Conversion of industrial solid wastes into functional materials has attracted considerable interest,as it can reduce environmental pollution and facilitate the sustainable development of relevant processes.Herein,spen...Conversion of industrial solid wastes into functional materials has attracted considerable interest,as it can reduce environmental pollution and facilitate the sustainable development of relevant processes.Herein,spent methanol-to-olefins(MTO)industrial catalyst was explored for the synthesis of DNL-6 molecular sieve,a promising SAPO-type adsorbent for CO_(2) capture.It was demonstrated that DNL-6 with high purity and crystallinity,and various silica contents can be readily synthesized.Na-exchanged DNL-6 was further prepared using the as-synthesized DNL-6 as the precursor,and its structure was investigated by Rietveld refinement,revealing that Na cations were mainly located in the single 8-rings(S8Rs).Na-DNL-6 with varied silica contents and Na contents were investigated for adsorption studies.Na-DNL-6 with a high Na exchange degree exhibited comparable CO_(2) uptake with H-DNL-6(298 K and 101 kPa);but superior separation selectivity for CO_(2)/CH4(as high as 1369,50/50 kPa);CO_(2)/N_(2)(∞,15/85 kPa)owing to the“trapdoor”effect associated with the Na cations sited in the S8Rs.This work provides an eco-friendly approach for the synthesis of efficient silicoaluminophosphate adsorbent for CO_(2) capture.展开更多
As the main contributor of the formation of particulate matter as well as ozone, volatile organic compounds(VOCs) greatly affect human health and the environmental quality. Catalytic combustion/oxidation has been view...As the main contributor of the formation of particulate matter as well as ozone, volatile organic compounds(VOCs) greatly affect human health and the environmental quality. Catalytic combustion/oxidation has been viewed as an efficient, economically feasible and environmentally friendly way for the elimination of VOCs. Supported metal catalyst is the preferred type of catalysts applied for VOCs catalytic combustion because of the synergy between active components and support as well as its flexibility in the composition. The presence of support not only plays the role of keeping the catalyst with good stability and mechanical strength, but also provides a large specific surface for the good dispersion of active components, which could effectively improve the performance of catalyst as well as decrease the usage of active components, especially the noble metal amount. Mesoporous molecular sieves, owing to their large surface area, unique porous structures, large pore size as well as uniform pore-size distribution, were viewed as superior support for dispersing active components. This review focuses on the recent development of mesoporous molecular sieve supported metal catalysts and their application in catalytic oxidation of VOCs. The effect of active component types, support structure, preparation method, precursors, etc. on the valence state, dispersion as well as the loading of active species were also discussed and summarized. Moreover, the corresponding conversion route of VOCs was also addressed.This review aims to provide some enlightment for designing the supported metal catalysts with superior activity and stability for VOCs removal.展开更多
A series of phenyl functionalized MSU mesoporous molecular sieves were synthesized under neutral condition in the presence of biodegradable non ionic polyethylene oxide(AEO 9). By subsequent sulphonation of the phenyl...A series of phenyl functionalized MSU mesoporous molecular sieves were synthesized under neutral condition in the presence of biodegradable non ionic polyethylene oxide(AEO 9). By subsequent sulphonation of the phenyl rings attached to the silica framework, the phenylsulphonic acid functionalized MSU derivatives could be obtained. Their structure and property of the organo modified mesoporous molecular sieves were studied by means of XRD, FT IR, TEM, HRTEM, 13 C MAS NMR, 29 Si MAS NMR, N 2 adsorption/desorption and probe reaction techniques. The results showed that the so produced organo modified mesoporous molecular sieves featured bimodal pore size distribution and the pore channel was similar to those in the \{MSU(worm like)\}. The organo modified mesoporous molecular sieves containing phenylsulphonic acid active sites, used as solid acid catalyst, showed a much higher catalytic activity for the formation of 2,2 pentamethylene 1,3 dioxolane(cyclic ketal) from ethylene glycol and cyclohexanone.[WT5HZ]展开更多
基金supported by the National Natural Science Foundation of China(Nos.21991090,21991091,22171259,22272173)the AI S&T Program of Yulin Branch,Dalian National Laboratory for Clean Energy,CAS(No.DNL-YL A202206)The authors thank to the funding from the Sino-French IRN(International Research Network).
文摘Conversion of industrial solid wastes into functional materials has attracted considerable interest,as it can reduce environmental pollution and facilitate the sustainable development of relevant processes.Herein,spent methanol-to-olefins(MTO)industrial catalyst was explored for the synthesis of DNL-6 molecular sieve,a promising SAPO-type adsorbent for CO_(2) capture.It was demonstrated that DNL-6 with high purity and crystallinity,and various silica contents can be readily synthesized.Na-exchanged DNL-6 was further prepared using the as-synthesized DNL-6 as the precursor,and its structure was investigated by Rietveld refinement,revealing that Na cations were mainly located in the single 8-rings(S8Rs).Na-DNL-6 with varied silica contents and Na contents were investigated for adsorption studies.Na-DNL-6 with a high Na exchange degree exhibited comparable CO_(2) uptake with H-DNL-6(298 K and 101 kPa);but superior separation selectivity for CO_(2)/CH4(as high as 1369,50/50 kPa);CO_(2)/N_(2)(∞,15/85 kPa)owing to the“trapdoor”effect associated with the Na cations sited in the S8Rs.This work provides an eco-friendly approach for the synthesis of efficient silicoaluminophosphate adsorbent for CO_(2) capture.
基金supported by the Open Research Fund Program of State Environmental Protection Key Laboratory of Food Chain Pollution Control (No. FC_(2)021YB05)the Opening Fund of State Key Laboratory of Heavy Oil Processing (No. SKLOP202002001)+1 种基金Fundamental Research Funds for the Central Universities (No. FRF-IDRY-20-004)National Natural Science Foundation of China (No. U20A20130)。
文摘As the main contributor of the formation of particulate matter as well as ozone, volatile organic compounds(VOCs) greatly affect human health and the environmental quality. Catalytic combustion/oxidation has been viewed as an efficient, economically feasible and environmentally friendly way for the elimination of VOCs. Supported metal catalyst is the preferred type of catalysts applied for VOCs catalytic combustion because of the synergy between active components and support as well as its flexibility in the composition. The presence of support not only plays the role of keeping the catalyst with good stability and mechanical strength, but also provides a large specific surface for the good dispersion of active components, which could effectively improve the performance of catalyst as well as decrease the usage of active components, especially the noble metal amount. Mesoporous molecular sieves, owing to their large surface area, unique porous structures, large pore size as well as uniform pore-size distribution, were viewed as superior support for dispersing active components. This review focuses on the recent development of mesoporous molecular sieve supported metal catalysts and their application in catalytic oxidation of VOCs. The effect of active component types, support structure, preparation method, precursors, etc. on the valence state, dispersion as well as the loading of active species were also discussed and summarized. Moreover, the corresponding conversion route of VOCs was also addressed.This review aims to provide some enlightment for designing the supported metal catalysts with superior activity and stability for VOCs removal.
文摘A series of phenyl functionalized MSU mesoporous molecular sieves were synthesized under neutral condition in the presence of biodegradable non ionic polyethylene oxide(AEO 9). By subsequent sulphonation of the phenyl rings attached to the silica framework, the phenylsulphonic acid functionalized MSU derivatives could be obtained. Their structure and property of the organo modified mesoporous molecular sieves were studied by means of XRD, FT IR, TEM, HRTEM, 13 C MAS NMR, 29 Si MAS NMR, N 2 adsorption/desorption and probe reaction techniques. The results showed that the so produced organo modified mesoporous molecular sieves featured bimodal pore size distribution and the pore channel was similar to those in the \{MSU(worm like)\}. The organo modified mesoporous molecular sieves containing phenylsulphonic acid active sites, used as solid acid catalyst, showed a much higher catalytic activity for the formation of 2,2 pentamethylene 1,3 dioxolane(cyclic ketal) from ethylene glycol and cyclohexanone.[WT5HZ]
