无机盐工业
主管:中海油天津化工研究设计院有限公司
主办:中海油天津化工研究设计院有限公司
   中海油炼油化工科学研究院(北京)有限公司
   中国化工学会无机酸碱盐专业委员会
ISSN 1006-4990 CN 12-1069/TQ
Catalytic Materials

钯负载锰氧化物基双金属复合氧化物催化氧化羰基化合成碳酸二苯酯

  • 苏伟 ,
  • 张林锋 ,
  • 吕庆阳 ,
  • 夏语嫣 ,
  • 袁华
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  • 武汉工程大学化学与环境工程学院,绿色化工过程省部共建教育部重点实验室,湖北武汉 430205
苏伟(1993— ),男,硕士研究生,研究方向为化工工艺、有机合成;E-mail: 380318211@qq.com。

收稿日期: 2019-03-19

  网络出版日期: 2020-06-10

基金资助

国家自然科学基金(51474160);湖北省自然科学基金(2016CFA079)

Synthesis of diphenyl carbonate by oxidative carbonylation over palladium loaded MnOx-based bimetallic oxide catalysis

  • Wei Su ,
  • Linfeng Zhang ,
  • Qingyang Lü ,
  • Yuyan Xia ,
  • Hua Yuan
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  • Key Laboratory for Green Chemical Process of Ministry of Education,Wuhan Institute of Technology School of Chemistry and Environmental Engineering,Wuhan,430205,China

Received date: 2019-03-19

  Online published: 2020-06-10

摘要

采用共沉淀法分别制备锰掺杂钨、钒、铋3种双金属复合氧化物载体,以氯化钯为活性组分制备负载型催化剂,并用于苯酚氧化羰基化合成碳酸二苯酯(DPC)。通过气相色谱(GC)、X射线衍射(XRD)、氢气程序升温还原(H2-TPR)、X射线光电子能谱(XPS)等表征手段,对催化剂结构和性能进行表征。结果表明:钨-锰载体随掺杂比例和焙烧温度升高,逐步形成四氧化三锰晶粒,同时钨渗入锰氧化物晶格中,在掺杂比(物质的量比)为1:1、焙烧温度为600 ℃条件下制备的催化剂性能最佳,DPC收率为5.20%;钒-锰载体在焙烧温度为400 ℃、掺杂比为1:5条件下形成二氧化锰晶相,催化剂性能明显提高,DPC收率为10.46%,而较高的焙烧温度会破坏晶型的完整;铋-锰载体在掺杂比为1:5、焙烧温度为400 ℃条件下制备的催化剂催化效果最好,DPC单程收率可达到13.13%。

本文引用格式

苏伟 , 张林锋 , 吕庆阳 , 夏语嫣 , 袁华 . 钯负载锰氧化物基双金属复合氧化物催化氧化羰基化合成碳酸二苯酯[J]. 无机盐工业, 2019 , 51(9) : 91 -96 . DOI: 10.11962/1006-4990.2018-0568

Abstract

The Mn-doped W,V and Bi bimetallic oxide supports were prepared by co-precipitation method.PdCl2 was used as the active component to prepare supported catalysts for synthesis of DPC by heterogeneous catalytic oxidation of phenol.The structure and properties were characterized by means of gas chromatography,X-ray diffraction,hydrogen temperature programmed reduction and X-ray photoelectron spectroscopy etc..Results showed that with the increase of tungsten-manganese doping ratio and calcination temperature,MnO grew into Mn3O4 grains gradually and infiltrated into the lattice of MnOx.Finally,the catalytic activity was best and the yield of DPC was 5.20% at a doping ratio(amount-of-substance ratio) of 1:1 and calcination at 600 ℃.For vanadium manganese oxide,higher calcination temperature will destroy the integrity of the crystal form,and formation of MnO2 at a doping ratio of 1:5 at 400 ℃ can significantly improve the property of activity,and the yield of DPC was 10.46%.The bismuth-manganese bimetallic oxide catalyst with doping ratio of 1:5 and calcination at 400 ℃ had the best catalytic effect,the one-way yield of DPC was 13.13%.

参考文献

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