Ligand engineering towards electrocatalytic urea synthesis on a molecular catalyst

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Окт. 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

Язык: Английский

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Electrocatalytic Reduction of Carbon Dioxide to High-Value Multicarbon Products with Metal–Organic Frameworks and Their Derived Materials

ACS Materials Letters, Год журнала: 2022, Номер 4(11), С. 2058 - 2079

Опубликована: Сен. 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

Язык: Английский

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Porphyrin- and phthalocyanine-based systems for rechargeable batteries

Energy storage materials, Год журнала: 2022, Номер 52, С. 495 - 513

Опубликована: Авг. 18, 2022

Язык: Английский

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A Machine Learning Model To Predict CO₂ Reduction Reactivity and Products Transferred from Metal-Zeolites

ACS Catalysis, Год журнала: 2022, Номер 12(19), С. 12336 - 12348

Опубликована: Сен. 27, 2022

Various reactive intermediates and Cn products from carbon dioxide reduction reaction (CO2RR) play critical roles in the chemical fuel industry. Developing easily accessible activity descriptors to predict possible of CO2RR is great importance. The free energy changes (ΔG) for all intermediate product probability (P) CO2 methanol, methane, formaldehyde on 26 single-atom catalysts (SACs) zeolites were predicted by density functional theory (DFT) calculations machine learning (ML) models. adsorption energies ΔG*OH ΔG*O*CH2 highly correlated with catalytic activity. Producing methanol was favorable metal-zeolites early transition metals main group elements. Methane production more feasible some systems such as Co-zeolite, due low high selectivity against hydrogen evolution reaction. Both XGBoost ExtraTrees algorithms could give satisfactory predictions ΔG P using pathways, metal, charge transfer (CT) between metal intermediate, bond interaction zeolite framework, geometry. global electronegativity difference (δχT) average ionization (δIE) metal-zeolite introduced features (along valence electron number atomic species) prediction CT values without need DFT calculations. feature be replaced additional band gap (Eg) or coordination training ML models prediction. an external test MOFs, 2D materials, molecular complex materials indicate that proposed are general change SACs CO2RR.

Язык: Английский

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Enhanced electronic interaction between iron phthalocyanine and cobalt single atoms promoting oxygen reduction in alkaline and neutral aluminum-air batteries

Chemical Engineering Journal, Год журнала: 2022, Номер 450, С. 138213 - 138213

Опубликована: Июль 21, 2022

Язык: Английский

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Iron and Nickel Phthalocyanine‐Modified Nanocarbon Materials as Cathode Catalysts for Anion‐Exchange Membrane Fuel Cells and Zinc‐Air Batteries**

ChemElectroChem, Год журнала: 2022, Номер 9(20)

Опубликована: Сен. 13, 2022

Abstract Iron and nickel phthalocyanines along with different carbon supports, i. e., multi‐walled nanotubes (MWCNT), graphene, carbide‐derived carbon, Vulcan mesoporous (MC, from Pajarito Powder, LLC), are used to prepare six bimetallic (Fe, Ni) N‐doped carbon‐based catalysts. The aim of this work is investigate the electrocatalytic activity bimetal phthalocyanine‐modified nanocarbon catalysts, e. g., effect supports on oxygen reduction reaction (ORR) evolution (OER), including anion‐exchange membrane fuel cell (AEMFC) rechargeable zinc‐air battery (RZAB) configuration. catalysts exhibit excellent as exemplified by their half‐wave potential ( E 1/2 ) for ORR at which OER current density reaches 10 mA cm −2 j =10 ), but best performing FeNiN−MC =0.88 V, =1.58 V) FeNiN−MWCNT =0.87 =1.59 V). In AEMFC analyses, cathode provides peak power P max 406 mW , slightly higher than that =386 ). Both a good RZAB performance 85 FeNiN−MWCNT). assembled RZABs run stably 48 h without any significant loss performance.

Язык: Английский

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Photoelectrochemical sensors based on paper and their emerging applications in point-of-care testing

Biosensors and Bioelectronics, Год журнала: 2023, Номер 236, С. 115400 - 115400

Опубликована: Май 28, 2023

Язык: Английский

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Developments in electrocatalysts for electrocatalytic hydrogen evolution reaction with reference to bio-inspired phthalocyanines

International Journal of Hydrogen Energy, Год журнала: 2023, Номер 48(44), С. 16569 - 16592

Опубликована: Фев. 2, 2023

Язык: Английский

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Organic macrocycle-polyoxometalate hybrids

Coordination Chemistry Reviews, Год журнала: 2023, Номер 481, С. 215039 - 215039

Опубликована: Фев. 3, 2023

Язык: Английский

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Mixed‐metal Ionothermal Synthesis of Metallophthalocyanine Covalent Organic Frameworks for CO₂ Capture and Conversion

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(38)

Опубликована: Авг. 3, 2023

Phthalocyanines (PCs) are intriguing building blocks owing to their stability, physicochemical and catalytic properties. Although PC-based polymers have been reported before, many suffer from relatively low crystallinity, surface areas. Utilizing a mixed-metal salt ionothermal approach, we report the synthesis of series metallophthalocyanine-based covalent organic frameworks (COFs) starting 1,2,4,5-tetracyanobenzene 2,3,6,7-tetracyanoanthracene form corresponding COFs named M-pPPCs M-anPPCs, respectively. The obtained followed Irving-Williams in metal contents, areas, pore volume featured excellent CO2 uptake capacities up 7.6 mmol g-1 at 273 K, 1.1 bar. We also investigated growth Co-pPPC Co-anPPC on highly conductive carbon nanofiber demonstrated high activity electrochemical reduction, which showed Faradaic efficiencies towards CO 74 % -0.64 V vs. RHE.

Язык: Английский

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