煅烧温度对磁性铁钛复合氧化物微观结构及脱硝活性的影响

doi:10.16085/j.issn.1000-6613.2017-2004

化工进展 ›› 2018, Vol. 37 ›› Issue (09): 3410-3415.DOI: 10.16085/j.issn.1000-6613.2017-2004

煅烧温度对磁性铁钛复合氧化物微观结构及脱硝活性的影响

周飞^1,2, 熊志波¹, 金晶¹, 武超¹, 陆威¹, 丁旭春²

1 上海理工大学能源与动力工程学院, 上海 200093;
2 江苏国信靖江发电有限公司, 江苏靖江 214500

收稿日期:2017-09-24 修回日期:2017-12-06 出版日期:2018-09-05 发布日期:2018-09-05
通讯作者: 熊志波,副教授,硕士生导师,研究方向为燃煤污染物排放控制。
作者简介:周飞(1986-),男,博士研究生,研究方向为氮氧化物排放控制。E-mail:zhoufei926@126.com。
基金资助:
国家自然科学基金（51406118）及上海市青年东方学者岗位计划（QD2015017）项目。

Influence of calcination temperature on the micro-structure and the NH₃-SCR activity of magnetic iron-titanium mixed oxide catalyst

ZHOU Fei^1,2, XIONG Zhibo¹, JIN Jing¹, WU Chao¹, LU Wei¹, DING Xuchun²

1 School of Energy and Power Engineering, University of Shanghai for Science and Technology, Shanghai 200093, China;
2 Jiangsu Guoxin Jingjiang Power Company, Jingjiang 214500, Jiangsu, China

Received:2017-09-24 Revised:2017-12-06 Online:2018-09-05 Published:2018-09-05

摘要/Abstract

摘要： 利用共沉淀微波法构筑新型磁性铁钛复合氧化物催化剂，研究了煅烧温度对其物性结构及NH₃-SCR脱硝性能的影响，揭示了钛掺杂对磁性γ-Fe₂O₃晶体高温热转化及其脱硝性能的优化机制。结果表明：当煅烧温度由300℃升至500℃时，磁性铁氧化物的比表面积、孔容先增大后减小，且较高的煅烧温度促使其γ-Fe₂O₃晶体逐步转变为α-Fe₂O₃晶体，导致磁性铁氧化物表面Fe²⁺和活性氧浓度增大，促使其NH₃-SCR脱硝性能降低；掺杂钛可提高磁性铁氧化物的热稳定性，抑制了高温煅烧下γ-Fe₂O₃晶体向α-Fe₂O₃晶体的不可逆转变和其孔隙结构的坍塌，增大了高温煅烧时磁性铁氧化物催化剂的比表面积和比孔容，合适的煅烧温度为400℃；该煅烧温度下，催化剂低温活性最佳，反应温度高于220℃、空速比60000h^-1时可获得80%以上的NO_x转化效率。

关键词: 污染, 选择催化还原, 催化剂, 共沉淀, 煅烧温度, 微观结构, 微波辐射

Abstract: A novel magnetic iron-titanium mixed oxide catalyst was prepared through the co-precipitation method under microwave irradiation. The effect of calcination temperature on its micro-structure and the NH₃-SCR activity was investigated. The mechanism of the enhancements on the NH₃-SCR activity and the high-temperature irreversible thermal transformation of magnetic γ-Fe₂O₃ crystal by the addtion of titanium was also revealed. The results indicated that the BET surface area and the pore volume of the prepared magnetic iron oxide firstly increased and then decreased when the calcination temperature increased from 300℃ to 500℃. Meanwhile, γ-Fe₂O₃ crystals irreversibly transformed into α-Fe₂O₃ after being calcined at high temperature, giving rise to the increase of the concentrations of Fe²⁺ and active oxygen on its surface, thereby decreased the NH₃-SCR activity of magnetic iron oxide catalyst. The addition of titanium oxide improved the thermal stability of γ-Fe₂O₃ crystals in magnetic iron oxide. The irreversible thermal transformation of γ-Fe₂O₃ crystal into α-Fe₂O₃ crystal and the collapsing of microscopic pore structure of the magnetic iron oxide were also depressed when it was calcined at high temperature. Therefore, the addition of titanium oxide improved the BET surface area and the pore volume of the magnetic iron oxide. The suitable calcination temperature for the magnetic iron oxide based catalysts prepared through the microwave irradiation assisted co-precipitation method is 400℃, under which the catalyst showed the best low-temperature catalytic activity. When the reaction temperature was higher than 220℃, the NO_x conversion was more than 80% under the gas space velocity of 60000 h^-1。

Key words: pollution, selective catalytic reduction (SCR), catalyst, co-precipitation, calcination temperature, micro-structure, microwave irradiation

中图分类号:

周飞, 熊志波, 金晶, 武超, 陆威, 丁旭春. 煅烧温度对磁性铁钛复合氧化物微观结构及脱硝活性的影响[J]. 化工进展, 2018, 37(09): 3410-3415.

ZHOU Fei, XIONG Zhibo, JIN Jing, WU Chao, LU Wei, DING Xuchun. Influence of calcination temperature on the micro-structure and the NH₃-SCR activity of magnetic iron-titanium mixed oxide catalyst[J]. Chemical Industry and Engineering Progress, 2018, 37(09): 3410-3415.

参考文献

[1] XIONG Z B, HU Q, LIU D Y, et al. Influence of partial substitution of iron oxide by titanium oxide on the structure and activity of iron-cerium mixed oxide catalyst for selective catalytic reduction of NO_x with NH₃[J]. Fuel, 2016, 165:432-439.
[2] 苏亚欣, 苏阿龙, 任立铭. 铁基催化剂脱除NO气体的研究现状[J]. 化工进展, 2012, 31(s1):154-157. SU Y X, SU A L, REN L M. Review on state-of-art of NO reduction by iron-based catalyst[J]. Chemical Industry and Engineering Progress, 2012, 31(s1):154-157.
[3] YAO G H, WANG F, WANG X B, et al. Magnetic field effects on selective catalytic reduction of NO by NH₃ over Fe₂O₃ catalyst in a magnetically fluidized bed[J]. Energy, 2010, 35(5):2295-2300.
[4] LIU C X, YANG S J, MA L, et al. Comparison on the performance of α-Fe₂O₃ and γ-Fe₂O₃ for selective catalytic reduction of nitrogen oxides with ammonia[J]. Catalysis Letters, 2013, 143(7):697-704.
[5] WU G X, LI J, FANG Z T, et al. FeVO₄ nanorods supported TiO₂ as a superior catalyst for NH₃-SCR reaction in a broad temperature range[J]. Catalysis Communications, 2015, 64:75-79.
[6] YANG S J, LI J H, WANG C Z, et al. Fe-Ti spinel for the selective catalytic reduction of NO with NH₃:mechanism and structureactivity relationship[J]. Applied Catalysis B:Environmental, 2012, 117/118(3):73-80.
[7] 武超, 熊志波, 周飞, 等. 磁性铁钛催化剂的制备及其NH₃选择性催化还原NO性能[J]. 上海理工大学学报, 2016, 37(5):427-432. WU C, XIONG Z B, ZHOU F, et al. Selective catalytic reduction of NO_x with NH₃ over magnetic iron-titanium mixed oxide catalysts[J]. Journal of University of Shanghai for Science and Technology, 2016, 37(5):427-432.
[8] 王芳, 姚桂焕, 归柯庭. 铁基催化剂选择性催化还原烟气脱硝特性比较研究[J]. 中国电机工程学报, 2009, 29:47-51. WANG F, YAO G H, GUI K T. Comparison about selective catalytic reduction of deNO_x on iron-based magnetic materials[J]. Proceedings of the CSEE, 2009, 29:47-51.
[9] SING K S W, EVERETT D H, HAUL R A W, et al. Reporting physisorption data for gas/solid systems with special reference to the determination of surface area and porosity[J]. Pure & Applied Chemistry, 1985, 57(4):603-619.
[10] FANG N J, GUO J X, SHU S, et al. Enhancement of low-temperature activity and sulfur resistance of Fe_0.3Mn_0.5Zr_0.2 catalyst for NO removal by NH₃-SCR[J]. Chemical Engineering Journal, 2017, 325:114-123.
[11] SHWAN S, NEDYAL K, JANSSON J, et al. Hydrothermal stability of Fe-BEA as an NH₃-SCR catalyst[J]. Industrial & Engineering Chemistry Research, 2012, 51(39):12762-12772.
[12] LI X, LI J H, PENG Y, et al. Selective catalytic reduction of NO with NH₃ over novel iron-tungsten mixed oxide catalyst in a broad temperature range[J]. Catalysis Science & Technology, 2015, 5(9):4556-4564.
[13] ZHANG S, QIU M, YANG S, et al. Facile preparation of MnO₂ doped Fe₂O₃ hollow nanofibers for low temperature SCR of NO with NH₃[J]. Journal of Materials Chemistry A, 2014, 2(48):20486-20493.
[14] YANG S J, GUO Y F, YAN N Q, et al. Capture of gaseous elemental mercury from flue gas using a magnetic and sulfur poisoning resistant sorbent Mn/γ-Fe₂O₃ at lower temperatures.[J]. Journal of Hazardous Materials, 2011, 186(1):508-515.
[15] YANG S J, GUO Y F, YAN N Q, et al. Remarkable effect of the incorporation of titanium on the catalytic activity and SO₂ poisoning resistance of magnetic Mn-Fe spinel for elemental mercury capture[J]. Applied Catalysis B:Environmental, 2011, 101(3/4):698-708.
[16] 陈亚南, 段钰峰, 朱纯, 等. Mo/Mn-TiO₂催化剂的脱硝活性剂抗SO₂ 性能[J]. 化工进展, 2017, 36(8):2941-2948. CHEN Y N, DUAN Y F, ZHU C, et al. NH₃-SCR catalytic activity and SO₂ resistance over Mo/Mn-TiO₂ catalyst[J]. Chemical Industry and Engineering Progress, 2017, 36(8):2941-2948.
[17] LIU F D, HE H, DING Y, et al. Effect of manganese substitution on the structure and activity of iron titanate catalyst for the selective catalytic reduction of NO with NH₃[J]. Applied Catalysis B:Environmental, 2009, 93(1):3760-3769.
[18] LIU F D, ASAKURA K, HE H, et al. Influence of sulfation on iron titanate catalyst for the selective catalytic reduction of NO_x with NH₃[J]. Applied Catalysis B:Environmental, 2011, 103(3):369-377.

煅烧温度对磁性铁钛复合氧化物微观结构及脱硝活性的影响

Influence of calcination temperature on the micro-structure and the NH₃-SCR activity of magnetic iron-titanium mixed oxide catalyst

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煅烧温度对磁性铁钛复合氧化物微观结构及脱硝活性的影响

Influence of calcination temperature on the micro-structure and the NH3-SCR activity of magnetic iron-titanium mixed oxide catalyst

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Influence of calcination temperature on the micro-structure and the NH₃-SCR activity of magnetic iron-titanium mixed oxide catalyst