Rh/UiO-66-NH_2催化1,4-丁炔二醇加氢性能研究
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摘要
采用浸渍法将Rh Cl3浸渍于Ui O-66-NH2上,用异丙醇还原,制得Rh/Ui O-66-NH2催化剂,考察了催化剂活性中心金属Rh与底物1,4-丁炔二醇(BYD)物质的量比、反应温度、H2压力、反应时间等因素对1,4-丁炔二醇加氢制备1,4-丁烯二醇的影响。结果表明,Rh/Ui O-66-NH2催化剂负载量为5%时,以甲醇作为溶剂,催化剂活性中心金属Rh与底物1,4-丁炔二醇物质的量比1∶4 000,反应温度为140℃,H2压力4 MPa,反应时间30 min时,1,4-丁炔二醇转化率99. 2%,1,4-丁烯二醇选择性90. 8%。
RhCl3 on Ui O-66-NH2,which prepared by hydrothermal synthesis of Zr Cl4 and 2-amino terephthalic acid,and followed reduced by isopropanol to obtain the Rh/Ui O-66-NH2 catalyst. The hydrogenation influencing factors of the preparation 2-butene-1,4-diol,which including the ratio of the amount of the catalyst active center Rh to substance 2-butyne-1,4-diol,and the reaction temperature,H2 pressure,reaction time were investigated. The results show that under the optimal conditions of the proportion of catalyst active center Rh and substrate was 1 ∶ 4 000,the reaction temperature was 140 ℃,H2 pressure was4 MPa,reaction time was 30 min,the 2-butyne-1,4-diol conversion rate was 99. 2%,and the selectivity2-butene-1,4-diol was 90. 8% respectively.
RhCl3 on Ui O-66-NH2,which prepared by hydrothermal synthesis of Zr Cl4 and 2-amino terephthalic acid,and followed reduced by isopropanol to obtain the Rh/Ui O-66-NH2 catalyst. The hydrogenation influencing factors of the preparation 2-butene-1,4-diol,which including the ratio of the amount of the catalyst active center Rh to substance 2-butyne-1,4-diol,and the reaction temperature,H2 pressure,reaction time were investigated. The results show that under the optimal conditions of the proportion of catalyst active center Rh and substrate was 1 ∶ 4 000,the reaction temperature was 140 ℃,H2 pressure was4 MPa,reaction time was 30 min,the 2-butyne-1,4-diol conversion rate was 99. 2%,and the selectivity2-butene-1,4-diol was 90. 8% respectively.
引文
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[2]王劭泓.丁炔二醇催化加氢制备丁烯二醇工艺研究[D].上海:华东理工大学,2004.
[3]李想,张艳梅,张静,等. Ui O-66-NH2负载Pd催化剂的合成、表征及其催化反应[J].辽宁石油化工大学学报,2017,37(1):8-13.
[4]张永飞.金属有机骨架材料及其复合物的制备和性能研究[D].合肥:安徽大学,2014:50-60.
[5] Xamena F X L I,Abad A,Corma A,et al. MOFs as catalysts:Activity,reusability and shape-selectivity of a Pdcontaining MOF[J]. Journal of Catalysis,2007,250(2):294-298.
[6] Zhang M,Yang Y,Li C,et al. PVP-Pd@ZIF-8 as highly efficient and stable catalysts for selective hydrogenation of1,4-butynediol[J]. Catalysis Science&Technology,2014,4(2):329-332.
[7]李闯,张明明,邸鑫,等.一步法合成Pt@ZIF-8及其在1,4-丁炔二醇选择加氢中的应用[J].催化学报,2016,37(9):1555-1561.
[8] Yin D,Li C,Ren H,et al. Efficient Pd@MIL-101(Cr)hetero-catalysts for 2-butyne-1,4-diol hydrogenation exhibiting high selectivity[J]. RSC Advances,2017,7(3):1626-1633.
[9] Yuan G,Tian Y,Liu J,et al. Schiff base anchored on metal-organic framework for Co(II)removal from aqueous solution[J]. Chemical Engineering Journal,2017,326:691-699.
[10]任勇,袁涛,刘德蓉,等.基于Cu-Fc配位聚合物衍生的Pt-Cu/CuxFeyO@C催化1,4-丁炔二醇加氢性能研究[J].分子催化,2018,32(1):8-17.
[11] Yuan Qingqing,Zhang Damin,Lennart van Haandel,et al. Selective liquid phase hydrogenation of furfural to furfuryl alcohol by Ru/Zr-MOFs[J]. Journal of Molecular Catalysis A:Chemical,2015(406):58-64.
[12]韩易潼,刘民,李克艳,等.高稳定性金属有机骨架Ui O-66的合成与应用[J].应用化学,2016,33(4):367-378.