木质素湿法氧化为芳香醛反应中LaMn_(1-x)Cu_xO_3催化机理的研究  

Studies on catalysis of Cu-doped Mn-based perovskite-type oxide in wet oxidation of lignin to produce aromatic aldehydes

作　　者：邓海波[1,2] 高磊[1] 龙柱[1] 刘德陶[2] 林鹿[2] 

机构地区：[1]江南大学生态纺织教育部重点实验室,江苏无锡214122 [2]华南理工大学制浆造纸工程国家重点实验室,广州510641

出　　处：《中华纸业》2012年第18期26-30,共5页China Pulp & Paper Industry

基　　金：国家"973"计划项目(2010CB732201);国家自然科学基金项目(31100441;31000285);华南理工大学制浆造纸工程国家重点实验室开放课题资助项目(200902)

摘　　要：研究了溶胶凝胶法得到的LaMn1-xCuxO3(x=0、0.1、0.2)催化剂在木质素湿法氧化为芳香醛反应中的活性差异,旨在探讨出Cu2+取代后LaMnO3催化剂的物理性质的变化与其催化活性的关联变化机理。XRD、XPS、TPR证实了Cu2+能进入LaMnO3格结点位置,且能导致Mn4+的含量以及表面吸附氧物种含量提高。该催化剂用于木质素的湿法氧化结果证明,其催化活性随着Cu2+含量的增加而增强。催化剂催化活性变化的原因归结于Cu2+取代后引起Mn4+的含量以及表面吸附氧物种含量的变化。这也说明只要提高LaMn1-xCuxO3(0<x<1)的Cu2+的含量,就能提高其在木质素湿法氧化为芳香醛反应中的催化活性。The difference in activity of LaMn1-xCuxO3（ x = 0, 0.1, and 0.2） prepared by the sol-gel method was studied to investigate the influence of Cu substitution on the physicochemical properties to clarify the relation between perovskite properties and their catalytic behaviors in the catalytic wet aerobic oxidation（CWAO） of lignin. X-ray diffraction （XRD）, temperature-programmed reduction of H2 （H2-TPR）, and X-ray photoelectron spectroscopy （XPS） indicated that Cu and Mn are finely dispersed on the perovskite framework of the samples and an interaction between the CuZ＋and Mn3＋ sites in the perovskite lattice occurs. The samples were applied to the CWAO of lignin, and the experimental results illustrated that the catalyst activity is improved with an increase in Cu2＋ content. The variation of the catalytic activity can be ascribed to the change of content of chemisorbed oxygen and Mn4＋ from Cu substitution, which indicated that improving the content of Cu2＋ in LaMn1-xCuxO3 （0〈x〈1） can enhance the catalytic activities in the catalytic wet aerobic oxidation（CWAO）.

关 键 词：木质素 催化湿法氧化 芳香醛 Cu取代 钙钛矿 LaMn1-xCuxO3(0 

分 类 号：O643.32[理学—物理化学]