Coordination Chemistry Reviews, Год журнала: 2025, Номер 540, С. 216763 - 216763
Опубликована: Май 15, 2025
Язык: Английский
Angewandte Chemie International Edition, Год журнала: 2025, Номер unknown
Опубликована: Март 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.
Язык: Английский
Процитировано
3
Advanced Functional Materials, Год журнала: 2024, Номер unknown
Опубликована: Окт. 29, 2024
Abstract Ethylene (C 2 H 4 ) electrosynthesis from the electrocatalytic CO reduction process holds enormous potential applications in industrial production. However, sluggish kinetics of C─C coupling often result low yield and poor selectivity for C Herein, performance Cu catalysts varying sizes is investigated, prepared via a cryo‐mediated liquid phase exfoliation technique, electrochemical to . The activity gradually increase as size decreases tens nanometers few nanometers. Impressively, 5 nm quantum dots (Cu‐5) achieve maximum Faradaic efficiency (FE) 81.5% half‐cell cathodic energy (CEE) 42.2% with large partial current density 1.1 A cm −2 at −0.93 V versus reversible hydrogen electrode. Structural characterization situ spectroscopic analysis reveal that Cu‐5 dots, dominated by (100) facet, provide an abundance active sites enhance adsorption activation, promoting formation *CO intermediates. accumulation intermediates on facilitates CO‐CHO reaction, thus enhancing production rate.
Язык: Английский
Процитировано
15
Advanced Materials, Год журнала: 2025, Номер unknown
Опубликована: Фев. 2, 2025
Abstract The electrochemical CO 2 reduction reaction (CO RR) to valuable C 2+ products emerges as a promising strategy for converting intermittent renewable energy into high‐energy‐density fuels and feedstock. Leveraging its substantial commercial potential compatibility with existing infrastructure, the conversion of multicarbon hydrocarbons oxygenates (C ) holds great industrial promise. However, process is hampered by complex multielectron‐proton transfer reactions difficulties in reactant activation, posing significant thermodynamic kinetic barriers commercialization production. Addressing these necessitates comprehensive approach encompassing multiple facets, including effective control C─C coupling electrolyzers using efficient catalysts optimized local environments. This review delves advancements outstanding challenges spanning from microcosmic macroscopic scales, design nanocatalysts, optimization microenvironment, development electrolyzers. By elucidating influence electrolyte environment, exploring flow cells, guidelines are provided future research aimed at promoting coupling, thereby bridging microscopic insights applications field electroreduction.
Язык: Английский
Процитировано
2
Journal of the American Chemical Society, Год журнала: 2025, Номер unknown
Опубликована: Апрель 24, 2025
The electrocatalytic conversion of carbon dioxide (CO2) to ethylene (C2H4) holds great promise for sustainable chemical synthesis, yet achieving industrially relevant production rates remains a significant challenge. Through computational screening, we have identified praseodymium (Pr) single-atom alloy embedded in copper (Cu) catalyst (Pr@Cu) that exhibits superior CO2 activation and remarkably low energy barrier asymmetric *CO-*CHO coupling, primarily by facilitating the *CHO intermediate formation. Our optimized catalyst, Pr@Cu-2 (6 wt % Pr), achieves C2H4 Faradaic efficiency (FE) 64.2% at -1.6 V versus reversible hydrogen electrode (RHE) under high current density 1200 mA cm-2 reduction reaction (CO2RR). Furthermore, when integrated into 100 cm2 membrane assembly (MEA) electrolyzer, demonstrates robust performance, maintaining continuous rate 21.3 mL min-1 20 A over 200 h. This work provides fundamental insights role Pr alloys CO2RR highlights their potential scalable electrosynthesis.
Язык: Английский
Процитировано
2
ACS Catalysis, Год журнала: 2024, Номер unknown, С. 17571 - 17581
Опубликована: Ноя. 14, 2024
Precise control and understanding of surface changes in indium (In)-based catalysts during the electrocatalytic CO2 reduction reaction (CO2RR) process are challenging. This study presents a series surface-reconstructed In2O3–Bi electrocatalysts, created by doping mesoporous In2O3 nanocubes with bismuth (Bi). introduces abundant bimetallic In–Bi sites at crystal–amorphous interfaces, enhancing CO2-to-formate conversion selectivity. Bi atoms accelerate reconstruction In2O3, reduce charge density around In atoms, promote partial amorphization. situ X-ray diffraction (XRD) Fourier-transform infrared spectroscopy (FT-IR) measurements functional theory (DFT) calculations show that lower energy barrier for HCOOH* intermediate, enhance H2O dissociation, inhibit hydrogen evolution (HER). The In1.8Bi0.2O3 electrocatalyst demonstrates Faradaic efficiency (FE) 92.6% current −28.5 mA·cm–2 operates stably 110 h H-type cell. flow cell, it achieves an FE formate (FEformate) 97.6% −1.4 VRHE maintains above 94% FEformate over potential window 800 mV (from −1.0 to −1.8 V vs RHE). offers effective approach designing high-performance electrocatalysts CO2RR based on reconstruction.
Язык: Английский
Процитировано
7
Green Energy & Environment, Год журнала: 2025, Номер unknown
Опубликована: Янв. 1, 2025
Язык: Английский
Процитировано
1
Proceedings of the National Academy of Sciences, Год журнала: 2025, Номер 122(8)
Опубликована: Фев. 20, 2025
Electrocatalytic reduction (ECR) of furfural represents a sustainable route for biomass valorization. Unfortunately, traditional Cu-catalyzed ECR suffers from diversified product distribution and industrial-incompatible production rates, mainly caused by the intricate mechanism-performance relationship. Here, we manipulate hydrogenation pathways on Cu introducing ceria as an auxiliary component, which enables mechanism switching proton-coupled electron transfer to electrochemical hydrogen-atom (HAT) thus high-speed furfural-to-furfuryl alcohol electroconversion. Theoretical kinetic analyses show that oxygen-vacancy-rich delivers efficient formation-diffusion-hydrogenation chain H* diminishing adsorption. Spectroscopic characterizations indicate Cu/ceria interfacial perimeter enriches local furfural, synergistically lowering barrier rate-determining HAT step across perimeter. Our catalyst realizes high-rate HAT-dominated electrosynthesis single-product furfuryl alcohol, achieving high rate 19.1 ± 0.4 mol h-1 m-2 Faradaic efficiency 97 1% at economically viable partial current density over 0.1 A cm-2. results demonstrate highly biofeedstock valorization with enhanced techno-economic feasibility.
Язык: Английский
Процитировано
1
Advanced Science, Год журнала: 2025, Номер unknown
Опубликована: Фев. 27, 2025
Abstract The electrocatalytic conversion of CO 2 into valuable multi‐carbon (C 2+ ) products using Cu‐based catalysts has attracted significant attention. This review provides a comprehensive overview recent advances in catalyst design to improve C selectivity and operational stability. It begins with an analysis the fundamental reaction pathways for formation, encompassing both established emerging mechanisms, which offer critical insights design. In situ techniques, essential validating these by real‐time observation intermediates material evolution, are also introduced. A key focus this is placed on how enhance through manipulation, particularly emphasizing catalytic site construction promote C─C coupling via increasing * coverage optimizing protonation. Additionally, challenge maintaining activity under conditions discussed, highlighting reduction active charged Cu species materials reconstruction as major obstacles. To address these, describes strategies preserve sites control including novel utilization mitigation reconstruction. By presenting developments challenges ahead, aims guide future conversion.
Язык: Английский
Процитировано
1
Angewandte Chemie, Год журнала: 2025, Номер unknown
Опубликована: Март 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.
Язык: Английский
Процитировано
1
ACS Catalysis, Год журнала: 2025, Номер unknown, С. 7390 - 7402
Опубликована: Апрель 19, 2025
Язык: Английский
Процитировано
1