碳氢化合物选择性催化还原(HC-SCR)NOx研究
氨选择性催化还原(NH3-SCR) NOx研究
柴油车污染排放控制应用研究
室内空气催化净化
非均相大气化学
您当前的位置:您当前的位置:首 页 -> 主要研究内容 -> 环境催化
 
碳氢化合物选择性催化还原(HC-SCR)NOx研究

    发展以车载燃料(如柴油)为还原剂来源的NOx选择性还原技术(HC-SCR)可免除基础设施布建、简化后处理系统,是柴油车NOx净化的终极目标。但是,直接以柴油为还原剂时,其NOx净化的效率还难以满足日益严格的排放法规的研究,因此迫切需要:厘清HC选择性还原NOx的微观机制与构效关系,并以此为指导,发展以车载燃料为还原剂来源的高效净化NOx的新原理和新方法。

一. HC-SCR反应高效还原剂特征

 

ü  首次在Ag/Al2O3催化乙醇部分氧化过程中发现了表面吸附态烯醇式物种(R-CH=CH-O-),证实该物种在乙醇-SCR反应中起到重要作用;

 

ü  醇类还原剂至少含一个α-HC-C键是其部分氧化过程中高活性烯醇式物种形成的先决条件,是决定醇-SCR反应中还原剂效率的内在标准;

 

ü  利用氢气效应提升不含氧HC选择性还原NOx低温活性的理论依据:还原剂HC至少含两个碳原子,促进部分氧化过程中烯醇式物种的形成。


不同结构丁醇选择性还原NOx活性与表面烯醇式物种形成

 


氢气促进HC-SCR反应中烯醇式物种形成与NOx净化效率的相关性

(Catal. Sci. Technol., 2014, 4: 1239; J. Catal., 2010, 271: 343)

 

 

二. 基于键合特征分析的HC-SCR构效关系

ü     Ag/Al2O3催化剂上氧化态Ag位及其与载体Al2O3的接触边界是烯醇式物种的吸附位

 

ü     Ag-O-AlIII结构中AgOAl之间的轨道杂化显著降低了能隙,提高了反应性能,是Ag/Al2O3催化剂上乙醇-SCR的活性中心

 


(ACS Catal., 2014, 4: 2776; J. Phys. Chem. C, 2015, 119: 3132; J. Catal., 2012, 293: 13)

 

 

三.未来柴油-SCR设计原理和方案

 

Ø              ü   未来柴油-SCR技术方案:柴油重整耦合HC-         SCR技术,以高效净化柴油车尾气NOx

 

ü   柴油重整设计原则与目标:

   1.  将柴油转化为活性小分子HC/小分子含 氧 HC(碳原子数≥ 2,以满足高活性烯醇式物种的形成条件);

   2.  原位制氢(利用氢气效应,提高低温活性、拓宽活性温度窗口)。



(Chem. Commun., 2014, 50: 8445)

   

 

相关论文:

35. Hua Deng, Yunbo Yu, Hong He*, Discerning the role of AgOAl entities on Ag/-Al2O3 surface in NOx Selective reduction by ethanol, J. Phys. Chem. C, 119, (2015) 31323142.

34. Yunbo Yu, Yi Li, Xiuli Zhang, Hua Deng, Hong He*, Yuyang Li, Promotion effect of H2 on the ethanol oxidation and NOx reduction with ethanol over Ag/Al2O3 catalyst, Environ. Sci. Technol., 49, (2015) 481488.

33. Hua Deng, Yunbo Yu, Fudong Liu, Jinzhu Ma, Yan Zhang, Hong He*, Nature of Ag Species on Ag/g-Al2O3: A Combined Experimental and theoretical study, ACS Catal., 4, (2014) 27762784.

32. Fudong Liu, Yunbo Yu, Hong He*, Environmentally-benign catalysts for the selective catalytic reduction of NOx from diesel engines: Structure-activity relationship and reaction mechanism aspects, Chem. Commun., 50 (62), (2014) 84458463.

31. Yunbo Yu, Hong He*, Xiuli Zhang, Hua Deng, A common feature of H2-assisted HC-SCR over Ag/Al2O3, Catal. Sci. Technol., 4, (2014) 12391245.

30. Zhao Jiaojiao, Yu Yunbo*, Han Xue, He Hong, Fuel reforming over Ni‐based catalysts coupled with selectivecatalytic reduction of NOx, Chin. J. Catal., 34, (2013) 1407–1417.

29. Yunbo Yu*, Jiaojiao Zhao, Yong Yan, Xue Han, Hong He, A cyclic reaction pathway triggered by ammonia for the selective catalytic reduction of NOx by ethanol over Ag/Al2O3, Appl.Catal. B, 136-137, (2013) 103111.

28. HeHong*, Liu Fudong, Yu Yunbo, ShanWenpo, Environmental-friendly SCR technique (selective catalytic reduction) for the deNOx process from diesel engines,SCIENCE CHINA: Chemistry,42, (2012) 446468. (in Chinese)

27. Yong Yan,Yunbo Yu*, Hong He, Jiaojiao Zhao, Intimate contact of enolic species with silver sites benefits the SCR of NOx by ethanol over Ag/Al2O3, J. Catal., 293, (2012) 1326.

26. He Hong*, Yu Yunbo, Li Yi, Wu Qiang, Zhang Xiuli, Zhang Changbin, Shi Xiaoyan, Song Xiaoping,Advances in mechanistic and practical studies on the selective catalytic reduction of NOx by oxygenated hydrocarbons over Ag/Al2O3, Chin. J. Catal., 31, (2010) 491501. (in Chinese)

25. Yunbo Yu, Xiaoping Song, Hong He*, Remarkable influence of reductant structure on the activity of alumina-supported silver catalyst for the selective catalytic reduction of NOx, J Catal.,271, (2010) 343350.

24. Yi Li, Xiuli Zhang, Hong He*, Yunbo Yu, Tao Yuan, Zhenyu Tian, Jing Wang, Yuyang Wang, Effect of the pressure on the catalytic oxidation of volatile organic compounds over Ag/Al2O3 catalyst,Appl. Catal. B, 89, (2009) 659664.

23. Xiuli Zhang, Hong He*, Hongwei Gao, Yunbo Yu, Experimental and theoretical studies of surface nitrate species on Ag/Al2O3 using DRIFTS and DFT, Spectrochim. Acta A,71, (2008) 14461451.

22. Hong He*, Xiuli Zhang, Qiang Wu, Changbin Zhang, Yunbo Yu, Review of Ag/Al2O3-reductant system in the selective catalytic reduction of NOx, Catal. Surv. Asia,12, (2008) 3855.

21. Xiuli Zhang, Yunbo Yu, Hong He*, Effect of hydrogen on reaction intermediates in the selective catalytic reduction of NOx by C3H6, Appl. Catal. B, 76, (2007) 241247.

20. Yunbo Yu, Xiuli Zhang, Hong He*, Evidence for the formation, isomerization and decomposition of organo-nitrite and -nitro species during the NOx reduction by C3H6 on Ag/Al2O3, Appl. Catal. B, 75, (2007) 298302.

19. Xiuli Zhang, Hong He*, Zichuan Ma, Hydrogen promotes the selective catalytic reduction of NOx by ethanol over Ag/Al2O3, Catal. Commun., 8, (2007) 187192.

18. Shuxia Xie, Jin Wang, Hong He*, Poisoning effect of sulphate on the selective catalytic reduction of NOx by C3H6 over Ag-Pd/Al2O3, J. Mol. Catal. A:Chem.,266, (2007) 166172.

17. Qiang Wu, Yunbo Yu, Hong He*, Mechanistic study of selective catalytic reduction of NOx with C2H5OH and CH3OCH3 over Ag/Al2O3 by in situ DRIFTS, Chin. J. Catal., 27(11), (2006) 993998.

16. Shuxia Xie, Yunbo Yu, Jin Wang, Hong He*, Effect of SO2 on the performance of Ag-Pd/Al2O3 for the selective catalytic reduction of NOx with C2H5OH, J. Environ. Sci.,18(5), (2006) 973978.

15. Qiang Wu, Hongwei Gao, Hong He*, Study on effect of SO2 on the selective catalytic reduction of NOx with propene over Ag/Al2O3 by in situ DRIFTS,Chin. J. Catal.,27(5), (2006) 403408.

14. Qiang Wu, Hongwei Gao, Hong He*, Conformational analysis of sulfate species on Ag/Al2O3 by means of theoretical and experimental vibration spectra, J. Phys. Chem. B, 110, (2006) 83208324.

13. Qiang Wu, Qingcai Feng, Hong He*, Disparate effects of SO2 on the selective catalytic reduction of NO by C2H5OH and IPA over Ag/Al2O3,Catal. Commun.,7, (2006) 657661.

12. Hongwei Gao, Hong He*, Yunbo Yu, Qingcai Feng, Density functional theory (DFT) and DRIFTS investigations of the formation and adsorption of enolic species on Ag/Al2O3 surface, J. Phys. Chem. B, 109, (2005) 1329113295.

11. Qiang Wu, Hong He*, Yunbo Yu, In situ DRIFTS study of the selective catalytic reduction of NOx with alcohols over Ag/Al2O3 catalyst: role of surface enolic species, Appl. Catal. B, 61, (2005) 107113.

10. Hong He*, Yunbo Yu, Selective catalytic reduction of NOx over Ag/Al2O3 catalyst: from reaction mechanism to diesel engine test, Catal. Today, 100, (2005) 3747.Invited paper

9Hongwei Gao, Hong He*, Conformational analysis and comparison between theoretical and experimental vibration spectra for isocyanate species on Ag/Al2O3 catalyst, Spectrochim. Acta A, 61, (2005) 12331238.

8 .Jin Wang, Hong He*, Shuxia Xie, Yunbo Yu, Novel Ag-Pd/Al2O3-SiO2 for lean NOx reduction by C3H6 with high tolerance of SO2, Catal. Commun., 6, (2005) 195200.

7. Jin Wang, Hong He*, Qingcai Feng, Yunbo Yu, Kiyohide Yoshida, Selective catalytic reduction of NOx by C3H6 over an Ag/Al2O3 catalyst with a small quantity of noble metal, Catal. Today, 9395, (2004) 783789.

6. Hong He*, Changbin Zhang, Yunbo Yu, A comparative study of Ag/Al2O3 and Cu/Al2O3 catalysts for the selective catalytic reduction of NO by C3H6,Catal. Today,90, (2004) 191197.

5. Yunbo Yu, Hong He*, Qingcai Feng, Hongwei Gao, Xin Yang, Mechanism of the selective catalytic reduction of NOx by C2H5OH over Ag/Al2O3, Appl. Catal. B,49, (2004) 159171.

4 . Yunbo Yu, Hong He*, Qingcai Feng, Novel enolic surface species during partial oxidation of CH3CHO, C2H5OH, and C3H6 on Ag/Al2O3: an in situ DRIFTS study, J. Phys. Chem. B,107, (2003) 1309013092.

3. Hong He*, Jin Wang, Qingcai Feng, Yunbo Yu, Kiyohide Yoshida, Novel Pd promoted Ag/Al2O3 catalyst for the selective reduction of NOx, Appl. Catal. B, 46, (2003) 365370.

2 Satosi Sumiya, Hong He, Akira Abe, Nobutsune Takezawa, Kiyohide Yoshida, Formation and reactivity of isocyanate (NCO) species on Ag/Al2O3, J. Chem. Soc., Faraday Trans., 94(15), (1998) 22172219.

1. Satoshi Sumiya,Mika Saito, Hong He, Qingcai Feng, Nobutsune Takezawa, Kiyohide Yoshida, Reduction of lean NOX by ethanol over Ag/Al2O3 catalysts in the presence of H2O and SO2, Catal. Lett., 50, (1998) 8791.

 
版权所有:贺泓研究组 | 技术支持:为您服务网络公司
Copyright Professor Hong He's Group 2005 All Rights Reserved Powed by cforu.com