Shikai Wang , Yafan Wang , Fei Zha , Xiaohua Tang , Yue Chang , Haifeng Tian
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引用次数: 0
摘要
由1,3-二异丙苯(DIPB)催化氧化得到的1,3-二异丙苯二氢过氧化氢(DHP)的分解被称为生产间苯二酚的主要工业工艺。采用配体辅助法合成了一种高分散Fe掺杂N-C (Fe- n /P-C)催化剂,并将其应用于DIPB的过氧化反应。SEM、TEM和HAADF-STEM分析表明,Fe均匀分布在N/P-C表面。XRD、拉曼光谱、N2吸附/解吸、XPS和O2-TPD均表明,在N-C中掺杂P物质,形成更多的介孔,无序程度增加,为DIPB中叔碳-氢键的活化提供了更多的活性位点。在Fe-N/P-C质量为1.0、反应温度为90℃、氧流量为100 mL/min、反应时间为8 h的条件下,DIPB转化率为97.8% %,DHP收率为67.2% %。自由基猝灭和质谱分析表明,Fe-N/P-C参与了链的引发和链的扩展。
Highly dispersed Fe in P dopped N-C for the catalytic peroxidation of 1,3-diisopropylbenzene with molecular oxygen
The decomposition of 1,3-diisopropylbenzene dihydroperoxide (DHP) obtained by the catalytic oxidation of 1,3-diisopropylbenzene (DIPB) is known as the main industrial process to produce resorcinol. A new catalyst of highly dispersed Fe in P-doped N-C (Fe-N/P-C) was synthesized using a ligand-assisted method, and was applied for the peroxidation of DIPB. SEM, TEM and HAADF-STEM revealed that Fe is uniformly dispersed on N/P-C. XRD, Raman spectra, N2 adsorption/desorption, XPS and O2-TPD showed that doping of P species in N-C leads to form more mesopore and increases the disorder degree, providing more active sites for the activation of tertiary C-H bonds in DIPB. The conversion of DIPB was 97.8 % and the yield of DHP was 67.2 % under mass of Fe-N/P-C to DIPB was 1.0, reaction temperature was 90°C, oxygen flow rate was 100 mL/min, and reaction time was 8 h. The investigation of radical quenching and mass spectrometry suggested that the increased oxidation rate is attributed to the involvement of Fe-N/P-C in both chain initiation and chain propagation.
期刊介绍:
Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications.
Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.