Ten concerns of Zn metal anode for rechargeable aqueous zinc batteries

Joule, Год журнала: 2023, Номер 7(6), С. 1145 - 1175

Опубликована: Июнь 1, 2023

Язык: Английский

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Boosting Oxygen Electrocatalytic Activity of Fe–N–C Catalysts by Phosphorus Incorporation

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(6), С. 3647 - 3655

Опубликована: Фев. 6, 2023

Nitrogen-doped graphitic carbon materials hosting single-atom iron (Fe-N-C) are major non-precious metal catalysts for the oxygen reduction reaction (ORR). The nitrogen-coordinated Fe sites described as first coordination sphere. As opposed to good performance in ORR, that evolution (OER) is extremely poor due sluggish O-O coupling process, thus hampering practical applications of rechargeable zinc (Zn)-air batteries. Herein, we succeed boosting OER activity Fe-N-C by additionally incorporating phosphorus atoms into second sphere, here denoted P/Fe-N-C. resulting material exhibits excellent 0.1 M KOH with an overpotential low 304 mV at a current density 10 mA cm-2. Even more importantly, they exhibit remarkably small ORR/OER potential gap 0.63 V. Theoretical calculations using first-principles functional theory suggest enhances electrocatalytic balancing *OOH/*O adsorption FeN4 sites. When used air cathode Zn-air battery, P/Fe-N-C delivers charge-discharge high peak power 269 mW cm-2, highlighting its role state-of-the-art bifunctional electrocatalyst.

Язык: Английский

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Long‐Range Interactions in Diatomic Catalysts Boosting Electrocatalysis

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(52)

Опубликована: Окт. 6, 2022

Abstract The simultaneous presence of two active metal centres in diatomic catalysts (DACs) leads to the occurrence specific interactions between sites. Such interactions, referred as long‐range (LRIs), play an important role determining rate and selectivity a reaction. optimal combination must be determined achieve targeted efficiency. To date, various types DACs have been synthesised applied electrochemistry. However, LRIs not systematically summarised. Herein, regulation, mechanism, electrocatalytic applications are comprehensively summarised discussed. In addition basic information above, challenges, opportunities, future development proposed order present overall view reference for research.

Язык: Английский

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High-Density Cobalt Single-Atom Catalysts for Enhanced Oxygen Evolution Reaction

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(14), С. 8052 - 8063

Опубликована: Март 30, 2023

Single atom catalysts (SACs) possess unique catalytic properties due to low-coordination and unsaturated active sites. However, the demonstrated performance of SACs is limited by low SAC loading, poor metal-support interactions, nonstable performance. Herein, we report a macromolecule-assisted synthesis approach that enabled us demonstrate high-density Co single atoms (10.6 wt % SAC) in pyridinic N-rich graphenic network. The highly porous carbon network (surface area ∼186 m2 g-1) with increased conjugation vicinal site decoration significantly enhanced electrocatalytic oxygen evolution reaction (OER) 1 M KOH (η10 at 351 mV; mass activity 2209 mA mgCo-1 1.65 V) more than 300 h stability. Operando X-ray absorption near-edge structure demonstrates formation electron-deficient Co-O coordination intermediates, accelerating OER kinetics. Density functional theory (DFT) calculations reveal facile electron transfer from cobalt species-accelerated OER.

Язык: Английский

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Tuning the spin state of Fe single atoms by Pd nanoclusters enables robust oxygen reduction with dissociative pathway

Chem, Год журнала: 2022, Номер 9(1), С. 181 - 197

Опубликована: Окт. 27, 2022

Язык: Английский

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Microenvironment Engineering of Single/Dual‐Atom Catalysts for Electrocatalytic Application

Advanced Materials, Год журнала: 2023, Номер 35(31)

Опубликована: Фев. 23, 2023

Single/dual-metal atoms supported on carbon matrix can be modulated by coordination structure and neighboring active sites. Precisely designing the geometric electronic uncovering structure-property relationships of single/dual-metal confront with grand challenges. Herein, this review summarizes latest progress in microenvironment engineering single/dual-atom sites via a comprehensive comparison single-atom catalyst (SACs) dual-atom catalysts (DACs) term design principles, modulation strategy, theoretical understanding structure-performance correlations. Subsequently, recent advances several typical electrocatalysis process are discussed to get general reaction mechanisms finely-tuned SACs DACs. Finally, full-scaled summaries challenges prospects given for This will provide new inspiration development atomically dispersed electrocatalytic application.

Язык: Английский

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Geminal-atom catalysis for cross-coupling

Nature, Год журнала: 2023, Номер 622(7984), С. 754 - 760

Опубликована: Сен. 20, 2023

Язык: Английский

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Multi-atom cluster catalysts for efficient electrocatalysis

Chemical Society Reviews, Год журнала: 2022, Номер 51(21), С. 8923 - 8956

Опубликована: Янв. 1, 2022

This review presents recent developments in the synthesis, modulation and characterization of multi-atom cluster catalysts for electrochemical energy applications.

Язык: Английский

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Challenges and Opportunities in Engineering the Electronic Structure of Single-Atom Catalysts

ACS Catalysis, Год журнала: 2023, Номер 13(5), С. 2981 - 2997

Опубликована: Фев. 14, 2023

Controlling the electronic structure of transition-metal single-atom heterogeneous catalysts (SACs) is crucial to unlocking their full potential. The ability do this with increasing precision offers a rational strategy optimize processes associated adsorption and activation reactive intermediates, charge transfer dynamics, light absorption. While several methods have been proposed alter characteristics SACs, such as oxidation state, band structure, orbital occupancy, spin, lack systematic approach application makes it difficult control effects. In Perspective, we examine how configuration SACs can be engineered for thermochemical, electrochemical, photochemical applications, exploring relationship activity, selectivity, stability. We discuss synthetic analytical challenges in controlling discriminating possible directions toward closing gap between computational experimental efforts. By bringing topic center, hope stimulate research understand, control, exploit effects ultimately spur technological developments.

Язык: Английский

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Inter‐Metal Interaction with a Threshold Effect in NiCu Dual‐Atom Catalysts for CO₂ Electroreduction

Advanced Materials, Год журнала: 2022, Номер 35(11)

Опубликована: Ноя. 26, 2022

Dual-atom catalysts (DACs) have become an emerging platform to provide more flexible active sites for electrocatalytic reactions with multi-electron/proton transfer, such as the CO2 reduction reaction (CRR). However, introduction of asymmetric dual-atom causes complexity in structure, leaving incomprehensive understanding inter-metal interaction and catalytic mechanism. Taking NiCu DACs example, herein, a rational structural model is proposed, distance-dependent investigated by combining theoretical simulations experiments, including density functional theory computation, aberration-corrected transmission electron microscopy, synchrotron-based X-ray absorption fine Monte Carlo experiments. A distance threshold around 5.3 Å between adjacent NiN4 CuN4 moieties revealed trigger effective electronic regulation boost CRR performance on both selectivity activity. universal macro-descriptor rigorously correlating intrinsic material features (e.g., metal loading thickness) established guide design synthesis advanced DACs. This study highlights significance identifying DACs, helps bridge gap experimental atomically dispersed highly correlated sites.

Язык: Английский

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