Defective-Engineered ZnO Encapsulated in N-Doped Carbon for Sustainable 2e^– ORR: Interfacial Zn–N Bond Regulated Oxygen Reduction Pathways

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(17), P. 12917 - 12927

Published: Aug. 13, 2024

Zinc oxide (ZnO), although known for its stability and safety, has shown limited catalytic activity in the two-electron oxygen reduction reaction (2e– ORR). In this context, we synthesized a robust defective-engineered ZnO/N-doped graphene heterojunction (ZnO-NG) featuring abundant Zn–N bonds at interface. The engineered composite exhibited remarkable H2O2 yield of 13.1 mg h–1 cm–2 25 mA with selectivity 85.0%, surpassing NG ZnO counterparts. Furthermore, exceptional long-term ZnO-NG was validated through chronoamperometric measurements 10 successive runs, highlighting great potential large-scale synthesis. Density functional theory calculations X-ray absorption near-edge structure analysis revealed that interfacial bridging N regulated local electron distribution, transferring unpaired electrons from Zn sites to adjacent N/C atoms. configuration facilitated hydrogenation step O2-to-OOH* more importantly inhibited O*-to–OH* conversion, thereby improving 2e– ORR toward water remediation.

Language: Английский

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Recent progress on graphene nanoribbon-based electrocatalysts for oxygen reduction reaction

Current Opinion in Electrochemistry, Journal Year: 2024, Volume and Issue: 47, P. 101554 - 101554

Published: June 13, 2024

Language: Английский

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Hydrogenated Pyridine‐Pyrrole Nitrogen‐Doped Carbon for High‐Efficiency Electrosynthesis of Hydrogen Peroxide in NaCl Electrolyte

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 26, 2024

Abstract Developing metal‐free carbon catalysts is critical to achieve the electrosynthesis of hydrogen peroxide (H 2 O ) via two‐electron oxygen reduction reaction (2e − ORR) using seawater as electrolyte. Herein, N‐rich doped (NC) synthesized by directly pyrolyzing guanine both N and C sources, which can facilitate formation ultrahigh‐N dopant (up 33.89 at.%), their ratios. The NC obtained at 700 °C with hydrogenated pyridine‐N pyrrole‐N (3:2) dopants exhibits a superior selectivity H 96%), high mass activity 545.5 A g −1 0.2 V versus RHE stable production 16.8 in 0.5 M NaCl. In situ Fourier transform infrared spectrum analysis proves that play role constructing active sites for synthesis . Meanwhile, theoretical calculations further reveal compared non‐hydrogenated dopants, pyridine pyrrole tune projected density states 2p z orbitals adjacent atoms approaching Fermi Level, enhancing * OOH through 2e ORR rather than 4e ORR. This work provides new insights developing efficient resources promising electrolytes.

Language: Английский

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Complete antihistamine degradation in wastewater matrix using a metal-free N-doped carbon with superior electrocatalytic performance for in-situ H2O2 production

Separation and Purification Technology, Journal Year: 2025, Volume and Issue: unknown, P. 131590 - 131590

Published: Jan. 1, 2025

Language: Английский

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Dual-Isolation Effect of Bismuth in Non-Noble BiNi Alloys for Enhanced Performance in H₂O₂ Electrosynthesis

ACS Catalysis, Journal Year: 2025, Volume and Issue: 15(3), P. 1819 - 1828

Published: Jan. 17, 2025

Noble-metal alloys are high-efficiency two-electron oxygen reduction reaction (2e– ORR) catalysts for the electrochemical production of H2O2. However, development noble-metal H2O2 is still in a bottleneck period due to their high cost, toxicity, low atom utilization, and limited reactivity. To solve these dilemmas alloys, developing non-noble can be an alternative. Herein, BiNi with uniform diameter ∼11 nm supported on carbon nanosheets (BiNi/C) synthesized by hydrothermal-pyrolysis method. The BiNi/C material exhibits 2e– ORR performance onset potential 0.76 V vs RHE selectivity ∼98% 0.1 M KOH. H-cell tests deliver yield ∼17 mM within 2 h at 0.4 RHE. then used fixed-bed Fenton process, degradation efficiencies RhB BPA maintain 100% ∼95% 10 h, respectively. Theoretical calculations reveal that Bi regulate electronic structure Ni through "dual-isolation" effect physical isolation. adsorption energy *OOH thus deceased, side-on sites achieved. Furthermore, itself lowest overpotential also serve as active site generation dual-isolation effect. Our study provides guidance synthesis alloy activity selectivity.

Language: Английский

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Charge Transfer Modulation in g-C₃N₄/CeO₂ Composites: Electrocatalytic Oxygen Reduction for H₂O₂ Production

Inorganic Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 4, 2025

The electrocatalytic two-electron oxygen reduction reaction (2e-ORR) represents one of the most prospective avenues for in situ synthesis hydrogen peroxide (H2O2). However, four-electron competition constrains efficiency H2O2 synthesis. Therefore, there is an urgent need to develop superior catalysts facilitate In this study, graphite-phase carbon nitride and cerium dioxide composites (g-C3N4/CeO2) with varying CeO2 loadings were prepared favorable 2e-ORR electrocatalysts. optimized composite, containing 20 wt % (g-C3N4/CeO2-20%) exhibited highest Faradaic (FE) 97% notable yielding 9.84 mol gcat.–1 h–1 at potential 0.3 V (vs RHE) a 0.1 M KOH electrolyte. Density functional theory calculations revealed that improvement selectivity yield attributed charge transfer between g-C3N4 CeO2, which causes active site C atom donating electrons form C+, thereby enhancing adsorption desorption *OOH intermediates. Additionally, g-C3N4/CeO2-20% composite exhibits excellent performance neutral acidic electrolytes demonstrates capability electro-Fenton degradation organic pollutants. This study not only provides new insights into mechanism g-C3N4/CeO2 but also effective method designing catalysts.

Language: Английский

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Biomass-derived carbon for solar H2O2 production: Current trends and future directions

Materials Today Energy, Journal Year: 2025, Volume and Issue: unknown, P. 101840 - 101840

Published: Feb. 1, 2025

Language: Английский

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Hydroxyl combined with nitrogen on biomass carbon promotes the electrocatalytic H\(_{2}\)O\(_{2}\) selectivity

Journal of Metals Materials and Minerals, Journal Year: 2025, Volume and Issue: 35(1), P. e2216 - e2216

Published: Feb. 22, 2025

Elevating the selectivity of two-electron oxygen reduction reaction (2e‒ ORR) is challenging. Herein, hydroxyl combined with nitrogen on biomass carbon exhibits a high H2O2 over wide potential range 0 V to 0.5 vs. RHE, which nearly 97% at 0.3 RHE. The combination and improves adsorption desorption intermediates, finally changing pathway promoting 2e‒ ORR. Faradaic efficiency (FE) reaches 98% Furthermore, typical organic pollutants were degraded site in flow cell. This work illustrates

Language: Английский

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Electrochemical Generation of Hydrogen Peroxide Using Cerium Oxide Nanostructures Supported on Graphene: Synthesis, Characterization, and Application in Wastewater Treatment

Electrochimica Acta, Journal Year: 2025, Volume and Issue: unknown, P. 145931 - 145931

Published: Feb. 1, 2025

Language: Английский

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The strong metal-support interaction regulation on cathode–anode coupling catalysts to boost the pollutant degradation

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 162015 - 162015

Published: March 1, 2025

Language: Английский

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