摘要
研究了粉煤灰(FA)-凹凸棒石(PG)负载MnO_(2)-CeO_(2)催化剂(MnO_(2)-CeO_(2)/FA-PG)的制备及其用于脱除模拟烟气(N_(2)+5%(体积分数,下同)O_(2)+0.15%SO_(2)+0.05%NO+5%H_(2)O)中的Hg^(0)的性能以及脱除Hg^(0)后MnO_(2)-CeO_(2)/FA-PG催化剂的再生。考察了MnO_(2)-CeO_(2)负载、制备温度、反应温度、空速、SO_(2)体积分数及催化剂再生方法对MnO_(2)-CeO_(2)/FA-PG催化剂脱除Hg^(0)的影响,探讨了Hg^(0)在Mn8-Ce0.5/FA-PG催化剂上的脱除过程。结果表明:350℃煅烧温度下制备的Mn8-Ce0.5/FA-PG催化剂脱除Hg^(0)的能力最高;MnO_(2)-CeO_(2)/FA-PG催化剂在120℃~210℃温度范围内具有良好的脱除Hg^(0)的能力和稳定性;在反应温度为150℃、空速为6000/h、Hg^(0)的质量浓度为160μg/m^(3)的条件下300 min时Hg^(0)脱除效率保持在97%以上,58 h时Hg^(0)的脱除效率仍能保持在87%左右;CeO_(2)提高了MnO_(2)-CeO_(2)/FA-PG催化剂的抗SO_(2)能力;Hg^(0)在MnO_(2)-CeO_(2)/FA-PG催化剂上被氧化生成了Hg^(2+)的化合物HgO和HgSO_(4)并吸附在MnO_(2)-CeO_(2)/FA-PG上;脱除Hg^(0)后的MnO_(2)-CeO_(2)/FA-PG经热再生-空气预氧化处理仍具有良好的脱除Hg^(0)的能力,MnO_(2)-CeO_(2)/FA-PG催化剂具有良好的再生循环使用性能。
MnO_(2)-CeO_(2)/FA-PG catalyst was prepared by using fly ash(FA)and attapulgite(PG)supported MnO_(2)-CeO_(2) catalyst and used to remove Hg^(0) in simulated flue gas(N_(2)+5%(volume fraction,the same below)O_(2)+0.15%SO_(2)+0.05%NO+5%H_(2)O).The effects of MnO_(2)-CeO_(2) loading,calcination temperature,reaction temperature,space velocity,volume fraction of SO_(2),and catalyst regeneration method on Hg^(0) removal using MnO_(2)-CeO_(2)/FA-PG were tested.The removal process of Hg^(0) removal over Mn8-Ce0.5/FA-PG was also discussed.The results show that Mn8-Ce0.5/FA-PG catalyst prepared at calcined temperature 350℃has the highest capacity.Mn8-Ce0.5/FA-PG catalyst exhibite an excellent Hg^(0) removal capability and stability at the temperature of 120℃-210℃.Hg^(0) removal efficiency is kept above 97%at 150℃for 300 min with the space velocity of 6000/h and Hg^(0) mass concentration of 160μg/m^(3) and maintained at about 87%for 58 h.CeO_(2) improves the SO_(2) resistance of the MnO_(2)-CeO_(2)/FA-PG catalyst.Hg^(0) is oxidized to Hg^(2+)compounds of HgO and HgSO_(4) and adsorbed on the MnO_(2)-CeO_(2)/FA-PG catalyst.The spent MnO_(2)-CeO_(2)/FA-PG still has high Hg^(0) removal capability after being treated with thermal regeneration and air pre-oxidation.MnO_(2)-CeO_(2)/PG-FA catalyst also exhibites excellent cyclic ability after Hg^(0) removal.
作者
王钧伟
姜彩虹
王柯佳
石李明
薛志锋
徐灿
秦伟
张建利
WANG Junwei;JIANG Caihong;WANG Kejia;SHI Liming;XUE Zhifeng;XU Can;QIN Wei;ZHANG Jianli(College of Chemistry and Chemical Engineering,Anqing Normal University,246011 Anqing,China;Development and Planning Department,Quality Control Center,Anqing Petrochemical Company,SINOPEC,246002 Anqing,China;State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering,Ningxia University,750021 Yinchuan,China)
出处
《煤炭转化》
CAS
CSCD
北大核心
2022年第5期89-96,共8页
Coal Conversion
基金
国家自然科学基金资助项目(21203003,51404014)
安徽省自然科学基金面上项目(1708085MB49)
安徽省高校学科(专业)拔尖人才学术资助重点项目(gxbjZD2021062)
省部共建煤炭高效利用与绿色化工国家重点实验室开放课题(2020-KF-28)
安徽省省级教学团队项目(2019jxtd079)
