Recent progress in electrocatalytic C-N coupling of CO2 and inorganic N-containing small molecules DOI
Huijuan Jing, Jun Long, Dunfeng Gao

et al.

Science China Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: March 5, 2025

Language: Английский

Isolated Metal Centers Activate Small Molecule Electrooxidation: Mechanisms and Applications DOI Open Access
Yanmin Hu,

Tingting Chao,

Yuhai Dou

et al.

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

Published: Jan. 26, 2025

Abstract Electrochemical oxidation of small molecules shows great promise to substitute oxygen evolution reaction (OER) or hydrogen (HOR) enhance kinetics and reduce energy consumption, as well produce high‐valued chemicals serve fuels. For these reactions, high‐valence metal sites generated at oxidative potentials are typically considered active trigger the process molecules. Isolated atom site catalysts (IASCs) have been developed an ideal system precisely regulate state coordination environment single‐metal centers, thus optimize their catalytic property. The isolated in IASCs inherently possess a positive state, can be more readily homogeneous under than nanoparticle counterparts. Meanwhile, merely centers but lack ensemble sites, which alter adsorption configurations compared with counterparts, induce various pathways mechanisms change product selectivity. More importantly, construction is discovered limit d‐electron back donation CO 2p * orbital overly strong on resolve poisoning problems most electro‐oxidation reactions improve stability. Based advantages fields electrochemical molecules, this review summarizes recent developments advancements focusing anodic HOR fuel cells OER electrolytic alternative such formic acid/methanol/ethanol/glycerol/urea/5‐hydroxymethylfurfural (HMF) key reactions. merits different decoding structure–activity relationships specifically discussed guide precise design structural regulation from perspective comprehensive mechanism. Finally, future prospects challenges put forward, aiming motivate application possibilities for diverse functional IASCs.

Language: Английский

Citations

1

Research Progress of Coordination Materials for Electrocatalytic Nitrogen Oxides Species Conversion into High-Value Chemicals DOI
Xianlong Liu, Peisen Liao, Weifang Liao

et al.

EnergyChem, Journal Year: 2025, Volume and Issue: unknown, P. 100146 - 100146

Published: Feb. 1, 2025

Language: Английский

Citations

1

Non-rigid metal–oxygen bonding empowered nitrate reduction on ruthenium catalysts DOI Creative Commons
Suwen Wang, Zechao Zhuang,

Jiawei Xu

et al.

Nano Energy, Journal Year: 2024, Volume and Issue: 130, P. 110088 - 110088

Published: Aug. 6, 2024

Electrocatalytic nitrate reduction (NitRR) offers exciting potential for mass production of ammonia (NH3) from renewables. However, the rigidity metal−ligand bonds in most electrocatalysts renders them unable to survive structural transformations required NitRR. Herein, we establish a type non-rigid metal−oxygen by employing graphene oxide (GO) sheets as 'micron-scale' ligand transition metals (TM). Because being confined interfaces between GO and TM, oxygenated groups can associate with dissociate TM response reaction dynamics. As proof-of-concept demonstration, an electrocatalyst was developed dispersing nanoscale ruthenium (Ru) on utilizing two-dimensional MXene compensate low electrical conductivity GO. This exhibits maximum NH3 yield over 5 mg cm−2 h−1, almost 100 % current-to-NH3 efficiency, far outperforming performance reported Ru-based materials. What's even more remarkable is achievement record-breaking performance: 200-hour stable electrolysis 40.2 using membrane electrode reactor. Our experimental theoretical investigations further reveal non-rigidity Ru–O how they self-regulate adapt diverse intermediates involved work provides approach fabricate high-performance featuring reversible bonds, opening new possibilities practical electrolysis.

Language: Английский

Citations

8

Advancing Heterogeneous Organic Synthesis With Coordination Chemistry‐Empowered Single‐Atom Catalysts DOI

Bo‐Chao Ye,

Wenhao Li, Xia Zhang

et al.

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

Published: Sept. 18, 2024

Abstract For traditional metal complexes, intricate chemistry is required to acquire appropriate ligands for controlling the electron and steric hindrance of active centers. Comparatively, preparation single‐atom catalysts much easier with more straightforward effective accesses arrangement control The presence coordination atoms or neighboring functional on supports' surface ensures stability single‐atoms their interactions individual substantially regulate performance Therefore, collaborative interaction between surrounding environment enhances initiation reaction substrates formation transformation crucial intermediate compounds, which imparts significant catalytic efficacy, rendering them a valuable framework investigating correlation structure activity, as well mechanism in organic reactions. Herein, comprehensive overviews both homogeneous complexes reactions are provided. Additionally, reflective conjectures about advancement synthesis also proposed present reference later development.

Language: Английский

Citations

6

Boosting Electroreduction of Nitrate and CO2 to Urea on a Tandem Fe1/MoS2 Catalyst DOI

Wenyu Du,

Zeyi Sun,

Shiyao Shang

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 23, 2024

Urea electrosynthesis by coelectrolysis of NO

Language: Английский

Citations

6

Theoretical Insights into the Selectivity of Nitrite Reduction to NH2OH on Single-Atom Catalysts DOI
Wei Zheng, Dingge Fan, Yang Yang

et al.

Nano Letters, Journal Year: 2024, Volume and Issue: 24(29), P. 9011 - 9016

Published: July 10, 2024

Electroreduction of nitrate/nitrite to high-value-added products, including NH

Language: Английский

Citations

5

Tailoring microenvironment for efficient CO2 electroreduction through nanoconfinement strategy DOI
Lulu Chen, Minhan Li, Jianan Zhang

et al.

Nano Research, Journal Year: 2024, Volume and Issue: 17(9), P. 7880 - 7899

Published: Aug. 7, 2024

Language: Английский

Citations

5

Tuning C─N Coupling Mode by Cu─In Dual Metal Sites in Covalent Organic Framework for Enhanced Urea Electrosynthesis DOI Open Access

Nan Wang,

Yuan Zhang, Chunfeng Shao

et al.

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

Published: Jan. 28, 2025

Abstract Electrochemical conversion of CO 2 and NO 3 − to high value‐added urea is a win–win strategy for both resources the environment. However, yield rate selectivity are still low. In this work, Cu metals grafted into interlayers an imine‐linked covalent organic framework (COF) form stable Cu─In dual metal sites by strong coordination hydroxyl O imine N atoms in framework. It found that optimal CuIn 1.07 ‐COF electrocatalyst exhibits impressive 2924.4 µg h −1 mg Faradaic efficiency (FE) 54.7% H‐cell, which surpasses most previously reported catalysts electrosynthesis. situ spectroscopy theoretical calculations reveal due stronger electronic interaction between In, * NH intermediate generated on site from reduction, then couples with neighbor produce lower energy barrier, effectively promotes electrochemical co‐reduction urea. The work provides new clues understanding structure‐performance relationship

Language: Английский

Citations

0

Regulation of Active Hydrogen and Nitrate Concentration: Pulsed Potential Strategies in Nitrate Electroreduction Microenvironments DOI Creative Commons
Jianping Yang, Lin Gu, Nan Song

et al.

Research Square (Research Square), Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 20, 2025

Abstract The electrochemical reduction of nitrate (NO3RR) plays a significant role in the nitrogen cycle and environmental remediation. dynamics active hydrogen NO3RR were studied depth by varying concentration applying pulsed-potential approach. effect both factors on regulation degree hydrogenation intermediates product distribution was evaluated. Density functional theory (DFT) calculations indicated that elevated levels decrease energy barrier for *NO to *N conversion, enhancing *N2 formation. experimental results indicate under high concentrations, copper-palladium (CuPd) catalysts exhibit faster reaction kinetics higher selectivity. In-situ characterizations illuminated critical intermediates. CuPd catalyst achieved 95% NO3-N conversion 99% N2 selectivity at 1 M pulse potential modulation surface. Finite element analysis (FEA) verified pulsed potentials modulate local ion concentrations. present work brings closer practical applications, aiding protection balance cycle.

Language: Английский

Citations

0

CuPt Alloy Enabling the Tandem Catalysis for Reduction of HCOOH and NO3 to Urea at High Current Density DOI Open Access

Yaodong Yu,

Jiani Han,

Haoran Li

et al.

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

Published: Feb. 21, 2025

The formation of urea by electrocatalytic reduction C1-reactants and NO3 - is an attractive way to store renewable electricity, close the carbon cycle, eliminate nitrate contaminants from wastewater. Involving insufficient supply C1 reactants multiple electron transfers makes reaction difficult achieve high Faraday efficiency yield at current density. Here, a synthesis approach presented via reductive coupling between liquid HCOOH on copper foam (CF) loaded Cu4Pt catalyst with optimized ratios. A 40.08 mg h-1 cm-2 achieved FE up 58.1% density -502.3 mA cm-2, superior productivity previously reported catalysts. No degradation observed over 120-h continuous operation such rate. highly efficient activity Cu4Pt/CF can be attributed synergetic effect Pt Cu sites tandem catalysis, in which doped enrich reactants, promote intermolecular dehydration, form adsorb large amounts *CO key intermediates. generate quantities intermediate *NH2. adsorbed intermediates *NH2 are basis for subsequent thermodynamic spontaneous C─N coupling.

Language: Английский

Citations

0