Development and Planning Department, SINOPEC Anqing Petrochemical Company Limited
College of Chemistry and Chemical Engineering, Anqing Normal University
Quality Control Center, SINOPEC Anqing Petrochemical Company Limited
College of Chemistry and Chemical Engineering, Hefei University of Technology

针对燃煤烟气汞排放污染问题,通过将V2O5负载到经H2SO4改性后的蒙脱石(montmorillonite,MMT)制备的V2O5/MMT催化剂用于脱除燃煤烟气中的汞,希望结合活性组分V2O5的催化氧化活性和载体改性后MMT的吸附性能实现燃煤烟气中汞的经济高效脱除。研究了V2O5/MMT催化剂脱除Hg0的性能及脱除Hg0后V2O5/MMT催化剂的再生性能,考察了H2SO4改性、催化剂制备条件、V2O5负载量、反应温度、烟气成分(O2,SO2,NO,H2O(g))、再生条件等对V2O5/MMT催化剂脱除Hg0的影响,采用XRD,BET,SEM-EDS,XPS和TPD等方法对脱除Hg0前后的V2O5/MMT催化剂进行了分析表征。结果表明:V2O5/MMT催化剂具有良好的脱除Hg0的能力,这主要是由于V2O5/MMT催化剂结合了V2O5的催化氧化活性和改性后MMT的吸附性能;3%V2O5/MMT催化剂(V2O5质量分数为3%)在反应温度为150℃、体积空速为6000/h条件下,对Hg0的脱除效率达到98%以上;O2和NO对V2O5/MMT催化剂脱除Hg0具有促进作用,SO2对V2O5/MMT催化剂脱除Hg0具有一定的促进作用,H2O(g)对V2O5/MMT催化剂脱除Hg0具有抑制作用;XRD和BET表征发现H2SO4改性可使MMT的比表面积增大,但层间距下降;SEM-EDS分析显示V2O5/MMT催化剂具有良好的孔隙结构,活性组分V2O5均匀分布在载体MMT表面;XPS和TPD表征证实Hg0在V2O5/MMT催化剂上被氧化生成了HgO和HgSO4并吸附在V2O5/MMT催化剂上;脱除Hg0后的V2O5/MMT催化剂具有良好的再生性能。

In order to solve the pollution problem of mercury emission from coal-fired flue gas, V2O5/MMT catalyst was prepared by loading V2O5 onto montmorillonite (MMT) modified by H2SO4 and used to remove mercury from coal-fired flue gas. The V2O5/MMT catalyst, which combined the catalytic oxidation activity of V2O5 and the adsorption performance of modified MMT, was expected to remove mercury cost-effectively. Its Hg0 removal capability in simulated flue gas and regeneration performance after Hg0 removal were studied. Meanwhile, the effects of H2SO4 modification, preparation condition, V2O5 loading amount, reaction temperature, flue gas components (O2, SO2, NO, H2O(g)) and regeneration condition on Hg0 removal by V2O5/MMT were investigated. The V2O5/MMT catalysts before and after Hg0 removal were charac-terized by XRD, BET, SEM-EDS, XPS and TPD. The results indicate that V2O5/MMT cata-lyst has a good Hg0 removal capability, which is mainly due to the co-effect between catalytic oxi-dation activity of V2O5 and adsorption ability of modified MMT. Hg0 removal efficiency by 3%V2O5/MMT catalyst (3% V2O5 loading) is over 98% at 150 ℃ with a space velocity of 6 000 h-1. O2 and NO have promoting effects on Hg0 removal by V2O5/MMT catalyst, SO2 has a slight promotion effect, while H2O has an inhibitory effect. The results of XRD and BET show that the specific surface area of MMT increases by H2SO4 modification, but the interlayer spacing decreases. SEM-EDS results indicate that the V2O5/MMT catalyst has a good pore structure, and the active component V2O5 distributes well on the surface of MMT support. The results of XPS and TPD confirme that Hg0 is oxidized to form HgO and HgSO4 on V2O5/MMT catalyst, which are then adsorbed on V2O5/MMT catalyst. V2O5/MMT catalyst has good regeneration performance after Hg0 removal.

国家自然科学 基 金 项 目 (21203003)、安 徽 省 自 然 科 学 基 金 项 目 (1708085MB49)、安 徽 省 高 校 学 科 (专 业)拔 尖 人 才 学 术 资 助 项 目(gxbjZD2021062)和安徽省高校优秀科研创新团队(2022AH010062).

杨 森,张 楠,魏 坤,等.改性蒙脱石负载 V2O5 脱除气态 Hg0 的性能研究[J].煤炭转化,2024,47(1):100-109

YANG Sen,ZHANG Nan,WEI Kun,et al.Performance of removal of vapor-phase Hg0 over V2O5/MMT catalyst[J].Coal Conversion,2024,47(1):100-109