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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Joule heating synthesis of NiFe alloy/MoO2 and in-situ transformed (Ni,Fe)OOH/MoO2 heterostructure as effective complementary electrocatalysts for overall splitting in alkaline seawater

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 340, P. 123277 - 123277

Published: Sept. 7, 2023

Language: Английский

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One stone for four birds: A “chemical blowing” strategy to synthesis wood-derived carbon monoliths for high-mass loading capacitive energy storage in low temperature

Journal of Colloid and Interface Science, Journal Year: 2023, Volume and Issue: 653, P. 1526 - 1538

Published: Sept. 29, 2023

Language: Английский

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H* Species Regulation by Mn‐Co(OH)₂ for Efficient Nitrate Electro‐reduction in Neutral Solution

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(11)

Published: Jan. 23, 2024

Abstract During the electrocatalytic NO 3 − reduction reaction (NO RR) under neutral condition, activation of H 2 O to generate H* and inhibition inter‐H* species binding, are critically important but remain challenging for suppressing non‐desirable hydrogen evolution (HER). Here, a Mn‐doped Co(OH) (named as Mn‐Co(OH) ) has been synthesized by in situ reconstruction electrolyte, which is able dissociate molecules inhibits binding between each other owing increased interatomic spacing Mn‐doping. The electrocatalyst offers faradaic efficiency (FE) high 98.9±1.7% at −0.6 V vs. reversible electrode (RHE) an energy (EE) 49.90±1.03% NH production RR, among highest recently reported state‐of‐the‐art catalysts electrolyte. Moreover, negligible degradation −200 mA cm −2 found least 500 h, longest catalytic durations ever reported. This work paves novel approach design synthesis efficient RR electrocatalysts.

Language: Английский

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Regulating the Spin‐State of Rare‐Earth Ce Single Atom Catalyst for Boosted Oxygen Reduction in Neutral Medium

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(47)

Published: July 16, 2023

Abstract The development of neutral zinc–air batteries (ZABs) is long been impeded by the sluggish oxygen reduction reaction (ORR) derived from insufficient O 2 activation and OH* blocking effect. Herein, synthesis a series rare‐earth Ce single‐atom catalysts (CeNCs) reported with enhanced spin‐state for boosting ORR. Experimental analysis theoretical calculations indicate that unique local coordination/geometric structure reshapes electronic configuration sites to achieve transition 4d 10 4f 1 8 3 . high‐spin active accelerate unpaired f electrons occupy anti‐π orbitals generate suitable binding strength intermediates. In conditions, CeNC‐40 exhibits excellent ORR performance half‐wave potentials 0.78 V negligible decay after 000 cycles. Additionally, self‐breathing ZABs based on demonstrates peak power density 81 mW cm −2 impressive long‐cycle stability (>1 600 cycles) at mA This work presents an effective strategy developing address challenges ZABs.

Language: Английский

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Modulation of the electronic structure of CoP by surface and interface codoping boosts electrocatalytic oxygen evolution reaction

International Journal of Hydrogen Energy, Journal Year: 2023, Volume and Issue: 51, P. 914 - 921

Published: Nov. 20, 2023

Language: Английский

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Activating lattice oxygen by a defect-engineered Fe₂O₃–CeO₂ nano-heterojunction for efficient electrochemical water oxidation

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(14), P. 5260 - 5272

Published: Jan. 1, 2024

Self-supporting Fe 2 O 3 –CeO nano-heterojunction electrodes with rich oxygen vacancies present high catalytic performance for evolution reaction, where defect-engineering promotes the interfacial interaction and activates lattice oxygens.

Language: Английский

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Enhancement of Nitrate‐to‐Ammonia on Amorphous CeO_x‐Modified Cu via Tuning of Active Hydrogen Supply

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 14(7)

Published: Dec. 22, 2023

Abstract The electrochemical nitrate reduction reaction (NO 3 RR) is an environment‐friendly and promising alternative to the conventional Haber–Bosch ammonia synthesis process, which a complex process of proton‐coupled electron transfer. Hereon, amorphous CeO x support introduced construct Cu/a‐CeO heterostructure prepared provide sufficient *H synergistically catalyze NO RR. achieves maximum yield 1.52 mmol h −1 mg cat . In flow cell, NH reaches 17.93 at 1 A cm −2 , exceeds most state‐of‐the‐art catalysts. situ X‐ray diffraction (XRD) in Raman observe that catalyst undergoes structural reconfiguration under operating conditions, thus confirming Cu 2 O not true active center catalytic process. Furthermore, characterizations density functional theory (DFT) calculations demonstrate modulates electronic structure overcomes higher potential barrier required for decomposition water on Cu, greatly facilitates hydrolysis provides H‐coverage rate hydrogenation − realizing dynamic equilibrium between production consumption hydrogen. This component design strategy centered opens up new pathway

Language: Английский

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Lattice Strain with Stabilized Oxygen Vacancies Boosts Ceria for Robust Alkaline Hydrogen Evolution Outperforming Benchmark Pt

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(33)

Published: June 12, 2024

Abstract Earth‐abundant metal oxides are usually considered as stable but catalytically inert toward hydrogen evolution reaction (HER) due to their unfavorable intermediate adsorption performance. Herein, a heavy rare earth (Y) and transition (Co) dual‐doping induced lattice strain oxygen vacancy stabilization strategy is proposed boost CeO 2 robust alkaline HER. The compression increased (O v ) concentration in synergistically improve the water dissociation on O sites sequential at activated ‐neighboring sites, leading significantly enhanced HER kinetics. Meanwhile, Y doping offers effect by its stronger Y─O bonding over Ce─O, which endows catalyst with excellent stability. Y,Co‐CeO electrocatalyst exhibits an ultra‐low overpotential (27 mV 10 mA cm −2 Tafel slope (48 dec −1 ), outperforming benchmark Pt electrocatalyst. Moreover, anion exchange membrane electrolyzer incorporated achieves stability of 500 h under 600 . This synergistic sheds new light rational development efficient oxide‐based electrocatalysts.

Language: Английский

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Stabilizing atomic Ru species in conjugated sp2 carbon-linked covalent organic framework for acidic water oxidation

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: June 26, 2024

Abstract Suppressing the kinetically favorable lattice oxygen oxidation mechanism pathway and triggering adsorbate evolution at expense of activity are state-of-the-art strategies for Ru-based electrocatalysts toward acidic water oxidation. Herein, atomically dispersed Ru species anchored into an stable vinyl-linked 2D covalent organic framework with unique crossed π-conjugation, termed as COF-205-Ru. The π-conjugated structure COF-205-Ru not only suppresses dissolution through strong Ru-N motifs, but also reduces state by multiple π-conjugations, thereby activating coordinated to stabilizing vacancies during process. Experimental results including X-ray absorption spectroscopy, in situ Raman powder diffraction patterns, theoretical calculations unveil activated elevated energy level O 2 p band, decreased vacancy formation energy, promoted electrochemical stability, significantly reduced barrier potential determining step Consequently, obtained displays a high mass 2659.3 A g −1 , which is 32-fold higher than commercial RuO retains long-term durability over 280 h. This work provides strategy simultaneously promote stability catalysts

Language: Английский

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