CO_(2)hydrogenation has been considered to be a highly promising route for the production of high-value olefins(HVOs)while also mitigating CO_(2)emissions.However,it is challenging to achieve high selectivity and main...CO_(2)hydrogenation has been considered to be a highly promising route for the production of high-value olefins(HVOs)while also mitigating CO_(2)emissions.However,it is challenging to achieve high selectivity and maintain stable performance for HVOs(ethylene,propylene,and linear a-olefins)over a prolonged reaction time due to the difficulty in precise control of carbon coupling and rapid catalyst deactivation.Herein,we present a selective Ba and Na co-modified Fe catalyst enriched with Fe_(5)C_(2)and Fe_(3)C active sites that can boost HVO synthesis with up to 66.1%selectivity at an average CO_(2)conversion of 38%for over 500 h.Compared to traditional NaFe catalyst,the combined effect of Ba and Na additives in the NaBaFe-0.5 catalyst suppressed excess oxidation of FeCxsites by H_(2)O.The absence of Fe3O4phase in the spent NaBaFe-0.5 catalyst reflects the stabilization effect of the co-modifiers on the FeCxsites.This study provides a strategy to design Fe-based catalysts that can be scaled up for the stable synthesis of HVOs from CO_(2)hydrogenation.展开更多
A 2 D-2 D titanium dioxide nanosheet-reduced graphene oxide(TNS-r GO)composite with better electronic conductivity and hydrophilicity was prepared by the hydrothermal method.The as-obtained TNS-r GO composite was furt...A 2 D-2 D titanium dioxide nanosheet-reduced graphene oxide(TNS-r GO)composite with better electronic conductivity and hydrophilicity was prepared by the hydrothermal method.The as-obtained TNS-r GO composite was further functionalized with 3-aminopropyltriethoxysilane(APTES)to provide a large amount of-NH2 groups on the surface for anchoring ultrafine Pd Ag alloy nanoparticles with an average particle size of 1.69 nm by a facile wet reduction approach.Benefiting from the combined effects of well-dispersed Pd Ag alloy nanoparticles,facilitated electron transfer from TNS-r GO to Pd,and increased electron density of active sites,the Pd8 Ag_(1)/NH_(2)-TNS-r GO catalyst exhibited excellent activity towards dehydrogenation of formic acid without adding any additives at 298 K,corresponding to an initial turn over frequency as high as 1090 h-1,which is much higher than that of most other state-of-theart catalysts.展开更多
Catalytic conversion of CO_(2) to high-value products is a crucial method to achieve targets of carbon dioxide emissions peak and carbon neutralization.However,realizing a controllable product distribution in a single...Catalytic conversion of CO_(2) to high-value products is a crucial method to achieve targets of carbon dioxide emissions peak and carbon neutralization.However,realizing a controllable product distribution in a single CO_(2) hydrogenation process is of great challenge.Herein,we prepared the CuFe nanoalloy catalyst that directly transforms CO_(2) to alkanes using physical sputtering method in mild condition.The characteristic results show that the proximity between Cu and Fe is the crucial factor to tunable products among the different catalysts.The formation of unique coordination of FeCu4 nanoalloys from high-energy sputtering process provides close interaction between Cu and Fe,which is favorable to formation of low carbon paraffin,however,a distant proximity and weak interaction will increase the selectivity of olefins and alcohols.This work provides a general strategy for tuning target chemicals and enriches the viewpoints in CO_(2) hydrogenation.展开更多
Direct synthesis of liquefied petroleum gas (LPG) from syngas was carried out over hybrid catalyst consisting of methanol synthesis catalyst and modified Y zeolite with Pd and Ca by different methods. The decrease o...Direct synthesis of liquefied petroleum gas (LPG) from syngas was carried out over hybrid catalyst consisting of methanol synthesis catalyst and modified Y zeolite with Pd and Ca by different methods. The decrease of CO conversion was mostly attributable to the sintering of Cu in methanol synthesis catalyst. On the other hand, coke deposition on Y zeolite was the reason for the decrease of LPG selectivity. The introduction of Ca decreased the strong acid sites of Y zeolite, suppressed coke formation, and thus improved the stability of hybrid catalyst.展开更多
A sustainable strategy for Fischer–Tropsch iron catalysts is successfully achieved by embedding of synergistic promoters from a renewable resource, corncob. The iron-based catalysts, named as 'corncob-driven'...A sustainable strategy for Fischer–Tropsch iron catalysts is successfully achieved by embedding of synergistic promoters from a renewable resource, corncob. The iron-based catalysts, named as 'corncob-driven'catalysts, are composed of iron species supported on carbon as primary active components and various minerals(K, Mg, Ca, and Si, etc.) as promoters. The corncob-driven catalysts are facilely synthesized by a one-pot hydrothermal treatment under mild conditions. The characterization results indicate that the formation of iron carbides from humboldtine is clearly enhanced and the morphology of catalyst particles tends to be more regular microspheres after adding corncob. It is observed that the optimized corncob-driven catalyst exhibits a higher conversion than without promoters' catalyst in Fischer–Tropsch synthesis(ca. 73% vs. ca. 49%). More importantly, a synergistic effect exists in multiple promoters from corncob that can enhance heavy hydrocarbons selectivity and lower CO_2 selectivity, obviously different from the catalyst with promoters from chemicals. The proposed synthesis route of corncob-driven catalysts provides new strategies for the utilization of renewable resources and elimination of environmental pollutants from chemical promoters.展开更多
基金supported by the National Natural Science Foundation of China(21802138,21773234 and 22078315)the‘‘Transformational Technologies for Clean Energy and Demonstration’’,Strategic Priority Research Program of the Chinese Academy of Sciences(XDA 21090203)+3 种基金the Youth Innovation Promotion Association of Chinese Academy of Sciences(2020189)the Natural Science Foundation of Liaoning Province(2022-MS-027)the Youth Science and Technology Star Project Support Program of Dalian City(2021RQ123),DICP(Grant:DICP I202138)the University of Chinese Academy of Sciences(UCAS)for UCAS Scholarship。
文摘CO_(2)hydrogenation has been considered to be a highly promising route for the production of high-value olefins(HVOs)while also mitigating CO_(2)emissions.However,it is challenging to achieve high selectivity and maintain stable performance for HVOs(ethylene,propylene,and linear a-olefins)over a prolonged reaction time due to the difficulty in precise control of carbon coupling and rapid catalyst deactivation.Herein,we present a selective Ba and Na co-modified Fe catalyst enriched with Fe_(5)C_(2)and Fe_(3)C active sites that can boost HVO synthesis with up to 66.1%selectivity at an average CO_(2)conversion of 38%for over 500 h.Compared to traditional NaFe catalyst,the combined effect of Ba and Na additives in the NaBaFe-0.5 catalyst suppressed excess oxidation of FeCxsites by H_(2)O.The absence of Fe3O4phase in the spent NaBaFe-0.5 catalyst reflects the stabilization effect of the co-modifiers on the FeCxsites.This study provides a strategy to design Fe-based catalysts that can be scaled up for the stable synthesis of HVOs from CO_(2)hydrogenation.
基金the financial supports from the Shandong Provincial Natural Science Foundation(Grant No.ZR201910220216)the Key Research and Development Plan of Shandong Province(2019GGX104034)+1 种基金the Foundation of State Key Laboratory of High-efficiency Utilization of Coal,and Green Chemical Engineering(Grant No.2020-KF-18)the Taishan Scholar Program of Shandong Province(No.ts201712045)。
文摘A 2 D-2 D titanium dioxide nanosheet-reduced graphene oxide(TNS-r GO)composite with better electronic conductivity and hydrophilicity was prepared by the hydrothermal method.The as-obtained TNS-r GO composite was further functionalized with 3-aminopropyltriethoxysilane(APTES)to provide a large amount of-NH2 groups on the surface for anchoring ultrafine Pd Ag alloy nanoparticles with an average particle size of 1.69 nm by a facile wet reduction approach.Benefiting from the combined effects of well-dispersed Pd Ag alloy nanoparticles,facilitated electron transfer from TNS-r GO to Pd,and increased electron density of active sites,the Pd8 Ag_(1)/NH_(2)-TNS-r GO catalyst exhibited excellent activity towards dehydrogenation of formic acid without adding any additives at 298 K,corresponding to an initial turn over frequency as high as 1090 h-1,which is much higher than that of most other state-of-theart catalysts.
基金the support of the“Transformational Technologies for Clean Energy and Demonstration”,Strategic Priority Research Program of the Chinese Academy of Sciences(XDA 21090203)the National Natural Science Foundation of China(22078315,22172169)+2 种基金the Youth Innovation Promotion Association of Chinese Academy of Sciences(2018214,2020189)the Liaoning Revitalization Talents Program(XLYC1907066)the Liaoning Bai Qian Wan Talents Program and DICP(Grant:DICP I202012)。
文摘Catalytic conversion of CO_(2) to high-value products is a crucial method to achieve targets of carbon dioxide emissions peak and carbon neutralization.However,realizing a controllable product distribution in a single CO_(2) hydrogenation process is of great challenge.Herein,we prepared the CuFe nanoalloy catalyst that directly transforms CO_(2) to alkanes using physical sputtering method in mild condition.The characteristic results show that the proximity between Cu and Fe is the crucial factor to tunable products among the different catalysts.The formation of unique coordination of FeCu4 nanoalloys from high-energy sputtering process provides close interaction between Cu and Fe,which is favorable to formation of low carbon paraffin,however,a distant proximity and weak interaction will increase the selectivity of olefins and alcohols.This work provides a general strategy for tuning target chemicals and enriches the viewpoints in CO_(2) hydrogenation.
基金supported by the National Key Technology R & D Program of China(No.2011BAD22B06)BP Company through the Clean Energy Facing the Future Program at Dalian Institute of Chemical Physics
文摘Direct synthesis of liquefied petroleum gas (LPG) from syngas was carried out over hybrid catalyst consisting of methanol synthesis catalyst and modified Y zeolite with Pd and Ca by different methods. The decrease of CO conversion was mostly attributable to the sintering of Cu in methanol synthesis catalyst. On the other hand, coke deposition on Y zeolite was the reason for the decrease of LPG selectivity. The introduction of Ca decreased the strong acid sites of Y zeolite, suppressed coke formation, and thus improved the stability of hybrid catalyst.
基金financially supported by the National Natural Science Foundation of China(21503215)
文摘A sustainable strategy for Fischer–Tropsch iron catalysts is successfully achieved by embedding of synergistic promoters from a renewable resource, corncob. The iron-based catalysts, named as 'corncob-driven'catalysts, are composed of iron species supported on carbon as primary active components and various minerals(K, Mg, Ca, and Si, etc.) as promoters. The corncob-driven catalysts are facilely synthesized by a one-pot hydrothermal treatment under mild conditions. The characterization results indicate that the formation of iron carbides from humboldtine is clearly enhanced and the morphology of catalyst particles tends to be more regular microspheres after adding corncob. It is observed that the optimized corncob-driven catalyst exhibits a higher conversion than without promoters' catalyst in Fischer–Tropsch synthesis(ca. 73% vs. ca. 49%). More importantly, a synergistic effect exists in multiple promoters from corncob that can enhance heavy hydrocarbons selectivity and lower CO_2 selectivity, obviously different from the catalyst with promoters from chemicals. The proposed synthesis route of corncob-driven catalysts provides new strategies for the utilization of renewable resources and elimination of environmental pollutants from chemical promoters.