Journal of Materials Chemistry A, Journal Year: 2023, Volume and Issue: 11(16), P. 8739 - 8746
Published: Jan. 1, 2023
Viologen-based MOFs were developed to show highly efficient electrocatalytic CO 2 reduction reaction with a high faradaic efficiency of 93.8% at 2.3 V and large partial current density 111.1 mA cm −2 2.9 V.
Language: Английский
Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)
Published: Oct. 14, 2024
Electrocatalytic C-N coupling from carbon dioxide and nitrate provides a sustainable alternative to the conventional energy-intensive urea synthetic protocol, enabling wastes upgrading value-added products synthesis. The design of efficient stable electrocatalysts is vital promote development electrocatalytic In this work, copper phthalocyanine (CuPc) adopted as modeling catalyst toward synthesis owing its accurate adjustable active configurations. Combining experimental theoretical studies, it can be observed that intramolecular Cu-N coordination strengthened with optimization in electronic structure by amino substitution (CuPc-Amino) electrochemically induced demetallation efficiently suppressed, serving origination excellent activity stability. Compared CuPc (the maximum yield rate 39.9 ± 1.9 mmol h
Language: Английский
Citations
19
Nature Communications, Journal Year: 2025, Volume and Issue: 16(1)
Published: March 27, 2025
Abstract Single-atom catalysts (SACs) have received increasing attention due to their 100% atomic utilization efficiency. The electrochemical CO 2 reduction reaction (CO RR) using SAC offers a promising approach for utilization, but achieving facile adsorption and desorption remains challenging traditional SACs. Instead of singling out specific atoms, we propose strategy utilizing atoms from the entire lanthanide (Ln) group facilitate RR. Density functional theory calculations, operando spectroscopy, X-ray absorption spectroscopy elucidate bridging mechanism representative erbium (Er) single-atom catalyst. As result, realize series Ln SACs spanning 14 elements that exhibit Faradaic efficiencies exceeding 90%. Er catalyst achieves high turnover frequency ~130,000 h − 1 at 500 mA cm . Moreover, 34.7% full-cell energy efficiency 70.4% single-pass conversion are obtained 200 with acidic electrolyte. This catalytic platform leverages collective potential group, introducing new possibilities efficient -to-CO beyond through exploration unique bonding motifs in catalysts.
Language: Английский
Citations
2
Advanced Materials, Journal Year: 2023, Volume and Issue: 35(52)
Published: Aug. 20, 2023
Abstract Electrochemical carbon dioxide reduction reaction (CO 2 RR) driven by renewable energy shows great promise in mitigating and potentially reversing the devastating effects of anthropogenic climate change environmental degradation. The simultaneous synthesis energy‐dense chemicals can meet global demand while decoupling emissions from economic growth. However, development CO RR technology faces challenges catalyst discovery device optimization that hinder their industrial implementation. In this contribution, a comprehensive overview current state research is provided, starting with background motivation for technology, followed fundamentals evaluated metrics. Then underlying design principles electrocatalysts are discussed, emphasizing structure–performance correlations advanced electrochemical assembly cells increase selectivity throughput. Finally, review looks to future identifies opportunities innovation mechanism discovery, material screening strategies, assemblies move toward carbon‐neutral society.
Language: Английский
Citations
38
Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(29)
Published: April 21, 2023
Abstract Exploring advanced co‐reaction accelerators with superior oxygen reduction activity that generate rich reactive species (ROS) has attracted great attention in boosting luminol‐O 2 electrochemiluminescence (ECL). However, tuning for efficient and selective catalytic O activation to switch anodic/cathodic ECL is very challenging. Herein, we report enzyme‐inspired Fe‐based single‐atom catalysts axial N/C coordination structures (FeN 5 , FeN 4 © SACs) can specific ROS cathodic/anodic conversion. Mechanistic studies reveal sites prefer produce highly active hydroxyl radicals afford direct cathodic luminescence by promoting the cleavage of O−O bonds through N‐induced electron redistribution. In contrast, tend superoxide radicals, resulting inefficient anodic ECL. Benefiting from enhanced ECL, SAC‐based immunosensor was constructed sensitive detection cancer biomarkers.
Language: Английский
Citations
35
Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(52)
Published: Oct. 2, 2023
Integration of CO2 capture capability from simulated flue gas and electrochemical reduction reaction (eCO2 RR) active sites into a catalyst is promising cost-effective strategy for carbon neutrality, but great difficulty. Herein, combining the mixed breakthrough experiments eCO2 RR tests, we showed that an Ag12 cluster-based metal-organic framework (1-NH2 , aka bpy-NH2 ), simultaneously possessing as "CO2 relays" sites, can not only utilize its micropores to efficiently (CO2 : N2 =15 85, at 298 K), also catalyze adsorbed CO with ultra-high conversion 60 %. More importantly, performance (a Faradaic efficiency (CO) 96 % commercial current density 120 mA cm-2 very low cell voltage -2.3 V 300 hours full-cell energy 56 %) under atmosphere close 100 atmosphere, higher than those all reported catalysts potentials atmosphere. This work bridges gap between enrichment/capture RR.
Language: Английский
Citations
34
SusMat, Journal Year: 2023, Volume and Issue: 3(4), P. 498 - 509
Published: Aug. 1, 2023
Abstract Nickel‐nitrogen‐carbon single‐atom catalysts have attracted widespread interest for CO 2 electroreduction but they suffer from poor stability. Herein, we report on the preparation of Cl‐ and N‐doped porous carbon nanosheets with atomically dispersed NiN 4 Cl active sites (NiN Cl‐ClNC) through a molten‐salt‐assisted pyrolysis strategy. The optimized Cl‐ClNC catalyst delivers exceptional conversion activity outstanding stability over 220 h at −0.7 V versus RHE high Faradaic efficiency 98.7% partial current density 12.4 mA cm ‒2 . Moreover, displays remarkable approximately 349.4 −2 in flow‐cell, meeting requirements industrial applications. Operando attenuated total reflectance surface‐enhanced infrared absorption spectroscopy functional theory calculations are used to understand Results reveal that introduced axial Ni‐Cl bond Ni center Cl─C support synergetically induce electronic delocalization, which not only stabilizes against leaching also facilitates formation COOH* intermediate is found be rate‐determining step.
Language: Английский
Citations
33
Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(19)
Published: Feb. 20, 2023
Abstract Single‐atom catalysts (SACs) are appealing next‐generation for various electrochemical technologies. Along with significant breakthroughs in their initial activity, SACs now face the next challenge viable applications, insufficient operational stability. In this Minireview, we summarize current knowledge of SAC degradation mechanisms mainly based on Fe−N−C SACs, some most investigated SACs. Recent studies isolated metal, ligand, and support degradations introduced, underlying fundamentals each path categorized into active site density (SD) turnover frequency (TOF) losses. Finally, discuss challenges prospects future outlook stable
Language: Английский
Citations
27
Journal of Materials Chemistry A, Journal Year: 2023, Volume and Issue: 11(24), P. 12643 - 12658
Published: Jan. 1, 2023
We provide comprehensive analyses of various methods to regulate the electronic structure single-atom catalysts, which have shown great promise for optimizing electrochemical energy conversion efficiency.
Language: Английский
Citations
27
Nano Letters, Journal Year: 2023, Volume and Issue: 23(15), P. 7046 - 7053
Published: July 20, 2023
Selective electroreduction of CO2 to C1 feed gas provides an attractive avenue store intermittent renewable energy. However, most the CO2-to-CO catalysts are designed from perspective structural reconstruction, and it is challenging precisely design a meaningful confining microenvironment for active sites on support. Herein, we report local sulfur doping method tune electronic structure isolated asymmetric nickel–nitrogen–sulfur motif (Ni1-NSC). Our Ni1-NSC catalyst presents >99% faradaic efficiency under high current density −320 mA cm–2. In situ attenuated total reflection surface-enhanced infrared absorption spectroscopy differential electrochemical mass spectrometry indicated that show significantly weaker binding strength *CO lower kinetic overpotential CO2-to-CO. Further theoretical analysis revealed enhanced reduction reaction performance was mainly due effectively decreased intermediate activation
Language: Английский
Citations
26
Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(42)
Published: Sept. 1, 2023
Solvent effect plays an important role in catalytic reaction, but there is little research and attention on it electrochemical CO2 reduction reaction (eCO2 RR). Herein, we report a stable covalent-organic framework (denoted as PcNi-im) with imidazole groups new electrocatalyst for eCO2 RR to CO. Interestingly, compared neutral conditions, PcNi-im not only showed high Faraday efficiency of CO product (≈100 %) under acidic conditions (pH ≈ 1), also the partial current density was increased from 258 320 mA cm-2 . No obvious degradation observed over 10 hours continuous operation at 250 The mechanism study shows that group can be protonated form cation media, hence reducing surface work function charge active metal center. As result, poisoning weakened key intermediate *COOH stabilized, thus accelerating rate.
Language: Английский
Citations
25