基于Cu/Beta沸石催化的生物质模型分子氧化裂解研究  

Oxidative cleavage of biomass model molecules catalyzed by Cu-Beta zeolite

作　　者：王鹏森 吴志强[1] P.Emayavaramban 杨伯伦[1,2] WANG Peng-sen;WU Zhi-qiang;P.Emayavaramban;YANG Bo-lun(School of Chemical Engineering and Technology,Xi’an Jiaotong University,Xi’an 710049,China;State Key Laboratory of Multiphase Flow in Power Engineering,Xi’an Jiaotong University,Xi’an 710049,China)

机构地区：[1]西安交通大学化学工程与技术学院,陕西西安710049 [2]西安交通大学动力工程多相流国家重点实验室,陕西西安710049

出　　处：《高校化学工程学报》2021年第6期1010-1019,共10页Journal of Chemical Engineering of Chinese Universities

基　　金：国家自然科学基金重点项目(22038011)。

摘　　要：为了裂解生物质有机大分子的C─C键,提出铜负载的脱铝H-Beta沸石作为催化剂的非均相氧化方法。以苯基乙二醇作为模型反应物,通过催化剂制备工艺探讨、物性测试、反应活性表征、稳定性试验等系列工作,考察所制催化剂的有效性。研究表明:断键反应需在催化剂和氧气同时存在的情况下才可以进行;使用高级醇代替甲醇作为溶剂时,反应有较高的转化率和较高的苯甲醛选择性。机理分析可知:1,2-二醇的氧化裂解是Bronsted酸和Lewis酸协同作用的结果,Cu对分子筛晶格中Al的取代,以及Cu^(+)变为Cu^(2+)的自身的循环,可有效提高催化剂C─C键的断裂能力。In order to cleave C─C bonds of biomass organic macromolecules,a copper-loaded dealuminated H-Beta zeolite catalyst was proposed for heterogeneous oxidation.Using 1-phenyl-1,2-ethanediol as a model reactant,the performance of the prepared catalysts was investigated through catalyst preparation process discussion,physical property testing,reactivity characterization and stability tests.The results show that the cleavage reaction can only be carried out in the presence of both catalyst and oxygen.The reaction had a high conversion and benzaldehyde selectivity when using higher alcohols instead of methanol as solvent.The mechanism analysis shows that the oxidative cleavage of 1,2-diol is resulted from synergistic effects of Bronsted acid and Lewis acid,and the substitution of Cu for Al in the lattice of molecular sieve,and in the cycle of Cu^(+) to Cu^(2+),can adjust the acidity and acid amount of the catalyst,which effectively improves C─C bond breaking ability of the catalyst.

关 键 词：生物质 苯基乙二醇 沸石改性 氧化裂解 反应机理分析 

分 类 号：TQ203.2[化学工程—有机化工]