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Evolution of C–C Bond Formation in the Methanol-to-Olefins Process: From Direct Coupling to Autocatalysis
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-07-11 00:00:00 , DOI: 10.1021/acscatal.8b02385 Xinqiang Wu 1, 2 , Shutao Xu 1 , Yingxu Wei 1 , Wenna Zhang 1, 2 , Jindou Huang 1 , Shuliang Xu 1 , Yanli He 1 , Shanfan Lin 1, 2 , Tantan Sun 1, 2 , Zhongmin Liu 1, 3
ACS Catalysis ( IF 11.3 ) Pub Date : 2018-07-11 00:00:00 , DOI: 10.1021/acscatal.8b02385 Xinqiang Wu 1, 2 , Shutao Xu 1 , Yingxu Wei 1 , Wenna Zhang 1, 2 , Jindou Huang 1 , Shuliang Xu 1 , Yanli He 1 , Shanfan Lin 1, 2 , Tantan Sun 1, 2 , Zhongmin Liu 1, 3
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Methanol conversion during the induction period of methanol-to-olefin (MTO) process has been investigated by solid-state nuclear magnetic resonance (ssNMR), diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), gas chromatography–mass spectroscopy (GC-MS), and time-of-flight mass spectroscopy (TOF-MS), over HSAPO-34 molecular sieve. The two-dimensional (2D) 13C–13C MAS NMR spectra revealed the correlation of surface methoxy species (SMS) and dimethyl ether (DME)/methanol was enhanced with the temperature increase, supporting that the carbon–carbon (C–C) bond can be possibly formed through the direct coupling of SMS and the surface-adsorbed C1 reactant. The evolution of surface species was monitored continuously by the aid of in situ ssNMR and in situ DRIFTS. With the consumption of SMS, alkenyl or/and phenyl carbocations were formed and accumulated as the successive intermediates for methanol conversion. Based on these direct observations, we propose that the first C–C bond is derived from SMS-mediated DME/methanol activation while alkenyl/phenyl carbocations can take over SMS and convert methanol efficiently in the autocatalysis stage of the MTO process.
中文翻译：
甲醇制烯烃过程中CC键形成的演变：从直接偶联到自动催化
已通过固态核磁共振（ssNMR），漫反射红外傅里叶变换光谱（DRIFTS），气相色谱-质谱（GC-MS）研究了甲醇制烯烃（MTO）过程诱导期间的甲醇转化，以及通过HSAPO-34分子筛的飞行时间质谱（TOF-MS）。二维（2D）13 C– 13C MAS NMR光谱显示，随着温度的升高，表面甲氧基物质（SMS）与二甲醚（DME）/甲醇的相关性增强，这表明碳-碳（CC）键可能通过直接偶联形成SMS和表面吸附的C1反应物。借助原位ssNMR和原位DRIFTS连续监测表面物质的演变。随着SMS的消耗，烯基或/和苯基碳正离子形成并积累为甲醇转化的连续中间体。基于这些直接观察，我们建议第一个C–C键源自SMS介导的DME /甲醇活化，而烯基/苯基碳正离子可以接管SMS并在MTO过程的自动催化阶段有效地转化甲醇。
更新日期：2018-07-11
中文翻译：
甲醇制烯烃过程中CC键形成的演变：从直接偶联到自动催化
已通过固态核磁共振（ssNMR），漫反射红外傅里叶变换光谱（DRIFTS），气相色谱-质谱（GC-MS）研究了甲醇制烯烃（MTO）过程诱导期间的甲醇转化，以及通过HSAPO-34分子筛的飞行时间质谱（TOF-MS）。二维（2D）13 C– 13C MAS NMR光谱显示，随着温度的升高，表面甲氧基物质（SMS）与二甲醚（DME）/甲醇的相关性增强，这表明碳-碳（CC）键可能通过直接偶联形成SMS和表面吸附的C1反应物。借助原位ssNMR和原位DRIFTS连续监测表面物质的演变。随着SMS的消耗，烯基或/和苯基碳正离子形成并积累为甲醇转化的连续中间体。基于这些直接观察，我们建议第一个C–C键源自SMS介导的DME /甲醇活化，而烯基/苯基碳正离子可以接管SMS并在MTO过程的自动催化阶段有效地转化甲醇。
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