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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Solvent Engineering of Oxygen‐Enriched Carbon Dots for Efficient Electrochemical Hydrogen Peroxide Production

Small, Journal Year: 2023, Volume and Issue: 19(43)

Published: June 27, 2023

The development of cost-effective and reliable metal-free carbon-based electrocatalysts has gained significant attention for electrochemical hydrogen peroxide (H2 O2 ) generation through a two-electron oxygen reduction reaction. In this study, scalable solvent engineering strategy is employed to fabricate oxygen-doped carbon dots (O-CDs) that exhibit excellent performance as electrocatalysts. By adjusting the ratio ethanol acetone solvents during synthesis, surface electronic structure resulting O-CDs can be systematically tuned. amount edge active CO group was strongly correlated with selectivity activity O-CDs. optimum O-CDs-3 exhibited extraordinary H2 up 96.55% (n = 2.06) at 0.65 V (vs RHE) achieved remarkably low Tafel plot 64.8 mV dec-1 . Furthermore, realistic productivity yield flow cell measured high 111.18 mg h-1 cm-2 duration 10 h. findings highlight potential universal approach enabling electrocatalytic materials improved performance. Further studies will undertaken explore practical implications advancing field electrocatalysis.

Language: Английский

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Advances on Axial Coordination Design of Single-Atom Catalysts for Energy Electrocatalysis: A Review

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 15(1)

Published: Oct. 13, 2023

Abstract Single-atom catalysts (SACs) have garnered increasingly growing attention in renewable energy scenarios, especially electrocatalysis due to their unique high efficiency of atom utilization and flexible electronic structure adjustability. The intensive efforts towards the rational design synthesis SACs with versatile local configurations significantly accelerated development efficient sustainable electrocatalysts for a wide range electrochemical applications. As an emergent coordination avenue, intentionally breaking planar symmetry by adding ligands axial direction metal single atoms offers novel approach tuning both geometric structures, thereby enhancing electrocatalytic performance at active sites. In this review, we briefly outline burgeoning research topic axially coordinated provide comprehensive summary recent advances synthetic strategies Besides, challenges outlooks field also been emphasized. present review provides in-depth understanding SACs, which could bring new perspectives solutions fine regulation structures catering high-performing electrocatalysis.

Language: Английский

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Review and perspectives on carbon-based electrocatalysts for the production of H₂O₂via two-electron oxygen reduction

Green Chemistry, Journal Year: 2023, Volume and Issue: 25(23), P. 9501 - 9542

Published: Jan. 1, 2023

As a versatile and environmentally friendly chemical, hydrogen peroxide (H 2 O ) is in high demand.

Language: Английский

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Phase Engineering of High‐Entropy Alloy for Enhanced Electrocatalytic Nitrate Reduction to Ammonia

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(35)

Published: May 4, 2024

Abstract Directly electrochemical conversion of nitrate (NO 3 − ) is an efficient and environmentally friendly technology for ammonia (NH production but challenged by highly selective electrocatalysts. High‐entropy alloys (HEAs) with unique properties are attractive materials in catalysis, particularly multi‐step reactions. Herein, we first reported the application HEA (FeCoNiAlTi) electrocatalytic NO reduction to NH (NRA). The bulk active NRA limited unsatisfied yield 0.36 mg h −1 cm −2 Faradaic efficiency (FE) 82.66 %. Through effective phase engineering strategy, uniform intermetallic nanoparticles introduced on increase surface area charge transfer efficiency. resulting nanostructured (n‐HEA) delivers enhanced performance terms (0.52 FE (95.23 %). Further experimental theoretical investigations reveal that multi‐active sites (Fe, Co, Ni) dominated electrocatalysis over n‐HEA. Notably, typical Co exhibit lowest energy barrier *NH 2 as rate‐determining step.

Language: Английский

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Metal-free carbon-based catalysts design for oxygen reduction reaction towards hydrogen peroxide: From 3D to 0D

Materials Today, Journal Year: 2023, Volume and Issue: 63, P. 339 - 359

Published: Feb. 26, 2023

Language: Английский

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Anthraquinone centers modified covalent organic frameworks for boosted photocatalytic O2-to-H2O2 synthesis: Inhibiting the in-situ decomposition of H2O2

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 481, P. 148494 - 148494

Published: Jan. 4, 2024

Language: Английский

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Isomerization Engineering of Oxygen‐Enriched Carbon Quantum Dots for Efficient Electrochemical Hydrogen Peroxide Production

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

Published: May 7, 2024

Abstract Hydrogen peroxide (H 2 O ) has emerged as a kind of multi‐functional green oxidants with extensive industrial utility. Oxidized carbon materials exhibit promises electrocatalysts in the two‐electron (2e − oxygen reduction reaction (ORR) for H production. However, precise identification and fabrication active sites that selectively yield present serious challenge. Herein, structural engineering strategy is employed to synthesize oxygen‐doped quantum dots (o‐CQD) 2e ORR. The surface electronic structure o‐CQDs systematically modulated by varying isomerization precursors, thereby demonstrating excellent electrocatalyst performance. Notably, o‐CQD‐3 emerges most promising candidate, showcasing remarkable selectivity 96.2% (n = 2.07) at 0.68 V versus RHE, coupled low Tafel diagram 66.95 mV dec −1 . In flow cell configuration, achieves productivity 338.7 mmol g catalyst h , maintaining consistent production stability over an impressive 120‐hour duration. Utilizing situ technology density functional theory calculations, it unveil edge are facilely functionalized C‐O‐C groups under alkaline ORR conditions. This approach advances forefront sustainable catalysis provides profound insight into carbon‐based design environmental‐friendly chemical synthesis processes.

Language: Английский

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Unveiling Favorable Microenvironment on Porous Doped Carbon Nanosheets for Superior H₂O₂ Electrosynthesis in Neutral Media

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(19)

Published: Feb. 21, 2024

Abstract Designing effective electrocatalysts tailored for targeted reactions requires fundamental insights into the structure dependence of reaction microenvironment. Herein, inspired by finite element simulations, N,O co‐doped carbon nanosheets featuring a hierarchical micro/mesoporous to form an oxygen‐rich and local alkaline‐like microenvironment two‐electron oxygen reduction (2e − ORR) in neutral medium are designed. The situ ex test results confirmed that architecture can elevate pH accelerate generation intermediates (*O 2 , *OOH), leading high‐efficiency H O production. Utilizing this favorable microenvironment, N,O‐CNS 0.5 demonstrated exceptional electrosynthesis performance media, achieving superior yield rate (6705 mmol g catalyst −1 h flow cell). Additionally, comparative experiments density‐functional theory calculations provided confirmation bi‐doping N as active origin responsible electrochemical 2e ORR. This study synergistically manipulates sites, providing opportunity efficient electro‐production medium.

Language: Английский

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Efficient Neutral H2O2 Electrosynthesis from Favorable Reaction Microenvironments via Porous Carbon Carrier Engineering

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(32)

Published: May 20, 2024

The efficient electrosynthesis of hydrogen peroxide (H

Language: Английский

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