Redistributing Cu species in Cu-SSZ-13 zeolite as NH3-SCR catalyst via a simple ion-exchange

doi:10.1016/j.cjche.2021.10.027

中国化学工程学报 ›› 2022, Vol. 41 ›› Issue (1): 329-341.DOI: 10.1016/j.cjche.2021.10.027

• Catalysis, Kinetics and Reaction Engineering • 上一篇下一篇

Redistributing Cu species in Cu-SSZ-13 zeolite as NH₃-SCR catalyst via a simple ion-exchange

Ben Liu¹, Nangui Lv², Chan Wang^1,2, Hongwei Zhang¹, Yuanyuan Yue^1,2, Jingdong Xu³, Xiaotao Bi^1,4, Xiaojun Bao^1,2,5

1 National Engineering Research Center of Chemical Fertilizer Catalyst, College of Chemical Engineering, Fuzhou University, Fuzhou 350002, China;
2 Qingyuan Innovation Laboratory, Quanzhou 362801, China;
3 Sinochem Quanzhou Energy Technology Co, Ltd, Quanzhou 362000, China;
4 Department of Chemical & Biological Engineering, University of British Columbia, 2360 East Mall, Vancouver, BC V6T 1Z3, Canada;
5 State Key Laboratory of Photocatalysis on Energy & Environment, College of Chemistry, Fuzhou University, Fuzhou 350116, China

收稿日期:2021-06-09 修回日期:2021-10-25 出版日期:2022-01-28 发布日期:2022-02-25
通讯作者: Yuanyuan Yue,E-mail address:yueyy@fzu.edu.cn
基金资助:
We gratefully acknowledge the financial supports from National Natural Science Foundation of China (Nos. 22178059 and 91934301), Natural Science Foundation of Fujian Province, China (2020J01513), Sinochem Quanzhou Energy Technology Co., Ltd. (ZHQZKJ-19-F-ZS-0076), Qingyuan Innovation Laboratory (No. 00121002), and Fujian Hundred Talent Program.

Redistributing Cu species in Cu-SSZ-13 zeolite as NH₃-SCR catalyst via a simple ion-exchange

Ben Liu¹, Nangui Lv², Chan Wang^1,2, Hongwei Zhang¹, Yuanyuan Yue^1,2, Jingdong Xu³, Xiaotao Bi^1,4, Xiaojun Bao^1,2,5

1 National Engineering Research Center of Chemical Fertilizer Catalyst, College of Chemical Engineering, Fuzhou University, Fuzhou 350002, China;
2 Qingyuan Innovation Laboratory, Quanzhou 362801, China;
3 Sinochem Quanzhou Energy Technology Co, Ltd, Quanzhou 362000, China;
4 Department of Chemical & Biological Engineering, University of British Columbia, 2360 East Mall, Vancouver, BC V6T 1Z3, Canada;
5 State Key Laboratory of Photocatalysis on Energy & Environment, College of Chemistry, Fuzhou University, Fuzhou 350116, China

Received:2021-06-09 Revised:2021-10-25 Online:2022-01-28 Published:2022-02-25
Contact: Yuanyuan Yue,E-mail address:yueyy@fzu.edu.cn
Supported by:
We gratefully acknowledge the financial supports from National Natural Science Foundation of China (Nos. 22178059 and 91934301), Natural Science Foundation of Fujian Province, China (2020J01513), Sinochem Quanzhou Energy Technology Co., Ltd. (ZHQZKJ-19-F-ZS-0076), Qingyuan Innovation Laboratory (No. 00121002), and Fujian Hundred Talent Program.

摘要/Abstract

摘要： The nature and distribution of Cu species in Cu-SSZ-13 play a vital role in selective catalytic reduction of NO by NH₃ (NH₃-SCR), but existing methods for adjusting the Cu distribution are complex and difficult to control. Herein, we report a simple and effective ion-exchange approach to regulate the Cu distribution in the one-pot synthesized Cu-SSZ-13 that possesses sufficient initial Cu species and thus provides a “natural environment” for adjusting Cu distribution precisely. By using this proposed strategy, a series of CuSSZ-13_x zeolites with different Cu contents and distributions were obtained. It is shown that the dealumination of the as-synthesized Cu-SSZ-13 during the ion-exchange generates abundant vacant sites in the double six-membered-rings of the SSZ-13 zeolite for relocating Cu²⁺ species and thus allows the redistribution of the Cu species. The catalytic results showed that the ion-exchanged Cu-SSZ-13 zeolites exhibit quite different catalytic performance in NH₃-SCR reaction but superior to the parent counterpart. The structure–activity relationship analysis indicates that the redistribution of Cu species rather than other factors (e.g., crystallinity, chemical composition, and porous structure) is responsible for the improved NH₃-SCR performance and SO₂ and H₂O resistance. Our work offers an effective method to precisely adjust the Cu distribution in preparing the industrial SCR catalysts.

关键词: Catalyst, Zeolite, Cu-SSZ-13, Ion-exchange, Redistribution of Cu species, Selective catalytic reduction (SCR)

Abstract: The nature and distribution of Cu species in Cu-SSZ-13 play a vital role in selective catalytic reduction of NO by NH₃ (NH₃-SCR), but existing methods for adjusting the Cu distribution are complex and difficult to control. Herein, we report a simple and effective ion-exchange approach to regulate the Cu distribution in the one-pot synthesized Cu-SSZ-13 that possesses sufficient initial Cu species and thus provides a “natural environment” for adjusting Cu distribution precisely. By using this proposed strategy, a series of CuSSZ-13_x zeolites with different Cu contents and distributions were obtained. It is shown that the dealumination of the as-synthesized Cu-SSZ-13 during the ion-exchange generates abundant vacant sites in the double six-membered-rings of the SSZ-13 zeolite for relocating Cu²⁺ species and thus allows the redistribution of the Cu species. The catalytic results showed that the ion-exchanged Cu-SSZ-13 zeolites exhibit quite different catalytic performance in NH₃-SCR reaction but superior to the parent counterpart. The structure–activity relationship analysis indicates that the redistribution of Cu species rather than other factors (e.g., crystallinity, chemical composition, and porous structure) is responsible for the improved NH₃-SCR performance and SO₂ and H₂O resistance. Our work offers an effective method to precisely adjust the Cu distribution in preparing the industrial SCR catalysts.

Key words: Catalyst, Zeolite, Cu-SSZ-13, Ion-exchange, Redistribution of Cu species, Selective catalytic reduction (SCR)

Ben Liu, Nangui Lv, Chan Wang, Hongwei Zhang, Yuanyuan Yue, Jingdong Xu, Xiaotao Bi, Xiaojun Bao. Redistributing Cu species in Cu-SSZ-13 zeolite as NH₃-SCR catalyst via a simple ion-exchange[J]. 中国化学工程学报, 2022, 41(1): 329-341.

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Redistributing Cu species in Cu-SSZ-13 zeolite as NH₃-SCR catalyst via a simple ion-exchange

Redistributing Cu species in Cu-SSZ-13 zeolite as NH₃-SCR catalyst via a simple ion-exchange

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