The microbial communities colonized on microplastics(MPs)have attracted widespread attention.However,few studies focused on the MPs impacts on mangrove ecosystems,particularly on bacterial communities.We investigated ...The microbial communities colonized on microplastics(MPs)have attracted widespread attention.However,few studies focused on the MPs impacts on mangrove ecosystems,particularly on bacterial communities.We investigated the MPs pollution in mangrove of Zhujiang(Pearl)River estuary(ZRE).To study the potential risk posed by MPs to the mangrove ecosystems,the differences in bacterial communities,functions,and complexity between MPs and sediment samples were reported for the first time.Microplastics(2991±1586 items/kg dry weight(dw))in sediment were mainly fibers and polyethylene,mostly transparent,and in size less than 0.5 mm.Bacterial communities and functions significantly differed from MPs in mangrove sediment.Compared with sediment,MPs significantly enriched members of Proteobacteria,Bacteroidetes,and Actinobacteria,as well as the bacteria associated with plastic-degrading and human diseases on their surface,suggesting that microbial communities on MPs may promote MPs degradation and the spread of diseases,posing potential risk to mangrove ecosystems and human health.Although bacteria on MPs exhibited a lower diversity,the co-occurrence network analysis indicated that network of bacteria colonized on MPs was bigger and more complex than those of mangrove sediment,illustrating that MPs can act as a distinct habitat in this special ecosystem.This study provides a new perspective for increasing our understanding of microplastic pollution in mangrove ecosystems.展开更多
The novel nickel-based catalysts with a nickel content of 12 wt% were prepared with the zirconia-alumina composite as the supports. The new carriers, ZrO2 improved alumina, were synthesized by three methods, i.e., imp...The novel nickel-based catalysts with a nickel content of 12 wt% were prepared with the zirconia-alumina composite as the supports. The new carriers, ZrO2 improved alumina, were synthesized by three methods, i.e., impregnation-precipitation, co-precipitation, and impregnation method. The catalytic properties of these catalysts were investigated in the methanation of carbon dioxide, and the samples were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscope (XPS), temperature-programmed reduction (TPR) and temperature-programmed desorption (TPD) techniques. The new catalysts showed higher catalytic activity and better stability than Ni/γ-Al2O3. Furthermore, as a support for new nickel catalyst, the ZrO2-Al2O3 composite prepared by the impregnation-precipitation method was more efficient than the other supports in the methanation of carbon dioxide. The highly dispersed zirconium oxide on the surface of γ-Al2O3 inhibited the formation of nickel aluminate-like phase, which was responsible for the better dispersion of Ni species and easier reduction of NiO species, leading to the enhanced catalytic performance of corresponding catalyst.展开更多
HNO 3 -pretreated CNTs were employed as supports, and a special ultrasound-assisted impregnation method was designed to prepare supported Cu-Co catalysts for higher-alcohol synthesis from syngas. The catalysts used in...HNO 3 -pretreated CNTs were employed as supports, and a special ultrasound-assisted impregnation method was designed to prepare supported Cu-Co catalysts for higher-alcohol synthesis from syngas. The catalysts used in this work were characterized by N 2 adsorption-desorption, TEM, XRD, H 2 -TPR, CO-TPD techniques. It was found that the pre-treatment procedure of CNTs remarkably promoted the catalytic properties of the Cu-Co/CNTs catalysts. For the Cu-Co catalyst supported on CNTs pre-treated by 68 wt% HNO 3 , some active components were introduced into the CNTs channels, their dispersions and the amount of strongly adsorbed CO-species were improved. The CO conversion and alcohol yield on the HNO 3 -pretreated Cu-Co/CNTs catalyst were increased by ～21% and ～69%, respectively, compared with those on the normal Cu-Co/CNTs catalyst.展开更多
The density functional theory was used to investigate the adsorption of CH_4 and H_2O on different rank coal surfaces.The coal rank is the dominant factor in affecting the adsorption capacity of coal.In order to bette...The density functional theory was used to investigate the adsorption of CH_4 and H_2O on different rank coal surfaces.The coal rank is the dominant factor in affecting the adsorption capacity of coal.In order to better understand gas and water interaction with coal of different maturity,we developed fourteen coal models to represent the different rank coal.The interactions of CH_4 and H_2O with coal surfaces were studied and characterized by their adsorption energies,Mulliken charges and electrostatic potential surfaces.The results revealed that the interaction between coal and CH_4 was weak physical adsorption,and that the interaction between coal and H_2 O consisted of physical and chemical adsorption.Adsorption energy of coal–H_2O system was larger than that of coal–CH_4 on all rank coals,suggesting that the adsorption priority in the coal models is H_2 O > CH_4.Consequently,the injection of H_2 O into the different rank coal could effectively enhance the coal bed methane(CBM) recovery.展开更多
Through our newly-developed "chemical vapor deposition integrated process (CVD-IP)" using carbon dioxide (CO2) as the raw material and only carbon source introduced, CO2 could be catalytically activated and ...Through our newly-developed "chemical vapor deposition integrated process (CVD-IP)" using carbon dioxide (CO2) as the raw material and only carbon source introduced, CO2 could be catalytically activated and converted to a new solid-form product, i.e., carbon nanotubes (CO2-derived) at a quite high yield (the single-pass carbon yield in the solid-form carbon-product produced from CO2 catalytic capture and conversion was more than 30% at a single-pass carbon-base). For comparison, when only pure carbon dioxide was introduced using the conventional CVD method without integrated process, no solid-form carbon-material product could be formed. In the addition of saturated steam at room temperature in the feed for CVD, there were much more end-opening carbon nano-tubes produced, at a slightly higher carbon yield. These inspiring works opened a remarkable and alternative new approach for carbon dioxide catalytic capture to solid-form product, comparing with that of CO2 sequestration (CCS) or CO2 mineralization (solidification), etc. As a result, there was much less body volume and almost no greenhouse effect for this solid-form carbon-material than those of primitive carbon dioxide.展开更多
The Co-incorporated Ce1-xZrxO2 catalysts were prepared by co-precipitation for carbon dioxide reforming of methane.The ratio of Ce to Zr was varied to optimize the performances of co-precipitated Co-Ce-Zr-Ox catalysts...The Co-incorporated Ce1-xZrxO2 catalysts were prepared by co-precipitation for carbon dioxide reforming of methane.The ratio of Ce to Zr was varied to optimize the performances of co-precipitated Co-Ce-Zr-Ox catalysts.The prepared catalysts were characterized by various physico-chemical characterization techniques including TPR,X-ray diffraction,N2 adsorption at low temperature,XPS and CO2-TPSR.The co-precipitated Co-Ce0.8Zr0.2O2 sample containing 16% CoO exhibited a higher catalytic activity among the five catalysts,and the activity was maintained without significant loss during the reaction for 60 h.Under the conditions of 750 ℃,0.1 MPa,36000 ml/(h gcat),and CO2/CH4 molar ratio of 1:1,the CO2 conversion over this catalyst was 75% while the CH4 conversion was 67%.The cubic Ce0.8Zr0.2O2 facilitated a higher dispersion and a higher reducibility of the cobalt component,and the apparent activation energy for Co-Ce0.8Zr0.2O2 sample was 49.1 kJ/mol in the CO2/CH4 reforming reaction.As a result,the Co-Ce0.8Zr0.2O2 sample exhibited a higher activity and stability for the reforming of CH4 with CO2.展开更多
The effects of CeO2 contents and silica carrier porosity with their pore diameters ranging from 5.2 nm to 12.5 nm of CuO-CeO2/SiO2 cata-lysts in CO oxidation were investigated.The catalysts were characterized by N2 ad...The effects of CeO2 contents and silica carrier porosity with their pore diameters ranging from 5.2 nm to 12.5 nm of CuO-CeO2/SiO2 cata-lysts in CO oxidation were investigated.The catalysts were characterized by N2 adsorption/desorption at low temperature,X-ray diffraction (XRD),temperature-programmed reduction by H2 (H2-TPR),oxygen temperature programmed desorption (O2-TPD) and X-ray photoelectron spectroscopy (XPS).The results suggested that,the ceria content and the porosity of SiO2 carrier possessed great impacts on the structures and catalytic performances of CuO-CeO2/SiO2 catalysts.When appropriate content of CeO2 (Ce content 8 wt%) was added,the catalytic activity was greatly enhanced.In the catalyst supported on silica carrier with larger pore diameter,higher dispersion of CuO was observed,better agglomeration-resistant capacity was displayed and more lattice oxygen could be found,thus the CuO-CeO2 supported on Si-1 showed higher catalytic activity for low-temperature CO oxidation.展开更多
The over-consumption of fossil fuels resulted in the large quantity emission of carbon dioxide(CO2), which was the main reason for the climate change and more extreme weathers. Hence, it is extremely pressing to explo...The over-consumption of fossil fuels resulted in the large quantity emission of carbon dioxide(CO2), which was the main reason for the climate change and more extreme weathers. Hence, it is extremely pressing to explore efficient and sustainable approaches for the carbon-neutral pathway of CO2 utilization and recycling. In our recent works with this context, we developed successfully a novel "chemical vapor deposition integrated process(CVD-IP)" technology to converting robustly CO2 into the value-added solid-form carbon materials.The monometallic Fe Ni0–Al2O3(FNi0) and bimetallic Fe Nix–Al2O3(FNi2, FNi4, FNi8 and FNi20) samples were synthesized and effective for this new approach. The catalyst labeled FNi8 gave the better performance, exhibited the single pass solid carbon yield of 30%. These results illustrated alternative promising cases for the CO2 capture utilization storage(CCUS), by means of the CO2 catalytic conversion into the solid-form nano carbon materials.展开更多
Doping effects of manganese(Mn) on catalytic performance and structure evolution of Ni Mg O catalysts for synthesis of multi-walled carbon nanotubes(MWCNTs) from methane were investigated for the first time. Addition ...Doping effects of manganese(Mn) on catalytic performance and structure evolution of Ni Mg O catalysts for synthesis of multi-walled carbon nanotubes(MWCNTs) from methane were investigated for the first time. Addition of Mn in Ni Mg O catalyst can greatly improve the MWCNTs yield. Mn0.2Ni Mg O catalyst among the tested ones gives the highest MWCNTs yield as 2244%, which is two times higher than that of the catalyst without Mn. The structure evolution, reduction behaviors and surface chemical properties of Mn Ni Mg O catalysts with various Mn contents were studied in detail. It was found that the stable solid solution of Ni Mg O2 formed in Ni Mg O catalyst was disturbed by the addition of Mn. Instead, another solid solution of Mn Mg6O8 is formed. More amount of Ni can be reduced and dispersed on the catalyst surface to be acted as active sites. Importantly, the changes of Ni content on the surface are correlated with the Ni particle size and the outer diameter of MWCNTs, suggesting the controllable synthesis of MWCNTs over Mn Ni Mg O catalysts.展开更多
Copper-promoted nickel-based metal nanoparticles(NPs) with high dispersion and good thermal stability were derived from layered-double hydroxides(LDHs) precursors that were facilely developed by a coprecipitation stra...Copper-promoted nickel-based metal nanoparticles(NPs) with high dispersion and good thermal stability were derived from layered-double hydroxides(LDHs) precursors that were facilely developed by a coprecipitation strategy.The copper-promoted Ni-based metal NPs catalysts were investigated for methane reforming with carbon dioxide to hydrogen and syngas.A series of characterization techniques including XRD,N_2 adsorption and desorption,H_2-TPR,XPS,CO_2-TPD,TEM,TGA and in situ CH_4-TPSR were utilized to determine the structure-function relationship for the obtained catalysts.The copper addition accelerated the catalyst reducibility as well as the methane activation,and made the Ni species form smaller NPs during both preparation and reaction by restricting the aggregation.However,with higher copper loading,the derived catalysts were less active during methane reforming with CO_2 to syngas.It was confirmed that the catalyst with 1 wt%Cu additive gave the higher catalytic activity and remained stable during long time reaction with excellent resistance to coking and to sintering.Furthermore,the mean size of metal NPs changed minimally from 6.6 to 7.9 nm even after 80 h of time on stream at temperature as high as700℃ for this optimized catalyst.Therefore,this high dispersed anti-coking copper-promoted nickel catalyst derived from LDHs precursor could be prospective catalyst candidate for the efficient heterogeneous catalysis of sustainable CO_2 conversion.展开更多
The catalytic performances of Co3O4/SiO2 catalysts prepared by incipient wetness impregnation for CO oxidation were investigated using three kinds of silica as carriers with different pore sizes of 7.7,14.0 and 27.0 n...The catalytic performances of Co3O4/SiO2 catalysts prepared by incipient wetness impregnation for CO oxidation were investigated using three kinds of silica as carriers with different pore sizes of 7.7,14.0 and 27.0 nm.The effects of calcination temperature on the catalyst surface and micro structure properties as well as catalytic performance for the oxidation of carbon monoxide were also studied.All catalysts were characterized by N2 adsorption-desorption,XRD,XPS,FTIR,H2-TPR and O2-TPD.It was found that the properties and crystal size of cobalt-containing species strongly depended on the pore size of silica carrier.While the silica pore size increased from 7.7 to 27.0 nm,the Co3O4 crystal size increased from 8.5 to 13.5 nm.Moreover,it was demonstrated that if the spinel crystal structure of Co3O4 was obtained at a calcination temperature as low as 150℃,the catalyst sample would have a high Co3O4 surface dispersion and an increase of surface active species,and thus exhibit a high activity for the oxidation of carbon monoxide.展开更多
In this work, a series of Ni-Mo-Mg-O catalysts with mesoporous structure prepared by sol-gel method were investigated for the oxidative dehydrogenation of propane (ODHP). The techniques of temperature-programmed reduc...In this work, a series of Ni-Mo-Mg-O catalysts with mesoporous structure prepared by sol-gel method were investigated for the oxidative dehydrogenation of propane (ODHP). The techniques of temperature-programmed reduction with H2 (H2-TPR), N2 adsorption-desorption, Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD) and X-ray photoelectron spectra (XPS) were employed for catalyst characterization. It is found that the activity of the catalysts for ODHP increases first and then decreases with the increase of Mo content. The catalyst with a Mo/Ni atomic ratio of 1/1 exhibits the best catalytic activity, which gives the propene selectivity of 81.4% at a propane conversion of 11.3% under 600°C and maintains the good catalytic performance for 22 h on stream. This is related not only to its high reducibility and dispersion as revealed by TPR and XRD, but also to the formation of more selective oxygen species on the MoOx-NiO interface as identified by XPS.展开更多
基金Supported by the National Natural Science Foundation of China(Nos.42177253,41807476,41706186)Natural Science Foundation of Guangdong Province,China(No.2022A1515010197)。
文摘The microbial communities colonized on microplastics(MPs)have attracted widespread attention.However,few studies focused on the MPs impacts on mangrove ecosystems,particularly on bacterial communities.We investigated the MPs pollution in mangrove of Zhujiang(Pearl)River estuary(ZRE).To study the potential risk posed by MPs to the mangrove ecosystems,the differences in bacterial communities,functions,and complexity between MPs and sediment samples were reported for the first time.Microplastics(2991±1586 items/kg dry weight(dw))in sediment were mainly fibers and polyethylene,mostly transparent,and in size less than 0.5 mm.Bacterial communities and functions significantly differed from MPs in mangrove sediment.Compared with sediment,MPs significantly enriched members of Proteobacteria,Bacteroidetes,and Actinobacteria,as well as the bacteria associated with plastic-degrading and human diseases on their surface,suggesting that microbial communities on MPs may promote MPs degradation and the spread of diseases,posing potential risk to mangrove ecosystems and human health.Although bacteria on MPs exhibited a lower diversity,the co-occurrence network analysis indicated that network of bacteria colonized on MPs was bigger and more complex than those of mangrove sediment,illustrating that MPs can act as a distinct habitat in this special ecosystem.This study provides a new perspective for increasing our understanding of microplastic pollution in mangrove ecosystems.
基金supported by the Science & Technology Support Plan Projects of Sichuan Province (2016GZ0371)National Natural Science Foun-dation of China (NNSFC,21476145,21506111)~~
基金supported by the Southwest Research & Design Institute of Chemical Industy (SKLIV GR-22010-01)the National Basic Research Program of China (973 Program, 2011CB201202) of Ministry of Science and Technology
文摘The novel nickel-based catalysts with a nickel content of 12 wt% were prepared with the zirconia-alumina composite as the supports. The new carriers, ZrO2 improved alumina, were synthesized by three methods, i.e., impregnation-precipitation, co-precipitation, and impregnation method. The catalytic properties of these catalysts were investigated in the methanation of carbon dioxide, and the samples were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscope (XPS), temperature-programmed reduction (TPR) and temperature-programmed desorption (TPD) techniques. The new catalysts showed higher catalytic activity and better stability than Ni/γ-Al2O3. Furthermore, as a support for new nickel catalyst, the ZrO2-Al2O3 composite prepared by the impregnation-precipitation method was more efficient than the other supports in the methanation of carbon dioxide. The highly dispersed zirconium oxide on the surface of γ-Al2O3 inhibited the formation of nickel aluminate-like phase, which was responsible for the better dispersion of Ni species and easier reduction of NiO species, leading to the enhanced catalytic performance of corresponding catalyst.
基金supported by the Foundation of Shaanxi Educational Committee (2010JK608)the Research Foundation of XATU (204-000092)supported by the National Natural Science Foundation of China (205903603)
文摘HNO 3 -pretreated CNTs were employed as supports, and a special ultrasound-assisted impregnation method was designed to prepare supported Cu-Co catalysts for higher-alcohol synthesis from syngas. The catalysts used in this work were characterized by N 2 adsorption-desorption, TEM, XRD, H 2 -TPR, CO-TPD techniques. It was found that the pre-treatment procedure of CNTs remarkably promoted the catalytic properties of the Cu-Co/CNTs catalysts. For the Cu-Co catalyst supported on CNTs pre-treated by 68 wt% HNO 3 , some active components were introduced into the CNTs channels, their dispersions and the amount of strongly adsorbed CO-species were improved. The CO conversion and alcohol yield on the HNO 3 -pretreated Cu-Co/CNTs catalyst were increased by ～21% and ～69%, respectively, compared with those on the normal Cu-Co/CNTs catalyst.
基金financially supported by the National Natural Science Foundation of China(21476145)the National 973 Program of Ministry of Sciences and Technologies of China(2011CB201202)
文摘The density functional theory was used to investigate the adsorption of CH_4 and H_2O on different rank coal surfaces.The coal rank is the dominant factor in affecting the adsorption capacity of coal.In order to better understand gas and water interaction with coal of different maturity,we developed fourteen coal models to represent the different rank coal.The interactions of CH_4 and H_2O with coal surfaces were studied and characterized by their adsorption energies,Mulliken charges and electrostatic potential surfaces.The results revealed that the interaction between coal and CH_4 was weak physical adsorption,and that the interaction between coal and H_2 O consisted of physical and chemical adsorption.Adsorption energy of coal–H_2O system was larger than that of coal–CH_4 on all rank coals,suggesting that the adsorption priority in the coal models is H_2 O > CH_4.Consequently,the injection of H_2 O into the different rank coal could effectively enhance the coal bed methane(CBM) recovery.
基金the National 973 Program of Ministry of Sciences and Technologies of China(2011CB201202)the National Natural Science Foundation of China(20776089)
文摘Through our newly-developed "chemical vapor deposition integrated process (CVD-IP)" using carbon dioxide (CO2) as the raw material and only carbon source introduced, CO2 could be catalytically activated and converted to a new solid-form product, i.e., carbon nanotubes (CO2-derived) at a quite high yield (the single-pass carbon yield in the solid-form carbon-product produced from CO2 catalytic capture and conversion was more than 30% at a single-pass carbon-base). For comparison, when only pure carbon dioxide was introduced using the conventional CVD method without integrated process, no solid-form carbon-material product could be formed. In the addition of saturated steam at room temperature in the feed for CVD, there were much more end-opening carbon nano-tubes produced, at a slightly higher carbon yield. These inspiring works opened a remarkable and alternative new approach for carbon dioxide catalytic capture to solid-form product, comparing with that of CO2 sequestration (CCS) or CO2 mineralization (solidification), etc. As a result, there was much less body volume and almost no greenhouse effect for this solid-form carbon-material than those of primitive carbon dioxide.
文摘The Co-incorporated Ce1-xZrxO2 catalysts were prepared by co-precipitation for carbon dioxide reforming of methane.The ratio of Ce to Zr was varied to optimize the performances of co-precipitated Co-Ce-Zr-Ox catalysts.The prepared catalysts were characterized by various physico-chemical characterization techniques including TPR,X-ray diffraction,N2 adsorption at low temperature,XPS and CO2-TPSR.The co-precipitated Co-Ce0.8Zr0.2O2 sample containing 16% CoO exhibited a higher catalytic activity among the five catalysts,and the activity was maintained without significant loss during the reaction for 60 h.Under the conditions of 750 ℃,0.1 MPa,36000 ml/(h gcat),and CO2/CH4 molar ratio of 1:1,the CO2 conversion over this catalyst was 75% while the CH4 conversion was 67%.The cubic Ce0.8Zr0.2O2 facilitated a higher dispersion and a higher reducibility of the cobalt component,and the apparent activation energy for Co-Ce0.8Zr0.2O2 sample was 49.1 kJ/mol in the CO2/CH4 reforming reaction.As a result,the Co-Ce0.8Zr0.2O2 sample exhibited a higher activity and stability for the reforming of CH4 with CO2.
基金supported by the National Natural Science Foundation of China(20590360)New Century Excellent Talent Project of China(NCET-05-0783)
文摘The effects of CeO2 contents and silica carrier porosity with their pore diameters ranging from 5.2 nm to 12.5 nm of CuO-CeO2/SiO2 cata-lysts in CO oxidation were investigated.The catalysts were characterized by N2 adsorption/desorption at low temperature,X-ray diffraction (XRD),temperature-programmed reduction by H2 (H2-TPR),oxygen temperature programmed desorption (O2-TPD) and X-ray photoelectron spectroscopy (XPS).The results suggested that,the ceria content and the porosity of SiO2 carrier possessed great impacts on the structures and catalytic performances of CuO-CeO2/SiO2 catalysts.When appropriate content of CeO2 (Ce content 8 wt%) was added,the catalytic activity was greatly enhanced.In the catalyst supported on silica carrier with larger pore diameter,higher dispersion of CuO was observed,better agglomeration-resistant capacity was displayed and more lattice oxygen could be found,thus the CuO-CeO2 supported on Si-1 showed higher catalytic activity for low-temperature CO oxidation.
基金support for this project from the National Natural Science Foundation of China (21476145)the National 973 Program of Ministry of Sciences and Technologies of China (2011CB201202)
文摘The over-consumption of fossil fuels resulted in the large quantity emission of carbon dioxide(CO2), which was the main reason for the climate change and more extreme weathers. Hence, it is extremely pressing to explore efficient and sustainable approaches for the carbon-neutral pathway of CO2 utilization and recycling. In our recent works with this context, we developed successfully a novel "chemical vapor deposition integrated process(CVD-IP)" technology to converting robustly CO2 into the value-added solid-form carbon materials.The monometallic Fe Ni0–Al2O3(FNi0) and bimetallic Fe Nix–Al2O3(FNi2, FNi4, FNi8 and FNi20) samples were synthesized and effective for this new approach. The catalyst labeled FNi8 gave the better performance, exhibited the single pass solid carbon yield of 30%. These results illustrated alternative promising cases for the CO2 capture utilization storage(CCUS), by means of the CO2 catalytic conversion into the solid-form nano carbon materials.
基金supported by the National Natural Science Foundation of China(20776089)the Fundamental Research Funds for the Central Universities(2014NZYQN20)
文摘Doping effects of manganese(Mn) on catalytic performance and structure evolution of Ni Mg O catalysts for synthesis of multi-walled carbon nanotubes(MWCNTs) from methane were investigated for the first time. Addition of Mn in Ni Mg O catalyst can greatly improve the MWCNTs yield. Mn0.2Ni Mg O catalyst among the tested ones gives the highest MWCNTs yield as 2244%, which is two times higher than that of the catalyst without Mn. The structure evolution, reduction behaviors and surface chemical properties of Mn Ni Mg O catalysts with various Mn contents were studied in detail. It was found that the stable solid solution of Ni Mg O2 formed in Ni Mg O catalyst was disturbed by the addition of Mn. Instead, another solid solution of Mn Mg6O8 is formed. More amount of Ni can be reduced and dispersed on the catalyst surface to be acted as active sites. Importantly, the changes of Ni content on the surface are correlated with the Ni particle size and the outer diameter of MWCNTs, suggesting the controllable synthesis of MWCNTs over Mn Ni Mg O catalysts.
基金supported by the Natural Science Foundation of China (21476145)the National Basic Research Program of China (973 Program,2011CB201202)
文摘Copper-promoted nickel-based metal nanoparticles(NPs) with high dispersion and good thermal stability were derived from layered-double hydroxides(LDHs) precursors that were facilely developed by a coprecipitation strategy.The copper-promoted Ni-based metal NPs catalysts were investigated for methane reforming with carbon dioxide to hydrogen and syngas.A series of characterization techniques including XRD,N_2 adsorption and desorption,H_2-TPR,XPS,CO_2-TPD,TEM,TGA and in situ CH_4-TPSR were utilized to determine the structure-function relationship for the obtained catalysts.The copper addition accelerated the catalyst reducibility as well as the methane activation,and made the Ni species form smaller NPs during both preparation and reaction by restricting the aggregation.However,with higher copper loading,the derived catalysts were less active during methane reforming with CO_2 to syngas.It was confirmed that the catalyst with 1 wt%Cu additive gave the higher catalytic activity and remained stable during long time reaction with excellent resistance to coking and to sintering.Furthermore,the mean size of metal NPs changed minimally from 6.6 to 7.9 nm even after 80 h of time on stream at temperature as high as700℃ for this optimized catalyst.Therefore,this high dispersed anti-coking copper-promoted nickel catalyst derived from LDHs precursor could be prospective catalyst candidate for the efficient heterogeneous catalysis of sustainable CO_2 conversion.
基金supported by the National Natural Science Foundation of China(NSFC 20776089)the 985 Project of Sichuan University
文摘The catalytic performances of Co3O4/SiO2 catalysts prepared by incipient wetness impregnation for CO oxidation were investigated using three kinds of silica as carriers with different pore sizes of 7.7,14.0 and 27.0 nm.The effects of calcination temperature on the catalyst surface and micro structure properties as well as catalytic performance for the oxidation of carbon monoxide were also studied.All catalysts were characterized by N2 adsorption-desorption,XRD,XPS,FTIR,H2-TPR and O2-TPD.It was found that the properties and crystal size of cobalt-containing species strongly depended on the pore size of silica carrier.While the silica pore size increased from 7.7 to 27.0 nm,the Co3O4 crystal size increased from 8.5 to 13.5 nm.Moreover,it was demonstrated that if the spinel crystal structure of Co3O4 was obtained at a calcination temperature as low as 150℃,the catalyst sample would have a high Co3O4 surface dispersion and an increase of surface active species,and thus exhibit a high activity for the oxidation of carbon monoxide.
基金supported by the National Natural Science Foundation of China (20776089)the New Century Excellent Talent Project of China(NCET-05-0783)
文摘In this work, a series of Ni-Mo-Mg-O catalysts with mesoporous structure prepared by sol-gel method were investigated for the oxidative dehydrogenation of propane (ODHP). The techniques of temperature-programmed reduction with H2 (H2-TPR), N2 adsorption-desorption, Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD) and X-ray photoelectron spectra (XPS) were employed for catalyst characterization. It is found that the activity of the catalysts for ODHP increases first and then decreases with the increase of Mo content. The catalyst with a Mo/Ni atomic ratio of 1/1 exhibits the best catalytic activity, which gives the propene selectivity of 81.4% at a propane conversion of 11.3% under 600°C and maintains the good catalytic performance for 22 h on stream. This is related not only to its high reducibility and dispersion as revealed by TPR and XRD, but also to the formation of more selective oxygen species on the MoOx-NiO interface as identified by XPS.
