Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 472, P. 144859 - 144859
Published: July 17, 2023
Language: Английский
Chemical Engineering Journal, Journal Year: 2023, Volume and Issue: 472, P. 144859 - 144859
Published: July 17, 2023
Language: Английский
Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(45)
Published: Oct. 6, 2023
Coordination assembly offers a versatile means to developing advanced materials for various applications. However, current strategies assembling metal-organic networks into nanoparticles (NPs) often face challenges such as the use of toxic organic solvents, cytotoxicity because synthetic ligands, and complex synthesis procedures. Herein, we directly assemble NPs using metal ions polyphenols (i.e., metal-phenolic (MPNs)) in aqueous solutions without templating or seeding agents. We demonstrate role buffers (e.g., phosphate buffer) governing NP formation engineering physicochemical properties tunable sizes from 50 270 nm) by altering conditions. A library MPN is prepared natural ions. Diverse functional cargos, including anticancer drugs proteins with different molecular weights isoelectric points, are readily loaded within applications biocatalysis, therapeutic delivery) direct mixing, surface modification, owing strong affinity guest molecules. This study provides insights mechanism complexes simple strategy engineer nanosized desired diverse biotechnological
Language: Английский
Citations
53eScience, Journal Year: 2023, Volume and Issue: 3(2), P. 100097 - 100097
Published: Jan. 18, 2023
Electroreduction of CO2 into value-added chemicals and fuels utilizing renewable electricity offers a sustainable way to meet the carbon-neutral goal viable solution for storage intermittent green energy sources. At core this technology is development electrocatalysts accelerate redox kinetics reduction reactions (CO2RR) toward high targeted-product yield at minimal input. This perspective focuses on unique category CO2RR embodying both inorganic organic components synergistically promote reaction activity, selectivity stability. First, we summarize recent progress design fabrication organic/inorganic hybrids electrocatalysts, with special attention assembly protocols structural configurations. We then carry out comprehensive discussion mechanistic understanding processes tackled jointly by phases, respect regulation mass charge transport, modification double-layer configuration, tailoring intermediates adsorption, establishment tandem pathways. end, outline future challenges in rational further extend scope device level. hope work could incentivize more research interests construct mobilizing electrocatalytic towards industrialization.
Language: Английский
Citations
47Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 494, P. 215333 - 215333
Published: July 28, 2023
Language: Английский
Citations
45Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(15), P. 5311 - 5335
Published: Jan. 1, 2024
The panorama of the latest developments emerging porphyrin-based MOFs for photo(electro)catalytic CO 2 reduction is shown.
Language: Английский
Citations
39Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(23)
Published: April 6, 2024
Abstract The development of a methodology for synthesizing value‐added urea (CO(NH 2 ) via renewable electricity‐driven C−N coupling reaction under mild conditions is highly anticipated. However, the complex catalytic active sites that act on carbon and nitrogen species make mechanism unclear, resulting in low efficiency from co‐reduction dioxide (CO nitrate (NO 3 − ). Herein, we propose novel tandem catalyst Mo‐PCN‐222(Co), which Mo serve to facilitate reduction *NH intermediate, while Co enhance CO carbonic oxide (CO), thus synergistically promoting coupling. synthesized Mo‐PCN‐222(Co) exhibited noteworthy yield rate 844.11 mg h −1 g , alongside corresponding Faradaic 33.90 % at −0.4 V vs. reversible hydrogen electrode (RHE). By combining situ spectroscopic techniques with density functional theory calculations, demonstrate efficient attributed system *CO intermediates produced by stabilize formation *CONH intermediate. This study provides an effective avenue design synthesis catalysts electrocatalytic synthesis.
Language: Английский
Citations
32Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(20)
Published: Feb. 26, 2024
Abstract The catalytic performance for electrocatalytic CO 2 reduction reaction (CO RR) depends on the binding strength of reactants and intermediates. Covalent organic frameworks (COFs) have been adopted to catalyze RR, their abilities are tuned via constructing donor‐acceptor (DA) systems. However, most DA COFs single donor acceptor units, which caused wide‐range but lacking accuracy in modulating More elaborate regulation interactions with intermediates necessary challenge construct high‐efficiency catalysts. Herein, three‐component COF D‐A‐A units was first constructed by introducing electron‐rich diarylamine unit, electron‐deficient benzothiazole Co‐porphyrin units. Compared two‐component COFs, designed exhibit elevated electronic conductivity, enhanced reducibility, high efficiency charge transfer, further improving RR faradic 97.2 % at −0.8 V activity partial current density 27.85 mA cm −2 −1.0 exceed other COFs. Theoretical calculations demonstrate that sites suitable ability intermediates, benefit formation *COOH desorption *CO. This work offers valuable insights advancement multi‐component enabling modulated transfer improve activity.
Language: Английский
Citations
22Chemical Reviews, Journal Year: 2025, Volume and Issue: unknown
Published: Feb. 18, 2025
The electrocatalytic technique, as an efficient energy storage and conversion technology, has attracted significant attention to address exhaustion environmental pollution. Usually, the activity selectivity of reactions are largely dominated by dynamic process occurring on electrocatalysts. Therefore, high-performance electrocatalysts, which can dominate pathway barrier reactions, great significance for advancement technique. Metal-organic frameworks (MOFs), emerging crystalline porous materials, present structural component advantages including well-defined structure, high surface area, large porosity, diverse components, easy tailorability, demonstrating fantastic potential precise fabrication In this Review, strategies in electrocatalysts based MOF-related materials specifically introduced from aspects catalytic site design microenvironment modulation around sites. Furthermore, representative progress achieved various applications employing MOF-based is systematically summarized, with special emphasis MOFs performance optimization. Finally, remaining challenges future perspectives further highlighted.
Language: Английский
Citations
4Exploration, Journal Year: 2025, Volume and Issue: unknown
Published: Feb. 12, 2025
ABSTRACT Copper (Cu) is the most promising catalyst for electrochemical CO 2 ‐to‐C 2+ conversion, whereas performance remains below practical thresholds due to high energy barrier of C−C coupling and lack effective approaches steer reaction pathway. Recent advances show that metal‐organic frameworks (MOF) could be a platform as support, pre‐catalyst, co‐catalyst modify electronic structure local environment Cu catalysts promoting reduction by virtue their great tunability over compositions pore architectures. In this review, we discussed general design principles, catalytic mechanisms, achievements MOF‐based catalysts, aiming boost refinement steering pathway C products. The fundamentals challenges are first introduced. Then, summarized conceptions from three aspects: engineering properties Cu, regulating environment, managing site exposure mass transport. Further, latest progress products namely Cu‐based MOF, MOF‐derived Cu@MOF hybrid discussed. Finally, future research opportunities strategies suggested innovate rational advanced electrifying transformation.
Language: Английский
Citations
2ACS Materials Letters, Journal Year: 2022, Volume and Issue: 4(11), P. 2058 - 2079
Published: Sept. 26, 2022
The electrocatalytic carbon dioxide reduction reaction (CO2RR) holds great potential in promoting neutral through effectively converting CO2 molecules to useful chemicals and fuels. high-efficiency electrochemical conversion of single-carbon products has been well realized, while more efforts are needed for the generation high-value multicarbon products. Metal–organic frameworks (MOFs), featuring porous structures, high chemical tunability, ultralarge surface area, have attracted increasing attention CO2RR. Herein, we review recent progress CO2RR on MOF-based materials toward First, structure MOFs is briefly introduced. Then, performance corresponding catalytic mechanism pristine (classified according kind organic ligands/linkers) MOF-derived (including metal nanomaterials, single-atom catalysts nanocomposites) product systematically discussed. Finally, critical challenges opportunities highlighted inspire rational design targeted synthesis advanced high-performance
Language: Английский
Citations
66Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 485, P. 215099 - 215099
Published: March 27, 2023
Language: Английский
Citations
37