Modulation of the Second-Beyond Coordination Structure in Single-Atom Electrocatalysts for Confirmed Promotion of Ammonia Synthesis DOI
Qinglin Li, Lin Luo, Xiangyang Guo

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 147(2), P. 1884 - 1892

Published: Dec. 30, 2024

Although microenvironments surrounding single-atom catalysts (SACs) have been widely demonstrated to a remarkable effect on their catalytic performances, it remains unclear whether the local structure beyond secondary coordination shells works as well or not. Herein, we employed series of metal-organic frameworks (MOFs) with well-defined and tunable second-beyond spheres model SAC electrocatalysts discuss influence long-distance ammonia synthesis from nitrate, which were synthesized denoted Cu12-NDI-X (X = NMe2, H, F). It is first experimentally confirmed that remote substitution function groups sphere can remarkably affect activity synthesis. Meanwhile, -H endowed Cu12-NND-H exhibits superior yield (35.1 mg·h-1·mgcat-1) FE (98.7%) those modified -NMe2 -F, also shows good stability at 100 mA·cm-2. The promotion modulated unraveled result adjustable d-band center Cu active site leading promoted adsorption NO3- protonation key intermediates. Encouraged by its extraordinary yield, electrode cathode assemble one rechargeable Zn-nitrate battery an impressive power density 34.0 mW·cm-2, demonstrating promising application in energy conversion storage.

Language: Английский

Balancing Hydrogen Evolution and Hydrogenation Reaction via Facet Engineering for Efficient Conversion of Nitrate to Ammonia in Actual Wastewater DOI Open Access

Wenye Zhong,

Yan Chen, Peiyan Chen

et al.

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: March 11, 2025

Abstract Due to the competitive relationship between nitrate reduction reaction (NO 3 − RR) and hydrogen evolution (HER), conventional approach improve Faradaic efficiency is select a catalyst without HER activity. Nevertheless, such strategy not only limits application of catalysts in NO RR, but also causes insufficient source, thereby sacrificing ammonia yield rate. We believe that should be excluded from hydrogenation reduction. Herein, taking traditional water electrolysis material Co O 4 as model system, we reveal oxygen vacancies on crystal facet can greatly promote dissociation capture intermediate for successfully shifting pathway hydrogenation. Beyond development, construct hybrid reactor achieve an recovery rate 1216.8 g‐N m −2 d −1 nuclear industry wastewater with ultra‐high concentration. This study breaks through limitation which provides significant insight into designing mechanism.

Language: Английский

Citations

0
Asymmetric active sites in ultra-thin high-entropy metal oxides nanosheets for enhanced electrochemical synthesis of ammonia DOI
Chuncheng Xu,

Hongyu Mou,

Dongrun Li

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125248 - 125248

Published: March 1, 2025

Language: Английский

Citations

0
Balancing Hydrogen Evolution and Hydrogenation Reaction via Facet Engineering for Efficient Conversion of Nitrate to Ammonia in Actual Wastewater DOI Open Access

Wenye Zhong,

Yan Chen, Peiyan Chen

et al.

Angewandte Chemie, Journal Year: 2025, Volume and Issue: unknown

Published: March 12, 2025

Abstract Due to the competitive relationship between nitrate reduction reaction (NO 3 − RR) and hydrogen evolution (HER), conventional approach improve Faradaic efficiency is select a catalyst without HER activity. Nevertheless, such strategy not only limits application of catalysts in NO RR, but also causes insufficient source, thereby sacrificing ammonia yield rate. We believe that should be excluded from hydrogenation reduction. Herein, taking traditional water electrolysis material Co O 4 as model system, we reveal oxygen vacancies on crystal facet can greatly promote dissociation capture intermediate for successfully shifting pathway hydrogenation. Beyond development, construct hybrid reactor achieve an recovery rate 1216.8 g‐N m −2 d −1 nuclear industry wastewater with ultra‐high concentration. This study breaks through limitation which provides significant insight into designing mechanism.

Language: Английский

Citations

0
Dual-active-site design of FeNi3 for electrocatalytic nitrate reduction to ammonia DOI

Kaiyu Qu,

Xiaojuan Zhu,

Leyang Song

et al.

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 161814 - 161814

Published: March 1, 2025

Language: Английский

Citations

0
Enabling High Performance in a Positive Potential of Nitrate‐to‐Ammonia Electrocatalysis Over Mesoporous Core@Shell Cu2O/Cu@PdCu Nanozyme DOI

Lizhi Sun,

Xiaowen Min,

Jingru Wang

et al.

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

Citations

0
Ni–Co bimetallic phosphide catalyst toward electrocatalytic ammonia synthesis under ambient conditions DOI Creative Commons

Dongnan Zhao,

Zhixian Mao,

Shengbo Zhang

et al.

RSC Advances, Journal Year: 2025, Volume and Issue: 15(13), P. 10390 - 10394

Published: Jan. 1, 2025

We have successfully synthesized a Ni–Co bimetallic phosphide catalyst for the electrocatalytic reduction of nitrate to produce ammonia.

Language: Английский

Citations

0
Plasmonic in-situ imaging of zeta potential distributions at electrochemical interfaces of 2D materials in water DOI Creative Commons
Xiaona Zhao, Xiaoli Zhou,

Cheng-Xin Cao

et al.

Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)

Published: April 12, 2025

Understanding the electrical double layer (EDL) at solid-liquid interfaces is pivotal across various fields, including energy storage, electrowetting, and electrocatalysis, yet probing its structure heterogeneity remains a considerable challenge. Here, we report an optical method for direct visualization quantification of zeta potential (ζ) between 2D materials aqueous solutions. By modulating surface charge density, map heterogenous distribution ζ MoS2 nanosheet interface, revealing how both external factors intrinsic material properties shape interfacial charge. This approach overcomes drawbacks conventional methods evaluating in materials, providing insights into elucidate complex interplay catalytic activity materials. Furthermore, it establishes robust framework exploring EDL electrochemical systems. Our findings reveal deeper understanding interface interactions, offering valuable fundamental processes governing these

Language: Английский

Citations

0
Metal-Support Interaction and Tip-Enhanced Electric Field Effect Co-Enhancing Oxygen Species Adsorption/Enrichment for Efficient Electrooxidation of Plastic Waste Derived Alcohol into Glycolic Acid DOI
Wenbo Li,

Qingshan Bao,

Fahao Ma

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125375 - 125375

Published: April 1, 2025

Language: Английский

Citations

0
Recent trends and prospects in electrochemical nitrate reduction to ammonia with an emphasis on cobalt catalysts DOI Creative Commons

Gaihong Wang,

Zhijie Chen, Jiangzhou Xie

et al.

Coordination Chemistry Reviews, Journal Year: 2025, Volume and Issue: 539, P. 216751 - 216751

Published: April 28, 2025

Language: Английский

Citations

0
Transition Metal‐Gallium Intermetallic Compounds with Tailored Active Site Configurations for Electrochemical Ammonia Synthesis DOI Creative Commons

Huaifang Zhang,

Chaoqun Ma,

Yichi Wang

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(49)

Published: Sept. 4, 2024

Abstract Gallium (Ga) with a low melting point can serve as unique metallic solvent in the synthesis of intermetallic compounds (IMCs). The negative formation enthalpy transition metal‐Ga IMCs endows them high catalytic stability. Meanwhile, their tunable crystal structures offer possibility to tailor configurations active sites meet requirements for specific applications. Herein, we present general method preparing range IMCs, including Co−Ga, Ni−Ga, Pt−Ga, Pd−Ga, and Rh−Ga IMCs. structurally ordered CoGa body‐centered cubic ( bcc ) structure are uniformly dispersed on nitrogen‐doped reduced graphene oxide substrate (O‐CoGa/NG) deliver outstanding nitrate reduction reaction (NO 3 RR) performance, making excellent catalysts construct highly efficient rechargeable Zn‐NO − battery. Operando studies theoretical simulations demonstrate that electron‐rich environments around Co atoms enhance adsorption strength *NO intermediate simultaneously suppress hydrogen, thus improving NO RR activity selectivity.

Language: Английский

Citations

3