钒钛催化剂表面硫酸氢铵的演化及对催化活性的影响  

Evolution of ABS on the Surface of Vanadium-Titanium Catalyst and Its Influence on Catalytic Activity

作　　者：黄林滨 何陆灿 陈国庆 谭锐 高行龙 张海峰 张萼松 于洁[4] HUANG Linbin;HE Lucan;CHEN Guoqing;TAN Rui;GAO Xinglong;ZHANG Haifeng;ZHANG Esong;YU Jie(State Key Laboratory of Low-Carbon Smart Coal-Fired Power Generation and Ultra-Clean Emission,National Energy Group Science and Technology Research Institute Co.,Ltd.,Nanjing 210023,Jiangsu Province,China;Guoneng Nanjing Electric Power Testing and Research Co.,Ltd.,Nanjing 210023,Jiangsu Province,China;Guoneng Changzhou Secondary Power Generation Co.,Ltd.,Changzhou 213000,Jiangsu Province,China;State Key Laboratory of Coal Combustion,Huazhong University of Science and Technology,Wuhan 430074,Hubei Province,China)

机构地区：[1]国家能源集团科学技术研究院有限公司低碳智能燃煤发电与超净排放全国重点实验室,江苏南京210023 [2]国能南京电力试验研究有限公司,江苏南京210023 [3]国能常州第二发电有限公司,江苏常州213000 [4]华中科技大学煤燃烧与低碳利用全国重点实验室,湖北武汉430074

出　　处：《动力工程学报》2025年第4期619-625,共7页Journal of Chinese Society of Power Engineering

基　　金：国家自然科学基金面上项目(52176186)。

摘　　要：探讨了钒钛催化剂表面硫酸氢铵(ABS)的演化特性及其对催化剂活性的影响。基于X射线衍射仪(XRD)、比表面积分析仪(BET)、傅里叶红外光谱分析仪(FTIR)和热重分析仪(TGA)等对催化剂负载ABS前后物理化学性质进行了表征,以期获得ABS对催化剂活性的影响;基于密度泛函理论(DFT)计算,对催化剂不同活性位点的作用机制进行了理论研究;对负载ABS的催化剂开展了脱硝台架实验研究。结果表明:ABS的沉积会导致催化剂比表面积降低;ABS含量低时,催化剂表面含硫基团主要以SO_(4)^(2-)形式存在;随着ABS含量增加,生成了HSO_(4)^(-)官能团;催化剂中主要反应活性位是钒氧化物的Lewis酸位点,催化剂内部ABS分解生成的硫化物具有的Br nsted酸位点能够起到储存NH 3的作用,对催化剂活性有一定的提升作用。负载ABS的催化剂在更高温下的脱硝活性更强,与DFT计算结果一致。从微观层面角度,微量ABS会提高催化剂活性。Evolution characteristics of ammonium bisulfate(ABS)on the surface of vanadium-titanium catalyst and its influence on catalytic activity were investigated.Physical and chemical properties of the catalyst before and after ABS loading were characterized to obtain the mechanism of the influence of ABS on catalytic activity through methods of XRD,BET,FTIR,TGA,etc.Density functional theory(DFT)calculation was employed to theoretically study the mechanism of different active sites of the catalyst.Denitrification bench experiments were conducted on the ABS-loaded catalyst.Results show that ABS deposition leads to a decrease in the specific surface area of the catalyst.When the ABS content is low,sulfur-containing groups on the catalyst surface primarily exist in the form of SO_(4)^(2-).As the ABS content increases,HSO-4 functional groups are generated.The main active sites for the reaction in the catalyst are the Lewis acid sites of vanadium oxide.Sulfide generated by the decomposition of ABS within the catalyst contains Br nsted acid sites which can store NH_(3),thus contributes to a certain improvement in catalytic activity.ABS-loaded catalyst exhibits stronger denitrification activity at higher temperature,consistent with DFT calculation results.From a microscopic perspective,trace amount of ABS can enhance catalytic activity.

关 键 词：硫酸氢铵 SCR催化剂 失活 密度泛函理论 

分 类 号：X701.3[环境科学与工程—环境工程]