Density Functional Theory for Electrocatalysis

Energy & environment materials, Год журнала: 2021, Номер 5(1), С. 157 - 185

Опубликована: Апрель 27, 2021

It is a considerably promising strategy to produce fuels and high‐value chemicals through an electrochemical conversion process in the green sustainable energy systems. Catalysts for electrocatalytic reactions, including hydrogen evolution reaction (HER), oxygen (OER), reduction (ORR), nitrogen (NRR), carbon dioxide (CO 2 RR), play significant role advanced technologies, such as water splitting devices, fuel cells, rechargeable metal‐air batteries. Developing low‐cost highly efficient electrocatalysts closely related establishing composition–structure–activity relationships fundamental understanding of catalytic mechanisms. Density functional theory (DFT) emerging important computational tool that can provide insights into relationship between performances physical/chemical properties catalysts. This article presents review on progress DFT, simulations, within framework processes, well designs virtual screenings new electrocatalysts. Some useful descriptors analysis tools evaluating are highlighted, formation energies, d ‐band model, scaling relation, e g orbital occupation, free energies adsorption. Furthermore, remaining questions perspectives development DFT electrocatalysis also proposed.

Язык: Английский

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Strategies for Designing High-Performance Hydrogen Evolution Reaction Electrocatalysts at Large Current Densities above 1000 mA cm^–2

ACS Nano, Год журнала: 2022, Номер 16(8), С. 11577 - 11597

Опубликована: Авг. 11, 2022

The depletion of fossil fuels and rapidly increasing environmental concerns have urgently called for the utilization clean sustainable sources future energy supplies. Hydrogen (H2) is recognized as a prioritized green resource with little impact to replace traditional fuels. Electrochemical water splitting has become an important method large-scale production hydrogen. hydrogen evolution reaction (HER) cathodic half-reaction that can be promoted produce pure H2 in large quantities by active electrocatalysts. However, unsatisfactory performance HER electrocatalysts cannot follow extensive requirements industrial-scale applications, including working efficiently stably over long periods time at high current densities (⩾1000 mA cm-2). In this review, we study crucial issues when work summarize several categories strategies design high-performance We also discuss challenges opportunities development catalysts.

Язык: Английский

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Design of a Multilayered Oxygen‐Evolution Electrode with High Catalytic Activity and Corrosion Resistance for Saline Water Splitting

Advanced Functional Materials, Год журнала: 2021, Номер 31(27)

Опубликована: Апрель 22, 2021

Abstract The realization of seawater electrolysis requires high‐performing anode materials that should possess good catalytic activity, stability, and specificity for the oxygen evolution reaction (OER) as well high resistance toward chloride corrosion. Herein, design a multilayered oxygen‐evolution electrode is reported to meet multiple needs material saline water splitting. synthesized through direct thermal boronization commercially available NiFe alloy plate with boron powder, followed by electrochemical oxidation. And this composed surface oxidized NiFeBx layer, interlayer, substrate. species are present in form metaborate outermost their existence conductive generation stabilization active phase γ‐(Ni,Fe)OOH. introduction interlayer effectively prevents excessive oxidative corrosion electrolyte containing ions.

Язык: Английский

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Decarboxylation‐Induced Defects in MOF‐Derived Single Cobalt Atom@Carbon Electrocatalysts for Efficient Oxygen Reduction

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(40), С. 21685 - 21690

Опубликована: Июль 31, 2021

Abstract Developing transition metal single‐atom catalysts (SACs) for oxygen reduction reaction (ORR) is of great importance. Zeolitic imidazolate frameworks (ZIFs) as a subgroup metal‐organic (MOFs) are distinguished SAC precursors, due to their large porosity and N content. However, the activity formed sites limited. Herein, we report decarboxylation‐induced defects strategy improve intrinsic via increasing defect density. Carboxylate/amide mixed‐linker MOF (DMOF) was chosen produce defective Co SACs (Co@DMOF) by gas‐transport species DMOF upon heating. Comparing with ZIF‐8 derived (Co@ZIF‐8‐900), Co@DMOF‐900 more yet one fifth content similar specific double‐layer capacitance show better ORR eight times higher turnover frequency (2.015 e s −1 site ). Quantum calculation confirms can weaken adsorption free energy OOH on further boost process.

Язык: Английский

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Advanced Oxygen Electrocatalysis in Energy Conversion and Storage

Advanced Functional Materials, Год журнала: 2020, Номер 31(12)

Опубликована: Окт. 29, 2020

Abstract Oxygen electrocatalysis is of great significance in electrochemical energy conversion and storage. Many strategies have been adopted for developing advanced oxygen electrocatalysts to promote these technologies. In this invited contribution, recent progress understanding the electrochemistry from theoretical experimental aspects summarized. The major categories electrocatalysts, namely, noble‐metal‐based compounds, transition‐metal‐based composites, nanocarbons, are successively discussed reduction evolution. Design various their relationship on structure–activity–performance comprehensively addressed with perspectives. Finally, challenge outlook toward storage

Язык: Английский

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Carbon-based bifunctional electrocatalysts for oxygen reduction and oxygen evolution reactions: Optimization strategies and mechanistic analysis

Journal of Energy Chemistry, Год журнала: 2022, Номер 71, С. 234 - 265

Опубликована: Март 25, 2022

Язык: Английский

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A Robust PtNi Nanoframe/N‐Doped Graphene Aerogel Electrocatalyst with Both High Activity and Stability

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(17), С. 9590 - 9597

Опубликована: Фев. 8, 2021

Abstract Insufficient catalytic activity and stability high cost are the barriers for Pt‐based electrocatalysts in wide practical applications. Herein, a hierarchically porous PtNi nanoframe/N‐doped graphene aerogel (PtNiNF‐NGA) electrocatalyst with outstanding performance toward methanol oxidation reaction (MOR) acid electrolyte has been developed via facile tert‐butanol‐assisted structure reconfiguration. The ensemble of high‐alloying‐degree‐modulated electronic correspondingly optimum MOR pathway, superiorities hierarchical porosity, thin edges, Pt‐rich corners, anchoring effect NGA, endow PtNiNF‐NGA both prominent electrocatalytic stability. mass specific (1647 mA mg Pt −1 , 3.8 cm −2 ) 5.8 7.8 times higher than those commercial Pt/C. It exhibits exceptional under 5‐hour chronoamperometry test 2200‐cycle cyclic voltammetry scanning.

Язык: Английский

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Multi‐Scale Design of Metal–Organic Framework‐Derived Materials for Energy Electrocatalysis

Advanced Energy Materials, Год журнала: 2021, Номер 12(4)

Опубликована: Янв. 18, 2021

Abstract The development of advanced energy conversion systems such as fuel cells and electrolyzers with desirable efficiency durability is great significance in order to power society a sustainable way, which highly depends on the fabrication electrocatalysts electrochemical performance. Multi‐scale design from atomic scale device‐scale crucial achieve optimal overall performance terms activity, selectivity, durability. Benefitting their diverse tunable structures compositions, metal–organic frameworks (MOFs) are promising platforms synthesize at multiple scales for electrocatalysis. Herein, fundamental principles recent progress multi‐scale MOF‐derived materials aspects active sites, interfaces, pore structures, morphologies summarized. Moreover, precise control these variables, meet requirements specific energy‐related reactions including oxygen reduction reaction, evolution hydrogen CO 2 reaction (CO RR), N critically discussed. Furthermore, challenges future research directions real‐world applications provided.

Язык: Английский

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Directional regulating dynamic equilibrium to continuously update electrocatalytic interface for oxygen evolution reaction

Chemical Engineering Journal, Год журнала: 2021, Номер 431, С. 134040 - 134040

Опубликована: Дек. 9, 2021

Язык: Английский

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Transition-Metal (Fe, Co, and Ni)-Based Nanofiber Electrocatalysts for Water Splitting

Advanced Fiber Materials, Год журнала: 2021, Номер 3(4), С. 210 - 228

Опубликована: Фев. 1, 2021

Язык: Английский

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