanistic aspects, key activity descriptors, local environment considerations, advances beyond computational electrode. Although it experimentally challenging to explore active sites mechanisms in process, show great potential identifying mechanisms. In this Review, especially focus depth on revealing designing HER. Major challenges ahead will also be discussed at end Review.

Language: Английский

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TURBOMOLE: Today and Tomorrow

Journal of Chemical Theory and Computation, Journal Year: 2023, Volume and Issue: 19(20), P. 6859 - 6890

Published: June 29, 2023

TURBOMOLE is a highly optimized software suite for large-scale quantum-chemical and materials science simulations of molecules, clusters, extended systems, periodic solids. uses Gaussian basis sets has been designed with robust fast applications in mind, ranging from homogeneous heterogeneous catalysis to inorganic organic chemistry various types spectroscopy, light-matter interactions, biochemistry. This Perspective briefly surveys TURBOMOLE's functionality highlights recent developments that have taken place between 2020 2023, comprising new electronic structure methods molecules solids, previously unavailable molecular properties, embedding, dynamics approaches. Select features under development are reviewed illustrate the continuous growth program suite, including nuclear orbital methods, Hartree-Fock-based adiabatic connection models, simplified time-dependent density functional theory, relativistic effects magnetic multiscale modeling optical properties.

Language: Английский

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Local reaction environment in electrocatalysis

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(4), P. 2022 - 2055

Published: Jan. 1, 2024

Beyond conventional electrocatalyst engineering, recent studies have unveiled the effectiveness of manipulating local reaction environment in enhancing performance electrocatalytic reactions. The general principles and strategies environmental engineering for different processes been extensively investigated. This review provides a critical appraisal advancements aiming to comprehensively assess this emerging field. It presents interactions among surface structure, ions distribution electric field relation environment. Useful protocols such as interfacial reactant concentration, mass transport rate, adsorption/desorption behaviors, binding energy are in-depth discussed toward modifying Meanwhile, electrode physical structures cell configurations viable optimization methods environments. In combination with

Language: Английский

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Different distributions of multi-carbon products in CO2 and CO electroreduction under practical reaction conditions

Nature Catalysis, Journal Year: 2023, Volume and Issue: 6(12), P. 1115 - 1124

Published: Dec. 20, 2023

Language: Английский

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Electrochemical Potential-Driven Shift of Frontier Orbitals in M–N–C Single-Atom Catalysts Leading to Inverted Adsorption Energies

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(46), P. 25264 - 25273

Published: Nov. 8, 2023

Electronic structure is essential to understanding the catalytic mechanism of metal single-atom catalysts (SACs), especially under electrochemical conditions. This study delves into nuanced modulation "frontier orbitals" in SACs on nitrogen-doped graphene (N-C) substrates by potentials. We observe shifts Fermi level and changes d-orbital occupation with alterations potentials, emphasizing a synergy between discretized atomic orbitals metals continuous bands N-C based environment. Using O2 CO2 as model adsorbates, we highlight direct consequences these adsorption energies, unveiling an intriguing inversion energies Co/N-C SAC negative Such insights are attributed role dxz dz2 orbitals, pivotal for stabilizing π* O2. Through this exploration, our work offers interplay electronic structures behaviors SACs, paving way enhanced catalyst design strategies processes.

Language: Английский

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Mechanism of Cations Suppressing Proton Diffusion Kinetics for Electrocatalysis

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(14)

Published: Feb. 10, 2023

Proton transfer is crucial for electrocatalysis. Accumulating cations at electrochemical interfaces can alter the proton rate and then tune electrocatalytic performance. However, mechanism regulating remains ambiguous. Here, we quantify cation effect on diffusion in solution by hydrogen evolution microelectrodes, revealing be suppressed more than 10 times. Different from prevalent opinions that transport slowed down modified electric field, found water structure imposes a evident kinetics. FTIR test path integral molecular dynamics simulation indicate prefers to wander within hydration shell of rather hop rapidly along wires. Low connectivity networks disrupted corrupts fast-moving bulk water. This study highlights promising way kinetics via structure.

Language: Английский

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Electric Double Layer Effects in Electrocatalysis: Insights from Ab Initio Simulation and Hierarchical Continuum Modeling

JACS Au, Journal Year: 2023, Volume and Issue: 3(10), P. 2640 - 2659

Published: Sept. 18, 2023

Structures of the electric double layer (EDL) at electrocatalytic interfaces, which are modulated by material properties, electrolyte characteristics (e.g., pH, types and concentrations ions), electrode potential, play crucial roles in reaction kinetics. Understanding EDL effects electrocatalysis has attracted substantial research interest recent years. However, intrinsic relationships between specific structures kinetics remain poorly understood, especially on atomic scale. In this Perspective, we briefly review advances deciphering mainly hydrogen oxygen through a multiscale approach, spanning from atomistic scale simulated ab initio methods to macroscale hierarchical approach. We highlight importance resolving local environment, bond network, understanding effects. Finally, some remaining challenges outlined, an outlook for future developments these exciting frontiers is provided.

Language: Английский

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Key Roles of Interfacial OH⁻ ion Distribution on Proton Coupled Electron Transfer Kinetics Toward Urea Oxidation Reaction

Small, Journal Year: 2023, Volume and Issue: 19(30)

Published: May 16, 2023

Enhancing alkaline urea oxidation reaction (UOR) activity is essential to upgrade renewable electrolysis systems. As a core step of UOR, proton-coupled electron transfer (PCET) determines the overall performance, and accelerating its kinetic remains challenge. In this work, newly raised electrocatalyst NiCoMoCuOx Hy with derived multi-metal co-doping (oxy)hydroxide species during electrochemical states reported, which ensures considerable UOR (10/500 mA cm-2 at 1.32/1.52 V vs RHE, respectively). Impressively, comprehensive studies elucidate correlation between electrode-electrolyte interfacial microenvironment electrocatalytic behavior. Specifically, featured dendritic nanostructure creates strengthened electric field distribution. This structural factor prompts local OH- enrichment in electrical double layer (EDL), so that dehydrogenative catalyst directly reinforced facilitate subsequent PCET kinetics nucleophilic urea, resulting high performance. practical utilization, -driven coupled cathodic hydrogen evolution (HER) carbon dioxide reduction (CO2 RR), harvested value-added products H2 C2 H4 , respectively. work clarifies novel mechanism improve performance through structure-induced modulation.

Language: Английский

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Electrochemically Driven Hydrogen Atom Transfer Catalysis: A Tool for C(sp³)/Si–H Functionalization and Hydrofunctionalization of Alkenes

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(13), P. 8731 - 8751

Published: June 16, 2023

Electrochemically driven hydrogen atom transfer (HAT) catalysis provides a complementary approach for the transformation of redox-inactive substrates that would be inaccessible to conventional electron (ET) catalysis. Moreover, electrochemically HAT could promote organic transformations with either abstraction or donation as key step. It versatile and effective tool direct functionalization C(sp3)–H/Si–H bonds hydrofunctionalization alkenes. Despite these attractive properties, has been largely overlooked due lack understanding both catalytic mechanism how catalyst selection should occur. In this Review, we give an overview applications in The mechanistic pathways, physical properties mediators, state-of-the-art examples are described discussed.

Language: Английский

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