DEGRADATION OF XYLENE BY DBD PLASMA IN COLLABORATION WITH Mn-TiO2/γ-Al2O3 CATALYST
-
摘要: 采用浸渍法制备Mn-TiO2/γ-Al2O3催化剂,协同介质阻挡放电(DBD)等离子体降解二甲苯。探究了不同放电功率、初始质量浓度、气体流量下DBD等离子体对二甲苯的氧化性能;利用XRD和FT-IR对催化剂进行表征,以分析DBD等离子体放电前后催化剂的晶型与性能。结果表明:在放电功率为20 W,二甲苯进气浓度为38.62 mg/m3,进气流量为0.65 L/min条件下,协同Mn-TiO2/γ-Al2O3催化剂后,二甲苯降解率达到75.8%,反应器的能效为0.1027 g/(kW·h),同时O3浓度降低至36.94 mg/m3。表征结果显示,DBD等离子体放电前后未改变催化剂晶型与性能。为进一步分析降解二甲苯过程中产生的中间产物,通过FT-IR、GC-MS及发射光谱法进行诊断,发现加入催化剂后中间产物的种类和数量减少、发射光谱强度增强、特征谱线的数量增多。研究结果可为DBD等离子体在降解二甲苯应用中的性能优化和催化剂的选择提供理论参考。Abstract: In this study, Mn-TiO2/γ-Al2O3 catalyst was prepared by impregnation method to degrade xylene with dielectric barrier discharge (DBD) plasma. The oxidation properties of xylene in DBD plasma under different discharge power, initial mass concentration, and gas flow were studied. The catalyst was characterized by XRD and FT-IR to analyze the crystal shape and properties of the catalyst before and after DBD plasma discharge. The results showed that under the conditions of discharge power of 20 W, inlet concentration of xylene 38.62 mg/m3 and inlet flow rate of 0.65 L/min, the degradation efficiency of xylene reached 75.8% and the energy efficiency of the reactor was 0.1027 g/(kW·h) after adding Mn-TiO2/γ-Al2O3 catalyst. At the same time, ozone concentration was reduced to 36.94 mg/m3. The characterization results showed that the crystal shape and properties of the catalyst were not changed before and after the DBD plasma discharge. To further analyze the intermediate products produced in the process of degradation of xylene, FT-IR, GC-MS, and emission spectroscopy were used for diagnosis. It was found that the types and quantity of intermediate products decreased, the emission spectral intensity increased, and the number of characteristic spectral lines increased after adding catalyst. This study can provide a theoretical reference for the performance optimization and catalyst selection of DBD plasma in the application of xylene degradation.
-
Key words:
- DBD plasma /
- xylene /
- catalyst /
- plasma diagnosis
-
[1] LIU R, WU H, SHI J H, et al. Recent progress on catalysts for catalytic oxidation of volatile organic compounds: a review[J]. Catalysis Science & Technology, 2022, 12(23): 6945-6991. [2] DAVIDSON C J, HANNIGAN J H, BOWEN S E. Effects of inhaled combined benzene, toluene, ethylbenzene, and xylenes (BTEX): toward an environmental exposure model[J]. Environmental toxicology and pharmacology, 2021, 81: 103518. [3] LIU B S, YANG Y, YANG T, et al. Effect of photochemical losses of ambient volatile organic compounds on their source apportionment[J]. Environment International, 2023,172: 107766. [4] YU B, YUAN Z, YU Z, et al. BTEX in the environment: an update on sources, fate, distribution, pretreatment, analysis, and removal techniques[J]. Chemical Engineering Journal, 2022,435(Part1): 134825. [5] MU Y B, WILLIAMS P T. Recent advances in the abatement of volatile organic compounds (VOCs) and chlorinated-VOCs by non-thermal plasma technology: a review[J]. Chemosphere, 2022,308(Part3): 136481. [6] LU W J, ABBAS Y, MUSTAFA M F, et al. A review on application of dielectric barrier discharge plasma technology on the abatement of volatile organic compounds[J]. Frontiers of Environmental Science & Engineering, 2019, 13(2): 1-19. [7] LI S J, DANG X Q, YU X, et al. The application of dielectric barrier discharge non-thermal plasma in VOCs abatement: a review[J]. Chemical Engineering Journal, 2020, 388: 124275. [8] PANDA P, MAHANTA R K, MOHANTY S, et al. Abatement of gas-phase VOCs via dielectric barrier discharge plasmas[J]. Environmental Science and Pollution Research, 2021, 28: 28666-28679. [9] ZHANG H, LI K, SUN T, et al. The removal of styrene using a dielectric barrier discharge (DBD) reactor and the analysis of the by-products and intermediates[J]. Research on Chemical Intermediates, 2013, 39(3): 1021-1035. [10] 刘鑫. 低温等离子体催化协同降解混合VOCs(甲苯、丙酮及乙酸乙酯)的研究[D]. 上海:东华大学, 2022. [11] 郑毅文. 介质阻挡放电协同催化降解邻二氯苯的实验研究[D]. 杭州:浙江大学, 2021. [12] LIU Z, ZHANG Y, JIANG S, et al. Enhanced catalytic performance and reduced by-products emission on plasma catalytic oxidation of high-concentration toluene using Mn-Fe/rGO catalysts[J]. Journal of Environmental Chemical Engineering, 2022, 10(6): 108770. [13] YANG J, LIU S Y, HE T Y, et al. Degradation of toluene by DBD plasma-catalytic method with Mn<em>xCo<em>yCe<em>zO<em>n catalysts: characterization of catalyst, catalytic activity and continuous test[J]. Journal of Environmental Chemical Engineering, 2021, 9(6): 106361. [14] LYU Y, LI C T, DU X Y, et al. Catalytic removal of toluene over manganese oxide-based catalysts: a review[J]. Environmental Science and Pollution Research, 2020, 27: 2482-2501. [15] CHANG T, MA C L, SHEN Z X, et al. Mn-based catalysts for post non-thermal plasma catalytic abatement of VOCs: a review on experiments, simulations and modeling[J]. Plasma Chemistry and Plasma Processing, 2021, 41(5): 1239-1278. [16] DONG S L, WANG Y F, YANG J, et al. Performance and mechanism analysis of degradation of toluene by DBD plasma-catalytic method with MnO<em>x/Al2O3 catalyst[J]. Fuel, 2022, 319: 123721. [17] JIANG L Y, WANG P J, ZHANG Y F, et al. Plasma-catalytic oxidation of chlorobenzene over Co-Mn/TiO2 catalyst in a dielectric barrier discharge reactor with the segmented electrodes[J]. Journal of Environmental Chemical Engineering, 2022, 10(4): 108021. [18] 姜理英, 张瑜芬, 胡俊,等. NTP协同双金属锰基催化剂降解氯苯的性能研究[J]. 环境科学学报, 2021, 41(3): 922-931. [19] AYUB K S, ZAMAN W Q, MIRAN W, et, al. Efficient post-plasma catalytic degradation of toluene via series of Co-Cu/TiO2 catalysts[J]. 2022, 8(48): 4227-4248. [20] LI W J, GU Z Y, TENG F H, et al. The synergetic effect of UV rays on the decomposition of xylene in dielectric barrier discharge plasma and photocatalyst process[J]. The European Physical Journal Applied Physics, 2018, 81(2): 20801. [21] WU Z L, ZHOU W L, ZHU Z B, et al. Enhanced oxidation of xylene using plasma activation of an Mn/Al2O3 catalyst[J]. IEEE Transactions on Plasma Science, 2020, 48(1): 163-172. [22] DONG S L, WANG Y F, YANG J, et al. Performance and mechanism analysis of degradation of toluene by DBD plasma-catalytic method with MnO<em>x/Al2O3 catalyst[J]. Fuel, 2022, 319: 123721. [23] ZENG X L, LI B, LIU R Q, et al. Investigation of promotion effect of Cu doped MnO2 catalysts on ketone-type VOCs degradation in a one-stage plasma-catalysis system[J]. Chemical Engineering Journal, 2020, 384: 123362. [24] 石秀娟, 梁文俊, 尹国彬, 等. 低温等离子体协同Mn基催化剂降解氯苯研究[J]. 化工学报, 2022, 73(10): 4472-4483. [25] 张益坤, 姚鑫, 陈铭夏, 等. 低温等离子体除苯过程中臭氧的演变与作用[J]. 工业催化, 2020, 28(4): 68-72. [26] 韩丰磊, 季纯洁, 张子琦, 等. 低温等离子体协同催化技术处理VOCs研究综述[J]. Clean Coal Technology, 2022, 28(2): 23-31. [27] LIU P F, HE L M, ZHAO B B. Discharge and optical emission spectrum characteristics of a coaxial dielectric barrier discharge plasma-assisted combustion actuator[J]. Journal of Spectroscopy, 2020, 2020: 6034848.
点击查看大图
计量
- 文章访问数: 55
- HTML全文浏览量: 7
- PDF下载量: 4
- 被引次数: 0