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HiGee strategy towards large-scale synthesis of soluble covalent organic frameworks
AIChE Journal ( IF 3.7 ) Pub Date : 2022-08-25 , DOI: 10.1002/aic.17864
Yun Zhao 1 , Xiaogang Yu 1 , Xin Wen 1 , Yong Luo 1 , Zhonghua Xiang 1 , Jian‐feng Chen 1
Affiliation  

The scale-up synthesis of covalent organic frameworks (COFs) with uniform structure and properties is of great importance for their practical applications. Here, we proposed a facile way to massively produce phthalocyanine-like COFs (COFBTC) via high-gravity intensified synthesis. Alcoholic solvent and basic catalyst were discovered synergically improved the formation of COFBTC. High concentration and reaction temperature were beneficial for high production as well. The intensified mass and heat transfer at high-gravity promoted the scaling-up of COFBTC with homogeneous structures and properties. A high space time yield of 305.9 kg∙(m3 D)−1 was achieved for Fe-COFBTC under optimized condition. The massively produced Fe-COFBTC presented good solubility in alkaline and polar organic solvents, thus allow to process as homogeneous or heterogenous electrocatalyst for oxygen reduction reaction. The catalyst exhibited good performance of 0.79 V (vs. RHE, half-wave) and >95% recovery in homogeneous electroreduction of O2 in 0.1 M KOH. A superior performance of 0.86 V was achieved by sol–gel-like processing of Fe-COFBTC on carbon paper due to the enhanced conductivity. The scale-up soluble catalysts with uniform properties provide more opportunities for practical applications of COFBTC.

中文翻译:

HiGee 大规模合成可溶性共价有机框架的策略

具有均匀结构和性能的共价有机框架(COF)的放大合成对其实际应用具有重要意义。在这里,我们提出了一种通过高重力强化合成大量生产类酞菁 COF (COF BTC ) 的简便方法。发现醇类溶剂和碱性催化剂可协同改善 COF BTC的形成。高浓度和高反应温度也有利于高产。高重力下强化的传质和传热促进了具有均匀结构和性能的 COF BTC的放大。Fe-COF BTC实现了305.9 kg∙(m 3  D) −1的高时空产率优化条件下。大量生产的 Fe-COF BTC在碱性和极性有机溶剂中具有良好的溶解性,因此可以作为均相或多相电催化剂进行氧还原反应。该催化剂在 0.1 M KOH 中的 O 2均相电还原中表现出 0.79 V(相对于 RHE,半波)和 >95% 回收率的良好性能。由于增强的导电性,通过类溶胶凝胶处理 Fe-COF BTC在碳纸上实现了 0.86 V 的优异性能。性能均匀的可溶性催化剂的放大为COF BTC的实际应用提供了更多机会。
更新日期:2022-08-25
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