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Fabrication of Yolk-Shell Cu@C Nanocomposites as High-Performance Catalysts in Oxidative Carbonylation of Methanol to Dimethyl Carbonate

机译:蛋黄壳Cu @ C纳米复合材料作为甲醇氧化羰基化合成碳酸二甲酯的高性能催化剂

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摘要

A facile way was developed to fabricate yolk-shell composites with tunable Cu cores encapsulated within hollow carbon spheres (Cu@C) with an average diameter about 210 nm and cavity size about 80 nm. During pyrolysis, the confined nanospace of hollow cavity ensures that the nucleation-and-growth process of Cu nanocrystals take place exclusively inside the cavities. The size of Cu cores can be easily tuned from 30 to 55 nm by varying the copper salt concentration. By deliberately creating shell porosity through KOH chemical activation, at an optimized KOH/HCS mass ratio of 1/4, the catalytic performance for the oxidative carbonylation of methanol to dimethyl carbonate (DMC) of the activated sample is enhanced remarkably with TOF up to 8.6 h−1 at methanol conversion of 17.1%. The activated yolk-shell catalyst shows promising catalytic properties involving the reusability with slight loss of catalytic activity and negligible leaching of activated components even after seven recycles, which is beneficial to the implementation of clean production for the eco-friendly chemical DMC thoroughly.Electronic supplementary materialThe online version of this article (doi:10.1186/s11671-017-2258-7) contains supplementary material, which is available to authorized users.
机译:已开发出一种简便的方法来制造卵黄壳复合材料,其具有可调谐的铜芯,该铜芯被封装在空心碳球(Cu @ C)中,平均直径约为210 nm,腔体尺寸约为80 nm。在热解过程中,空心空腔的有限纳米空间确保了Cu纳米晶体的成核和生长过程仅发生在空腔内部。通过改变铜盐浓度可以很容易地将Cu核的尺寸从30 nm调节到55 nm。通过以KOH / HCS最佳质量比1/4的方式通过KOH化学活化故意产生壳层孔隙,使用TOF可以显着提高活化样品的甲醇氧化羰基化为碳酸二甲酯(DMC)的催化性能。 h −1 在甲醇转化率为17.1%时。活化的蛋黄-壳型催化剂显示出令人鼓舞的催化性能,包括可重复使用,催化活性略有下降,并且即使经过7次循环后活化组分的浸出也可忽略不计,这有利于彻底实现环保型化学DMC的清洁生产。材料本文的在线版本(doi:10.1186 / s11671-017-2258-7)包含补充材料,授权用户可以使用。

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