Promotion of Au nanoparticles on carbon frameworks for alkali-free aerobic oxidation of benzyl alcohol

IF 2.5 Q3 BIOTECHNOLOGY & APPLIED MICROBIOLOGY Frontiers in chemical engineering Pub Date : 2023-01-23 DOI:10.3389/fceng.2022.1116366
Zhongtian Du, Sen Zhang, S. Yang, Wenhao Yang, Jingjie Luo, Changhai Liang
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Abstract

We synthesized a series of modified Co-ZIF-67 materials with tunable morphology to support fine Au nanoparticles for the alkali-free aerobic oxidation of benzyl alcohol. Structure promotion was performed using Stöber silica as a hard template, which was subsequently removed by NaOH etching before gold immobilization. The texture structure of Au/(Si)C was greatly improved with increasing surface area and volume. CoOx was simultaneously introduced into the carbon shell from the Co-ZIF-67 precursor, which consequently facilitated the specific Au-support interaction via bimetallic synergy. XRD, XPS, and TEM images demonstrated the redispersion of both Au and CoOx as well as the electronic delivery between metals. Analysis of the chemical and surface composition suggested a surface rich in Auδ+ with abundant lattice oxygen contributed by CoOx in the final Au/(Si)C, which improved the transformation rate of benzyl alcohol even in an alkali-free condition. Au/(Si)C with finely dispersed Au particles showed excellent catalytic performance in the alkali-free environment, with 89.3% benzyl conversion and 74.5% benzaldehyde yield under very mild conditions.
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金纳米颗粒在碳骨架上对苯甲醇无碱好氧氧化的促进作用
我们合成了一系列具有可调形貌的改性Co-ZIF-67材料,以支持精细的金纳米颗粒用于苯甲醇的无碱好氧氧化。使用Stöber二氧化硅作为硬模板进行结构提升,随后在固定金之前通过NaOH蚀刻去除。随着表面积和体积的增加,Au/(Si)C的织构结构得到了很大的改善。CoOx同时从Co-ZIF-67前体引入碳壳,从而通过双金属协同作用促进了特定的au支持相互作用。XRD, XPS和TEM图像显示了Au和CoOx的再分散以及金属之间的电子传递。化学成分和表面组成分析表明,在最终Au/(Si)C中,表面富含Auδ+, CoOx贡献了丰富的晶格氧,即使在无碱条件下也提高了苯甲醇的转化率。Au/(Si)C在无碱环境下表现出优异的催化性能,在非常温和的条件下,苯转化率为89.3%,苯甲醛收率为74.5%。
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CiteScore
3.50
自引率
0.00%
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0
审稿时长
13 weeks
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