抗硫抗水性三元复合催化剂脱硝协同氯苯脱除性能研究

林静仁; 纵宇浩; 岳彦伟; 刘猛; 韦红旗

doi:10.19805/j.cnki.jcspe.2026.240813

欢迎来到能源电力期刊网！

English Version 期刊登录

您当前的位置：

首页 >

文章列表页 >

抗硫抗水性三元复合催化剂脱硝协同氯苯脱除性能研究

绿色低碳 | 更新时间：2026-10-10

- 抗硫抗水性三元复合催化剂脱硝协同氯苯脱除性能研究
- Study on the NO_x-Chlorobenzene Synergistic Removal Performance of Sulfur and Water Resistance Ternary Composite Catalyst
- 动力工程学报 2026年46卷第4期页码：181-190
- 作者机构：
  
  1. 大唐南京环保科技有限责任公司,江苏,南京,211100
  2. 东南大学能源与环境学院,江苏,南京,210096
- 作者简介：
  
  林静仁(1976—),男,江苏徐州人,高级工程师,硕士,研究方向为催化剂污染物脱除。刘猛(通信作者),男,副教授,博士,E-mail:101011778@seu.edu.cn。
- 基金信息：
  
  国家重点研发计划资助项目(2022YFB4100301)
- DOI：10.19805/j.cnki.jcspe.2026.240813
  中图分类号： X511
- 纸质出版：2026
- 稿件说明：
移动端阅览
林静仁, 纵宇浩, 岳彦伟, 刘猛, 韦红旗. 抗硫抗水性三元复合催化剂脱硝协同氯苯脱除性能研究[J]. 动力工程学报, 2026, 46(4): 181-190.
林静仁, 纵宇浩, 岳彦伟, 刘猛, 韦红旗. 抗硫抗水性三元复合催化剂脱硝协同氯苯脱除性能研究[J]. 动力工程学报, 2026, 46(4): 181-190. DOI： 10.19805/j.cnki.jcspe.2026.240813.

DOI： 10.19805/j.cnki.jcspe.2026.240813

摘要

针对钢铁烧结、垃圾焚烧等烟气中氮氧化物(NOx)与氯代芳香化合物协同脱除难题

以及现有商用催化剂活性温度窗口偏高、易生成剧毒副产物的问题

以氯苯(CB)为氯代芳香化合物替代物

开展复合金属氧化物催化剂的低温协同脱除性能研究。研究对象为CeMnNb三元复合金属氧化物催化剂

采用共沉淀法制备不同Ce/Nb物质的量比的催化剂样品

通过固定床活性测试系统考察反应温度、氨氮比(NSR)、O2体积分数、空速等操作参数的影响

结合X射线光电子能谱(XPS)表征探究催化剂在H2O和SO2存在下的结构演变与抗硫抗水机理。结果表明:在优化条件(反应温度为280 ℃

NH3、NO、CB、O2的体积分数为600×10-6、600×10-6、300×10-6、8%

空速为60 000 h-1)下

Ce、Mn、Nb的物质的量比为1∶1∶2的CeMnNb催化剂可实现97.2%的CB脱除率和88.3%的NOx转化率;H2O和SO2对催化剂协同脱除性能均有抑制作用

且共存时抑制更显著

其中SO2的毒害作用不可逆;表征显示

3种反应条件下催化剂中Mn4+相对含量均显著降低

H2O存在时Cl与低价Mn形成Mn-Cl键

SO2存在时表面有机氯相对含量上升

而H2O与SO2共存时易形成硫酸盐

可减少含氯化合物沉积。

Abstract

In response to the challenges associated with the synergistic removal of nitrogen oxides (NOx) and chlorinated aromatic compounds from flue gases generated during steel sintering

waste incineration

and other processes

as well as the issues with existing commercial catalysts

such as a relatively high active temperature window and the tendency to produce highly toxic by-products

a study was conducted on the low-temperature synergistic removal performance of composite metal oxide catalysts

using chlorobenzene (CB) as a surrogate for chlorinated aromatic compounds. The research focused on a CeMnNb ternary composite metal oxide catalyst. Catalyst samples with varying Ce/Nb molar ratios were prepared via the co-precipitation method. The effects of operating parameters

including reaction temperature

ammonia-nitrogen ratio (NSR)

O2 volume fraction

and space velocity

were investigated using a fixed-bed activity testing system. Additionally

X-ray photoelectron spectroscopy (XPS) characterization was employed to explore the structural evolution and sulfur/water resistance mechanisms of the catalyst in the presence of H2O and SO2. Results demonstrate that under the optimized condition (a reaction temperature of 280 ℃

volume fractions of NH3

CB and O2 of 600×10-6

600×10-6

300×10-6

and 8%

respectively

and a space velocity of 60 000 h-1)

the CeMnNb catalyst with a Ce/Mn/Nb molar ratio of 1∶1∶2 can achieve a CB removal efficiency of 97.2% and a NOx conversion efficiency of 88.3%. Both H2O and SO2 are found to inhibit the synergistic removal performance of the catalyst

with a more pronounced inhibitory effect observed when they coexist. Notably

the poisoning effect of SO2 is irreversible. XPS characterization results reveal that the relative content of Mn4+ in the catalyst decreases significantly under all three reaction conditions. In the presence of H2O

Cl formes Mn-Cl bonds with low-valent Mn species. When SO2 is present

the relative content of surface organic chlorine increases. However

when H2O and SO2 coexist

sulfates are readily formed

which is conductive to reduce the deposition of chlorinated compounds.

关键词

Keywords

references

朱廷钰, 叶猛, 齐枫, 等. 钢铁烧结烟气多污染物协同控制技术及示范[J]. 科技资讯, 2016, 14(10): 166-167. ZHU Tingyu, YE Meng, QI Feng, et al. The collaborative control technology and demonstrations for steel sintering flue gas pollutants[J]. Science & Technology Information, 2016, 14(10): 166-167.

蒋海威, 高明明, 张开萍, 等. 循环流化床大气污染物机理模型及关键状态变量研究[J]. 动力工程学报, 2024, 44(4): 622-631.JIANG Haiwei, GAO Mingming, ZHANG Kaiping, et al. Study on mechanism model and key state variables of air pollutants in circulating fluidized bed[J]. Journal of Chinese Society of Power Engineering, 2024, 44(4): 622-631.

朱法华, 徐静馨, 王圣, 等. 中国燃煤电厂大气污染物治理历程及展望[J]. 电力科技与环保, 2023, 39(5): 371-384. ZHU Fahua, XU Jingxin, WANG Sheng, et al. Processes and prospects of air pollutant control in coal-fired power plants in China[J]. Electric Power Technology and Environmental Protection, 2023, 39(5): 371-384.

戴豪波, 王健, 张琪. 钒基催化剂降解氯苯的原位红外分析[J]. 环境工程学报, 2020, 14(1): 144-153.DAI Haobo, WANG Jian, ZHANG Qi. In-situ FT-IR analysis of chlorobenzene degradation by vanadia based catalysts[J]. Chinese Journal of Environmental Engineering, 2020, 14(1): 144-153.

黄宇, 魏家璇, 张雄, 等. SCR脱硝系统的RBF条件积分滑模参数优化控制[J]. 动力工程学报, 2024, 44(8): 1244-1252.HUANG Yu, WEI Jiaxuan, ZHANG Xiong, et al. Parameter optimization control of RBF conditional integral sliding mode for SCR denitration system[J]. Journal of Chinese Society of Power Engineering, 2024, 44(8): 1244-1252.

任鹏, 宋学伟, 刘海秋. 宽温脱硝催化剂性能试验研究[J]. 电力科技与环保, 2023, 39(1): 49-58.REN Peng, SONG Xuewei, LIU Haiqiu. Experimental study on the performance of wide temperature denitration catalyst[J]. Electric Power Technology and Environmental Protection, 2023, 39(1): 49-58.

DAI Qiguang, SHEN Kai, DENG Wei, et al. HCl-tolerant HxPO4/RuOx-CeO2 catalysts for extremely efficient catalytic elimination of chlorinated VOCs[J]. Environmental Science & Technology, 2021, 55(6): 4007-4016.

JONES J, ROSS J R H. The development of supported vanadia catalysts for the combined catalytic removal of the oxides of nitrogen and of chlorinated hydrocarbons from flue gases[J]. Catalysis Today, 1997, 35(1/2): 97-105.

汪振辉, 顾秋香, 杨波, 等. MnCeTiOx协同催化脱除氮氧化物与氯苯研究[J]. 环境科学学报, 2024, 44(3): 345-353.WANG Zhenhui, GU Qiuxiang, YANG Bo, et al. Study on the synergistic catalytic removal of nitrogen oxides and chlorobenzene over MnCeTiOx[J]. Acta Scientiae Circumstantiae, 2024, 44(3): 345-353.

戴毅, 梅超强, 李雪, 等. 前驱体对MnO2同时催化脱除氮氧化物与氯苯性能的影响[J]. 环境工程, 2022, 40(4): 57-63, 105.DAI Yi, MEI Chaoqiang, LI Xue, et al. Effect of precursors on simultaneous catalytic removal of nitrogen oxides and chlorobenzene by MnO2[J]. Environmental Engineering, 2022, 40(4): 57-63, 105.

杨波, 陈子伦, 徐海涛, 等. VOx-MnOx/TiO2催化脱除氮氧化物与二噁英研究[J]. 环境科学学报, 2020, 40(3): 838-845.YANG Bo, CHEN Zilun, XU Haitao, et al. Synergistic removal of nitrogen oxides and dioxins by VOx-MnOx/TiO2[J]. Acta Scientiae Circumstantiae, 2020, 40(3): 838-845.

贾晖杰, 熊小鹤. 300 MW机组锅炉效率和NOx排放协同优化试验研究[J]. 电力科技与环保, 2023, 39(4): 338-344.JIA Huijie, XIONG Xiaohe. Collaborative optimization study on between boiler efficiency and NOx emission in a 300 MW unit[J]. Electric Power Technology and Environmental Protection, 2023, 39(4): 338-344.

许晓龙, 童翠香, 蔡佳凤, 等. 制备条件对脱硝脱二噁英V2O5-CeO2/TiO2催化剂协同性能的影响[J]. 安徽化工, 2024, 50(1): 51-53, 61.XU Xiaolong, TONG Cuixiang, CAI Jiafeng, et al. Effect of preparation conditions on the synergistic performance of V2O5-CeO2/TiO2 catalysts for denitrification and dioxin removal[J]. Anhui Chemical Industry, 2024, 50(1): 51-53, 61.

XU Wenqing, YU Yunbo, ZHANG Changbin, et al. Selective catalytic reduction of NO by NH3 over a Ce/TiO2 catalyst[J]. Catalysis Communications, 2008, 9(6): 1453-1457.

DAI Qiguang, BAI Shuxing, WANG Jianwei, et al. The effect of TiO2 doping on catalytic performances of Ru/CeO2 catalysts during catalytic combustion of chlorobenzene[J]. Applied Catalysis B: Environmental, 2013, 142-143: 222-233.

YANG Yang, HUANG Jun, WANG Siwen, et al. Catalytic removal of gaseous unintentional POPs on[KG(1x]manganese oxide octahedral molecular sieves[J].[KG)]Applied Catalysis B: Environmental, 2013, 142-143: 568-578.

MA Xiaodong, SHEN Jinshan, PU Weiya, et al. Water-resistant Fe-Ca-Ox/TiO2 catalysts for low temperature 1, 2-dichlorobenzene oxidation[J]. Applied Catalysis A: General, 2013, 466: 68-76.

施琦, 丁龙, 龙红明, 等. 基于XRD和FITR的Ce-V-Ti催化剂减排烧结烟气二噁英的活性分析(英文)[J]. 光谱学与光谱分析, 2021, 41(1): 327-332. SHI Qi, DING Long, LONG Hongming, et al. Study on catalytic combustion of dioxins from iron ore sintering flue gas over Ce-V-Ti catalysts by XRD and FTIR[J]. Spectroscopy and Spectral Analysis, 2021, 41(1): 327-332.

邓丽萍, 张琪, 姜雅洲, 等. 多功能催化蓄热体的制备及特性研究[J]. 能源工程, 2024, 44(3): 40-46.DENG Liping, ZHANG Qi, JIANG Yazhou, et al. Preparation of multifunctional catalytic-heat accumulator and its catalytic characteristics[J]. Energy Engineering, 2024, 44(3): 40-46.

SUN Pengfei, CHEN Jingkun, ZAI Shaiying, et al. Regeneration mechanism of a deactivated zeolite-supported catalyst for the combustion of chlorinated volatile organic compounds[J]. Catalysis Science & Technology, 2021, 11(3): 923-933.

WANG Qiulin, LIN Feng, ZHOU Jianjian, et al. Effect of HCl and o-DCBz on NH3-SCR of NO over MnOx/TiO2 and MnOx-CeO2/TiO2 catalysts[J]. Applied Catalysis A: General, 2020, 605: 117801.

郑足红, 童华, 童志权, 等. 低温高活性NO氧化催化剂Mn-V-Ce/TiO2的制备与性能[J]. 过程工程学报, 2008, 8(6): 1204-1212.ZHENG Zuhong, TONG Hua, TONG Zhiquan, et al. Preparation of low temperature and high activity Mn-V-Ce/TiO2 catalyst and its catalytic performance on NO oxidation[J]. The Chinese Journal of Process Engineering, 2008, 8(6): 1204-1212.

ROMANO E J, SCHULZ K H. A XPS investigation of SO2 adsorption on ceria-zirconia mixed-metal oxides[J]. Applied Surface Science, 2005, 246(1/2/3): 262-270.

浏览量

下载量

CSCD

文章被引用时，请邮件提醒。

提交

工具集

关联资源

沿面介质阻挡放电协同催化剂脱除NO/SO2/Hg0实验研究

奇异值分解用于早期摩擦故障诊断的研究

计入工业园区电热负荷需求的源网荷储优化调度方法研究

分形特征对漂浮式风力机仿生平台动态响应的影响

融合长短期依赖的双通道短期风电功率预测