A Rapid, Sustainable, One‐step Mechanochemical Strategy for Synthesizing Gold Nanoparticle‐Doped Covalent Organic Frameworks

作者：Yogendra Nailwal, Qingsong Zhang, Normanda Brown, Ziad Alsudairy, Chelsea Harrod, Md Hanif Uddin, Fazli Akram, Junrui Li, Yi Liu, Xinle Li · 发表于：Chemistry - A European Journal · 年份：2025 · DOI：10.1002/chem.202500339 · 被引用次数：11 · 研究领域：Nanomaterials for catalytic reactions、Covalent Organic Framework Applications、Catalytic Processes in Materials Science

Doping gold nanoparticles within covalent organic frameworks (AuNPs@COFs) has garnered enormous momentum due to their unique properties and broad applications. Nevertheless, prevailing multi-step synthesis is plagued with low time efficiency, eco-unfriendliness, and tedious protocols. Herein, we introduce a rapid, sustainable, scalable, one-step mechanochemical strategy for synthesizing up to four AuNPs-doped COFs via steel ball milling within an hour under ambient conditions. This approach overcomes the synthetic barriers of conventional multi-step solution-based methods, such as extended reaction times (5 days), milligram scale, the use of toxic solvents, elevated temperatures, and reliance on external reducing agents. One exemplary AuNPs@COF (AuNPs@DMTP-TPB) exhibits high crystallinity, porosity, small AuNP size, and uniform dispersion (5.4±0.6 nm), surpassing its counterpart synthesized via multi-step solution-based methods (6.4±1.1 nm). Notably, the gram-scale synthesis of AuNPs@DMTP-TPB can be successfully achieved. Control experiments suggest that the in situ formation of AuNPs is attributed to the galvanic reduction of gold precursor by stainless steel apparatus. As a proof-of-concept catalytic application, AuNPs@DMTP-TPB demonstrates remarkable catalytic activity and recyclability for the aqueous reduction of 4-nitrophenol under ambient conditions. This study provides an environmentally benign and fast pathway to synthesize AuNPs@COFs via mechanochemistry for the fir...