Simultaneous removal of sulfur dioxide and nitrogen oxide from flue gas by phosphorus sludge: The performance and absorption mechanism

doi:10.1016/j.cjche.2023.09.001

中国化学工程学报 ›› 2024, Vol. 65 ›› Issue (1): 212-221.DOI: 10.1016/j.cjche.2023.09.001

• Full Length Article • 上一篇下一篇

Simultaneous removal of sulfur dioxide and nitrogen oxide from flue gas by phosphorus sludge: The performance and absorption mechanism

Yuanyuan Yin^1,2,3, Xujun Wang^1,2,3, Lei Xu^1,2,3, Binbin He^1,2,3, Yunxiang Nie^1,2,3, Yi Mei^1,2,3

1 Faculty of Chemical Engineering, Kunming University of Science and Technology, Kunming 650500, China;
2 Yunnan Provincial Key Laboratory of Energy Saving in Phosphorus Chemical Engineering and New Phosphorus Materials, Kunming 650500, China;
3 The Higher Educational Key Laboratory for Phosphorus Chemical Engineering of Yunnan Province, Kunming 650500, China

收稿日期:2023-06-12 修回日期:2023-09-08 出版日期:2024-01-28 发布日期:2024-04-17
通讯作者: Yunxiang Nie, E-mail:YunxiangNie@126.com;Yi Mei,E-mail:meiyi412@126.com
基金资助:
The National Natural Science Foundation of China (22068019) and Yunnan Major Scientific and Technological Projects (202202AG050001) are gratefully acknowledged for financial support of this research work.

Simultaneous removal of sulfur dioxide and nitrogen oxide from flue gas by phosphorus sludge: The performance and absorption mechanism

Yuanyuan Yin^1,2,3, Xujun Wang^1,2,3, Lei Xu^1,2,3, Binbin He^1,2,3, Yunxiang Nie^1,2,3, Yi Mei^1,2,3

1 Faculty of Chemical Engineering, Kunming University of Science and Technology, Kunming 650500, China;
2 Yunnan Provincial Key Laboratory of Energy Saving in Phosphorus Chemical Engineering and New Phosphorus Materials, Kunming 650500, China;
3 The Higher Educational Key Laboratory for Phosphorus Chemical Engineering of Yunnan Province, Kunming 650500, China

Received:2023-06-12 Revised:2023-09-08 Online:2024-01-28 Published:2024-04-17
Contact: Yunxiang Nie, E-mail:YunxiangNie@126.com;Yi Mei,E-mail:meiyi412@126.com
Supported by:
The National Natural Science Foundation of China (22068019) and Yunnan Major Scientific and Technological Projects (202202AG050001) are gratefully acknowledged for financial support of this research work.

摘要/Abstract

摘要： Developing low-cost and green simultaneous desulfurization and denitrification technologies is of great significance for sulfur dioxide (SO₂) and nitrogen oxide (NO_x) emission control at low temperatures, especially for small and medium-sized coal-fired boilers and furnaces. Herein, phosphorus sludge, an industrial waste from the production process of yellow phosphorus, has been developed to simultaneously eliminate SO₂ and NO_x from coal-fired flue gas. The key factors affecting the experimental results indicate that desulfurization and denitrification efficiency of over 95% can be achieved at a low temperature of 55 ℃. Further, the absorption mechanism was investigated by characterizing the solid and liquid phases of the phosphorus sludge during the absorption process. The efficient removal of SO₂ is attributed to the abundance of iron (Fe³⁺) and manganese (Mn₂₊) in the absorbent. SO₂ can be rapidly catalyzed and converted to SO₄^2- by them. The key to NO_x removal is the oxidation of NO toward watersoluble high-valent nitrogen oxides by oxidizing reactive substances induced via yellow phosphorus, which are then absorbed by water and converted to NO₃^-. Meanwhile, yellow phosphorus is oxidized to phosphoric acid (H₃PO₄). The spent absorption slurry can be reused through wet process phosphoric acid production, as it contains sulfuric acid (H₂SO₄), nitric acid (HNO₃), and H₃PO₄. Accordingly, this is a technology with broad application prospects.

关键词: Absorption, Oxidation, Multiphase reaction, Phosphorus sludge, Yellow phosphorus, Low temperature

Abstract: Developing low-cost and green simultaneous desulfurization and denitrification technologies is of great significance for sulfur dioxide (SO₂) and nitrogen oxide (NO_x) emission control at low temperatures, especially for small and medium-sized coal-fired boilers and furnaces. Herein, phosphorus sludge, an industrial waste from the production process of yellow phosphorus, has been developed to simultaneously eliminate SO₂ and NO_x from coal-fired flue gas. The key factors affecting the experimental results indicate that desulfurization and denitrification efficiency of over 95% can be achieved at a low temperature of 55 ℃. Further, the absorption mechanism was investigated by characterizing the solid and liquid phases of the phosphorus sludge during the absorption process. The efficient removal of SO₂ is attributed to the abundance of iron (Fe³⁺) and manganese (Mn₂₊) in the absorbent. SO₂ can be rapidly catalyzed and converted to SO₄^2- by them. The key to NO_x removal is the oxidation of NO toward watersoluble high-valent nitrogen oxides by oxidizing reactive substances induced via yellow phosphorus, which are then absorbed by water and converted to NO₃^-. Meanwhile, yellow phosphorus is oxidized to phosphoric acid (H₃PO₄). The spent absorption slurry can be reused through wet process phosphoric acid production, as it contains sulfuric acid (H₂SO₄), nitric acid (HNO₃), and H₃PO₄. Accordingly, this is a technology with broad application prospects.

Key words: Absorption, Oxidation, Multiphase reaction, Phosphorus sludge, Yellow phosphorus, Low temperature

Yuanyuan Yin, Xujun Wang, Lei Xu, Binbin He, Yunxiang Nie, Yi Mei. Simultaneous removal of sulfur dioxide and nitrogen oxide from flue gas by phosphorus sludge: The performance and absorption mechanism[J]. 中国化学工程学报, 2024, 65(1): 212-221.

参考文献

[1] C.Q. Zhu, J.B. Ru, S.Q. Gao, C.M. Li, The simultaneous removal of NO_x and SO₂ from flue gas by direct injection of sorbents in furnace of waste incinerator, Fuel 333(2023)126464.
[2] X. Kang, X.X. Ma, J.A. Yin, X.C. Gao, A study on simultaneous removal of NO and SO₂ by using sodium persulfate aqueous scrubbing, Chin. J. Chem. Eng. 26(7)(2018)1536-1544.
[3] K. Li, Q.Y. Li, H.D. Fan, Y.H. Wang, S.C. Chang, C.H. Zhao, Soft sensing of SO₂ emission for ultra-low emission coal-fired power plant with dynamic model and segmentation model, Fuel 332(2023)125921.
[4] Y.X. Zhang, C. Luo, Y. Lu, Y. Zhang, C. Zhou, Z.Y. Zhou, X.C. Wu, C.H. Zheng, X. Gao, Technology development and cost analysis of multiple pollutant abatement for ultra-low emission coal-fired power plants in China, J. Environ. Sci.(China)123(2023)270-280.
[5] N.E. Altun, Assessment of marble waste utilization as an alternative sorbent to limestone for SO₂ control, Fuel Process. Technol 128(2014)461-470.
[6] K.J. He, Q. Song, Z.N. Yan, N. Zheng, Q. Yao, Study on competitive absorption of SO₃ and SO₂ by calcium hydroxide, Fuel 242(2019)355-361.
[7] T.S. Zhang, C. Wu, B. Li, J.W. Wang, R. Ravat, X.Z. Chen, J.X. Wei, Q.J. Yu, Linking the SO₂ emission of cement plants to the sulfur characteristics of their limestones:A study of 80 NSP cement lines in China, J. Clean. Prod. 220(2019)200-211.
[8] S. Mohan, P. Dinesha, S. Kumar, NO_x reduction behaviour in copper zeolite catalysts for ammonia SCR systems:A review, Chem. Eng. J. 384(2020)123253.
[9] S.L. Zhao, J.L. Peng, R.Q. Ge, S.Y. Wu, K.H. Zeng, H.J. Huang, K.B. Yang, Z.Q. Sun, Research progress on selective catalytic reduction (SCR) catalysts for NO_x removal from coal-fired flue gas, Fuel Process. Technol. 236(2022)107432.
[10] H.H. Li, W. Zhao, L.C. Wu, Q. Wang, D.H. Shang, Q. Zhong, Boosting lowtemperature selective catalytic reduction of NO_x with NH₃ of V₂O₅/TiO₂ catalyst via B-doping, Chin. J. Chem. Eng. 44(2022)377-383.
[11] X. Yong, H. Chen, H.W. Zhao, M. Wei, Y.N. Zhao, Y.D. Li, Insight into SO₂ poisoning and regeneration of one-pot synthesized Cu-SSZ-13 catalyst for selective reduction of NO_x by NH₃, Chin. J. Chem. Eng. 46(2022)184-193.
[12] G.Y. Xu, X.L. Guo, X.X. Cheng, J. Yu, B.Z. Fang, A review of Mn-based catalysts for low-temperature NH₃-SCR:NO_x removal and H₂O/SO₂ resistance, Nanoscale 13(15)(2021)7052-7080.
[13] M.S. Kang, J. Shin, T.U. Yu, J. Hwang, Simultaneous removal of gaseous NO_x and SO₂ by gas-phase oxidation with ozone and wet scrubbing with sodium hydroxide, Chem. Eng. J. 381(2020)122601.
[14] Y. Zou, Y. Wang, X.L. Liu, T.Y. Zhu, M.K. Tian, M.Y. Cai, Simultaneous removal of NO_x and SO₂ using two-stage O₃ oxidation combined with Ca (OH)2 absorption, Korean J. Chem. Eng. 37(11)(2020)1907-1914.
[15] Y. Xing, L.L. Li, P. Lu, J.S. Cui, Q.L. Li, B.J. Yan, B. Jiang, M.S. Wang, Simultaneous purifying of Hg⁰, SO₂, and NO_x from flue gas by Fe³⁺/H₂O₂:The performance and purifying mechanism, Environ. Sci. Pollut. Res. Int. 25(7)(2018)6456-6465.
[16] S.H. Jia, G. Pu, J. Gao, C. Yuan, Oxidationeabsorption process for simultaneous removal of NO_x and SO₂ over Fe/Al₂O₃@SiO₂ using vaporized H₂O₂, Chemosphere 291(Pt 3)(2022)133047.
[17] B.R. Deshwal, H.K. Lee, Mass transfer in the absorption of SO₂ and NO_x using aqueouseuchlorine scrubbingsolution, J. Environ. Sci. China21(2)(2009)155-161.
[18] J. Johansson, A.H. Hultén, F. Normann, K. Andersson, Simultaneous removal of NO_x and SO_x from flue gases using ClO₂:Process scaling and modeling simulations, Ind. Eng. Chem. Res. 60(2021)1774-1783.
[19] J.C. Bao, K. Li, P. Ning, C. Wang, X. Song, Y.S. Luo, X. Sun, Study on the role of copper converter slag in simultaneously removing SO₂ and NO_x using KMnO₄/copper converter slag slurry, J. Environ. Sci.(China)108(2021)33-43.
[20] J.G. Wang, H.H. Yi, X.L. Tang, S.Z. Zhao, F.Y. Gao, Simultaneous removal of SO₂ and NO_x by catalytic adsorption using γ-Al₂O₃ under the irradiation of nonthermal plasma:Competitiveness, kinetic, and equilibrium, Chem. Eng. J. 384(2020)123334.
[21] B.M. Obradovi c, G.B. Sretenovi c, M.M. Kuraica, A dual-use of DBD plasma for simultaneous NO_x and SO₂ removal from coal-combustion flue gas, J. Hazard. Mater. 185(2-3)(2011)1280-1286.
[22] H. Yamasaki, Y. Mizuguchi, R. Nishioka, Y. Fukuda, T. Kuroki, H. Yamamoto, M. Okubo, Pilot-scale NO_x and SO_x aftertreatment by semi-dry plasmaechemical hybrid process in glass-melting-furnace exhaust gas, Plasma Chem. Plasma Process. 42(1)(2022)51-71.
[23] H. Fujishima, K. Takekoshi, T. Kuroki, A. Tanaka, K. Otsuka, M. Okubo, Towards ideal NO_x control technology for bio-oils and a gas multi-fuel boiler system using a plasmaechemical hybrid process, Appl. Energy 111(2013)394-400.
[24] M. Okubo, Recent development of technology in scale-up of plasma reactors for environmental and energy applications, Plasma Chem. Plasma Process. 42(1)(2022)3-33.
[25] W.Y. Sun, S.L. Ding, S.S. Zeng, S.J. Su, W.J. Jiang, Simultaneous absorption of NO_x and SO₂ from flue gas with pyrolusite slurry combined with gas-phase oxidation of NO using ozone, J. Hazard. Mater. 192(1)(2011)124-130.
[26] J.C. Bao, P. Ning, F. Wang, X. Sun, C. Wang, X. Song, Y.S. Luo, K. Li, Thermal modification ofcopper slag via phase transformation for simultaneous removal of SO₂ and NO_x from acid-making tail gas, Chem. Eng. J. 425(2021)131646.
[27] Y.X. Nie, S.A. Li, C.J. Wu, C. Wang, D.D. He, Y. Mei, Efficient removal of SO₂ from flue gas with phosphate rock slurry and investigation of reaction mechanism, Ind. Eng. Chem. Res. 57(44)(2018)15138-15146.
[28] Y.S. Luo, P. Ning, C. Wang, F. Wang, Y.X. Ma, J.C. Bao, X. Sun, K. Li, Pretreated water-quenched-manganese-slag slurry for high-efficiency one-step desulfurization and denitrification, Sep. Purif. Technol. 250(2020)117164.
[29] E. Fois, A. Lallai, G. Mura, Sulfur dioxide absorption in a bubbling reactor with suspensions of bayer red mud, Ind. Eng. Chem. Res. 46(21)(2007)6770-6776.
[30] Z.H. Meng, C.Y. Wang, X.R. Wang, Y. Chen, H.Q. Li, Simultaneous removal of SO₂ and NO_x from coal-fired flue gas using steel slag slurry, Energy Fuels 32(2)(2018)2028-2036.
[31] Y.X. Nie, X.J. Wang, J.F. Dai, C. Wang, D.D. He, Y. Mei, Mutual promotion effect of SO₂ and NO_x during yellow phosphorus and phosphate rock slurry adsorption process, AIChE. J. 67(8)(2021) -17236.
[32] Y.X. Nie, J.F. Dai, Y.D. Hou, Y.Z. Zhu, C. Wang, D.D. He, Y. Mei, An efficient and environmentally friendly process for the reduction of SO₂ by using waste phosphate mine tailings as adsorbent, J. Hazard. Mater. 388(2020)121748.
[33] H.M. Rietveld, The Rietveld method, Phys. Scr. 89(9)(2014)098002.
[34] Y. Zhang, J.T. Zhou, C.Y. Li, G.D. Wang, S.Y. Guo, Research progress on liquidphase catalysis of SO₂ oxidation by transition metal ions, in:2011 International Conference on Remote Sensing, Environment and Transportation Engineering, IEEE, Nanjing, China, 2011.
[35] D. Karatza, M. Prisciandaro, A. Lancia, D. Musmarra, Calcium bisulfite oxidation in the flue gas desulfurization process catalyzed by iron and manganese ions, Ind. Eng. Chem. Res. 43(16)(2004)4876-4882.
[36] Y.X. Nie, S. Li, J.F. Dai, D.D. He, Y. Mei, Catalytic effect of Mn₂₊, Fe³⁺ and Mg²⁺ ions on desulfurization using phosphate rock slurry as absorbent, Chem. Eng. J. 390(2020)124568.
[37] Y.X. Nie, L. Xu, Y.F. Yang, D.D. He, Y. Mei, Mechanism investigation on yellow phosphorus inducing O, O₃ and OH$radicals in phosphate rock slurry for high-efficiency NO oxidation, Sep. Purif. Technol. 312(2023)123435.
[38] L.J. Jia, X. Song, L.N. Sun, S.T. Zhang, K. Li, P. Ning, Catalytic effect of phosphorus on SO₂ oxidation in liquid phase:Experimental and theoretical studies, Chem. Eng. J. 429(2022)132376.
[39] S.A. Li, J.Q. Yang, C. Wang, D.L. Xie, Y.M. Luo, K. Li, D.D. He, Y. Mei, Removal of NO_x from flue gas using yellow phosphorus and phosphate slurry as adsorbent, Energy Fuels 32(4)(2018)5279-5288.
[40] B.D. Wang, Y.X. Zhou, L. Li, H. Xu, Y.L. Sun, Y. Wang, Novel synthesis of cyanofunctionalized mesoporous silica nanospheres (MSN) from coal fly ash for removal of toxic metals from wastewater, J. Hazard. Mater. 345(2018)76-86.
[41] A. Huss, P.K. Lim, C. A Eckert, Oxidation of aqueous sulfur dioxide. 1. Homogeneous manganese (II) and iron (II) catalysis at low pH, J. Phys. Chem. 86(21)(1982)4224-4228.
[42] X. Wang, Y. Mei, Y. Yang, C. Ye, D. He, L. Xu, B. He, Y. Nie, The effect of primary components of phosphate rock on wet flue gas desulfurization, Chin. J. Environ. Eng. 16(9)(2022)2921-2929.(in Chinese)

Simultaneous removal of sulfur dioxide and nitrogen oxide from flue gas by phosphorus sludge: The performance and absorption mechanism

Simultaneous removal of sulfur dioxide and nitrogen oxide from flue gas by phosphorus sludge: The performance and absorption mechanism

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 15

编辑推荐

Metrics

本文评价

[1]	Songling Guo, Xun Tao, Fan Zhou, Mengyan Yu, Yufan Wu, Yunfei Gao, Lu Ding, Fuchen Wang. Investigation of oxy-fuel combustion for methane and acid gas in a diffusion flame[J]. 中国化学工程学报, 2024, 65(1): 106-116.
[2]	Binxia Zhao, Yijia Gao, Tiancheng Hun, Xiaoxiao Fan, Nan Shao, Xiaoqian Chen. Preparation of PrFe_xCo_1-xO₃/Mt catalyst and study on degradation of 2-hydroxybenzoic acid wastewater by catalytic wet peroxide oxidation[J]. 中国化学工程学报, 2024, 65(1): 286-297.
[3]	Jinpei Huang, Xingwei Lu, Xuejing Zhang, Yiqiang Jin, Yifeng Zhou. Continuous, efficient and safe synthesis of 1-oxa-2-azaspiro [2.5] octane in a microreaction system[J]. 中国化学工程学报, 2023, 61(9): 37-42.
[4]	Wenjian Yue, Xiaojiang Li, Junhao Jing, Li Tong, Na Wang, Hongsheng Lu, Zhiyu Huang. A CO₂-controllable phase change absorbent solvent used to waste recycling of dining lampblack[J]. 中国化学工程学报, 2023, 61(9): 110-117.
[5]	Xun Tao, Fan Zhou, Xinlei Yu, Songling Guo, Yunfei Gao, Lu Ding, Guangsuo Yu, Zhenghua Dai, Fuchen Wang. Effect of carbon dioxide on oxy-fuel combustion of hydrogen sulfide: An experimental and kinetic modeling[J]. 中国化学工程学报, 2023, 59(7): 105-117.
[6]	Zijie Zhang, Qianyu Zha, Ying Liu, Zhibing Zhang, Jia Liu, Zheng Zhou. Study on the epoxidation of olefins with H₂O₂ catalyzed by biquaternary ammonium phosphotungstic acid[J]. 中国化学工程学报, 2023, 58(6): 146-154.
[7]	Shuangtai Liu, Lei He, Qiuxiang Yao, Xi Li, Linyang Wang, Jing Wang, Ming Sun, Xiaoxun Ma. Separation and analysis of six fractions in low temperature coal tar by column chromatography[J]. 中国化学工程学报, 2023, 58(6): 256-265.
[8]	Yutong Jiang, Yifeng Chen, Fuliu Yang, Jixue Fan, Jun Li, Zhuhong Yang, Xiaoyan Ji. Efficient SO₂ removal using aqueous ionic liquid at low partial pressure[J]. 中国化学工程学报, 2023, 58(6): 355-363.
[9]	Chenyang Zhao, Yinhan Cheng, Guangfei Qu, Yongheng Yuan, Fenghui Wu, Ye Liu, Shan Liu, Junyan Li, Ping Ning. High-performance liquid-phase catalytic purification of phosphine in tail gas using Pd(II)/Cu(II) composite[J]. 中国化学工程学报, 2023, 57(5): 98-108.
[10]	Qi Yang, Weikang Dai, Maoshuai Li, Jie Wei, Yi Feng, Cheng Yang, Wanxin Yang, Ying Zheng, Jie Ding, Mei-Yan Wang, Xinbin Ma. Enhanced selective hydrogenation of glycolaldehyde to ethylene glycol over Cu⁰-Cu⁺ sites[J]. 中国化学工程学报, 2023, 57(5): 141-150.
[11]	Feng Pan, Sugang Ma, Yu Ge, Chuanlin Fan, Qingshan Zhu. Fluidization thermal decomposition of sodium fluosilicate[J]. 中国化学工程学报, 2023, 57(5): 329-337.
[12]	Bingxiao Feng, Lining Hao, Chaoting Deng, Jiaqiang Wang, Hongbing Song, Meng Xiao, Tingting Huang, Quanhong Zhu, Hengjun Gai. A highly hydrothermal stable copper-based catalyst for catalytic wet air oxidation of m-cresol in coal chemical wastewater[J]. 中国化学工程学报, 2023, 57(5): 338-348.
[13]	Shengfeng Luo, Song Zhang, Yiping Zeng, Hui Zhang, Lili Zheng, Zhaopeng Xu. Study on oxygen transport and titanium oxidation in coating cracks under parallel gas flow based on LBM modelling[J]. 中国化学工程学报, 2023, 56(4): 15-24.
[14]	Yuxi Chai, Yanan Zhang, Yannan Tan, Zhiwei Li, Huangzhao Wei, Chenglin Sun, Haibo Jin, Zhao Mu, Lei Ma. Life cycle assessment of high concentration organic wastewater treatment by catalytic wet air oxidation[J]. 中国化学工程学报, 2023, 56(4): 80-88.
[15]	Peiyin Chen, Yanxiong Fang, Kaihong Xie, Yao Chen, Yang Liu, Hongliang Zuo, Weijian Lu, Baoyu Liu. Lacunary silicotungstic heteropoly salts as high-performance catalysts in oxidation of cyclopentene[J]. 中国化学工程学报, 2023, 56(4): 152-159.