Engineering Dual Sites into the Confined Nanospace of the Porphyrinic Metal–Organic Framework for Tandem Transformation of CO₂ to Ethylene

ACS Sustainable Chemistry & Engineering, Год журнала: 2024, Номер 12(16), С. 6093 - 6101

Опубликована: Март 12, 2024

The electrocatalytic CO2 reduction reaction (CO2RR) to produce multicarbon (C2+) products such as ethylene (C2H4) is a promising method achieve carbon neutrality, but it very difficult due the high activation barrier of and low selectivity CO2RR especially for C2+ products. Herein, copper single atoms (Cu-SAs) were confined into nanospace an iridium porphyrin-based metal–organic framework (Ir-PCN-222) form (MOF) composite (Cu-SAs@Ir-PCN-222-PA) with dual active sites Ir-porphyrin Cu-SAs through precoordination confinement strategy. Catalytic results disclosed that Cu-SAs@Ir-PCN-222-PA could drive C2H4 faradaic efficiency (FE) (70.9%) current density 20.4 mA·cm–2. When H-cell was replaced by flow cell, be increased 161 mA·cm–2 still FE (66.9%). Mechanism studies suggested in Cu-SAs@Ir-PCN-222-PA-catalyzed electroreduction reaction, CO first generated on then moved adsorbed *CO intermediate nearby Cu-SAs, after that, C–C coupling process carried out provide product C2H4. This work offers new kind MOF electrocatalysts generate

Язык: Английский

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Acceleration of the charge transfer rate for efficient photocatalytic hydrogen production via adjusting modulator and introducing electronic bridge dual strategies

Fuel, Год журнала: 2024, Номер 366, С. 131252 - 131252

Опубликована: Март 8, 2024

Язык: Английский

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Precise immobilization of metal single atoms into a porphyrinic metal-organic framework for an efficient alkene hydrosilylation

Nano Research, Год журнала: 2024, Номер 17(7), С. 5914 - 5921

Опубликована: Апрель 11, 2024

Язык: Английский

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2D Copper–Porphyrin Metal–Organic Framework Nanosheet‐Photosensitized TiO₂ for Efficiently Broadband Light‐Driven Conversion of CO₂ to CH₄

Solar RRL, Год журнала: 2024, Номер 8(9)

Опубликована: Март 26, 2024

The effective utilization of light is crucial in the use solar energy for CO 2 conversion into valuable fuels and chemicals, which improving photocatalytic materials’ capacity to absorb a key. Herein, 2D copper–porphyrin metal−organic framework (MOF)‐photosensitized titania, TiO /Zn–CuTCPP, reported, can wide range photoreduce with high efficiency under full spectrum irradiation. Fluorescence spectral analysis elucidates relationship between activity electron–hole separation efficiency. In addition, mechanistic information obtained from electron paramagnetic resonance situ infrared analyses demonstrates that presence Cu–N 4 site MOF structure conducive generation hydrogen free radicals (•H), plays key role formation intermediates, thus facilitating hydrogenation reaction process. Consequently, /Zn–CuTCPP significantly enhances CH yield 14 times higher than P25.

Язык: Английский

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One-pot synthesis of multivariate porphyrinic metal-organic frameworks with the insertion of metallobipyridine and the cooperative catalysis for carbonyl hydrosilylation

Applied Materials Today, Год журнала: 2024, Номер 38, С. 102208 - 102208

Опубликована: Апрель 30, 2024

Язык: Английский

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Carbon Capture Advancements in Metal-Organic Frameworks

Опубликована: Авг. 9, 2024

Global growth and sustainability highly depend upon the output of industries, corporations, governments, non-governmental organisations requiring comprehensive energy transition in face a worldwide crisis demanding carbon neutralisation. The neutralisation challenges required for could be overcome by detailed surveying, recording analysis dioxide emissions. It is crucial to study innovative materials like metal-organic frameworks their transdisciplinary applications towards capture have sustainable strategy harmful In addition, CO2 solubility, adsorption absorption capacity, several reinforcing characteristics factors using MOFs are discussed detail. Further, various multidisciplinary commercialisation, parameters were considered. Moreover, essential organic qualities organo-derivatives considerably elaborated. Overall, align with current development goals, it significant that emissions must reduced along its scientific manner. Relevant projections through been reviewed industrially universally alignment United Nations Sustainable Development Goals (UNSDGs).

Язык: Английский

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Engineering a pyrene MOF composite photocatalyst toward the formation of carbon dioxide radical anion through regulating the charge transfer from type-II to Z-scheme via a chemical bond-modulated strategy

Inorganic Chemistry Frontiers, Год журнала: 2024, Номер 11(23), С. 8489 - 8501

Опубликована: Янв. 1, 2024

A new approach was reported for regulating the charge transfer mechanism in a pyrene-based MOF composite, transitioning from type-II to Z-scheme configuration.

Язык: Английский

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Precise Control of Regioselective N¹ and N²-Alkylation of Benzotriazoles with α-Diazoacetates by Metalloporphyrin

Inorganic Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Янв. 2, 2025

Regioselective

Язык: Английский

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Influence of Electron-Inducted effect of ligand on electrocatalytic reduction of CO2 by copper phthalocyanine

Chemical Engineering Journal, Год журнала: 2025, Номер unknown, С. 160154 - 160154

Опубликована: Фев. 1, 2025

Язык: Английский

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Achieving Diverse CO₂ Conversions through On-Demand Installation of Multivariate Catalytic Sites into One Prototypical Metal–Organic Framework

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Май 30, 2025

The programmable design and construction of multirole or swing-role metal-organic frameworks (MR/SR-MOFs) for variable CO2 conversions are appealing green sustainable chemistry. Herein, we describe a facile MR/SR-MOF synthetic strategy on-demand engineering the catalytic pore spaces in primitive MOF diverse chemical fixation. Distinct functional groups can be precisely quantitively immobilized into prototypical LIFM-28 (proto-LIFM-28) by virtue postsynthesis based on its solid-state dynamic attribute, generating different suitable hydrosilylation, N-methylation, cycloaddition, cyclization reactions CO2. Remarkably, resultant LIFM-DSL-3 carrying amino CO2-masked N-heterocyclic carbene (NHC-CO2) sites presents an excellent hydrosilylation performance with complete Ph2SiH2 conversion (>99%) high silyl methoxide (SMO) selectivity (95%) under atmospheric pressure, achieving extraordinary turnover number (TON) 4367 frequency (TOF) 6221 h-1 beneficial efficient methanol release upon hydrolysis. Moreover, exceptionally N-methylation efficiency is obtained transformation via N-methylation. This work demonstrates how to MR/SR-MOFs as multivariate platform cost-saving applications through manipulation installation active single matrix without de novo synthesis.

Язык: Английский

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