工业MnOx颗粒催化剂的制备及其低温脱硝应用研究  

Preparation and industrial application of MnOx particle catalyst for low temperature denitration

作　　者：张霄玲 鲍佳宁 李运甲 皇甫林 李文松[3] 高士秋[2] 许光文[4] 李长明[2] 余剑[2] ZHANG Xiaoling;BAO Jianing;LI Yunjia;HUANGFU Lin;LI Wensong;GAO Shiqiu;XU Guangwen;LI Changming;YU Jian(School of Chemistry and Chemical Engineering,University of Chinese Academy of Science,Beijing 100049,China;State Key Laboratory of Multi-phase Complex System,Institute of Process Engineering,Chinese Academy of Sciences,Beijing 100190,China;School of Chemical Engineering,Xiangtan University,Xiangtan 411105,Hunan,China;Shenyang University of Chemical Technology,Shenyang 110142,Liaoning,China;School of Environmental Health and Engineering,University of Johns Hopkins,Baltimore 21287,Maryland,USA)

机构地区：[1]中国科学院大学化学与化工学院,北京100049 [2]中国科学院过程工程研究所多相复杂系统国家重点实验室,北京100190 [3]湘潭大学化工学院,湖南湘潭411105 [4]沈阳化工大学,辽宁沈阳110142 [5]约翰斯∙霍普金斯大学环境健康与工程系,美国马里兰州巴尔的摩市21287

出　　处：《化工学报》2020年第11期5169-5177,共9页CIESC Journal

基　　金：国家自然科学基金青年基金项目(21601192);多相实验室开放课题(MPCS-2019-0-03)。

摘　　要：以工业硫酸锰为前体,通过沉淀、洗涤、挤出、煅烧步骤批量制备了高活性颗粒状低温MnOx脱硝催化剂(ϕ5mm×30mm)。针对天然气冷热电三联供高含水低含硫烟气开展应用示范,研究催化剂在不同工况下的脱硝性能与长周期活性稳定性,结果表明:在入口NOx浓度850~1000mg/m³、床层温度145~175℃、空速4405h-1工况条件下,脱硝率达到87.88%~97.47%,连续运行1180h后脱硝效率有约3%的微弱衰减。对长周期运行后催化剂进行取样,进行XRD、BET、SEM表征及活性测试结果表明:该催化剂在该高湿烟气长时间运行中发生了一定程度的晶型转变,颗粒烧结、尺寸变大以及比表面积降低,导致其脱硝活性降低。该研究结果将为高活性锰基催化剂的制备及其低温脱硝工业应用提供参考和借鉴。Powder nano-manganese oxide(MnOx)material with excellent low-temperature denitration activity was prepared by precipitation-calcination method with manganese sulfate as precursor.The industrial catalyst ofϕ5 mm×30 mm granular MnOx was successfully produced by continuous extrusion molding technology.The produced industrial catalyst was applied in the denitration purification of low-temperature flue gas from cold,hot&electric triple supply(CCHP)system on the conditions of 5000 m3/h gas flow,850—1000 mg/m3 inlet NOx and the temperature from 145 to175℃.The NO conversion can achieve to 87.88%—97.47%under the GHSV of 4405 h-1,and 3%decline of denitration efficiency was observed after use for 1180 hours.The laboratory test also confirmed the reduced activity for the used sample.Moreover,XRD,BET and SEM results showed the crystal transition,increased particle size and decreased surface area for the used MnOx sample,which accounted for the observed decline of denitration efficiency after long term use on the industrial conditions.The results of this study will provide references for the preparation of highly active manganese-based catalysts and their industrial application in low-temperature denitrification.

关 键 词：锰氧化物 低温脱硝 选择性催化还原 失活 工业应用 

分 类 号：TQ137.1[化学工程—无机化工]