Designing a Built-In Electric Field for Efficient Energy Electrocatalysis

ACS Nano, Journal Year: 2022, Volume and Issue: 16(12), P. 19959 - 19979

Published: Dec. 15, 2022

To utilize intermittent renewable energy as well achieve the goals of peak carbon dioxide emissions and neutrality, various electrocatalytic devices have been developed. However, reactions, e.g., hydrogen evolution reaction/oxygen reaction in overall water splitting, polysulfide conversion lithium–sulfur batteries, formation/decomposition lithium peroxide lithium–oxygen nitrate reduction to degrade sewage, suffer from sluggish kinetics caused by multielectron transfer processes. Owing merits accelerated charge transport, optimized adsorption/desorption intermediates, raised conductivity, regulation microenvironment, ease combine with geometric characteristics, built-in electric field (BIEF) is expected overcome above problems. Here, we give a Review about very recent progress BIEF for efficient electrocatalysis. First, construction strategies characterization methods (qualitative quantitative analysis) are summarized. Then, up-to-date overviews engineering electrocatalysis, attention on electron structure optimization microenvironment modulation, analyzed discussed detail. In end, challenges perspectives proposed. This gives deep understanding design electrocatalysts next-generation storage devices.

Language: Английский

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Enabling Internal Electric Fields to Enhance Energy and Environmental Catalysis

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(11)

Published: Jan. 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.

Language: Английский

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Mo‐Modified ZnIn₂S₄@NiTiO₃ S‐Scheme Heterojunction with Enhanced Interfacial Electric Field for Efficient Visible‐Light‐Driven Hydrogen Evolution

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(15)

Published: Feb. 26, 2023

Abstract Designing and developing visible‐light‐responsive materials for solar to chemical energy is an efficient promising approach green sustainable carbon‐neutral systems. Herein, a facile in situ growth hydrothermal strategy using Mo‐modified ZnIn 2 S 4 (Mo‐ZIS) nanosheets coupled with NiTiO 3 (NTO) microrods synthesize multifunctional ZIS wrapped NTO (Mo‐ZIS@NTO) photocatalyst enhanced interfacial electric field (IEF) effect typical S‐scheme heterojunction reported. Mo‐ZIS@NTO catalyst possesses wide‐spectrum light absorption properties, excellent visible light‐to‐thermal effect, electron mobility, charges transfer, strong IEF exhibits solar‐to‐chemical conversion visible‐light‐driven photocatalytic hydrogen evolution. Notably, the engineered Mo 1.4 ‐ZIS@NTO superior performance H evolution rate of up 14.06 mmol g −1 h − 1 apparent quantum efficiency 44.1% at 420 nm. The scientific explorations provide in‐depth understanding microstructure, heterojunction, IEF, Mo‐dopant facilitation effect. Moreover, theoretical simulations verify critical role element promoting adsorption activation O molecules, modulating behavior on active sites, thus accelerating overall catalytic efficiency. mechanism via adjustable regulation over also demonstrated.

Language: Английский

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Optimizing Electrocatalytic Nitrogen Reduction via Interfacial Electric Field Modulation: Elevating d‐Band Center in WS₂‐WO₃ for Enhanced Intermediate Adsorption

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(29)

Published: May 25, 2023

Electrocatalytic nitrogen reduction reaction (ENRR) has emerged as a promising approach to synthesizing green ammonia under ambient conditions. Tungsten (W) is one of the most effective ENRR catalysts. In this reaction, protonation intermediates rate-determining step (RDS). Enhancing adsorption crucial increase intermediates, which can lead improved catalytic performance. Herein, we constructed strong interfacial electric field in WS2 -WO3 elevate d-band center W, thereby strengthening intermediates. Experimental results demonstrated that led significantly Specifically, exhibited high NH3 yield 62.38 μg h-1 mgcat-1 and promoted faraday efficiency (FE) 24.24 %. Furthermore, situ characterizations theoretical calculations showed upshifted W towards Fermi level, leading enhanced -NH2 -NH on catalyst surface. This resulted rate RDS. Overall, our study offers new insights into relationship between provides strategy enhance during process.

Language: Английский

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Tunable Built‐In Electric Field in Ru Nanoclusters‐Based Electrocatalyst Boosts Water Splitting and Simulated Seawater Electrolysis

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(7)

Published: Oct. 31, 2023

Abstract The development of bifunctional electrocatalysts suitable for a wide pH range and seawater splitting under simulated industrial electrolysis conditions is expected to advance practical applications clean hydrogen energy. Here, the study reports built‐in electric field approach assemble heterogeneous Ru nanoclusters (Ru NCs) anchored in P,O co‐doped NiFe layered double hydroxide NCs/P,O‐NiFe LDH) overall water splitting. It revealed that BEF ensures electron enrichment via unidirectional transfer from P,O‐NiFe LDH due difference corresponding Fermi levels. optimized LDH/NF shows excellent electrocatalytic activity toward evolution reaction, oxygen range, as well industry‐relevant conditions. long‐term catalyst stability high currents process temperatures also demonstrated. Density functional theory calculations further confirm active sites at interface effectively reduce energy barrier electrolysis, thereby facilitating processes.

Language: Английский

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Tailoring the d‐Band Center over Isomorphism Pyrite Catalyst for Optimized Intrinsic Affinity to Intermediates in Lithium–Oxygen Batteries

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(15)

Published: Feb. 15, 2023

Abstract Rechargeable lithium–oxygen batteries (LOBs) are regarded as one of the most promising candidates for next generation energy storage devices. Nevertheless, lack understanding relationships between structure, property, and performance catalysts limits rational development efficient cathode catalysts, therefore, hinders commercial application LOBs. Herein, a d‐band center regulation strategy is proposed to construct an isomorphism composite NiS 2 ‐CoS @nitrogen‐doped carbon (NiS @NC) advanced catalyst boosting electrocatalytic activities Density functional theory calculations reveal that introduction Ni atoms not only redistributes internal charges on structure but also modulates adsorption capacities intermediates by tuning center, thus promoting oxygen reduction reaction/oxygen evolution reaction kinetics reducing overpotentials. As expected, @NC catalyzed LOBs present superior electrochemical including large initial discharge/charge specific capacity 14 551/13 563 mAh g −1 , ultralong cycle life over 490 cycles at current density 500 mA excellent rate performance. The insight into tailoring its facilitates construction electrocatalysts other systems.

Language: Английский

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Solvation Structure with Enhanced Anionic Coordination for Stable Anodes in Lithium‐Oxygen Batteries

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(30)

Published: June 7, 2023

Li-O2 batteries have garnered much attention due to their high theoretical energy density. However, the irreversible lithium plating/stripping on anode limits performance, which has been paid little attention. Herein, a solvation-regulated strategy for stable anodes in tetraethylene glycol dimethyl ether (G4) based electrolyte is attempted batteries. Trifluoroacetate anions (TFA- ) with strong Li+ affinity are incorporated into bis(fluorosulfonyl)imide (LiTFSI)/G4 attenuate -G4 interaction and form anion-dominant solvates. The bisalt 0.5 M LiTFA LiTFSI mitigates G4 decomposition induces an inorganic-rich solid interphase (SEI). This contributes decreased desolvation barrier from 58.20 46.31 kJ mol-1 , compared 1.0 LiTFSI/G4, facile interfacial diffusion efficiency. It yields extended lifespan of 120 cycles battery limited Li (7 mAh cm-2 ). work gains comprehensive insights rational design

Language: Английский

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Engineering the Electronic Interaction between Atomically Dispersed Fe and RuO ₂ Attaining High Catalytic Activity and Durability Catalyst for Li‐O ₂ Battery

Advanced Science, Journal Year: 2023, Volume and Issue: 10(9)

Published: Jan. 22, 2023

Abstract It is significant to develop catalysts with high catalytic activity and durability improve the electrochemical performances of lithium‐oxygen batteries (LOBs). While electronic metal‐support interaction (EMSI) between metal atoms support has shown great potential in field. Hence, effectively performance LOBs, atomically dispersed Fe modified RuO 2 nanoparticles are designed be loaded on hierarchical porous carbon shells (Fe SA ‐RuO /HPCS) based EMSI criterion. revealed that Ru‐O‐Fe 1 structure formed surrounding Ru sites through electron interaction, this could act as ultra‐high driving force center oxygen reduction/evolution reaction (ORR/OER). Specifically, enhances kinetics ORR a certain extent, optimizes morphology discharge products by reducing adsorption energy catalyst for O LiO ; while during OER process, not only greatly OER, but also catalyzes efficient decomposition Li favorable transfer active products. LOBs FeSA‐RuO /HPCS cathodes show an ultra‐low over‐potential, capacity superior durability.

Language: Английский

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Complementary Weaknesses: A Win‐Win Approach for rGO/CdS to Improve the Energy Conversion Performance of Integrated Photorechargeable Li−S Batteries

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(22)

Published: March 15, 2024

Integrating solar energy into rechargeable battery systems represents a significant advancement towards sustainable storage solutions. Herein, we propose win-win solution to reduce the shuttle effect of polysulfide and improve photocorrosion stability CdS, thereby enhancing conversion efficiency rGO/CdS-based photorechargeable integrated lithium-sulfur batteries (PRLSBs). Experimental results show that CdS can effectively anchor under sunlight irradiation for 20 minutes. Under high current density (1 C), discharge-specific capacity PRLSBs increased 971.30 mAh g

Language: Английский

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Field-assisted metal-air batteries: Recent progress, mechanisms, and challenges

Nano Energy, Journal Year: 2024, Volume and Issue: 125, P. 109550 - 109550

Published: March 28, 2024

Language: Английский

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