醋酸溶液中Pd/C催化瓦斯选择氧化制甲醇  

Selective Oxidation of Mine Gas to Methanol in Acetic Acid Solution over Pd /C Catalyst

作　　者：徐锋[1] 贾韶洋 朱丽华[1] 胡成秋 陈文胜[1] 李定启[1] 王伟[1] 

机构地区：[1]黑龙江科技大学安全工程学院,黑龙江哈尔滨150022 [2]七台河宝泰隆煤化工股份有限公司,黑龙江七台河154603

出　　处：《佳木斯大学学报（自然科学版）》2014年第3期471-474,共4页Journal of Jiamusi University：Natural Science Edition

基　　金：黑龙江省教育厅科学技术研究项目(12511481)

摘　　要：为有效利用瓦斯资源,研究了瓦斯选择氧化制甲醇的反应条件及机理.以PdCl2为前驱体,采用浸渍法制备了Pd/C催化剂,进而对醋酸水溶液中Pd/C催化瓦斯选择氧化制甲醇的反应条件进行了实验研究,结果表明,目标产物甲醇生成量与催化剂添加量、对苯醌用量、溶剂中CH3COOH与H2O的混合比例、反应温度和反应时间正相关.采用3%Pd/C为催化剂时,在3%Pd/C添加量2g、对苯醌用量1000μmol、CH3COOH与H2O体积比4:1、反应温度130℃、反应时间3h条件下,甲醇的生成量为1960μmol.此外,利用瓦斯选择氧化实验和XRD谱图表征技术研究了Pd/C催化剂循环使用对瓦斯氧化制甲醇的影响.分析实验结果,认为Pd/C在醋酸溶液中催化瓦斯选择氧化制甲醇反应,既遵循亲电取代机理,又遵循活性氧物种氧化机理.This paper referred to the catalyst prepared by taking PdCl 2 as the precursor , and investigated the reaction conditions of the selective oxidation of mine gas to methanol in the aqueous solution of acetic acid o -ver Pd/C catalyst.The results show that the production of the target product , i.e.methanol is positively related to the addition of the catalyst , the addition of p-benzoquinone , the mixing proportion of CH 3 COOH and H2 O in the solvent , the temperature and time of reaction .In case of the use of 3%Pd/C as the catalyst , the production of methanol is 1960μmol in the condition that the addition of the 3%Pd/C is 2g, the addition of p-benzoqui-none is 1000μmol, the volume ratio between CH 3 COOH and H2 O is 4：1, the temperature is 130℃, and the re-action time is 3h.Moreover, effect of recycled Pd/C catalyst on selective oxidation of mine gas to methanol is studied .The methanol synthesized by catalyzing the selective oxidation of gas in the acetic acid solution through Pd/C may be the result for the joint action of electrophilic substitution reaction and oxidation of reactive oxygen species .

关 键 词：PD C 醋酸 瓦斯 甲醇 机理 选择氧化 

分 类 号：X936[环境科学与工程—安全科学] TQ223.1[化学工程—有机化工]