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※

doi:10.6023/A22010014

化学学报 ›› 2022, Vol. 80 ›› Issue (5): 590-597.DOI: 10.6023/A22010014 上一篇下一篇

所属专题：中国科学院青年创新促进会合辑

研究论文

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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摘要/Abstract

HMOR分子筛在二甲醚羰基化反应中具有类似酶催化的优异性能. 关于骨架铝的分布和反应活性位的识别是研究该反应机理的关键科学问题. 早期的工作是基于理论计算研究二甲醚羰基化活性位点, 但缺乏直接的谱学证据. 通过在不同温度下焙烧NH₄MOR制备了一系列HMOR催化剂, 通过多种谱学表征手段研究分子筛骨架铝的稳定性以及铝原子落位信息, 进一步通过二甲醚羰基化反应活性关联MOR分子筛的酸性和铝分布关系获得反应机理的谱学证据. 首先从XRD (X-Ray diffraction)和SEM (Scanning electron microscope)发现经过不同温度焙烧, MOR分子筛结晶度和宏观形貌没有发生明显变化, 但是通过一维²⁹Si, ²⁷Al和¹H魔角旋转固体核磁谱(MAS NMR)发现分子筛局部环境发生了脱铝现象, 产生了明显的缺陷羟基以及B酸量的下降. 焙烧温度对HMOR分子筛骨架Al稳定性的影响较大, 随着温度升高, 脱铝逐渐加剧. 定量¹H MAS NMR结合红外(IR)光谱提供了HMOR分子筛不同孔道B酸含量的分布. 进一步使用2D ²⁷Al MQ MAS NMR的方法以及结合切片分峰拟合技术区分出分子筛骨架中的四种不同T位点, 发现当温度低于600 ℃, 不同T位脱铝速率相当; 当焙烧温度为600 ℃时, T3位点的Al原子脱除速率加快. 最后研究了二甲醚羰基化反应性能与酸分布和铝分布的关系, 获得羰基化反应活性中心的确凿谱学证据, T3-O33位置的Al位是羰基化反应的活性中心.

关键词: HMOR, 酸性, 铝分布, 固体核磁, 二甲醚羰基化

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

引用此文

张瑾, 丁湘浓, 刘红超, 樊栋, 徐舒涛, 魏迎旭, 刘中民. 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^※[J]. 化学学报, 2022, 80(5): 590-597.

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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图/表 10

图1. Mordenite分子筛骨架结构示意图(沿[010]方向)

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

图2. NH4MOR和不同温度焙烧后样品的XRD谱图

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

表1. NH4MOR及其在不同焙烧温度下获得HMOR样品的物理化学性质

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

图3. NH4MOR, HMOR-450-4, HMOR-500-4, HMOR-550-4和HMOR-600-4样品的29Si MAS NMR谱图

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

图4. NH4MOR, HMOR-450-4, HMOR-500-4, HMOR-550-4和HMOR-600-4样品的27Al MAS NMR谱图

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

图5. 不同焙烧温度HMOR样品的1H MAS NMR谱图(A), 红外光谱图以及在3608 cm-1处B酸信号的分峰拟合结果(B)

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

表2. 基于1H MAS NMR和FTIR的HMOR样品的B酸分布

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

图6. 系列HMOR分子筛的27Al MQ MAS NMR谱图及分峰拟合曲线: HMOR-450-4 (a), HMOR-500-4 (b), HMOR-550-4 (c)和HMOR-600-4 (d). 左图为选择F1维度(各向同性化学位移)不同T位点对应的平行于F2维度(各向异性化学位移)的切片信号以及拟合曲线. 通过左图获得的四极核参数对1D 27Al MAS NMR谱图进行四极线型分峰拟合曲线在F2维正上方

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

表3. Al(Ⅳ)-1和Al(Ⅳ)-2物种的物质的量的相对量和对应浓度

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

图7. 系列HMOR样品的DME转化率和乙酸甲酯(methyl acetate, MAc)选择性(a)、时空产率与8MR中B酸中心浓度(b)、以及与Al (T3)原子绝对浓度的关系图(c). 反应条件: 反应温度T=200 ℃, 反应总压pT=2.0 MPa, 反应气组成V(DME)∶V(CO)∶V(H2)=5∶35∶60, 空速GHSV=1800 mL•gcat–1•h–1

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

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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^※

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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※

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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^※