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摘要
采用溶胶-凝胶法合成具有高比表面积(959.72 m2/g)的发散状介孔SiO2(MSNs),制备了不同Ag负载量的Ag-CeO2/MSNs催化剂,探究了其对四氢糠醇(THFA)选择性氧化生成乙酸四氢糠酯的催化效果。当Ag的负载量为10%时催化效果最佳。在反应温度为145℃、反应压力为4 MPa、转速为325 r/min、催化剂质量为1 g的条件下,反应转化率为84%,产物选择性为81.03%。用N2-吸附脱附、XRD、XPS、SEM、TEM、FT-IR等手段对催化剂进行表征,结果表明,Ag和CeO2粒子以稳定且高度分散的状态负载于MSNs表面及发散状孔道内部;Ag-Ce存在双金属协同作用,Ag易使环氧化物C—C键断裂开环,Ce能使Ag容易吸附氧气,从而提高催化效率。催化剂重复使用5次后THFA转化率仍可达73.85%,产物选择性为78.43%。
Abstract
The sol-gel method is employed to synthesize divergent mesoporous SiO2 (MSNs) with high specific surface area (959.72 m2·g-1), from which Ag-CeO2/MSNs catalysts with different Ag loadings are prepared, and their catalytic effect on the selective oxidation of tetrahydrofurfuryl alcohol to tetrahydrofurfuryl acetate.It is found that the best catalytic effect is achieved when the loading rate of Ag is 10%.The reaction conversion reaches 84% and the selectivity of tetrahydrofurfuryl acetate reaches 81.03% at 145℃, 4 MPa, 325 r·min-1 and 1 g of catalyst.The prepared catalysts are characterized by means of N2-sorption desorption, XRD, XPS, SEM, TEM and FT-IR.It is shown that Ag and CeO2 particles are successfully loaded on the surface of MSNS and inside the divergent pore channel in a stable and highly dispersed state.There exists a bimetallic synergy between Ag and Ce.Ag can easily break out the ring of C-C bond in epoxides, while Ce can make Ag easily adsorb oxygen, thus improving the catalytic efficiency.The conversion of THFA still reaches 73.85% and the product selectivity reaches 78.43% after the catalyst has been reused for five times.
关键词
介孔二氧化硅
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四氢糠醇
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选择性氧化
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Ag-CeO2催化剂
Key words
mesoporous silica
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tetrahydrofurfuryl alcohol
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selective oxidation
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Ag-CeO2 catalyst
Author summay
陈小妮(1998-),女,硕士生,研究方向为多孔氧化硅的制备及应用,1669725303@qq.com。
发散状介孔SiO2负载Ag-CeO2催化剂选择性氧化THFA的研究[J].
现代化工, 2023, 43(12): 149-155 DOI:10.16606/j.cnki.issn0253-4320.2023.12.028