MOF-derived CoP-nitrogen-doped carbon@NiFeP nanoflakes as an efficient and durable electrocatalyst with multiple catalytically active sites for OER, HER, ORR and rechargeable zinc-air batteries

Chemical Engineering Journal, Journal Year: 2021, Volume and Issue: 428, P. 131115 - 131115

Published: July 5, 2021

Language: Английский

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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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Functional Carbon Nitride Materials in Photo‐Fenton‐Like Catalysis for Environmental Remediation

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 32(24)

Published: May 12, 2022

Abstract Among various advanced oxidation processes, coupled photocatalysis and heterogeneous Fenton‐like catalysis (known as photo‐Fenton‐like catalysis) to generate highly reactive species for environmental remediation has attracted wide interests. As an emerging metal‐free photocatalyst, graphitic carbon nitride (g‐C 3 N 4 , CN) been recently recognized a promising candidate catalyze robustly reactions wastewater remediation. This review summarizes recent progress in fabricating types of CN‐based catalysts the reaction process. Innovative engineering strategies on CN matrix are outlined, ranging from morphology control, defect engineering, nonmetal atom doping, organic molecule doping modification by metal‐containing species. The catalytic activities loaded with auxiliary sub‐nanoscale (e.g., quantum dots, organometallic molecules, metal cations, single metals) nanoscale metal‐based materials critically evaluated. Hybridization bandgap‐matching semiconductors construction type‐II Z‐scheme heterojunctions also examined. critical factors morphology, dimensionality, light absorption, charge excitation/migration, sites, H 2 O generation activation) that determine performance photocatalysts systematically discussed. After examining structure–activity relationship, research perspectives proposed further development toward more efficient their application practical water treatment.

Language: Английский

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A Pentagonal Defect-Rich Metal-Free Carbon Electrocatalyst for Boosting Acidic O₂ Reduction to H₂O₂ Production

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: unknown

Published: May 9, 2023

Metal-free carbon-based materials are considered one of the most promising two-electron oxygen reduction reaction (2e– ORR) electrocatalysts for green synthesis hydrogen peroxide (H2O2). However, reported carbon perform much more effectively in alkalis than acids. Herein, by creatively using fullerene (C60) as precursor subject to ammonia treatment, we designed and synthesized a pentagonal defect-rich nitrogen-doped nanomaterial (PD/N–C). It achieves outstanding ORR activity, 2e– selectivity, stability acidic electrolytes, surpassing benchmark PtHg4 alloy catalyst. Impressively, flow cell based on PD/N–C catalyst nearly 100% Faraday efficiency with remarkable H2O2 yield, representing best improvement among all metal-free catalysts. Experimental theoretical results reveal that such superb performance originates from synergism between defects nitrogen dopants. This work presents an effective strategy design construction highly efficient acid-resistant production beyond.

Language: Английский

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High‐Loading Co Single Atoms and Clusters Active Sites toward Enhanced Electrocatalysis of Oxygen Reduction Reaction for High‐Performance Zn–Air Battery

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 33(4)

Published: Nov. 18, 2022

Abstract The development of precious‐metal alternative electrocatalysts for oxygen reduction reaction (ORR) is highly desired a variety fuel cells, and single atom catalysts (SACs) have been envisaged to be the promising choice. However, there remains challenges in synthesis high metal loading SACs (>5 wt.%), thus limiting their electrocatalytic performance. Herein, facile self‐sacrificing template strategy developed fabricating Co atoms along with atomic clusters co‐anchored on porous‐rich nitrogen‐doped graphene (Co SAs/AC@NG), which implemented by pyrolysis dicyandiamide formation layered g‐C 3 N 4 as sacrificed templates, providing rich anchoring sites achieve up 14.0 wt.% SAs/AC@NG. Experiments combined density functional theory calculations reveal that co‐existence underlying nitrogen doped carbon optimized 40 SAs/AC@NG synergistically contributes enhanced electrocatalysis ORR, outperforms state‐of‐the‐art Pt/C presenting half‐wave potential ( E 1/2 = 0.890 V) robust long‐term stability. Moreover, presents excellent performance Zn–air battery high‐peak power (221 mW cm −2 ) strong cycling stability, demonstrating great energy storage applications.

Language: Английский

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FeCo alloy entrapped in N-doped graphitic carbon nanotubes-on-nanosheets prepared by coordination-induced pyrolysis for oxygen reduction reaction and rechargeable Zn-air battery

Journal of Colloid and Interface Science, Journal Year: 2023, Volume and Issue: 639, P. 424 - 433

Published: Feb. 15, 2023

Language: Английский

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Nitrogen‐Rich Carbonaceous Materials for Advanced Oxygen Electrocatalysis: Synthesis, Characterization, and Activity of Nitrogen Sites

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 32(31)

Published: May 31, 2022

Abstract Nitrogen‐doped carbons are among the fastest‐growing class of materials used for oxygen electrocatalysis, namely, reduction reaction (ORR) and evolution (OER), thanks to their low cost, environmental friendliness, excellent electrical conductivity, scalable synthesis. The perspective replacing precious metal‐based electrocatalysts with nitrogen‐doped carbon is highly desirable reducing costs in energy conversion storage systems. In this review, role nitrogen N‐induced structural defects on enhanced performance N‐doped toward OER ORR as well applications technologies summarized. synthesis characterization functional groups active sites also reviewed. electrocatalytic main types OER/ORR electrocatalysis then discussed. Finally, major challenges future opportunities advanced highlighted.

Language: Английский

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Metal‐Free Carbon‐Based Covalent Organic Frameworks with Heteroatom‐Free Units Boost Efficient Oxygen Reduction

Advanced Materials, Journal Year: 2022, Volume and Issue: 35(7)

Published: Nov. 25, 2022

Accurate identification of carbon-based metal-free electrocatalyst (CMFE) activity and enhancing their catalytic efficiency for O2 conversion is an urgent challenging task. This study reports a promising strategy to simultaneously develop series covalent organic frameworks (COFs) with well-defined heterocyclic-free biphenyl or fluorenyl units. Unlike heteroatom doping, the developed method not only supplies methyl-induced molecular configuration promote activity, but also provides direct opportunity identify heteroatom-free carbon active centers. The introduction methyl groups (MGs) reversible valence bonds into pristine biphenyl-based COF results in excellent performance half-wave potential 0.74 V versus hydrogen electrode (RHE), which among highest values CMFE-COFs as oxygen reduction reaction (ORR) electrocatalysts. Combined situ Raman spectra theoretical calculations, MG-bound skeleton (DAF-COF) found produce ortho activation, confirming (site-5) adjacent MGs may be attributed opening binding MGs, effectively regulate charge redistribution, well improve transfer reduce energy barrier. insight design highly efficient electrocatalysts via regulation bonds.

Language: Английский

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Intermetallic Nanocrystals for Fuel-Cells-Based Electrocatalysis

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(22), P. 12507 - 12593

Published: Nov. 1, 2023

Electrocatalysis underpins the renewable electrochemical conversions for sustainability, which further replies on metallic nanocrystals as vital electrocatalysts. Intermetallic have been known to show distinct properties compared their disordered counterparts, and long explored functional improvements. Tremendous progresses made in past few years, with notable trend of more precise engineering down an atomic level investigation transferring into practical membrane electrode assembly (MEA), motivates this timely review. After addressing basic thermodynamic kinetic fundamentals, we discuss classic latest synthetic strategies that enable not only formation intermetallic phase but also rational control other catalysis-determinant structural parameters, such size morphology. We demonstrate emerging nanomaterials potentially advancement energy electrocatalysis. Then, state-of-the-art characterizations representative electrocatalysts emphasis oxygen reduction reaction evaluated a MEA setup. summarize review by laying out existing challenges offering perspective future research directions toward practicing conversions.

Language: Английский

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Steering the oxygen reduction reaction pathways of N-carbon hollow spheres by heteroatom doping

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 327, P. 122470 - 122470

Published: Feb. 13, 2023

Language: Английский

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