Dual Single‐Atomic Ni‐N₄ and Fe‐N₄ Sites Constructing Janus Hollow Graphene for Selective Oxygen Electrocatalysis

Advanced Materials, Journal Year: 2020, Volume and Issue: 32(30)

Published: June 22, 2020

Nitrogen-coordinated metal single atoms in carbon have aroused extensive interest recently and been growing as an active research frontier a wide range of key renewable energy reactions devices. Herein, step-by-step self-assembly strategy is developed to allocate nickel (Ni) iron (Fe) respectively on the inner outer walls graphene hollow nanospheres (GHSs), realizing separate-sided different single-atom functionalization graphene. The Ni or Fe atom demonstrated be coordinated with four N via formation Ni-N4 Fe-N4 planar configuration. /GHSs/Fe-N4 Janus material exhibits excellent bifunctional electrocatalytic performance, which clusters dominantly contribute high activity toward oxygen reduction reaction (ORR), while are responsible for evolution (OER). Density functional theory calculations demonstrate structures reactivities ORR OER. endows rechargeable Zn-air battery efficiency cycling stability air-cathode, outperforming that benchmark Pt/C+RuO2 air-cathode. current work paves new avenue precise control sites surface high-performance selective electrocatalysts.

Language: Английский

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Co/CoP Heterojunction on Hierarchically Ordered Porous Carbon as a Highly Efficient Electrocatalyst for Hydrogen and Oxygen Evolution

Advanced Energy Materials, Journal Year: 2021, Volume and Issue: 11(42)

Published: Oct. 8, 2021

Abstract Designing non‐precious electrocatalysts to synergistically achieve a facilitated mass/electron transfer and exposure of abundant active sites is highly desired but remains significant challenge. Herein, composite electrocatalyst consisting dispersed Co/CoP heterojunction embedded within hierarchically ordered macroporous‐mesoporous‐microporous carbon matrix (Co/CoP@HOMC) rationally designed through the pyrolysis polystyrene sphere‐templated zeolite imidazolate framework‐67 (ZIF‐67) assemblies. The combined experimental theoretical calculations reveal that interfaces not only provide richly exposed also optimize hydrogen/water absorption free energy via electronic coupling, while interconnected macroporous structure enables superior mass all accessible sites. As result, as‐developed Co/CoP@HOMC composites exhibit outstanding catalytic activity with overpotentials 120 260 mV at 10 mA cm −2 for hydrogen evolution reaction oxygen in 1.0 m KOH, respectively. Moreover, an alkaline electrolyzer constructed by requires ultralow cell voltage 1.54 V , outperforming Pt@C||IrO 2 @C couple (1.64 V).

Language: Английский

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Gd-induced electronic structure engineering of a NiFe-layered double hydroxide for efficient oxygen evolution

Journal of Materials Chemistry A, Journal Year: 2021, Volume and Issue: 9(5), P. 2999 - 3006

Published: Jan. 1, 2021

A novel rare earth hybrid electrocatalyst, consisting of a gadolinium-doped hierarchal NiFe-layered double hydroxide, is developed for improving the OER activity.

Language: Английский

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Ce‐Induced Differentiated Regulation of Co Sites via Gradient Orbital Coupling for Bifunctional Water‐Splitting Reactions

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(30)

Published: June 22, 2023

Abstract Rare‐earth (RE) elements have emerged as crucial promoters to regulate the electrocatalysis of transition metals (TM), but knowledge about RE‐enhanced mechanism TM in is limited. Herein, an array‐like Ce‐CoP catalyst constructed explore origin and distinction Ce‐induced enhanced Co sites both hydrogen evolution reaction (HER) oxygen (OER). Compared with individual CoP, developed exhibits superior bifunctional electrocatalytic activity overpotentials 81 240 mV at 10 mA cm −2 , respectively for HER OER, excellent stability. Theoretical calculations show that unique 4 f valence electron structure Ce endows differentiated regulation OER through f‐p‐d gradient orbital coupling. In HER, retained Ce‐4 state induces spin parallelism surrounding sites, promoting adsorption *H intermediates. While band acts sacrificing protect from overoxidation Ce‐O‐Co chain optimized Co‐3 d state, providing additional coupling These findings provide new insights into comprehending present valuable design guidelines development efficient multi‐functional electrocatalysts.

Language: Английский

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Recent advances in rare-earth-based materials for electrocatalysis

Chem Catalysis, Journal Year: 2022, Volume and Issue: 2(5), P. 967 - 1008

Published: March 3, 2022

Language: Английский

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Defect Engineering on CeO₂‐Based Catalysts for Heterogeneous Catalytic Applications

Small Structures, Journal Year: 2021, Volume and Issue: 2(12)

Published: July 14, 2021

With abundant crystal defects, cerium oxide (CeO 2 ), widely used in heterogeneous catalysis, has attracted extensive attention. In recent years, researchers have investigated that the defect chemistry of CeO plays a vital role its catalytic activity and developed various introduction methods to synthesize stable efficient defective ‐based catalysts. Herein, understanding, introduction, applications catalysis are reviewed, structure–activity relationship between engineering performance is recommended with great emphasis. Interests put into investigation how defects influence stability catalysts effective strategies for fabricating efficient, stable, Finally, existing problems perspectives displayed. This review provides reference in‐depth understanding design more catalysis.

Language: Английский

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Plasma‐induced Mo‐doped Co₃O₄ with enriched oxygen vacancies for electrocatalytic oxygen evolution in water splitting

Carbon Energy, Journal Year: 2022, Volume and Issue: 5(3)

Published: Oct. 27, 2022

Abstract Heteroatomic substitution and vacancy engineering of spinel oxides can theoretically optimize the oxygen evolution reaction (OER) through charge redistribution d ‐band center modification but still remain a great challenge in both preparation catalytic mechanism. Herein, we proposed novel efficient Ar‐plasma (P)‐assisted strategy to construct heteroatom Mo‐substituted vacancies enriched hierarchical Co 3 O 4 porous nanoneedle arrays situ grown on carbon cloth (denoted P‐Mo‐Co @CC) improve OER performance. technology efficiently generate sites at surface hydroxide, which induces anchoring Mo anion salts electrostatic interaction, finally facilitating atoms formation surface. The @CC affords low overpotential only 276 mV 10 mA cm −2 for OER, is 58 superior that Mo‐free surpasses commercial RuO 2 catalyst. robust stability satisfactory selectivity (nearly 100% Faradic efficiency) are also demonstrated. Theoretical studies demonstrate with variable valance states regulates atomic ratio 3+ /Co 2+ increases number vacancies, thereby inducing tuning , adsorption energy intermediates (e.g., *OOH) during OER. Furthermore, two‐electrode OER//HER electrolyzer equipped as anode displays operation potential 1.54 V deliver current density exhibits good reversibility anticurrent fluctuation ability under simulated real supply conditions, demonstrating water electrolysis.

Language: Английский

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Multiphase nanosheet-nanowire cerium oxide and nickel-cobalt phosphide for highly-efficient electrocatalytic overall water splitting

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 316, P. 121678 - 121678

Published: June 28, 2022

Language: Английский

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Surface chemical reconstruction of hierarchical hollow inverse-spinel manganese cobalt oxide boosting oxygen evolution reaction

Chemical Engineering Journal, Journal Year: 2021, Volume and Issue: 431, P. 133829 - 133829

Published: Nov. 26, 2021

Language: Английский

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Interface Engineering of Anti-Perovskite Ni3FeN/VN Heterostructure for High-Performance Rechargeable Zinc–Air batteries

Chemical Engineering Journal, Journal Year: 2022, Volume and Issue: 437, P. 135291 - 135291

Published: Feb. 16, 2022

Language: Английский

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