Citation: ZHANG Shuan-Qin, KONG Ling-Dong, ZHAO Xi, Roel JANSEN, CHEN Jian-Min. Effects of Ammonia and Amines on Heterogeneous Oxidation of Carbonyl Sulfide on Hematite[J]. Acta Physico-Chimica Sinica, ;2013, 29(09): 2027-2034. doi: 10.3866/PKU.WHXB201306171 shu

Effects of Ammonia and Amines on Heterogeneous Oxidation of Carbonyl Sulfide on Hematite

1.
Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention, Department of Environmental Science & Engineering, Fudan University, Shanghai 200433, P. R. China

Received Date: 22 March 2013
Available Online: 17 June 2013
Fund Project: 国家自然科学基金(21077025, 21277028, 21190053) (21077025, 21277028, 21190053)上海市科学技术委员会项目(10231203801, 10JC1401600)资助 (10231203801, 10JC1401600)

The heterogeneous oxidation of carbonyl sulfide (COS) on hematite pre-adsorbed with ammonia and methylamine, trimethylamine, triethylamine, phenylamine, pyridine, and pyrrole was investigated using in situ diffuse-reflectance infrared Fourier-transform spectroscopy (DRIFTS) at room temperature. The products and kinetics of the heterogeneous reaction were investigated. The results showed that adsorbed COS could be oxidized on the surface of hematite pre-adsorbed with these basic substances, forming gaseous carbon dioxide (CO₂), surface bicarbonate (HCO₃^-), surface carbonate (CO₃^2-), and surface SO₄^2-. Ammonia and amines pre-adsorbed on hematite significantly enhanced the reactivity of COS. Hematite with pre-adsorbed methylamine exhibited the highest reactivity, about 4.5 times higher than that of pure hematite, whereas the effects of phenylamine and pyrrole were not obvious. The reaction rates with the basic substances were in the order of methylamine>trimethylamine>ammonia>triethylamine>pyridine> pyrrole> phenylamine≈pure hematite. The basic substances changed the reaction order from first to second. Coverage by the basic substances and surface water also played important roles in the heterogeneous reaction of COS. These experimental results indicated that surface oxygen species (M―O^-) were the key factor contributing to oxidizing activities in the presence of basic substances. The heterogeneous oxidation mechanism of COS on hematite with pre-adsorbed basic substances is discussed on the basis of the experimental results.
- Carbonyl sulfide,
- Ammonia,
- Amine,
- Hematite,
- Heterogeneous reaction
1. [1]
  
  (1) Turco, R. P.;Whitten, R. C.; Toon, O. B.; Pollack, J. B.; Hamill,P. Nature 1980, 283, 283. doi: 10.1038/283283a0
2. [2]
  (2) Sze, N. D.; Ko, M. K. W. Nature 1979, 278, 731. doi: 10.1038/278731a0
3. [3]
  (3) Sze, N. D.; Ko, M. K. W. Nature 1979, 280, 308. doi: 10.1038/280308a0
4. [4]
  (4) Sze, N. D.; Ko, M. K. W. Atmos. Environ. 1980, 14, 1223. doi: 10.1016/0004-6981(80)90225-5
5. [5]
  (5) Svoronos, P. D. N.; Bruno, T. J. Ind. Eng. Chem. Res. 2002, 41,5321. doi: 10.1021/ie020365n
6. [6]
  (6) Torres, A. L.; Maroulis, P. J.; ldberg, A. B.; Bandy, A. R. J. Geophys. Res. 1980, 85, 7357. doi: 10.1029/JC085iC12p07357
7. [7]
  (7) Rasmussen, R. A.; Khalil, M. A. K.; Hoyt, S. D. Atmos. Environ.1982, 16, 1591. doi: 10.1016/0004-6981(82)90111-1
8. [8]
  (8) Watts, S. F. Atmos. Environ. 2000, 34, 761. doi: 10.1016/S1352-2310(99)00342-8
9. [9]
  (9) Wu, H. B.; Wang, X.; Chen, J. M.; Yu, H. K.; Xue, H. X.; Pan,X. X.; Hou, H. Q. Chin. Sci. Bull. 2004, 49, 739. [吴洪波,王晓, 陈建民,俞宏坤, 薛华欣,潘循晳, 侯惠奇.科学通报,2004, 49, 739.] doi: 10.1360/03wb0132
10. [10]
  (10) He, H.; Liu, J. F.; Mu, Y. J.; Yu, Y. B.; Chen, M. X. Environ. Sci. Technol. 2005, 39, 9637. doi: 10.1021/es048865q
11. [11]
  (11) Liu, J. F.; Yu, Y. B.; Mu, Y. J.; He, H. J. Phys. Chem. B 2006,110, 3225. doi: 10.1021/jp055646y
12. [12]
  (12) Liu, Y. C.; He, H.; Xu, W. Q.; Yu, Y. B. J. Phys. Chem. A 2007,111, 4333. doi: 10.1021/jp069015v
13. [13]
  (13) Liu, Y. C.; He, H. J. Phys. Chem. A 2009, 113, 3387. doi: 10.1021/jp809887c
14. [14]
  (14) Chen, H. H.; Kong, L. D.; Chen, J. M.; Zhang, R. Y.; Wang, L.Environ. Sci. Technol. 2007, 41, 6484. doi: 10.1021/es070717n
15. [15]
  (15) Yu, Y. J.; Zhang, S. Q.; Kong, L. D.; Lin, L.; Cheng, T. T.; Chen,J. M. Acta Phys. -Chim. Sin. 2011, 27, 2275. [俞偐偼,张拴勤,孔令东,林立,成天涛,陈建民. 物理化学学报, 2011, 27,2275.] doi: 10.3866/PKU.WHXB20110912
16. [16]
  (16) Usher, C. R.; Michel, A. E.; Grassian, V. H. Chem. Rev. 2003,103, 4883. doi: 10.1021/cr020657y
17. [17]
  (17) Wang, X. F.; Gao, S.; Yang, X.; Chen, H.; Chen, J. M.; Zhuang,G. S.; Surratt, J. D.; Chan, M. N.; Seinfeld, J. H. Environ. Sci. Technol. 2010, 44, 4441. doi: 10.1021/es1001117
18. [18]
  (18) Cadle, S. H.; Mulawa, P. A. Environ. Sci. Technol. 1980, 14,718. doi: 10.1021/es60166a011
19. [19]
  (19) Westerholm, R.; Li, H.; Almen, J. Chemosphere 1993, 27, 1381.doi: 10.1016/0045-6535(93)90231-S
20. [20]
  (20) Chen, C. P.; Veregin, R. P.; Harbour, J. R.; Hair, M. L. Chin. Sci. Bull. 1994, 39, 744. [陈次平, Veregin, R. P., Harbour, J. R.,Hair, M. L.科学通报, 1994, 39, 744.]
21. [21]
  (21) Vanneste, A.; Duce, R. A.; Lee, C. Geophys. Res. Lett. 1987, 14,711. doi: 10.1029/GL014i007p00711
22. [22]
  (22) Zhang, Q.; Anastasio, C. Atmos. Environ. 2003, 37, 2247. doi: 10.1016/S1352-2310(03)00127-4
23. [23]
  (23) Lavalley, J. C. Catal. Today 1996, 27, 377. doi: 10.1016/0920-5861(95)00161-1
24. [24]
  (24) Lercher, J. A.; Grundling, C.; EderMirth, G. Catal. Today 1996,27, 353. doi: 10.1016/0920-5861(95)00248-0
25. [25]
  (25) Sarria, F. R.; Blasin-Aube, V.; Saussey, J.; Marie, O.; Daturi, M.J. Phys. Chem. B 2006, 110, 13130. doi: 10.1021/jp061729i
26. [26]
  (26) Qiu, C.; Zhang, R. Y. Environ. Sci. Technol. 2012, 46, 4474.doi: 10.1021/es3004377
27. [27]
  (27) Gai, Y. B.; Ge, M. F.; Wang, W. G. Acta Phys. -Chim. Sin. 2010,26, 1768. [盖艳波, 葛茂发, 王玮罡. 物理化学学报, 2010,26, 1768.] doi: 10.3866/PKU.WHXB20100705
28. [28]
  (28) Yin, S.; Ge, M. F.; Wang, W. G.; Liu, Z.; Wang, D. X. Chin. Sci. Bull. 2011, 56, 1241. [殷实,葛茂发,王炜罡,刘泽,王殿勋.科学通报, 2011, 56, 1241.]
29. [29]
  (29) Qiu, C.; Wang, L.; Lal, V.; Khalizov, A. F.; Zhang, R. Y.Environ. Sci. Technol. 2011, 45, 4748. doi: 10.1021/es1043112
30. [30]
  (30) Dohrmann, J.; Glebov, A.; Toennies, J. P.; Weiss, H. Surf. Sci .1996, 368, 118. doi: 10.1016/S0039-6028(96)01038-2
31. [31]
  (31) Amenomiya, Y.; Morikawa, Y.; Pleizier, G. J. Catal. 1977, 46,431. doi: 10.1016/0021-9517(77)90230-5
32. [32]
  (32) Turek, A. M.; Wachs, I. E.; Decanio, E. J. Phys. Chem. 1992,96, 5000. doi: 10.1021/j100191a050
33. [33]
  (33) Lavalley, J. C.; Travert, J.; Chevreau, T.; Lamotte, J.; Saur, O. J.Chem. Sci. Chem. Commun. 1979, 146.
34. [34]
  (34) Morterra, C.; Zecchina, A.; Coluccia, S.; Chiorino, A. J. Chem. Soc. Faraday Trans I. 1977, 73, 1544. doi: 10.1039/f19777301544
35. [35]
  (35) Molina, R.; Centeno, M. A.; Poncelet, G. J. Phys. Chem. B1999, 103, 6036.
36. [36]
  (36) The Sadtler Handbook of Infrared Spectra. Bio-RadLaboratories, Inc., Informatics Divison: Htercules, California,USA, 1978-2004.
37. [37]
  (37) Finlayson-Pitts, B. J.; Wingen, L. M.; Sumber, A. L.; Syomin,D.; Ramazan, K. A. Phys. Chem. Chem. Phys. 2003, 5, 223. doi: 10.1039/b208564j
38. [38]
  (38) Xu, B. Y.; Zhu, T.; Tang, X. Y.; Ding, J.; Li, H. J. Chem. J. Chin. Univ. 2006, 27, 1912. [徐冰烨,朱彤,唐孝炎,丁杰,李宏军.高等学校化学学报, 2006, 27, 1912.]
39. [39]
  (39) Borensen, C.; Kirchner, U.; Scheer, V.; Vogt, R.; Zellner, R.J. Phys. Chem. A 2000, 104, 5036. doi: 10.1021/jp994170d
40. [40]
  (40) Li, Q. X.; Hou, S. Z.; Xing, Y. Z.; Wei, H. W.; Li, M. China Surfactant Detergent & Consmetics 2000, 30, 50. [李秋小,侯素珍, 邢英站, 魏海威,李明. 日用化学工业, 2000, 30,50.]
41. [41]
  (41) Rhodes, C.; Riddel, S. A.; West, J.;Williams, B. P.; Hutchings,G. J. Catal. Today 2000, 59, 443. doi: 10.1016/S0920-5861(00)00309-6
42. [42]
  (42) Simmons, G. W.; Beard, B. C. J. Phys. Chem. 1987, 91, 1143.doi: 10.1021/j100289a025
1. [1]
  Haojie Duan , Hejingying Niu , Lina Gan , Xiaodi Duan , Shuo Shi , Li Li . Reinterpret the heterogeneous reaction of α-Fe₂O₃ and NO₂ with 2D-COS: The role of SDS, UV and SO₂. Chinese Chemical Letters, 2024, 35(6): 109038-. doi: 10.1016/j.cclet.2023.109038
2. [2]
  Hong CAI , Jiewen WU , Jingyun LI , Lixian CHEN , Siqi XIAO , Dan LI . Synthesis of a zinc-cobalt bimetallic adenine metal-organic framework for the recognition of sulfur-containing amino acids. Chinese Journal of Inorganic Chemistry, 2025, 41(1): 114-122. doi: 10.11862/CJIC.20240382
3. [3]
  Cailiang Yue , Nan Sun , Yixing Qiu , Linlin Zhu , Zhiling Du , Fuqiang Liu . A direct Z-scheme 0D α-Fe₂O₃/TiO₂ heterojunction for enhanced photo-Fenton activity with low H₂O₂ consumption. Chinese Chemical Letters, 2024, 35(12): 109698-. doi: 10.1016/j.cclet.2024.109698
4. [4]
  Yinuo Wang , Siran Wang , Yilong Zhao , Dazhen Xu . Selective Synthesis of Diarylmethyl Anilines and Triarylmethanes via Multicomponent Reactions: Introduce a Comprehensive Experiment of Organic Chemistry. University Chemistry, 2024, 39(8): 324-330. doi: 10.3866/PKU.DXHX202401063
5. [5]
  Jun Dong , Senyuan Tan , Sunbin Yang , Yalong Jiang , Ruxing Wang , Jian Ao , Zilun Chen , Chaohai Zhang , Qinyou An , Xiaoxing Zhang . Spatial confinement of free-standing graphene sponge enables excellent stability of conversion-type Fe₂O₃ anode for sodium storage. Chinese Chemical Letters, 2025, 36(3): 110010-. doi: 10.1016/j.cclet.2024.110010
6. [6]
  Weina Wang , Lixia Feng , Fengyi Liu , Wenliang Wang . Computational Chemistry Experiments in Facilitating the Study of Organic Reaction Mechanism: A Case Study of Electrophilic Addition of HCl to Asymmetric Alkenes. University Chemistry, 2025, 40(3): 206-214. doi: 10.12461/PKU.DXHX202407022
7. [7]
  Youlin SI , Shuquan SUN , Junsong YANG , Zijun BIE , Yan CHEN , Li LUO . Synthesis and adsorption properties of Zn(Ⅱ) metal-organic framework based on 3, 3', 5, 5'-tetraimidazolyl biphenyl ligands. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1755-1762. doi: 10.11862/CJIC.20240061
8. [8]
  Xiaoling LUO , Pintian ZOU , Xiaoyan WANG , Zheng LIU , Xiangfei KONG , Qun TANG , Sheng WANG . Synthesis, crystal structures, and properties of lanthanide metal-organic frameworks based on 2, 5-dibromoterephthalic acid ligand. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1143-1150. doi: 10.11862/CJIC.20230271
9. [9]
  Fan Wu , Wenchang Tian , Jin Liu , Qiuting Zhang , YanHui Zhong , Zian Lin . Core-Shell Structured Covalent Organic Framework-Coated Silica Microspheres as Mixed-Mode Stationary Phase for High Performance Liquid Chromatography. University Chemistry, 2024, 39(11): 319-326. doi: 10.12461/PKU.DXHX202403031
10. [10]
  Jun LUO , Baoshu LIU , Yunchang ZHANG , Bingkai WANG , Beibei GUO , Lan SHE , Tianheng CHEN . Europium(Ⅲ) metal-organic framework as a fluorescent probe for selectively and sensitively sensing Pb²⁺ in aqueous solution. Chinese Journal of Inorganic Chemistry, 2024, 40(12): 2438-2444. doi: 10.11862/CJIC.20240240
11. [11]
  Mengzhen JIANG , Qian WANG , Junfeng BAI . Research progress on low-cost ligand-based metal-organic frameworks for carbon dioxide capture from industrial flue gas. Chinese Journal of Inorganic Chemistry, 2025, 41(1): 1-13. doi: 10.11862/CJIC.20240355
12. [12]
  Zelong LIANG , Shijia QIN , Pengfei GUO , Hang XU , Bin ZHAO . Synthesis and electrocatalytic CO₂ reduction performance of metal-organic framework catalysts loaded with silver particles. Chinese Journal of Inorganic Chemistry, 2025, 41(1): 165-173. doi: 10.11862/CJIC.20240409
13. [13]
  Shasha Ma , Zujin Yang , Jianyong Zhang . Facile Synthesis of FeBTC Metal-Organic Gel and Its Adsorption of Cr₂O₇²⁻: A Physical Chemistry Innovation Experiment. University Chemistry, 2024, 39(8): 314-323. doi: 10.3866/PKU.DXHX202401008
14. [14]
  Jinyao Du , Xingchao Zang , Ningning Xu , Yongjun Liu , Weisi Guo . Electrochemical Thiocyanation of 4-Bromoethylbenzene. University Chemistry, 2024, 39(6): 312-317. doi: 10.3866/PKU.DXHX202310039
15. [15]
  Houjin Li , Wenjian Lan . Name Reactions in University Organic Chemistry Laboratory. University Chemistry, 2024, 39(4): 268-279. doi: 10.3866/PKU.DXHX202310016
16. [16]
  Wenxiu Yang , Jinfeng Zhang , Quanlong Xu , Yun Yang , Lijie Zhang . Bimetallic AuCu Alloy Decorated Covalent Organic Frameworks for Efficient Photocatalytic Hydrogen Production. Acta Physico-Chimica Sinica, 2024, 40(10): 2312014-. doi: 10.3866/PKU.WHXB202312014
17. [17]
  Aiai WANG , Lu ZHAO , Yunfeng BAI , Feng FENG . Research progress of bimetallic organic framework in tumor diagnosis and treatment. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1825-1839. doi: 10.11862/CJIC.20240225
18. [18]
  Feng Sha , Xinyan Wu , Ping Hu , Wenqing Zhang , Xiaoyang Luan , Yunfei Ma . Design of Course Ideology and Politics for the Comprehensive Organic Synthesis Experiment of Benzocaine. University Chemistry, 2024, 39(2): 110-115. doi: 10.3866/PKU.DXHX202307082
19. [19]
  Xinyu Zhu , Meili Pang . Application of Functional Group Addition Strategy in Organic Synthesis. University Chemistry, 2024, 39(3): 218-230. doi: 10.3866/PKU.DXHX202308106
20. [20]
  Tianyun Chen , Ruilin Xiao , Xinsheng Gu , Yunyi Shao , Qiujun Lu . Synthesis, Crystal Structure, and Mechanoluminescence Properties of Lanthanide-Based Organometallic Complexes. University Chemistry, 2024, 39(5): 363-370. doi: 10.3866/PKU.DXHX202312017

Get Citation

PDF

XML

Metrics

PDF Downloads(517)
Abstract views(760)
HTML views(5)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142