Heterogeneous β-Co(OH)2/Cu2(OH)3Cl bifunctional electrocatalyst for superior concurrent conversion of glycerol and nitrite

Journal of Energy Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

Language: Английский

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A Copper–Zinc Cyanamide Solid-Solution Catalyst with Tailored Surface Electrostatic Potentials Promotes Asymmetric N-Intermediate Adsorption in Nitrite Electroreduction

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: 147(9), P. 8012 - 8023

Published: Feb. 18, 2025

The electrocatalytic nitrite reduction (NO2RR) converts nitrogen-containing pollutants to high-value ammonia (NH3) under ambient conditions. However, its multiple intermediates and multielectron coupled proton transfer process lead low activity NH3 selectivity for the existing electrocatalysts. Herein, we synthesize a solid-solution copper-zinc cyanamide (Cu0.8Zn0.2NCN) with localized structure distortion tailored surface electrostatic potential, allowing asymmetric binding of NO2-. It exhibits outstanding NO2RR performance Faradaic efficiency ∼100% an yield 22 mg h-1 cm-2, among best such process. Theoretical calculations in situ spectroscopic measurements demonstrate that Cu-Zn sites coordinated linear polarized [NCN]2- could transform symmetric [Cu-O-N-O-Cu] CuNCN-NO2- [Cu-N-O-Zn] configuration Cu0.8Zn0.2NCN-NO2-, thus enhancing adsorption bond cleavage. A paired electro-refinery Cu0.8Zn0.2NCN cathode reaches 2000 mA cm-2 at 2.36 V remains fully operational industrial-level 400 >140 h production rate ∼30 mgNH3 cm-2. Our work opens new avenue tailoring potentials using strategy advanced electrocatalysis.

Language: Английский

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Recent Breakthroughs in Electrocatalytic Reduction of Nitrogen-Oxyanions for Environmentally Benign Ammonia Synthesis

Nano Energy, Journal Year: 2025, Volume and Issue: unknown, P. 110683 - 110683

Published: Jan. 1, 2025

Language: Английский

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Laser-induced PdCu alloy catalysts for highly efficient and stable electrocatalytic nitrate reduction to ammonia

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 1, 2025

Language: Английский

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Integrated Three-in-one to Boost Nitrate Electroreduction to Ammonia Utilizing a 1D Mesoporous Carbon Cascade Nanoreactor

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: March 10, 2025

The electrochemical reduction of nitrate (NO3-) offers a promising waste-to-value strategy for synthesizing ammonia (NH3), yet it involves complex multi-interface system with several stages such as mass transport, species enrichment, and interfacial transformation. This complexity necessitates catalysts diverse structural characteristics across multiple temporal spatial scales. Herein, three-in-one nanoreactor is designed 1D geometry, open mesochannels, synergistic active sites optimized NH3 synthesis. Guided by finite element simulations, mesoporous carbon carrier engineered to create distinctive microenvironment that enhances NO3- transfer adsorption while confining reaction intermediates. Meanwhile, iron single atomic (Fe-N4 SAs) nanoclusters (Fe4 NCs) are embedded in situ into the carrier, yielding an efficient cascade nanoreactor. design demonstrates large Faraday efficiencies, rapid removal rates, impressive yield rates under both neutral alkaline conditions. Detailed experimental results theoretical analysis reveal Fe-N4 SAs Fe4 NCs can adapt their electronic structures tandem, allowing effectively reduce oxidize H2O. As demonstration, assembled Zn-NO3- battery achieves power density 20.12 mW cm-2 coupled excellent rechargeability.

Language: Английский

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Enabling High Performance in a Positive Potential of Nitrate‐to‐Ammonia Electrocatalysis Over Mesoporous Core@Shell Cu₂O/Cu@PdCu Nanozyme

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 2, 2025

Electrocatalytic tandem nitrate reduction to ammonia (NO3 --to-NH3) offers a promising pathway for energy and environmental sustainability. Although considerable efforts have been presented modulate the reaction pathways enhanced NO3 --to-NH3 electrocatalysis, these advances often require relatively high overpotentials balance yield rate selectivity of NH3, resulting in remarkable inefficiency. Inspired by enzyme catalysis nature, herein enzyme-like electrocatalyst is designed consisting core Cu2O/Cu heterojunction surrounded mesoporous PdCu shell (Cu2O/Cu@mesoPdCu) that accelerated electrocatalysis positive potentials. Impressively, Cu2O/Cu@mesoPdCu nanozymes hold superior performance robust NH3 electrosynthesis fairly potential 0.10 V (versus reversible hydrogen electrode), having Faraday efficiency 96.2%, 13.3 mg h-1 mg-1, half-cell 46.0%. Kinetic studies, situ spectra density functional theory calculations revealed preferentially adsorbed - further reduced *NO2, while active radicals enriched on promoted multistep hydrodeoxygenation *NO2 within "semi-closed" microenvironment, both which synergistically enabled Moreover, this disclosed better more energy-efficient manner when coupling with thermodynamically favorable ethanol oxidation reaction.

Language: Английский

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Multiple Functional Engineering Strategies and Active Site Identification in Ru‐Based Electrocatalysts for Catalytic Conversion Reactions

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 3, 2025

Electrochemical conversion has been regarded as an ideal technology for achieving clean and sustainable energy, showing significant promise in addressing the increasingly serious energy crisis environmental pollution. Ru-containing electrocatalysts (RUCE) outperform other precious metals due to elevated intrinsic activity superior cost-effectiveness, developing into a promising candidate electrochemical reactions. A challenge field of catalyst discovery lies its heavy reliance on empirical methods, rather than approaches that are rooted rational design principles. This review first concentrates catalytically active sites critical factors governing catalytic performance durability. Then, comprehensive summary multifunctional modification strategies ranging from nanoscale atomic scale is explored control structure improve performance. By unveiling roles each component modified RUCE at level, their identified discussed establish structure-performance relationship catalysts. Finally, challenges perspectives Ru-based materials hydrogen, oxygen, nitrogen reactions presented inspire further efforts toward understanding meet ever-growing demand future.

Language: Английский

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A bifunctional CoNi alloy for electrocatalytically coupled cathodic nitrate reduction and anodic HPAM oxidation

Journal of Electroanalytical Chemistry, Journal Year: 2025, Volume and Issue: unknown, P. 119105 - 119105

Published: April 1, 2025

Language: Английский

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Revitalizing lithium-mediated ammonia electrosynthesis activity over heterogeneous lithiophobic-lithiophilic solid electrolyte interphase

Journal of Energy Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: April 1, 2025

Language: Английский

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Anion‐Regulated Active Nickel Site for Nitrate Reduction in Efficient Ammonia Electrosynthesis and Zn‐Nitrate Battery

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 14, 2025

Abstract Electrocatalytic nitrate reduction (NO 3 RR) to ammonia (NH ) has great potential address the challenges caused by Habor‐Bosch process. However, sluggish kinetic, complex mechanisms and competitive reactions seriously reduce Faradaic efficiency (FE) yield of NH . Transition metal‐based compounds are promising catalysts for electrocatalytic NO RR, where anions can tune electronic structure metal cation sites. In this work, oxygen (O) phosphorus (P) introduced regulate nickel (Ni) reveal mechanism anion regulation in RR. The electrosynthesis performance is ranked as follows: Ni 2 P surpasses Ni, which turn outperforms NiO. Notably, nanosheets exhibit a maximum FE 97.4% 15.4 mg h − ¹ cm −2 Characterization theoretical calculation indicate that introduction moderately alters resulting reduced energy barriers rate‐limiting step RR improved H O decomposition generate active hydrogen, subsequently enhances production. This work highlights critical role

Language: Английский

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