中试研究了好氧膨胀床(OEB)反应器处理甲醇制烯烃(MTO)废水的稳定运行过程,考察了COD去除效果、填料层膨胀情况、反应器压降、反应器排泥及其它运行情况。试验过程运行稳定,膨胀填料层负荷在0.5~1.4 kg COD/m^3/d,COD去除率一直稳定在80...中试研究了好氧膨胀床(OEB)反应器处理甲醇制烯烃(MTO)废水的稳定运行过程,考察了COD去除效果、填料层膨胀情况、反应器压降、反应器排泥及其它运行情况。试验过程运行稳定,膨胀填料层负荷在0.5~1.4 kg COD/m^3/d,COD去除率一直稳定在80%以上,DO比耗基本在1~3,而且废水浊度也可以得到明显去除。确认了自主开发的OEB反应器是稳定和有效的,值得进一步优化并推广使用。展开更多
An effective route to improve the catalytic performance of SAPO-34 in the methanol-to-olefin reaction by simple oxalic acid treatment was investigated. The samples were characterized by XRD, SEM, N2 adsorption-desorpt...An effective route to improve the catalytic performance of SAPO-34 in the methanol-to-olefin reaction by simple oxalic acid treatment was investigated. The samples were characterized by XRD, SEM, N2 adsorption-desorption, XRF, TG, 29Si MAS NMR and NH3-TPD techniques. The results indicated that the external surface acidity of SAPO-34 was finely tuned by oxalic acid treatment, and the selectivity to C2H4 on SAPO-34 and the catalyst lifetime in the methanol-to-olefin reaction were greatly improved.展开更多
A series of SAPO-34 molecular sieves with different SiO_(2)/Al_(2)O_(3)ratios have been synthesized for the methanol-to-olefin(MTO)reaction.Their physico-chemical properties are characterized by various techniques suc...A series of SAPO-34 molecular sieves with different SiO_(2)/Al_(2)O_(3)ratios have been synthesized for the methanol-to-olefin(MTO)reaction.Their physico-chemical properties are characterized by various techniques such as X-ray diffraction(XRD),scanning electron microscopy(SEM),energy dispersive spectroscopy(EDS),Fourier transform infrared spectroscopy(FT-IR)and N2 adsorption-desorption.The results are compared with those of the commercial HZSM-5,which show that the crystallinity and particle diameter of SAPO-34 as well as HZSM-5 increase with SiO_(2)/Al_(2)O_(3)ratio.The variation of BET surface area of SAPO-34 is different from that of HZSM-5 and the sample with SiO_(2)/Al_(2)O_(3)ratio of 0.4 exhibits the highest BET surface area.FT-IR spectra indicate that HZSM-5 has both Brǿnsted and Lewis acid sites and Brǿnsted acid sites are stronger,whereas SAPO-34 samples are dominated only by Lewis acid sites.When the SiO_(2)/Al_(2)O_(3)ratio increases,propylene and butylenes become the predominant product of the MTO reaction over HZSM-5.In contrast,the main products of this reaction catalyzed by SAPO-34 are ethylene and propylene.According to the product distribution,the reaction mechanism over HZSM-5 catalysts is proposed.展开更多
Methanol-to-olefins(MTO)reaction is one of the important non-petroleum routes to produce light olefinsover acidic molecular sieves.In this study,the complete reaction course of MTO on SAPO-34 molecular sieve with reta...Methanol-to-olefins(MTO)reaction is one of the important non-petroleum routes to produce light olefinsover acidic molecular sieves.In this study,the complete reaction course of MTO on SAPO-34 molecular sieve with retained organics evolution from induction period to deactivation period was investigated systematically at different weight hourly space velocities(WHSV)of methanol.By the aid of 12C/3C-methanol isotopic switch experiment,the dual cycle mechanism involving aromatics-based cycle and alkenes-based cycle was evaluated during the whole reac-tion process.The detailed reaction route varied with the evolution of the retained organics in the catalyst at different reaction stages.The aromatics-based cycle and alkenes-based cycle alternately dominate the reaction process.In the efficient reaction period,aromatics-based cvcle is the main reaction mechanism,while in the induction and deactiva-tion periods.the contribution of alkenes-based cvcle mechanism will become more important.展开更多
文摘中试研究了好氧膨胀床(OEB)反应器处理甲醇制烯烃(MTO)废水的稳定运行过程,考察了COD去除效果、填料层膨胀情况、反应器压降、反应器排泥及其它运行情况。试验过程运行稳定,膨胀填料层负荷在0.5~1.4 kg COD/m^3/d,COD去除率一直稳定在80%以上,DO比耗基本在1~3,而且废水浊度也可以得到明显去除。确认了自主开发的OEB反应器是稳定和有效的,值得进一步优化并推广使用。
文摘An effective route to improve the catalytic performance of SAPO-34 in the methanol-to-olefin reaction by simple oxalic acid treatment was investigated. The samples were characterized by XRD, SEM, N2 adsorption-desorption, XRF, TG, 29Si MAS NMR and NH3-TPD techniques. The results indicated that the external surface acidity of SAPO-34 was finely tuned by oxalic acid treatment, and the selectivity to C2H4 on SAPO-34 and the catalyst lifetime in the methanol-to-olefin reaction were greatly improved.
基金This research was supported financially by the National High Technology Research and Development Program of China(863 Program)(Grant Nos.2006AA06Z371 and 2008AA06Z324)the Innovation Project of Institute of Process Engineering,Chinese Academy of Sciences(No.082702).
文摘A series of SAPO-34 molecular sieves with different SiO_(2)/Al_(2)O_(3)ratios have been synthesized for the methanol-to-olefin(MTO)reaction.Their physico-chemical properties are characterized by various techniques such as X-ray diffraction(XRD),scanning electron microscopy(SEM),energy dispersive spectroscopy(EDS),Fourier transform infrared spectroscopy(FT-IR)and N2 adsorption-desorption.The results are compared with those of the commercial HZSM-5,which show that the crystallinity and particle diameter of SAPO-34 as well as HZSM-5 increase with SiO_(2)/Al_(2)O_(3)ratio.The variation of BET surface area of SAPO-34 is different from that of HZSM-5 and the sample with SiO_(2)/Al_(2)O_(3)ratio of 0.4 exhibits the highest BET surface area.FT-IR spectra indicate that HZSM-5 has both Brǿnsted and Lewis acid sites and Brǿnsted acid sites are stronger,whereas SAPO-34 samples are dominated only by Lewis acid sites.When the SiO_(2)/Al_(2)O_(3)ratio increases,propylene and butylenes become the predominant product of the MTO reaction over HZSM-5.In contrast,the main products of this reaction catalyzed by SAPO-34 are ethylene and propylene.According to the product distribution,the reaction mechanism over HZSM-5 catalysts is proposed.
基金Supported by the National Key R&D Program of China(No.2018YFB0604901)the National Natural Science Foundation of China(Nos.21991090,21991092.21972142.91834302,91745109)+4 种基金the Liaoning Revitalization Talents Program,China(Nos.XLYC1808014,XLYC1807227)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.2014165)the Key Research Program of Frontier Sciences of the Chinese Academy of Sciences(Nos.OYZDY-SSW-JSC024.OYZDB-ssw-SLH026)the International Partnership Program of the Chinese Academy of Sciences(No.121421KYSB20180007)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA21030200)。
文摘Methanol-to-olefins(MTO)reaction is one of the important non-petroleum routes to produce light olefinsover acidic molecular sieves.In this study,the complete reaction course of MTO on SAPO-34 molecular sieve with retained organics evolution from induction period to deactivation period was investigated systematically at different weight hourly space velocities(WHSV)of methanol.By the aid of 12C/3C-methanol isotopic switch experiment,the dual cycle mechanism involving aromatics-based cycle and alkenes-based cycle was evaluated during the whole reac-tion process.The detailed reaction route varied with the evolution of the retained organics in the catalyst at different reaction stages.The aromatics-based cycle and alkenes-based cycle alternately dominate the reaction process.In the efficient reaction period,aromatics-based cvcle is the main reaction mechanism,while in the induction and deactiva-tion periods.the contribution of alkenes-based cvcle mechanism will become more important.