Hydrophobicity Tailoring of Ferric Covalent Organic Framework/MXene Nanosheets for High‐Efficiency Nitrogen Electroreduction to Ammonia

Advanced Science, Journal Year: 2023, Volume and Issue: 10(15)

Published: March 30, 2023

Abstract Electrocatalytic nitrogen reduction reaction (NRR) represents a promising sustainable approach for NH 3 synthesis. However, the poor NRR performance of electrocatalysts is great challenge at this stage, mainly owing to their low activity and competitive hydrogen evolution (HER). Herein, 2D ferric covalent organic framework/MXene (COF‐Fe/MXene) nanosheets with controllable hydrophobic behaviors are successfully prepared via multiple‐in‐one synthetic strategy. The boosting hydrophobicity COF‐Fe/MXene can effectively repel water molecules inhibit HER enhanced performances. By virtue ultrathin nanostructure, well‐defined single Fe sites, enrichment effect, high hydrophobicity, 1H,1H,2H,2H‐perfluorodecanethiol modified hybrid shows yield 41.8 µg h −1 mg cat. Faradaic efficiency 43.1% −0.5 V versus RHE in 0.1 m Na 2 SO 4 solution, which vastly superior known Fe‐based catalysts even noble metal catalysts. This work provides universal strategy design synthesis non‐precious high‐efficiency N .

Language: Английский

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Structural Regulation of Covalent Organic Frameworks for Catalysis

Accounts of Chemical Research, Journal Year: 2024, Volume and Issue: 57(8), P. 1214 - 1226

Published: March 29, 2024

ConspectusChemical reactions can be promoted at lower temperatures and pressures, thereby reducing the energy input, by introducing suitable catalysts. Despite its significance, quest for efficient stable catalysts remains a significant challenge. In this context, addressing efficiency of stands out as paramount concern. However, challenges posed vague structure limited tailorability traditional would make it highly desirable to fabricate optimized based on understanding structure–activity relationships. Covalent organic frameworks (COFs), subclass fully designed crystalline materials formed polymerization building blocks through covalent bonds have garnered widespread attention in catalysis. The precise customizable structures COFs, coupled with attributes such high surface area facile functional modification, COFs attractive molecular platforms catalytic applications. These inherent advantages position ideal catalysts, facilitating elucidation structure-performance relationships further improving Nevertheless, there is lack systematic emphasis summary structural regulation atomic/molecular level COF Consequently, growing need summarize research field provide deep insights into COF-based catalysis promote development.In Account, we will recent advances achieved placing an design enhanced Considering unique components present fundamental principles rational This Account starts presenting overview explaining why are promising Then, introduce principle Next, following three aspects specific strategies catalysts: (1) By designing different groups integrating metal species unit, activity and/or selectivity finely modulated. (2) Regulating linkage facilitates charge transfer modulates electronic sites, accordingly, intrinsic activity/selectivity improved. (3) means pore wall/space engineering, microenvironment surrounding sites modulated optimize performance. Finally, current future developments discussed detail. provides insight toward their performance, which inspiration other heterogeneous

Language: Английский

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Covalent Organic Frameworks as Promising Platforms for Efficient Electrochemical Reduction of Carbon Dioxide: A Review

Small Structures, Journal Year: 2024, Volume and Issue: 5(5)

Published: Feb. 5, 2024

In current research, achieving carbon neutrality has become a primary focus through the utilization of various conversion technologies that transform dioxide (CO 2 ) into valuable chemicals or fuels. Covalent organic frameworks (COFs), as emerging crystalline polymers, offer distinct advantages in CO compared to other materials. These include controllable nanoscale pores, predefined functional units, editable framework structures, and rich conjugated systems. The unique characteristics COFs make them highly promising electrocatalysts for conversion. This review provides comprehensive overview pioneering works recent research on COF‐based materials electrochemical reduction reaction. offers analysis design principles reactive sites, skeleton pore functionalities, 3D frameworks, morphologies, composite COFs, aiming enhance electrocatalysis. Finally, this presents some recommendations material design, reaction mechanisms, theoretical computations understanding mechanisms further facilitate high‐performance electrocatalysts.

Language: Английский

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Asymmetric Atomic Dual‐Sites for Photocatalytic CO₂ Reduction

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(38)

Published: July 23, 2024

Abstract Atomically dispersed active sites in a photocatalyst offer unique advantages such as locally tuned electronic structures, quantum size effects, and maximum utilization of atomic species. Among these, asymmetric dual‐sites are particular interest because their charge distribution generates local built‐in electric potential to enhance separation transfer. Moreover, the dual provide flexibility for tuning complex multielectron multireaction pathways, CO 2 reduction reactions. The coordination opens new possibilities engineering structure–activity–selectivity relationship. This comprehensive overview discusses efficient sustainable photocatalysis processes photocatalytic reduction, focusing on strategic active‐site design future challenges. It serves timely reference development conversion processes, specifically exploring here exemplified by into valuable chemicals.

Language: Английский

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Harnessing visible light for sustainable biodiesel production with Ni/Si/MgO photocatalyst

Renewable and Sustainable Energy Reviews, Journal Year: 2024, Volume and Issue: 208, P. 115033 - 115033

Published: Nov. 2, 2024

Language: Английский

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