Citation: Li Shihan, Zhao Zhenchao, Li Shikun, Xing Youdong, Zhang Weiping. Aluminum Distribution and Brønsted Acidity of Al-Rich SSZ-13 Zeolite: A Combined DFT Calculation and Solid-State NMR Study[J]. Acta Physico-Chimica Sinica, ;2020, 36(4): 190302. doi: 10.3866/PKU.WHXB201903021 shu

Aluminum Distribution and Brønsted Acidity of Al-Rich SSZ-13 Zeolite: A Combined DFT Calculation and Solid-State NMR Study

State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, Liaoning Province, P. R. China

Corresponding author: Zhang Weiping, wpzhang@dlut.edu.cn
Received Date: 11 March 2019
Revised Date: 11 April 2019
Accepted Date: 11 April 2019
Available Online: 18 April 2019
Fund Project: the National Natural Science Foundation of China 21603022the Fundamental Research Funds for the Central Universities in China DUT17TD04the National Natural Science Foundation of China 21872017The project was supported by the National Natural Science Foundation of China (21872017, 21603022), the Fundamental Research Funds for the Central Universities in China (DUT17TD04) and the Supercomputing Center of Dalian University of Technology, China

SSZ-13 zeolite with a chabazite (CHA) topology structure has important applications for methanol to olefin (MTO) conversion and selective catalytic reduction of nitrogen oxides (NO_x) by ammonia (NH₃-SCR) to reduce diesel engine exhaust emissions. It has been reported that the Al-rich SSZ-13 zeolite can be used to tune the selectivity of olefins in the MTO reaction, and significantly enhance NO conversions at lower temperatures in NH₃-SCR. Thus, the aluminum content and distribution as well as the corresponding acidity in SSZ-13 zeolite determine the catalytic performance of the zeolite for different catalytic reactions. Herein, quantum chemical computing using density functional theory (DFT) combined with multinuclear solid-state nuclear- magnetic-resonance (NMR) experiments were performed to investigate the correlation of Al location and Brønsted acidity of H-SSZ-13 zeolite with the Si/Al ratio varying from 5.8 to 25. The most favorable acid site in the 1Al model is O(1)―H in which a proton is bonded with the O(1) atom near the isolated Al atom of the zeolite framework. Nevertheless, energy differences were rather small when comparing the substitution energies of an Al atom replacing a Si atom in the zeolite framework with a proton located in different O sites. As the Si/Al ratio decreased, the Al-rich SSZ-13 zeolite contained more Al substitutions in its framework. This system exhibited the lowest substitution energy when two Al atoms were located at the diagonal of the same six-membered ring for the Al-Si-Si-Al (NNNN) sequence in the framework of the Al-rich SSZ-13 zeolite. However, for the Al-Si-Al (NNN) sequence, the most favorable distribution involved two Al atoms located in different six-membered rings of the double six-membered ring units (D6R). The proton affinities (PA), NH₃ desorption energies, and ¹H NMR chemical shifts after d3-acetonitrile adsorption were calculated in the most stable models to characterize the Brønsted acid strength of the SSZ-13 zeolite with different Si/Al ratios. All computing results suggested that the Al-rich SSZ-13 zeolite exhibited weaker Brønsted acid strength than that of the Si-rich counterpart due to the presence of Si(2Al) groupings with the NNN sequence in the framework. Quantitative ²⁹Si magic-angle spinning (MAS) NMR measurements after deconvolution demonstrated that the content of Si(2Al) groupings in the Al-rich SSZ-13 was > 43%. The ¹H MAS NMR experiments after d3-acetonitrile adsorption showed that the chemical shift of the bridging hydroxyls in the Al-rich SSZ-13 moved to the lower field, further confirming that it had a weaker Brønsted acid strength than the Si-rich counterpart.
- DFT,
- Solid-state NMR,
- SSZ-13 zeolite,
- Al distribution,
- Brønsted acidity
1. [1]
  Yang, B.; Guo, C.; Cheng, J. Chem. Eng. Prog. 2014, 33, 368. doi: 10.3969/j.issn.1000-6613.2014.02.018
2. [2]
  Zhang, R.; Liu, N.; Lei, Z.; Chen, B. Chem. Rev. 2016, 116, 3658. doi: 10.1021/acs.chemrev.5b00474 doi: 10.1021/acs.chemrev.5b00474
3. [3]
  Zhou, Z.; Wang, Z.; Liu, Z. Sci. China Chem. 2018, 48, 562. doi: 10.1360/N032017-00215
4. [4]
  Bull, I.; Boorse, R. S.; Jaglowski, W. M.; Koermer, G. S.; Moini, A.; Patchett, J. A.; Xue, W.; Burk, P.; Dettling, J. C.; Caudle, M. T. Processes for Reducing Nitrogen Oxides Using Copper Cha Zeolite Catalysts. U.S. Patent 8404203.B2, 3013-03-26
5. [5]
  Beale, A. M.; Gao, F.; Lezcano-Gonzalez, I.; Peden, C. H. F.; Szanyi, J. Chem. Soc. Rev. 2015, 44, 7371. doi: 10.1039/c5cs00108k doi: 10.1039/c5cs00108k
6. [6]
  Song, J.; Wang, Y.; Walter, E. D.; Washton, N. M.; Mei, D.; Kovarik, L.; Engelhard, M. H.; Prodinger, S.; Wang, Y.; Peden, C. H. F.; et al. ACS Catal. 2017, 7, 8214. doi: 10.1021/acscatal.7b03020 doi: 10.1021/acscatal.7b03020
7. [7]
  Yu, H.; Zhang, G.; Han, L.; Chang, L.; Bao, W.; Wang, J. Acta Phys. -Chim. Sin. 2015, 31, 2165. doi: 10.3866/PKU.WHXB201509184
8. [8]
  Zhao, Z.; Yu, R.; Zhao, R.; Shi, C.; Gies, H.; Xiao, F.; De Vos, D.; Yokoi, T.; Bao, X.; Kolb, U.; et al. Appl. Catal. B: Environ. 2017, 217, 421. doi: 10.1016/j.apcatb.2017.06.013 doi: 10.1016/j.apcatb.2017.06.013
9. [9]
  Gao, F.; Wang, Y.; Washton, N. M.; Kollar, M.; Szanyi, J.; Peden, C. H. F. J. Catal. 2015, 331, 25. doi: 10.1016/j.jcat.2015.08.004 doi: 10.1016/j.jcat.2015.08.004
10. [10]
  Deimund, M. A.; Harrison, L.; Lunn, J. D.; Liu, Y.; Malek, A.; Shayib, R.; Davis, M. E. ACS Catal. 2016, 6, 542. doi: 10.1021/acscatal.5b01450 doi: 10.1021/acscatal.5b01450
11. [11]
  Di Iorio, J. R.; Nimlos, C. T.; Gounder, R. ACS Catal. 2017, 7, 6663. doi: 10.1021/acscatal.7b01273 doi: 10.1021/acscatal.7b01273
12. [12]
  Zhao, Z.; Xing, Y.; Li, S.; Meng, X.; Xiao, F.; McGuire, R.; Parvulescu, A. N.; Müller, U.; Zhang, W. J. Phys. Chem. C 2018, 122, 9973. doi: 10.1021/acs.jpcc.8b01423 doi: 10.1021/acs.jpcc.8b01423
13. [13]
  Civalleri, B.; Ferrari, A. M.; Llunell, M.; Orlando, R.; Mérawa, M.; Ugliengo, P. Chem. Mater. 2003, 15, 3996. doi: 10.1021/cm0342804 doi: 10.1021/cm0342804
14. [14]
  Zheng, A.; Chen, L.; Yang, J.; Zhang, M.; Su, Y.; Yue, Y.; Ye, C.; Deng, F. J. Phys. Chem. B 2005, 109, 24273. doi: 10.1021/jp0527249 doi: 10.1021/jp0527249
15. [15]
  Zheng, A.; Liu, S. B.; Deng, F. Chem. Rev. 2017, 117, 12475. doi: 10.1021/acs.chemrev.7b00289 doi: 10.1021/acs.chemrev.7b00289
16. [16]
  Li, S.; Li, J.; Zheng, A.; Deng, F. Acta Phys. -Chim. Sin. 2017, 33, 270. doi: 10.3866/PKU.WHXB201611022
17. [17]
  Sazama, P.; Tabor, E.; Klein, P.; Wichterlova, B.; Sklenak, S.; Mokrzycki, L.; Pashkkova, V.; Ogura, M.; Dedecek, J. J. Catal. 2016, 333, 102. doi: 10.1016/j.jcat.2015.10.010 doi: 10.1016/j.jcat.2015.10.010
18. [18]
  Zhang, W.; Xu, S.; Han, X.; Bao, X. Chem. Soc. Rev. 2012, 41 (1), 192. doi: 10.1039/c1cs15009j doi: 10.1039/c1cs15009j
19. [19]
  Shah, R.; Gale, J. D.; Payne, M. C. J. Phys. Chem-Us 1996, 100, 11688. doi: 10.1021/Jp960365z doi: 10.1021/Jp960365z
20. [20]
  Lo, C.; Trout, B. L. J. Catal. 2004, 227 (1), 77. doi: 10.1016/j.jcat.2004.06.018 doi: 10.1016/j.jcat.2004.06.018
21. [21]
  Solans-Monfort, X.; Sodupe, M.; Branchadell, V.; Sauer, J.; Orlando, R.; Ugliengo, P. J. Phys. Chem. B 2005, 109, 3539. doi: 10.1021/jp045531e doi: 10.1021/jp045531e
22. [22]
  Haw, J. F.; Hall, M. B.; Alvarado-Swaisgood, A. E.; Munson, E. J.; Lin, Z.; Beck, L. W.; Howard, T. J. Am. Chem. Soc. 1994, 116, 7308. doi: 10.1021/ja00095a039 doi: 10.1021/ja00095a039
23. [23]
  Gil, B.; Zones, S. I.; Hwang, S. J.; Bejblová, M.; Čejka, J. J. Phys. Chem. C 2008, 112, 2997. doi: 10.1021/jp077687v doi: 10.1021/jp077687v
24. [24]
  Calligaris, M.; Nardin, G.; Randaccio, L. Zeolites 1983, 3, 205. doi: 10.1016/0144-2449(83)90008-8 doi: 10.1016/0144-2449(83)90008-8
25. [25]
  Zheng, A.; Zhang, H.; Chen, L.; Yue, Y.; Ye, C.; Deng, F. J. Phys. Chem. B 2007, 111, 3085. doi: 10.1021/jp067340c doi: 10.1021/jp067340c
26. [26]
  Dunning, T. H. J. Phys. Chem. A 2000, 104, 9062. doi: 10.1021/jp001507z doi: 10.1021/jp001507z
27. [27]
  Frisch, M. J.; Trucks, G. W.; Schlegel, H. B.; Scuseria, G. E.; Robb, M. A.; Cheeseman, J.R.; Scalmani, G.; Barone, V.; Mennucci, B.; Petersson, G. A.; et al. Gaussian 09, Revision D.01; Gaussian Inc: Wallingford, CT, 2013
28. [28]
  Jobic, H.; Tuel, A.; Krossner, M.; Sauer, J. J. Phys. Chem. C 1996, 100, 19545. doi: 10.1021/jp9619954 doi: 10.1021/jp9619954
29. [29]
  Zygmunt, S. A.; Curtiss, L. A.; Iton, L. E.; Erhardt, M. K. J. Phys. Chem-Us 1996, 100, 6663. doi: 10.1021/Jp952913z doi: 10.1021/Jp952913z
30. [30]
  Ryder, J. A.; Chakraborty, A. K.; Bell, A. T. J. Phys. Chem. B 2000, 104, 6998. doi: 10.1021/jp9943427 doi: 10.1021/jp9943427
31. [31]
  Wang, J.; Li, S.; Zhao, Z.; Zhou, D.; Lu, A.; Zhang, W. Acta Phys. -Chim. Sin. 2016, 32, 1666. doi: 10.3866/PKU.WHXB201604012
32. [32]
  Li, S.; Zhao, Z.; Zhao, R.; Zhou, D.; Zhang, W. ChemCatChem 2017, 9, 1494. doi: 10.1002/cctc.201601623 doi: 10.1002/cctc.201601623
33. [33]
  Zhao, R.; Zhao, Z.; Li, S.; Zhang, W. J. Phys. Chem. Lett. 2017, 8, 2323. doi: 10.1021/acs.jpclett.7b00711 doi: 10.1021/acs.jpclett.7b00711
34. [34]
  Calligaris, M.; Nardin, G.; Randaccio, L.; Chiaramonti, P. C. Acta Crystallogr. B 1982, 38, 602. doi: Doi10.1107/S0567740882003483 doi: 10.1107/S0567740882003483
35. [35]
  Jeanvoine, Y.; Angyan, J. G.; Kresse, G.; Hafner, J. J. Phys. Chem. B 1998, 102, 5573. doi: 10.1021/Jp980341n doi: 10.1021/Jp980341n
36. [36]
  Nielsen, M.; Brogaard, R. Y.; Falsig, H.; Beato, P.; Swang, O.; Svelle, S. ACS Catal. 2015, 5, 7131. doi: 10.1021/acscatal.5b01496 doi: 10.1021/acscatal.5b01496
37. [37]
  Smith, L. J.; Davidson, A.; Cheetham, A. K. Catal. Lett. 1997, 49, 143. doi: 10.1023/A:1019097019846 doi: 10.1023/A:1019097019846
38. [38]
  Wang, N.; Zhang, M.; Yu, Y. Micropor. Mesopor. Mat. 2013, 169, 47. doi: 10.1016/j.micromeso.2012.10.019 doi: 10.1016/j.micromeso.2012.10.019
39. [39]
  Chai, J. D.; Head-Gordon, M. Phys. Chem. Chem. Phys. 2008, 10, 6615. doi: 10.1039/b810189b doi: 10.1039/b810189b
40. [40]
  Jänchen, J.; Van Wolput, J. H. M. C.; Van de Ven, L. J. M.; De Haan, J. W.; Van Santen, R. A. Catal. Lett. 1996, 39, 147. doi: 10.1007/bf00805574 doi: 10.1007/bf00805574
41. [41]
  Dai, W.; Sun, X.; Tang, B.; Wu, G.; Li, L.; Guan, N.; Hunger, M. J. Catal. 2014, 314, 10. doi: 10.1016/j.jcat.2014.03.006 doi: 10.1016/j.jcat.2014.03.006
1. [1]
  Jie ZHAO , Sen LIU , Qikang YIN , Xiaoqing LU , Zhaojie WANG . Theoretical calculation of selective adsorption and separation of CO₂ by alkali metal modified naphthalene/naphthalenediyne. Chinese Journal of Inorganic Chemistry, 2024, 40(3): 515-522. doi: 10.11862/CJIC.20230385
2. [2]
  Xiaochen Zhang , Fei Yu , Jie Ma . 多角度数理模拟在电容去离子中的前沿应用. Acta Physico-Chimica Sinica, 2024, 40(11): 2311026-. doi: 10.3866/PKU.WHXB202311026
3. [3]
  Hao Wu , Zhen Liu , Dachang Bai . ¹H NMR Spectrum of Amide Compounds. University Chemistry, 2024, 39(3): 231-238. doi: 10.3866/PKU.DXHX202309020
4. [4]
  Yufang GAO , Nan HOU , Yaning LIANG , Ning LI , Yanting ZHANG , Zelong LI , Xiaofeng LI . Nano-thin layer MCM-22 zeolite: Synthesis and catalytic properties of trimethylbenzene isomerization reaction. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1079-1087. doi: 10.11862/CJIC.20240036
5. [5]
  Jinkang Jin , Yidian Sheng , Ping Lu , Zhan Lu . Introducing a Website for Learning Nuclear Magnetic Resonance (NMR) Spectrum Analysis. University Chemistry, 2024, 39(11): 388-396. doi: 10.12461/PKU.DXHX202403054
6. [6]
  Maitri Bhattacharjee , Rekha Boruah Smriti , R. N. Dutta Purkayastha , Waldemar Maniukiewicz , Shubhamoy Chowdhury , Debasish Maiti , Tamanna Akhtar . Synthesis, structural characterization, bio-activity, and density functional theory calculation on Cu(Ⅱ) complexes with hydrazone-based Schiff base ligands. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1409-1422. doi: 10.11862/CJIC.20240007
7. [7]
  Zhuoming Liang , Ming Chen , Zhiwen Zheng , Kai Chen . Multidimensional Studies on Ketone-Enol Tautomerism of 1,3-Diketones By ¹H NMR. University Chemistry, 2024, 39(7): 361-367. doi: 10.3866/PKU.DXHX202311029
8. [8]
  Runze Liu , Yankai Bian , Weili Dai . Qualitative and quantitative analysis of Brønsted and Lewis acid sites in zeolites: A combined probe-assisted 1H MAS NMR and NH3-TPD investigation. Chinese Journal of Structural Chemistry, 2024, 43(4): 100250-100250. doi: 10.1016/j.cjsc.2024.100250
9. [9]
  Yuhao SUN , Qingzhe DONG , Lei ZHAO , Xiaodan JIANG , Hailing GUO , Xianglong MENG , Yongmei GUO . Synthesis and antibacterial properties of silver-loaded sod-based zeolite. Chinese Journal of Inorganic Chemistry, 2024, 40(4): 761-770. doi: 10.11862/CJIC.20230169
10. [10]
  Yong Shu , Xing Chen , Sai Duan , Rongzhen Liao . How to Determine the Equilibrium Bond Distance of Homonuclear Diatomic Molecules: A Case Study of H₂. University Chemistry, 2024, 39(7): 386-393. doi: 10.3866/PKU.DXHX202310102
11. [11]
  Jia Yao , Xiaogang Peng . Theory of Macroscopic Molecular Systems: Theoretical Framework of the Physical Chemistry Course in the Chemistry “101 Plan”. University Chemistry, 2024, 39(10): 27-37. doi: 10.12461/PKU.DXHX202408117
12. [12]
  Sinong Wang , Shanshan Jin , Xue Yang , Yanyan Huang , Peng Liu , Yi Tang , Yuliang Yang . Development of Mg-Al LDH and LDO as novel protective materials for deacidification of paper-based relics. Chinese Chemical Letters, 2024, 35(9): 109890-. doi: 10.1016/j.cclet.2024.109890
13. [13]
  Lumin Zheng , Ying Bai , Chuan Wu . Multi-electron reaction and fast Al ion diffusion of δ-MnO₂ cathode materials in rechargeable aluminum batteries via first-principle calculations. Chinese Chemical Letters, 2024, 35(4): 108589-. doi: 10.1016/j.cclet.2023.108589
14. [14]
  Chuanming GUO , Kaiyang ZHANG , Yun WU , Rui YAO , Qiang ZHAO , Jinping LI , Guang LIU . Performance of MnO₂-0.39IrO_x composite oxides for water oxidation reaction in acidic media. Chinese Journal of Inorganic Chemistry, 2024, 40(6): 1135-1142. doi: 10.11862/CJIC.20230459
15. [15]
  Xingyang LI , Tianju LIU , Yang GAO , Dandan ZHANG , Yong ZHOU , Meng PAN . A superior methanol-to-propylene catalyst: Construction via synergistic regulation of pore structure and acidic property of high-silica ZSM-5 zeolite. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1279-1289. doi: 10.11862/CJIC.20240026
16. [16]
  Hongyi LI , Aimin WU , Liuyang ZHAO , Xinpeng LIU , Fengqin CHEN , Aikui LI , Hao HUANG . Effect of Y(PO₃)₃ double-coating modification on the electrochemical properties of Li[Ni_0.8Co_0.15Al_0.05]O₂. Chinese Journal of Inorganic Chemistry, 2024, 40(7): 1320-1328. doi: 10.11862/CJIC.20230480
17. [17]
  Yanhui XUE , Shaofei CHAO , Man XU , Qiong WU , Fufa WU , Sufyan Javed Muhammad . Construction of high energy density hexagonal hole MXene aqueous supercapacitor by vacancy defect control strategy. Chinese Journal of Inorganic Chemistry, 2024, 40(9): 1640-1652. doi: 10.11862/CJIC.20240183
18. [18]
  Cheng PENG , Jianwei WEI , Yating CHEN , Nan HU , Hui ZENG . First principles investigation about interference effects of electronic and optical properties of inorganic and lead-free perovskite Cs₃Bi₂X₉ (X=Cl, Br, I). Chinese Journal of Inorganic Chemistry, 2024, 40(3): 555-560. doi: 10.11862/CJIC.20230282
19. [19]
  Hua Hou , Baoshan Wang . Course Ideology and Politics Education in Theoretical and Computational Chemistry. University Chemistry, 2024, 39(2): 307-313. doi: 10.3866/PKU.DXHX202309045
20. [20]
  Lu XU , Chengyu ZHANG , Wenjuan JI , Haiying YANG , Yunlong FU . Zinc metal-organic framework with high-density free carboxyl oxygen functionalized pore walls for targeted electrochemical sensing of paracetamol. Chinese Journal of Inorganic Chemistry, 2024, 40(5): 907-918. doi: 10.11862/CJIC.20230431

Get Citation

PDF

XML

Metrics

PDF Downloads(5)
Abstract views(512)
HTML views(28)

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