沉淀过程对锰孔雀石结构及其演化过程的影响  

Influence of the precipitation process on the structure and evolution of manganese malachite

作　　者：陈帅帅[1] 陈鑫超 凌晨[1] 蒋新[1] CHEN Shuaishuai;CHEN Xinchao;LING Chen;JIANG Xin(Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology,College of Chemical and Biological Engineering,Zhejiang University,Hangzhou 310027,Zhejiang,China)

机构地区：[1]浙江大学化学工程与生物工程学院,浙江省化工高效制造技术重点实验室,浙江杭州310027

出　　处：《化工进展》2020年第5期1707-1713,共7页Chemical Industry and Engineering Progress

基　　金：国家自然科学基金(21676236);国家重点研发计划(2017YFC0211802)。

摘　　要：锰孔雀石中的Mn含量对其后续演变和Cu-Mn催化剂的活性有重要的影响。本文利用搅拌釜反应器和微反应器制备了铜锰的碱式碳酸盐共沉淀物,研究了混合过程对Cu^2+、Mn^2+的共沉淀反应过程及共沉淀产物的后续演变过程的影响。采用X射线衍射(XRD)、热重质谱联用(TG-MS)、氢气程序升温还原(H2-TPR)分析了前体、催化剂的结构及演变过程。研究发现,在混合较好的微反应器制备的样品中,锰孔雀石中的极限Mn质量分数为25%左右,明显高于文献研究从搅拌釜中得到的数值。通过对扩散-反应过程的分析发现,反应过程中的混合效果越好,制备得到的前体中锰孔雀石的含量越多且其中的锰含量越高。高锰含量的锰孔雀石在焙烧时会形成更多的Cu-Mn界面,进而产生更多的高温碳酸盐,最终的铜锰催化剂中Cu、Mn相互作用更强,催化活性更高。The Mn content in manganese malachite has an important influence on its subsequent evolution and the activity of Cu-Mn catalyst.A series of copper manganese co-precipitate were prepared by using a batch reactor and several different microreactors,and the effect of the mixing on the coprecipitation of Cu2+and Mn2+and the evolution of precipitate was investigated.X-ray diffraction(XRD),thermogravimetry-mass spectrometry(TG-MS)and hydrogen temperature programmed reduction(H2-TPR)were used for analyzing the structure of the precursors and catalysts.The results indicated that the limit Mn content in manganese malachite prepared by the microreactors with better mixing was about 25%,which was significantly higher than the value reported in the literature.The analysis of diffusionreaction process revealed that as the mixing increased during the precipitation process,more manganese malachite with higher Mn content was formed in precursors.During the subsequent calcination,these precursors decomposed into mixed oxides with more Cu-Mn interfaces,leading to the preservation of more high-temperature carbonate.The catalysts prepared in flow pattern with excellent mixing had stronger Cu-Mn interaction and better catalytic performance.

关 键 词：锰孔雀石 微反应器 沉淀 锰含量 混合 

分 类 号：TQ426.6[化学工程]