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
Molybdenum carbides are highly active for CO2 conversion to CO via the reverse water-gas shift(RWGS)reaction, however the large grain size up to micrometers renders its relatively lower active sites utilization effici...Molybdenum carbides are highly active for CO2 conversion to CO via the reverse water-gas shift(RWGS)reaction, however the large grain size up to micrometers renders its relatively lower active sites utilization efficiency while generating CH4 as a by-product. In this work, a homogeneously dispersed molybdenum carbide hybrid catalyst with sub-nanosized cluster(the average size as small as 0.5 nm) is prepared via a facile carbothermal treatment for highly selective CO2-CO reduction. The partially disordered Mo2C clusters are characterized by synchrotron high-resolution XRD and atomic resolution HAADF-STEM analysis, for which the source cause of the disorder is pinpointed by XAFS analysis to be the nitrogen intercalants from the carbonaceous precursor. The partially disordered Mo2C clusters show a RWGS rate as high as 184.4 μmol gMo2C-1s-1 at 400 ℃ with a superior selectivity toward CO(> 99.5%). This work 2 highlights a facile strategy for fabricating highly dispersed and partially disordered Mo2C clusters at a sub-nano size with beneficial N-doping for delivering high catalytic activity and operational stability.展开更多
Two type zirconia(monoclinic and tetragonal phase ZrO_2) carriers were synthesized via hydrothermal route,and nano-sized zirconia supported nickel catalysts were prepared by incipient impregnation then followed therma...Two type zirconia(monoclinic and tetragonal phase ZrO_2) carriers were synthesized via hydrothermal route,and nano-sized zirconia supported nickel catalysts were prepared by incipient impregnation then followed thermal treatment at 300℃ to 500℃,for the CO_2 selective hydrogenation to synthetic natural gas(SNG).The catalysts were characterized by XRD,CO_2-TPD-MS,XPS,TPSR(CH_4,CO_2) techniques.For comparison,the catalyst NZ-W-400(monoclinic) synthesized in water solvent exhibited a better catalytic activity than the catalyst NZ-M-400(tetragonal) prepared in methanol solvent.The catalyst NZ-W-400 displayed more H_2 absorbed sites,more basic sites and a lower temperature of initial CO_2 activation.Then,the thermal treatment of monoclinic ZrO_2 supported nickel precursor was manufactured at three temperature of 350,400,500℃.The TPSR experiments displayed that there were the lower temperature for CO_2 activation and initial conversion(185℃) as well as the lower peak temperature of CH_4 generation(318℃),for the catalyst calcined at 500℃.This sample contained the more basic sites and the higher catalytic activity,evidenced byCO_2-TPD-MS and performance measurement.As for the NZ-W-350 sample,which exhibited the less basic sites and the lower catalytic activity,its initial temperature for CO_2 activation and conversion was higher(214℃) as well as the higher peak temperature of CH_4 formation(382℃).展开更多
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the National Natural Science Foundation of China(21872144,21972140 and 91645117)Liaoning Revitalization Talents Program(XLYC1907053)+2 种基金CAS Youth Innovation Promotion Association(2018220)Talents Innovation Project of Dalian City(2017RQ032 and 2016RD04)China Postdoctoral Science Foundation(2019TQ0314,2018M641726 and 2019M661146)。
文摘Molybdenum carbides are highly active for CO2 conversion to CO via the reverse water-gas shift(RWGS)reaction, however the large grain size up to micrometers renders its relatively lower active sites utilization efficiency while generating CH4 as a by-product. In this work, a homogeneously dispersed molybdenum carbide hybrid catalyst with sub-nanosized cluster(the average size as small as 0.5 nm) is prepared via a facile carbothermal treatment for highly selective CO2-CO reduction. The partially disordered Mo2C clusters are characterized by synchrotron high-resolution XRD and atomic resolution HAADF-STEM analysis, for which the source cause of the disorder is pinpointed by XAFS analysis to be the nitrogen intercalants from the carbonaceous precursor. The partially disordered Mo2C clusters show a RWGS rate as high as 184.4 μmol gMo2C-1s-1 at 400 ℃ with a superior selectivity toward CO(> 99.5%). This work 2 highlights a facile strategy for fabricating highly dispersed and partially disordered Mo2C clusters at a sub-nano size with beneficial N-doping for delivering high catalytic activity and operational stability.
基金supported by National Natural Science Foundation of China (21476145)
文摘Two type zirconia(monoclinic and tetragonal phase ZrO_2) carriers were synthesized via hydrothermal route,and nano-sized zirconia supported nickel catalysts were prepared by incipient impregnation then followed thermal treatment at 300℃ to 500℃,for the CO_2 selective hydrogenation to synthetic natural gas(SNG).The catalysts were characterized by XRD,CO_2-TPD-MS,XPS,TPSR(CH_4,CO_2) techniques.For comparison,the catalyst NZ-W-400(monoclinic) synthesized in water solvent exhibited a better catalytic activity than the catalyst NZ-M-400(tetragonal) prepared in methanol solvent.The catalyst NZ-W-400 displayed more H_2 absorbed sites,more basic sites and a lower temperature of initial CO_2 activation.Then,the thermal treatment of monoclinic ZrO_2 supported nickel precursor was manufactured at three temperature of 350,400,500℃.The TPSR experiments displayed that there were the lower temperature for CO_2 activation and initial conversion(185℃) as well as the lower peak temperature of CH_4 generation(318℃),for the catalyst calcined at 500℃.This sample contained the more basic sites and the higher catalytic activity,evidenced byCO_2-TPD-MS and performance measurement.As for the NZ-W-350 sample,which exhibited the less basic sites and the lower catalytic activity,its initial temperature for CO_2 activation and conversion was higher(214℃) as well as the higher peak temperature of CH_4 formation(382℃).