Science China Chemistry, Journal Year: 2025, Volume and Issue: unknown
Published: March 5, 2025
Language: Английский
Science China Chemistry, Journal Year: 2025, Volume and Issue: unknown
Published: March 5, 2025
Language: Английский
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
1EnergyChem, Journal Year: 2025, Volume and Issue: unknown, P. 100146 - 100146
Published: Feb. 1, 2025
Language: Английский
Citations
1Nano 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
8Advanced 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
6ACS Nano, Journal Year: 2024, Volume and Issue: unknown
Published: Sept. 23, 2024
Urea electrosynthesis by coelectrolysis of NO
Language: Английский
Citations
6Nano 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
5Nano Research, Journal Year: 2024, Volume and Issue: 17(9), P. 7880 - 7899
Published: Aug. 7, 2024
Language: Английский
Citations
5Advanced 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
0Research Square (Research Square), Journal Year: 2025, Volume and Issue: unknown
Published: Feb. 20, 2025
Language: Английский
Citations
0Advanced 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