改性钴催化剂催化燃烧二溴甲烷  

Catalytic combustion of dibromomethane on modified cobalt catalysts

作　　者：卢媛娇 缪长喜[1] 蒋见[1] 宋磊[1] 孙清[1] Lu Yuanjiao;Miao Changxi;Jiang Jian;Song Lei;Sun Qing(Sinopec Shanghai Research Institute of Petrochmeical Technology,Shanghai 201208,China)

机构地区：[1]中国石化上海石油化工研究院,上海201208

出　　处：《石油化工》2021年第9期872-878,共7页Petrochemical Technology

摘　　要：采用溶胶凝胶法制备了Mn和/或Fe掺杂的Co基复合氧化物催化剂,利用XRD、N2吸附-脱附、ICP、Raman光谱、XPS、H_(2)-TPR等方法表征了催化剂的结构和氧化还原性能,并考察了催化剂对模拟对苯二甲酸(PTA)装置尾气的催化燃烧性能。实验结果表明,掺杂前后催化剂均为Co_(3)O_(4)尖晶石结构,Mn和/或Fe的掺杂能够影响催化剂的氧化还原能力和表面吸附氧物种的含量,而二溴甲烷的反应速率与催化剂表面吸附氧物种的含量呈正相关。由于Mn和Fe两种元素的协同作用,使同时掺杂两种元素的Co_(8)Mn_(0.5)Fe_(0.5)O_(x)催化剂表现出较好的氧化还原能力和氧流动性,从而提高了催化剂的活性和抗溴中毒的能力。以乙酸甲酯(MA)、对二甲苯(PX)、二溴甲烷的混合反应物为模拟PTA工业装置尾气,在反应物组成为1500×10^(-6)(φ)MA、300×10^(-6)(φ)PX、100×10^(-6)(φ)CH2Br2及10%(φ)O_(2),气态空速为60000 mL/(g·h)的条件下,Co_(8)Mn_(0.5)Fe_(0.5)O_(x)催化剂在280℃时对二溴甲烷的转化率达到93%。Cobalt oxides catalysts modified with Fe and Mn were prepared by sol-gel method and tested in the catalytic combustion of methyl acetate(MA),paraxylene(PX)and dibromomethane(CH_(2)Br_(2))(as the simulated p-phthalic acid exhaust gas).The physicochemical properties and redox ability of the catalysts were characterized by XRD,N2 adsorptiondesorption,ICP,Raman,XPS and H_(2)-TPR.The spinel structure of Co_(3)O_(4) can be prepared by sol-gel method.The addition of Mn and Fe could affect the redox ability and the amount of adsorbed surface oxygen species of the catalysts,the latter has a positive correlation with the reaction rate of CH_(2)Br_(2).Due to the synergetic effect of Co,Mn and Fe,Co_(8)Mn_(0.5)Fe_(0.5)O_(x) exhibited a better Br poisoning resistance which was attributed to its good oxygen fluidity and strong redox ability.Under the conditions of 1500×10^(-6)(φ)of MA,300×10^(-6)(φ)of PX,100×10^(-6)(φ)of CH2Br2 and 10%(φ)of O2,GHSV of 60000 mL/(g·h),the conversion of CH2Br2 could reach 93%at 280℃with Co_(8)Mn_(0.5)Fe_(0.5)O_(x) as catalyst.

关 键 词：钴基氧化物 改性 催化燃烧 二溴甲烷 对苯二甲酸装置尾气 

分 类 号：TQ426[化学工程]