Study on the Framework Aluminum Distributions of HMOR Zeolite and Identification of Active Sites for Dimethyl Ether Carbonylation Reaction※

doi:10.6023/A22010014

Acta Chimica Sinica ›› 2022, Vol. 80 ›› Issue (5): 590-597.DOI: 10.6023/A22010014 Previous Articles Next Articles

Special Issue: 中国科学院青年创新促进会合辑

Article

HMOR分子筛骨架铝分布研究及二甲醚羰基化反应活性中心的辨识^※

张瑾^a^,^c, 丁湘浓^a, 刘红超^a, 樊栋^a, 徐舒涛^a^,^*(), 魏迎旭^a, 刘中民^a^,^b^,^c

a 中国科学院大连化学物理研究所甲醇制烯烃国家工程实验室辽宁大连 116023
b 中国科学院大连化学物理研究所催化基础国家重点实验室辽宁大连 116023
c 中国科学院大学化学工程学院北京 100049

投稿日期:2022-01-09 发布日期:2022-05-31
通讯作者: 徐舒涛
作者简介:
^※庆祝中国科学院青年创新促进会十年华诞.
基金资助:
国家自然科学基金(21972142); 国家自然科学基金(22022202); 国家自然科学基金(21991092); 国家自然科学基金(21991090); 大连市杰出青年基金项目(2021RJ01); 中国科学院前沿科学重点研究计划(QYZDY-SSW-JSC024); 中国科学院国际合作(121421KYSB20180007)

Study on the Framework Aluminum Distributions of HMOR Zeolite and Identification of Active Sites for Dimethyl Ether Carbonylation Reaction^※

Jin Zhang^a^,^c, Xiangnong Ding^a, Hongchao Liu^a, Dong Fan^a, Shutao Xu^a(), Yingxu Wei^a, Zhongmin Liu^a^,^b^,^c

a National Engineering Laboratory for Methanol to Olefins, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning 116023
b State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, Liaoning 116023
c School of Chemical Engineering, University of Chinese Academy of Sciences, Beijing 100049

Received:2022-01-09 Published:2022-05-31
Contact: Shutao Xu
About author:
^※Dedicated to the 10th anniversary of the Youth Innovation Promotion Association, CAS.
Supported by:
National Natural Science Foundation of China(21972142); National Natural Science Foundation of China(22022202); National Natural Science Foundation of China(21991092); National Natural Science Foundation of China(21991090); Dalian Outstanding Young Scientist Foundation(2021RJ01); Key Research Program of Frontier Sciences, Chinese Academy of Sciences(QYZDY-SSW-JSC024); International Partnership Program of Chinese Academy of Sciences(121421KYSB20180007)

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Abstract

HMOR zeolites has an excellent performance similar to enzyme catalysis in the carbonylation of dimethyl ether (DME). The distribution of framework aluminum and the identification of the active site of the reaction are the key issues in the study of the reaction mechanism. The early work was based on theoretical calculation to study the active site of DME carbonylation, but lacked direct experimental evidence. In this work, a series of HMOR catalysts were prepared by calcination of NH₄MOR at various temperatures. The stability and location of framework aluminum were studied by a variety of spectroscopic characterization methods. Moreover, the evidence of reaction mechanism was obtained by the carbonylation reaction activity of dimethyl ether related to the acidity of MOR zeolite and aluminum distribution. Firstly, it was found that the crystallinity and morphology of MOR zeolites did not change significantly after calcination at different temperatures by XRD (X-Ray diffraction) and SEM (Scanning electron microscope). However, it was found by ²⁹Si, ²⁷Al and ¹H Magic angle spinning (MAS) solid-state nuclear magnetic resonance (NMR) that the local environment of HMORs was dealuminated, which resulted in obvious defect hydroxyl groups and the decrease of Brönsted acid sites (BASs) content. In addition, the calcination temperature has a great influence on the stability of framework Al of HMORs. Increase of calcination temperature will accelerate the occurrence of dealumination. Quantitative¹H MAS NMR combined with Fourier transform infrared spectra (FTIR) provided the distribution of BASs content in different channels of HMOR zeolites. By using 2D ²⁷Al multiple quantum (MQ) MAS NMR method combined with the representative slices parallel to the F2 dimension of MQMAS NMR spectra at selected F1 chemical shift to distinguish the framework Al sites, it was found that when the temperature was lower than 600 ℃, framework Al atoms located in the different T-sites had the similar dealumination rate. But when the calcination temperature was increased to 600 ℃, the removal rate of Al atom at T3 site was accelerated. Furthermore, the relationship between the carbonylation performance of dimethyl ether and the distribution of Brønsted acid and aluminum was studied, and the definitive spectral evidence of the carbonylation activity center was obtained, that is, the Al site at T3-O33 was the active site of the carbonylation reaction.

Key words: HMOR, acidity, aluminum distribution, solid-state NMR, DME carbonylation

Cite this article

Jin Zhang, Xiangnong Ding, Hongchao Liu, Dong Fan, Shutao Xu, Yingxu Wei, Zhongmin Liu. Study on the Framework Aluminum Distributions of HMOR Zeolite and Identification of Active Sites for Dimethyl Ether Carbonylation Reaction^※[J]. Acta Chimica Sinica, 2022, 80(5): 590-597.

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Fig. & Tab. 10

Figure 1. Framework structure of Mordenite (viewed along [010])

Figure 2. X-ray diffraction patterns of NH4MOR and calcination treated samples at different temperature.

Sample	C_XRD/%	Si/Al ratio	Surface area/(m²•g^-1)			Pore volume/(cm³•g^-1)
Sample	C_XRD/%	Si/Al ratio	BET	Micro*	Ext*	Total	Micro*	Meso*
NH₄MOR	100	7.3	—	—	—	—	—	—
HMOR-450-4	90.3	9.1	446.3	409.7	36.5	0.23	0.19	0.06
HMOR-500-4	91.1	9.7	432.9	395.9	37.0	0.22	0.18	0.06
HMOR-550-4	90.8	10.9	454.5	414.1	40.3	0.24	0.20	0.06
HMOR-600-4	90.9	12.5	400.2	366.0	34.2	0.21	0.18	0.05

Table 1. Physicochemical properties of NH4MOR and its calcined samples under different temperatures

Figure 3. 29Si MAS NMR spectra of NH4MOR, HMOR-450-4, HMOR-500-4, HMOR-550-4, and HMOR-600-4

Figure 4. 27Al MAS NMR spectra of NH4MOR, HMOR-450-4, HMOR-500-4, HMOR-550-4 and HMOR-600-4

Figure 5. The 1H MAS NMR of HMOR samples (A), the FTIR spectra and the deconvoluted results of signal at 3608 cm-1 of HMOR samples (B)

Sample	¹H MAS NMR/(mmol•g^–1)	FTIR^a/(mmol•g^–1)
Sample	Total	8MR	12MR
HMOR-450-4	1.62	0.98	0.64
HMOR-500-4	1.86	1.00	0.86
HMOR-550-4	1.36	0.83	0.53
HMOR-600-4	0.9	0.52	0.38

Table 2. Brönsted acid distribution of the HMOR samples derived from 1H MAS NMR and FTIR

Figure 6. 27Al MQ MAS NMR spectra and their fitting curves of HMOR zeolites: HMOR-450-4 (a), HMOR-500-4 (b), HMOR-550-4 (c) and HMOR-600-4 (d). The representative slices parallel to the F2 acquisition dimension (the anisotropic chemical shift dimension) at selected F1 dimensions (the isotropic chemical shift dimension) with the fitting lines are on the left, and deconvoluted 1D 27Al MAS NMR spectra by using quadrupole line shapes are on the top of F2 dimension

Sample	Al(Ⅳ)-1
	T2		T1		T4		T3
	(%)	mmol•g^–1	(%)	mmol•g^–1	(%)	mmol•g^–1	(%)	mmol•g^–1	(%)	mmol•g^–1
HMOR-450-4	9.93	0.1639	18.11	0.299	40.69	0.671	31.27	0.516	—	—
HMOR-500-4	10.20	0.1589	18.37	0.286	40.63	0.633	30.8	0.480	—	—
HMOR-550-4	9.95	0.1394	15.38	0.215	24.80	0.347	23.66	0.331	26.2	0.367
HMOR-600-4	9.11	0.1125	14.80	0.183	24.16	0.298	13.73	0.170	38.20	0.471

Table 3. Relative percentage concentration for amount of substance and corresponding concentration of Al(Ⅳ)-1 at different T sites and Al(Ⅳ)-2 species

Figure 7. DME conversion and MAc selectivity (a), Space Time Yield plotted against the concentration of B acid site in 8MR (b) and the number of Al (T3) (c), respectively over HMOR-450-4, HMOR-500-4, HMOR-550-4 and HMOR-600-4. The reaction conditions are as follows: reaction temperature T=200 ℃, total reaction pressure pT=2.0 MPa, composition of reaction gas V(DME)∶V(CO)∶V(H2)=5∶35∶60, gas hourly space velocity (GHSV)=1800 mL•gcat–1•h–1

References 60

[1]	Sun, D.; Sun, B.; Pei, Y.; Yan, S. R.; Fan, K. N.; Qiao, M. H.; Zhang, X. X.; Zong, B. N. Acta Chim. Sinica 2021, 79, 771. (in Chinese) doi: 10.6023/A20120563
	(孙冬, 孙博, 裴燕, 闫世润, 范康年, 乔明华, 张晓昕, 宗保宁, 化学学报, 2021, 79, 771.) doi: 10.6023/A20120563
[2]	Zhang, M. T.; Yan, T. T.; Dai, W. L.; Guan, N. J.; Li, L. D. Acta Chim. Sinica 2020, 78, 1404. (in Chinese) doi: 10.6023/A20080346
	(张梦婷, 颜婷婷, 戴卫理, 关乃佳, 李兰冬, 化学学报, 2020, 78, 1404.) doi: 10.6023/A20080346
[3]	Yao, X. T.; Huang, X.; Lin, Y. X.; Liu, Y. M. Acta Chim. Sinica 2020, 78, 1111. (in Chinese) doi: 10.6023/A20060246
	(姚旭婷, 黄鑫, 林玉霞, 刘月明, 化学学报, 2020, 78, 1111.) doi: 10.6023/A20060246
[4]	Liu, Y. H.; Zhao, N.; Xian, H.; Cheng, Q. P.; Tan, Y. S.; Tsubaki, N.; Li, X. G. ACS Appl. Mater. Inter. 2015, 7, 8398. doi: 10.1021/acsami.5b01905
[5]	Li, Y.; Sun, Q.; Huang, S. Y.; Cheng, Z. Z.; Cai, K.; Lv, J.; Ma, X. B. Catal. Today 2018, 311, 81. doi: 10.1016/j.cattod.2017.08.050
[6]	Zhao, N.; Cheng, Q. P.; Lyu, S. S.; Guo, L. H.; Tian, Y.; Ding, T.; Xu, J.; Ma, X. B.; Li, X. G. Catal. Today. 2020, 339, 86. doi: 10.1016/j.cattod.2019.01.013
[7]	Huo, H.; Peng, L. M.; Gan, Z. H.; Grey, C. P. J. Am. Chem. Soc. 2012, 134, 9708. doi: 10.1021/ja301963e
[8]	Lukyanov, D. B.; Vazhnova, T.; Cherkasov, N.; Casci, J. L.; Birtill, J. J. J. Phys. Chem. C 2014, 118, 23918. doi: 10.1021/jp5086334
[9]	Cai, K.; Huang, S. Y.; Li, Y.; Cheng, Z. Z.; Lv, J.; Ma, X. B. ACS Sustain. Chem. Eng. 2019, 7, 2027. doi: 10.1021/acssuschemeng.8b04388
[10]	Yi, X. F.; Xiao, Y.; Li, G. C.; Liu, Z. Q.; Chen, W.; Liu, S. B.; Zheng, A. M. Chem. Mater. 2020, 32, 1332. doi: 10.1021/acs.chemmater.0c00005
[11]	Gong, K.; Liu, Z. M.; Liang, L. X.; Zhao, Z. C.; Guo, M. L.; Liu, X. B.; Han, X. W.; Bao, X. H.; Hou, G. J. J. Phys. Chem. Lett. 2021, 12, 2413. doi: 10.1021/acs.jpclett.0c03610 pmid: 33661009
[12]	Cao, K. P.; Fan, D.; Gao, M. B.; Fan, B. H.; Chen, N.; Wang, L. Y.; Tian, P.; Liu, Z. M. ACS Catal. 2021, 12, 1. doi: 10.1021/acscatal.1c04966
[13]	Bajpai, P. K. Zeolites 1986, 6, 2. doi: 10.1016/0144-2449(86)90002-3
[14]	Bajpai, P. K.; Rao, M. S.; Gokhale, K. V. G. K. Ind. Eng. Chem. Prod. Res. Dev. 1981, 20, 721. doi: 10.1021/i300004a026
[15]	Bhan, A.; Allian, A. D.; Sunley, G. J.; Law, D. J.; Iglesia, E. J. Am. Chem. Soc. 2007, 129, 4919. doi: 10.1021/ja070094d
[16]	Boronat, M.; Martinez-Sanchez, C.; Law, D.; Corma, A. J. Am. Chem. Soc. 2008, 130, 16316. doi: 10.1021/ja805607m
[17]	Cheung, P.; Bhan, A.; Sunley, G. J.; Iglesia, E. Angew. Chem., Int. Ed. 2006, 45, 1617. doi: 10.1002/anie.200503898
[18]	Cheung, P.; Bhan, A.; Sunley, G.; Law, D.; Iglesia, E. J. Catal. 2007, 245, 110. doi: 10.1016/j.jcat.2006.09.020
[19]	Jiang, Y. J.; Hunger, M.; Wang, W. J. Am. Chem. Soc. 2006, 128, 11679. doi: 10.1021/ja061018y
[20]	Chu, Y. Y.; Lo, A. Y.; Wang, C.; Deng, F. J. Phys. Chem. C 2019, 123, 15503. doi: 10.1021/acs.jpcc.9b01874
[21]	Blasco, T.; Boronat, M.; Concepcion, P.; Corma, A.; Law, D.; Vidal-Moya, J. A. Angew. Chem., Int. Ed. 2007, 46, 3938.
[22]	He, T.; Ren, P. J.; Liu, X. C.; Xu, S. T.; Han, X. W.; Bao, X. H. Chem. Commun. 2015, 51, 16868. doi: 10.1039/C5CC07201H
[23]	Li, B. J.; Xu, J.; Han, B.; Wang, X. M.; Qi, G. D.; Zhang, Z. F.; Wang, C.; Deng, F. J. Phys. Chem. C 2013, 117, 5840. doi: 10.1021/jp400331m
[24]	Xue, H. F.; Huang, X. M.; Ditzel, E.; Zhan, E. S.; Ma, M.; Shen, W. J. Ind. Eng. Chem. Res. 2013, 52, 11510. doi: 10.1021/ie400909u
[25]	Wang, S. R.; Guo, W. W.; Zhu, L. J.; Wang, H. X.; Qiu, K. Z.; Cen, K. F. J. Phys. Chem. C 2014, 119, 524. doi: 10.1021/jp511543x
[26]	Liu, S. P.; Liu, H. C.; Ma, X. G.; Liu, Y.; Zhu, W. L.; Liu, Z. M. Catal. Sci. Technol. 2020, 10, 4663. doi: 10.1039/D0CY00125B
[27]	Cao, K. P.; Fan, D.; Li, L. Y; Fan, B. H.; Wang, L. Y.; Zhu, D. L.; Wang, Q. Y.; Tian, P.; Liu, Z. M. ACS Catal. 2020, 10, 3372. doi: 10.1021/acscatal.9b04890
[28]	Wang, X. S.; Li, R. J.; Yu, C. C.; Liu, Y. X.; Zhang, L. Y.; Xu, C. M.; Zhou, H. J. Fuel 2019, 239, 794. doi: 10.1016/j.fuel.2018.10.147
[29]	Reule, A. A. C.; Sawada, J. A.; Sema gina, N. J. Catal. 2017, 349, 98. doi: 10.1016/j.jcat.2017.03.010
[30]	Li, Y.; Li, Z. H.; Huang, S. Y.; Cai, K.; Qu, Z.; Zhang, J. F.; Wang, Y.; Ma, X. B. ACS Appl. Mater. Inter. 2019, 11, 24000. doi: 10.1021/acsami.9b03588
[31]	Paul, G.; Bisio, C.; Braschi, I.; Cossi, M.; Gatti, G.; Gianotti, E.; Marchese, L. Chem. Soc. Rev. 2018, 47, 5684. doi: 10.1039/c7cs00358g pmid: 30014075
[32]	Chen, X.; Fu, Y. Y.; Yue, B.; He, H. Y. Chin. J. Magn. Reson. 2021, 38, 491. (in Chinese)
	(陈欣, 付颖懿, 岳斌, 贺鹤勇, 波谱学杂志, 2021, 38, 491.)
[33]	Gao, S. S.; Xu, S. T.; Wei, Y. X.; Liu, Z. M. Chin. J. Magn. Reson. 2021, 38, 433. (in Chinese)
	(高树树, 徐舒涛, 魏迎旭, 刘中民, 波谱学杂志, 2021, 38, 433.)
[34]	Xao, Y.; Xia, C. J.; Yi, X. F.; Liu, F. Q.; Liu, S. B.; Zheng, A. M. Chin. J. Magn. Reson. 2021, 38, 571. (in Chinese)
	肖瑶, 夏长久, 易先锋, 刘凤庆, 刘尚斌, 郑安民, 波谱学杂志, 2021, 38, 571.)
[35]	Chen, H. D.; Kong, H. Y.; Zhao, Z. C.; Zhang, W. P. Chin. J. Magn. Reson. 2021, 38, 543. (in Chinese)
	(陈翰迪, 孔海宇, 赵侦超, 张维萍, 波谱学杂志, 2021, 38, 543.)
[36]	Yang, W. J.; Huang, J. Chin. J. Magn. Reson. 2021, 38, 460. (in Chinese)
	(杨文杰, 黄骏, 波谱学杂志, 2021, 38, 460.)
[37]	Wang, Y. X. Wang, Q.; Xu, J.; Xia, Q. H.; Deng, F. Chin. J. Magn. Reson. 2021, 38, 514. (in Chinese)
	(王永祥, 王强, 徐君, 夏清华, 邓风, 波谱学杂志, 2021, 38, 514.)
[38]	Xia, X. F.; Zhang, W. J.; Lin, Z. Y.; Ke, X. K.; Wen, Y. J.; Wang, F.; Chen, J. C.; Peng, L. M. Chin. J. Magn. Reson. 2021, 38, 533. (in Chinese)
	(夏锡锋, 张文静, 林芝晔, 柯晓康, 温玉洁, 王芳, 陈俊超, 彭路明, 波谱学杂志, 2021, 38, 533.)
[39]	Fyfe, C. A.; Gobbi, G. C.; Murphy, W. J.; Ozubko, R. S.; Slack, D. A. J. Am. Chem. Soc. 1984, 106, 4435. doi: 10.1021/ja00328a024
[40]	Yokoi, T.; Mochizuki, H.; Namba, S.; Kondo, J. N.; Tatsumi, T. J. Phys. Chem. C 2015, 119, 15303. doi: 10.1021/acs.jpcc.5b03289
[41]	Kneller, J. M.; Pietraß, T.; Ott, K. C.; Labouriau, A. Micropor. Mesopor. Mater. 2003, 62, 121. doi: 10.1016/S1387-1811(03)00400-1
[42]	Ravi, M.; Sushkevich, V. L.; van Bokhoven, J. A. Chem. Sci. 2021, 12, 4094. doi: 10.1039/D0SC06130A
[43]	Medek, A.; Harwood, J. S.; Frydman, L. J. Am. Chem. Soc. 1995, 117, 12779. doi: 10.1021/ja00156a015
[44]	Massiot, D.; Fayon, F.; Capron, M.; King, I.; Le Calvé, S.; Alonso, B.; Durand, J.-O.; Bujoli, B.; Gan, Z. H.; Hoatson, G. Magn. Reason. Chem. 2002, 40, 70.
[45]	Hu, J. Z.; Wan, C.; Vjunov, A.; Wang, M.; Zhao, Z. C.; Hu, M. Y.; Camaioni, D. M.; Lercher, J. A. J. Phys. Chem. C. 2017, 121, 12849. doi: 10.1021/acs.jpcc.7b03517
[46]	Frydman, L.; Harwood, J. S. J. Am. Chem. Soc. 1995, 117, 5367. doi: 10.1021/ja00124a023
[47]	Sarv, P.; Tuherm, T.; Lippmaa, E.; Keskinen, K.; Root, A. J. Phys. Chem. 1995, 99, 13763. doi: 10.1021/j100038a003
[48]	Maache, M.; Janin, A.; Lavalley, J. C.; Benazzi, E. Zeolites 1995, 15, 507. doi: 10.1016/0144-2449(95)00019-3
[49]	Pastvova, J.; Pilar, R.; Moravkova, J.; Kaucky, D.; Rathousky, J.; Sklenak, S.; Sazama, P. Appl. Catal. A. 2018, 562, 159. doi: 10.1016/j.apcata.2018.05.035
[50]	Wakabayashi, F.; Kondo, J.; Wada, A.; Domen, K.; Hirose, C. J. Phys. Chem. 1996, 100, 4154. doi: 10.1021/jp9522775
[51]	Zholobenko, V. L.; Makarova, M. A.; Dwyer, J. J. Phys. Chem. 2002, 97, 5962. doi: 10.1021/j100124a030
[52]	Engelhardt, G.; Kentgens, A. P. M.; Koller, H.; Samoson, A. Solid State Nucl. Magn. Reson. 1999, 15, 171. pmid: 10672941
[53]	Liu, R. S.; Fan, B. H.; Zhang, W. N.; Wang, Y. L.; Qi, L.; Xu, S. T.; Yu, Z. X.; Wei, Y. X.; Liu, Z. M. Angew. Chem., Int. Ed. 2022, e202116990.
[54]	Jeffroy, M.; Nieto-Draghi, C.; Boutin, A. Chem. Mater. 2017, 29, 513. doi: 10.1021/acs.chemmater.6b03011
[55]	Chen, K.; Horstmeier, S.; Nguyen, V. T.; Wang, B.; Crossley, S. P.; Pham, T.; Gan, Z.; Hung, I.; White, J. L. J. Am. Chem. Soc. 2020, 142, 7514. doi: 10.1021/jacs.0c00590
[56]	Chen, K.; Gan, Z.; Horstmeier, S.; White, J. L. J. Am. Chem. Soc. 2021, 143, 6669. doi: 10.1021/jacs.1c02361
[57]	Bodart, P.; Nagy, J. B.; Debras, G.; Gabelica, Z.; Jacobs, P. A. J. Phys. Chem. 1986, 90, 5183. doi: 10.1021/j100412a058
[58]	Debras, G.; Nagy, J. B.; Gabelica, Z.; Bodart, P.; Jacobs, P. A. Chem. Lett. 1983, 12, 199. doi: 10.1246/cl.1983.199
[59]	Schroeder, K. P.; Sauer, J. J. Phys. Chem. 1993, 97, 6579.
[60]	Amoureux, J. P.; Fernandez, C.; Steuernagel, S. J. Magn. Reson. A 1996, 123, 116. doi: 10.1006/jmra.1996.0221

HMOR分子筛骨架铝分布研究及二甲醚羰基化反应活性中心的辨识^※

Study on the Framework Aluminum Distributions of HMOR Zeolite and Identification of Active Sites for Dimethyl Ether Carbonylation Reaction^※

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[10]	Chen Jianshe;Lu Gui;Wei Danyi;Yao Kemin;Shen Lianfang. Studies on the acidity properties of Eu(Ⅲ) complexes with α-amino acids by ^1^3C NMR [J]. Acta Chimica Sinica, 1998, 56(9): 892-899.
[11]	XIA SHIJUN;CHENG DEPING. Studies on the directional reaction of silver coordination compounds with hydrazine [J]. Acta Chimica Sinica, 1990, 48(3): 251-255.
[12]	YANG SHUXUN;TONG HUAXIANG;WANG WENXIANG. Kinetic study on the reaction system of Tl^3^+-H2O2-Fe^2^+ [J]. Acta Chimica Sinica, 1989, 47(9): 831-837.
[13]	LIU CHENGMIN;WANG YAHUI;CHI XIZENG;LIANG SHUQUAN. The additivity of the absorbances of Europium (or other Lanthanides)-Bivalent metal ions-xylenol orange [J]. Acta Chimica Sinica, 1989, 47(6): 563-567.
[14]	PANG WENQIN;QIU SHILUN;DI BIN;ZHOU FENGQI. Synthesis and characterization of Ga-ZSM-5 zeolite in a slightly acidic medium [J]. Acta Chimica Sinica, 1989, 47(5): 476-480.
[15]	LU QIN;WANG GUOXIONG;ZANG YAN;ZENG CHENG. Correlation between acid strengths and quantum chemical parameters of some oxygen-containing acids [J]. Acta Chimica Sinica, 1989, 47(3): 284-287.

HMOR分子筛骨架铝分布研究及二甲醚羰基化反应活性中心的辨识※

Study on the Framework Aluminum Distributions of HMOR Zeolite and Identification of Active Sites for Dimethyl Ether Carbonylation Reaction※

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HMOR分子筛骨架铝分布研究及二甲醚羰基化反应活性中心的辨识^※

Study on the Framework Aluminum Distributions of HMOR Zeolite and Identification of Active Sites for Dimethyl Ether Carbonylation Reaction^※