FeCeLaO/粉煤灰基SiO2-Al2O3中低温烟气脱砷及抗硫性能

王凯; 张凯华; 张锴

doi:10.19805/j.cnki.jcspe.2025.240039

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FeCeLaO/粉煤灰基SiO₂-Al₂O₃中低温烟气脱砷及抗硫性能

绿色低碳 | 更新时间：2025-11-28

- FeCeLaO/粉煤灰基SiO₂-Al₂O₃中低温烟气脱砷及抗硫性能
- Middle-Low-temperature Flue Gas Arsenic Removal and Sulfur Resistance Performance of FeCeLaO/Fly Ash-based SiO₂-Al₂O₃
- 动力工程学报 2025年45卷第4期页码：602-611
- 作者机构：
  
  华北电力大学热电生产过程污染物监测与控制北京市重点实验室,北京,102206
- 作者简介：
  
  [ "王凯(1999—),男,内蒙古呼伦贝尔人,硕士研究生,研究方向为燃煤烟气脱砷吸附剂" ]
  [ "张凯华(通信作者),女,副教授,博士,E-mail:khzhang@ncepu.edu.cn" ]
- 基金信息：
  
  国家重点研发计划资助项目(2020YFB0606201);国家自然科学基金委与山西煤基低碳联合基金重点资助项目(U1910215)
- DOI：10.19805/j.cnki.jcspe.2025.240039
  中图分类号： X773
- 网络出版：2025-04-28，
  
  纸质出版：2025
- 稿件说明：
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王凯,张凯华,张锴. FeCeLaO/粉煤灰基SiO₂-Al₂O₃中低温烟气脱砷及抗硫性能动力工程学报, 2025, 45(4): 602-611 https://doi.

org/10.19805/j.cnki.jcspe.2025.240039
王凯,张凯华,张锴. FeCeLaO/粉煤灰基SiO₂-Al₂O₃中低温烟气脱砷及抗硫性能动力工程学报, 2025, 45(4): 602-611 https://doi. DOI： 10.19805/j.cnki.jcspe.2025.240039.

org/10.19805/j.cnki.jcspe.2025.240039 DOI：

摘要

采用碱熔-酸洗法对粉煤灰表面进行改性

制备活性Si-Al载体

同时以Fe、Ce、La复合氧化物为活性组分

采用共沉淀法制备FeCeLaO/活性Si-Al载体复合吸附剂

通过X射线荧光光谱、比表面积测定、X射线衍射图谱等对吸附剂进行表征

进而研究温度、Si/Al质量分数比、FeCeLaO负载率对复合吸附剂脱砷和抗硫中毒能力的影响。结果表明:活性Si-Al载体的脱砷能力随Si/Al质量分数比的增大和吸附温度的升高均先升高后降低

最佳Si/Al质量分数比为1.85

此时脱砷效率最高为78.7%

为原灰的2.8倍;最佳吸附温度位于高温段600 ℃

此时脱砷效率为84.8%;而FeCeLaO/活性Si-Al载体复合吸附剂最佳吸附温度位于中低温段400 ℃

脱砷效率高达96.9%

活性组分最佳负载率为1∶1。活性Si-Al载体的抗硫中毒能力随Si/Al质量分数比的增大而增强;引入FeCeLaO活性组分

有利于增强吸附剂的抗硫中毒能力

且负载率越高

抗硫中毒能力越强;FeCeLaO/活性Si-Al氧化物抗硫中毒能力强的原因主要是SiO

的表面酸性和Ce元素对Fe、La、Al等活性组分的保护效应。

Abstract

The surface of fly ash was modified using an alkali fusion-acid washing method to prepare an active Si-Al carrier. And Fe

La composite oxides were used as the active components to prepare FeCeLaO/active Si-Al carrier composite adsorbent by co-precipitation method. The adsorbents were characterized by X-ray fluorescence spectroscopy (XRF)

specific surface area measurements

and X-ra

y diffraction (XRD) patterns. Effects of temperature

Si/Al mass ratio

FeCeLaO loading ratio on arsenic removal efficiency and sulfur poisoning resistance of the composite adsorbent were investigated. Results show that the arsenic removal capacity of active Si-Al carrier increases first and then decreases with the increase of Si/Al mass ratio and adsorption temperature. The optimal Si/Al mass fraction ratio is 1.85

achieved a maximum arsenic removal efficiency of 78.7%

which is 2.8 times higher than that of raw fly ash. The highest removal efficiency of 84.8% is located in the high temperature range of 600 ℃. The best adsorption temperature of FeCeLaO/active Si-Al carrier composite adsorbent is located in the middle and low temperature section of 400 ℃

the arsenic removal efficiency is as high as 96.9%

and the best loading ratio of active components is 1∶1. The anti-sulfur poisoning ability of active Si-Al carriers is enhanced with the increase Si/Al mass fraction ratio. The introduction of FeCeLaO active component is conducive to the enhancement of the antisulfur poisoning ability of the adsorbent

and the higher the loading ratio

the stronger the anti-sulfur poisoning ability. The reason for the strong anti-sulfur poisoning ability of FeCeLaO/active Si-Al oxides is mainly due to the surface acidity of SiO

and the protective effect of elemental Ce on the active components

such as Fe

etc.

关键词

Keywords

references

岑可法, 倪明江, 高翔, 等. 煤炭清洁发电技术进展与前景[J]. 中国工程科学, 2015, 17(9): 49-55. CEN Kefa, NI Mingjiang, GAO Xiang, et al. Progress and prospects on clean coal technology for power generation[J]. Strategic Study of CAE, 2015, 17(9): 49-55.

TIAN Hezhong, WANG Yan, XUE Zhigang, et al. Atmospheric emissions estimation of Hg, As, and Se from coal-fired power plants in China, 2007[J]. Science of the Total Environment, 2011, 409(16): 3078-3081.

陈超, 刘卫平, 汤国锋, 等. 400 MW对冲燃烧亚临界和1 000 MW切圆燃烧超超临界燃煤机组烟气挥发性有机物排放特征研究[J/OL]. 洁净煤技术[2024-01-10]. https://doi.org/10.13226/j.issn.1006-6772.23100201. CHEN Chao, LIU Weiping, TANG Guofeng, et al. Study on VOCs emission characteristics of 400 MW opposed firing subcritical and 1 000 MW tangential firing ultra-supercritical coal-fired units[J]. Clean Coal Technology[2024-01-10]. https://doi.org/10.13226/j.issn.1006-6772.23100201.

任少君, 朱保宇, 翁琪航,等. 基于物理信息神经网络的燃煤锅炉NOx排放浓度预测方法[J]. 中国电机工程学报, 2024, 44(20): 8157-8165. REN Shaojun, ZHU Baoyu, WENG Qihang, et al. Forecasting method for NOx emission in coal fired boiler based on physics-informed neural network[J]. Proceedings of the CSEE, 2024, 44(20): 8157-8165.

董静兰, 马凯. 富氧气氛下煤与生物质掺烧时砷的释放研究[J]. 动力工程学报, 2017, 37(3): 237-241. DONG Jinglan, MA Kai. Arsenic release from co-firing of coal and biomass in oxygen-enriched atmosphere[J]. Journal of Chinese Society of Power Engineering, 2017, 37(3): 237-241.

黄永达, 胡红云, 龚泓宇, 等. 燃煤电厂砷、硒、铅的排放与控制技术研究进展[J]. 燃料化学学报, 2020, 48(11): 1281-1297. HUANG Yongda, HU Hongyun, GONG Hongyu, et al. Research progress on emission and control technologies of arsenic, selenium and lead in coal-fired power plants[J]. Journal of Fuel Chemistry and Technology, 2020, 48(11): 1281-1297.

郑刘根, 刘桂建, CHOU Chenlin, 等. 中国煤中砷的含量分布、赋存状态、富集及环境意义[J]. 地球学报, 2006, 27(4): 355-366. ZHENG Liugen, LIU Guijian, CHOU Chenlin, et al. Arsenic in Chinese coals: its abundance, distribution, modes of occurrence, enrichment processes, and environmental significance[J]. Acta Geoscientica Sinica, 2006, 27(4): 355-366.

杨希刚, 许月阳, 王圣, 等. 燃煤烟气对商用SCR催化剂氧化SO2性能的影响[J]. 洁净煤技术, 2023, 29(增刊2): 499-504. YANG Xigang, XU Yueyang, WANG Sheng, et al. Effect of coal combustion flue gas on the oxidation characteristics of SO2 by commercial SCR catalyst[J]. Clean Coal Technology, 2023, 29(Sup2): 499-504.

李想, 李俊华, 何煦, 等. 烟气脱硝催化剂中毒机制与再生技术[J]. 化工进展, 2015, 34(12): 4129-4138. LI Xiang, LI Junhua, HE Xu, et al. Poisoning mechanism and regeneration process of the denitration catalyst[J]. Chemical Industry and Engineering Progress, 2015, 34(12): 4129-4138.

吴江, 陈玉年, 张鑫, 等. 碳中和背景下燃煤烟气重金属污染物控制技术展望[J]. 上海电力大学学报, 2022, 38(5): 427-432. WU Jiang, CHEN Yunian, ZHANG Xin, et al. Prospects of control technology for heavy metal pollutants in coal-fired flue gas under the background of carbon neutrality[J]. Journal of Shanghai University of Electric Power, 2022, 38(5): 427-432.

唐朝春, 朱蓓, 许荣明, 等. 金属基吸附剂除砷技术研究进展[J]. 环境科学与技术, 2020, 43(10): 221-228. TANG Chaochun, ZHU Bei, XU Rongming, et al. Progress in research on arsenic removal technology with metal-based adsorbents[J]. Environmental Science & Technology, 2020, 43(10): 221-228.

袁媛, 赵永椿, 张军营, 等. TiO2-硅酸铝纤维纳米复合材料光催化脱硫脱硝脱汞的实验研究[J]. 中国电机工程学报, 2011, 31(11): 79-85. YUAN Yuan, ZHAO Yongchun, ZHANG Junying, et al. Study on photocatalytic experiments of desulfurization, denitrification and mercury removal using a TiO2-aluminum silicate fiber nanocomposite[J]. Proceedings of the CSEE, 2011, 31(11): 79-85.

SHI Xueke, GUO Jiaxiu, SHEN Ting, et al. Improvement of NH3-SCR activity and resistance to SO2 and H2O by Ce modified La-Mn perovskite catalyst[J]. Journal of the Taiwan Institute of Chemical Engineers, 2021, 126: 102-111.

夏新星, 马腾, 王志强, 等. 载铁活性炭烧结滤芯的制备及其除砷性能[J]. 环境工程学报, 2019, 13(7): 1534-1540. XIA Xinxing, MA Teng, WANG Zhiqiang, et al. Preparation of sintered iron-loaded activated carbon filter core and its arsenic removal performance[J]. Chinese Journal of Environmental Engineering, 2019, 13(7): 1534-1540.

LPEZ-ANTN M A, DIAZ-SOMOANO M, SPEARS D A, et al. Arsenic and selenium capture by fly ashes at low temperature[J]. Environmental Science & Technology, 2006, 40(12): 3947-3951.

洪剑东. 改性CaO脱除燃煤烟气砷的实验和理论研究[D]. 上海: 上海电力大学, 2022.

李扬, 陈伟, 赵永椿, 等. Fe/Al-SiO2复合金属氧化物用于燃煤烟气中汞的脱除[J]. 燃料化学学报, 2019, 47(12): 1409-1416. LI Yang, CHEN Wei, ZHAO Yongchun, et al. Removal of elemental mercury from flue gas by Fe/Al-SiO2 complex[J]. Journal of Fuel Chemistry and Technology, 2019, 47(12): 1409-1416.

王鹏, 张凯华, 王传风, 等. 氧化剂-Fe2O3复合吸附剂强化脱除气相砷的研究[J]. 中国电机工程学报, 2019, 39(15): 4497-4504. WANG Peng, ZHANG Kaihua, WANG Chuanfeng, et al. Studies on oxidant-Fe2O3 composite adsorbent and its enhanced removal of gas-phase arsenic[J]. Proceedings of the CSEE, 2019, 39(15): 4497-4504.

HU Hongyun, CHEN Dunkui, LIU Huan, et al. Adsorption and reaction mechanism of arsenic vapors over γ-Al2O3 in the simulated flue gas containing acid gases[J]. Chemosphere, 2017, 180: 186-191.

ZHAO Haitao, MU Xueliang, YANG Gang, et al. Graphene-like MoS2 containing adsorbents for Hg0 capture at coal-fired power plants[J]. Applied Energy, 2017, 207: 254-264.

JIANG Lijun, LIANG Ya, LIU Weizao, et al. Synergistic effect and mechanism of FeOx and CeOx co-doping on the superior catalytic performance and SO2 tolerance of Mn-Fe-Ce/ACN catalyst in low-temperature NH3-SCR of NOx[J]. Journal of Environmental Chemical Engineering, 2021, 9(6): 106360.

张月, 李文瀚, 王春波, 等. 超声波辅助浸渍法制备Fe2O3/γ-Al2O3吸附剂脱除气相As2O3的实验研究[J]. 燃料化学学报, 2015, 43(9): 1134-1141. ZHANG Yue, LI Wenhan, WANG Chunbo, et al. Experimental study on As2O3 capture from gas phase using ultrasound-assisted prepared Fe2O3/γ-Al2O3 sorbent[J]. Journal of Fuel Chemistry and Technology, 2015, 43(9): 1134-1141.

JADHAV R A, FAN L S. Capture of gas-phase arsenic oxide by lime: kinetic and mechanistic studies[J]. Environmental Science & Technology, 2001, 35(4): 794-799.

侯书阳, 张凯华, 王传风, 等. Fe-Ce-La复合氧化物在中低温烟气脱砷过程中的协同作用[J]. 中国电机工程学报, 2023, 43(2): 640-650. HOU Shuyang, ZHANG Kaihua, WANG Chuanfeng, et al. Synergistic effect of Fe-Ce-La composite oxide in the process of arsenic removal from flue gas at middle-low-temperatures[J]. Proceedings of the CSEE, 2023, 43(2): 640-650.

ZHANG Kaihua, HU Lintao, WANG Chuanfeng, et al. Middle-low-temperature oxidation and adsorption of arsenic from flue gas by Fe-Ce-based composite catalyst[J]. Chemosphere, 2022, 288: 132425.

LIN Jinru, CHEN Ning, PAN Yuanming. Uptake mechanisms of arsenate in gypsum: structural incorporation versus surface adsorption and implications for remediation of arsenic contamination[J]. Earth Science Frontiers, 2020, 27(5): 227-237.

ZHANG Yue, WANG Chunbo, LIU Huimin. Experiment and mechanism research on gas-phase As2O3 adsorption of Fe2O3/γ-Al2O3[J]. Fuel, 2016, 181: 1034-1040.

LI Yuzhong, TONG Huiling, ZHUO Yuqun, et al. Simultaneous removal of SO2 and trace As2O3 from flue gas: mechanism, kinetics study, and effect of main gases on arsenic capture[J]. Environmental Science & Technology, 2007, 41(8): 2894-2900.

屈湃, 高翔, 王倩, 等. 碱水热处理粉煤灰及其吸附性能探究[J]. 山西化工, 2021, 41(6): 1-2, 9. QU Pai, GAO Xiang, WANG Qian, et al. Study on alkali hydrothermal treatment of fly ash and its adsorption properties[J]. Shanxi Chemical Industry, 2021, 41(6): 1-2, 9.

SOMERSET V S, PETRIK L F, WHITE R A, et al. Alkaline hydrothermal zeolites synthesized from high SiO2 and Al2O3 co-disposal fly ash filtrates[J]. Fuel, 2005, 84(18): 2324-2329.

赵永椿, 张军营, 刘晶, 等. 燃煤飞灰吸附脱汞能力的实验研究[J]. 中国科学: 技术科学, 2010, 40(4): 385-391. ZHAO Yongchun, ZHANG Junying, LIU Jing, et al. Experimental study on fly ash capture mercury in flue gas[J]. Science China Technological Sciences, 2010, 40(4): 385-391.

赵永椿, 张军营, 王宗华, 等. 高钙飞灰的矿物学组成及微区特征研究[J]. 工程热物理学报, 2008, 29(8): 1427-1430. ZHAO Yongchun, ZHANG Junying, WANG Zonghua, et al. Study on mineralogy and micro-structure of high-calcium fly ash[J]. Journal of Engineering Thermophysics, 2008, 29(8): 1427-1430.

QI Liqiang, WANG Xu, WANG Wen, et al. Mercury removal from coal combustion flue gas by pyrite-modified fly ash adsorbent[J]. Environmental Science and Pollution Research, 2022, 29(26): 39228-39238.

邹潺, 王春波, 王贺飞, 等. 燃煤过程中砷挥发特性及动力学特性的研究[J]. 动力工程学报, 2017, 37(5): 349-355, 378. ZOU Chan, WANG Chunbo, WANG Hefei, et al. Volatilization and kinetic characteristics of arsenic during coal combustion[J]. Journal of Chinese Society of Power Engineering, 2017, 37(5): 349-355, 378.

侯书阳. Fe-Ce-La复合氧化物中低温烟气脱砷及抗硫中毒实验研究[D]. 北京: 华北电力大学, 2023.

耿俊, 柯权力, 周文茜, 等. 催化燃烧催化剂抗硫性的研究进展[J]. 燃料化学学报, 2022, 50(5): 564-575. GENG Jun, KE Quanli, ZHOU Wenqian, et al. Research progress in the sulfur resistance of catalytic combustion catalysts[J]. Journal of Fuel Chemistry and Technology, 2022, 50(5): 564-575.

JIANG Lijun, LIU Qingcai, RAN Guangjing, et al. V2O5-modified Mn-Ce/AC catalyst with high SO2 tolerance for low-temperature NH3-SCR of NO[J]. Chemical Engineering Journal, 2019, 370: 810-821.

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