p–d Orbital Hybridization Induced by p-Block Metal-Doped Cu Promotes the Formation of C₂₊ Products in Ampere-Level CO₂ Electroreduction

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(8), С. 4675 - 4682

Опубликована: Фев. 17, 2023

Large-current electrolysis of CO2 to multi-carbon (C2+) products is critical realize the industrial application conversion. However, poor binding strength *CO intermediates on catalyst surface induces multiple competing pathways, which hinder C2+ production. Herein, we report that p-d orbital hybridization induced by Ga-doped Cu (CuGa) could promote efficient electrocatalysis at ampere-level current density. It was found CuGa exhibited highest productivity with a remarkable Faradaic efficiency (FE) 81.5% density 0.9 A/cm2, and potential such high -1.07 V versus reversible hydrogen electrode. At 1.1 still maintained an FE 76.9%. Experimental theoretical studies indicated excellent performance results from Ga, not only enriches reactive sites but also enhances intermediate facilitates C-C coupling. The strategy can be extended other p-block metal-doped catalysts, as CuAl CuGe, boost electroreduction for As far know, this first work electrochemical reduction reaction generate product interaction using catalyst.

Язык: Английский

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CxNy-based materials as gas sensors: Structure, performance, mechanism and perspective

Coordination Chemistry Reviews, Год журнала: 2024, Номер 503, С. 215653 - 215653

Опубликована: Янв. 9, 2024

Carbon nitride (CxNy) materials, characterized by an ordered two-dimensional without metal ions structure high N:C ratio, phase transition transformation, predispose them for promising applications in catalytic reaction, flexible electronics, broadband photodetectors and battery. However, up to now, its potential advantages gas sensor have yet be fully explored. This review provides a comprehensive overview of recent advances CxNy-based materials applied as substrates covering structure, properties, synthesis methods, enhancement strategies. A rigorous assessment their sensing capabilities, including sensitivity, selectivity, stability was critically summarized. Additionally, the molecule-level mechanistic aspects underlying gas-sensing working principles insights into functional properties were discussed. Furthermore, thorough investigations utilizing density theory (DFT) studies, aimed illuminating fundamental governing behavior presented detail. Finally, futuristic along with challenges CxNy deliberated herein.

Язык: Английский

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Steering the Reaction Pathway of CO₂ Electroreduction by Tuning the Coordination Number of Copper Catalysts

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(23), С. 15917 - 15925

Опубликована: Май 28, 2024

Cu-based catalysts are optimal for the electroreduction of CO2 to generate hydrocarbon products. However, controlling product distribution remains a challenging topic. The theoretical investigations have revealed that coordination number (CN) Cu considerably influences adsorption energy *CO intermediates, thereby affecting reaction pathway. with different CNs were fabricated by reducing CuO precursors via cyclic voltammetry (Cyc-Cu), potentiostatic electrolysis (Pot-Cu), and pulsed (Pul-Cu), respectively. High-CN predominantly C2+ products, while low-CN favors CH4 production. For instance, over high-CN Pot-Cu, is main product, Faradaic efficiency (FE) reaching 82.5% partial current density (j) 514.3 mA cm–2. Conversely, Pul(3)-Cu production CH4, achieving highest FECH4 value 56.7% jCH4 234.4 In situ X-ray absorption spectroscopy Raman studies further confirm adsorptions CN, directing pathway CO2RR.

Язык: Английский

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Emerging two-dimensional materials: Synthesis, physical properties, and application for catalysis in energy conversion and storage

The Innovation Materials, Год журнала: 2024, Номер 2(1), С. 100060 - 100060

Опубликована: Янв. 1, 2024

<p>Inorganic, organic, and hybrid two-dimensional (2D) materials are being developed for ever-expanding numbers of applications, though energy catalysis remain the main drivers their development. We present overviews bottom-up top-down synthetic strategies such examine manufacturing scalability issues. Mechanical, electrical, thermal properties modulation highlighted because they fundamental to above-mentioned drivers. The burgeoning importance heterostructures in materials, particularly electrode design function is stressed. Detailed attention given applications 2D electrocatalysis reactions: oxygen reduction, evolution, hydrogen carbon dioxide nitrogen reduction. Water splitting, reduction by photocatalysis also examined. A perspective expected advances expansion types with a focus on heterostructure development, presented conclusion.</p>

Язык: Английский

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The green chemistry paradigm in modern organic synthesis

Russian Chemical Reviews, Год журнала: 2023, Номер 92(12), С. RCR5104 - RCR5104

Опубликована: Дек. 1, 2023

After the appearance of green chemistry concept, which was introduced in vocabulary early 1990s, its main statements have been continuously developed and modified. Currently, there are 10–12 cornerstones that should form basis for an ideal chemical process. This review analyzes accumulated experience achievements towards design products processes reduce or eliminate use generation hazardous substances. The presents views leading Russian scientists specializing various fields this subject, including homogeneous heterogeneous catalysis, fine basic organic synthesis, electrochemistry, polymer chemistry, based on bio-renewable feedstocks energetic compounds materials. A new approach to quantitative evaluation environmental friendliness by authors is described. <br> bibliography includes 1761.

Язык: Английский

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Ternary Ionic-Liquid-Based Electrolyte Enables Efficient Electro-reduction of CO₂ over Bulk Metal Electrodes

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(21), С. 11512 - 11517

Опубликована: Май 17, 2023

Using bulk metals as catalysts to get high efficiency in electro-reduction of CO2 is ideal but challenging. Here, we report the coupling metal electrodes and a ternary ionic-liquid-based electrolyte, 1-butyl-3-methylimidazolium tetrafluoroborate/1-dodecyl-3-methylimidazolium tetrafluoroborate/MeCN realize highly efficient CO. Over various electrodes, electrolyte not only increases current density also suppresses hydrogen evolution reaction obtain Faradaic (FE) toward FECO could maintain ∼100% over wide potential range, showed very stability electrolyte. It demonstrated that aggregation behavior arrangement two kinds IL cations with different chain lengths electrochemical double layer increase wettability electrode adsorption extend diffusion channel H+, rendering FECO.

Язык: Английский

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Emerging heterostructured C₃N₄photocatalysts for photocatalytic environmental pollutant elimination and sterilization

Inorganic Chemistry Frontiers, Год журнала: 2023, Номер 10(13), С. 3756 - 3780

Опубликована: Янв. 1, 2023

Photocatalysis is deemed a highly prominent technology to solve environmental problems such as pollution, CO 2 emission and bacterial contamination.

Язык: Английский

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Lattice Strain Engineering Boosts CO₂ Electroreduction to C₂₊ Products

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(38)

Опубликована: Июль 1, 2024

Regulating the binding effect between surface of an electrode material and reaction intermediates is essential in highly efficient CO

Язык: Английский

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Improved metal-organic frameworks (MOFs) and their application in catalytic CO2 reduction: A review

Materials Today Sustainability, Год журнала: 2024, Номер 26, С. 100745 - 100745

Опубликована: Март 12, 2024

Язык: Английский

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Manipulation of Oxygen Species on an Antimony-Modified Copper Surface to Tune the Product Selectivity in CO₂ Electroreduction

Journal of the American Chemical Society, Год журнала: 2024, Номер unknown

Опубликована: Сен. 10, 2024

Rational regulation of the electrochemical CO

Язык: Английский

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