An activated carbon pore-expanding technique was achieved through innovative reactivation by CO_2/microwave.The original and modified activated carbons were characterized by nitrogen adsorption–desorption,scanning el...An activated carbon pore-expanding technique was achieved through innovative reactivation by CO_2/microwave.The original and modified activated carbons were characterized by nitrogen adsorption–desorption,scanning electron microscopy,transmission electron microcopy,and Fourier transform infrared spectroscopy.The mesopore volume increased from 0.122 cm^3·g^(-1) to 0.270 cm^3·g^(-1),and a hierarchical pore structure was formed.A gradual decrease in the phenolic hydroxyl and carboxyl groups on the surface of activated carbon enhanced the surface inertia of granular activated carbon(GAC).The toluene desorption rate of the modified sample increased by 8.81% compared with that of the original GAC.Adsorption isotherm fittings revealed that the Langmuir model was applicable for the original and modified activated carbons.The isosteric adsorption heat of toluene on the activated carbon decreased by approximately 50%,which endowed the modified sample with excellent stability in application.The modified samples showed an enhanced desorption performance of toluene,thereby opening a way to extend the cycle life and improve the economic performance of carbon adsorbent in practical engineering applications.展开更多
The CO2reforming of CH4is studied over MgO‐promoted Ni catalysts,which were supported on alumina prepared from hydrotalcite.This presents an improved stability compared with non‐promoted catalysts.The introduction o...The CO2reforming of CH4is studied over MgO‐promoted Ni catalysts,which were supported on alumina prepared from hydrotalcite.This presents an improved stability compared with non‐promoted catalysts.The introduction of the MgO promoter was achieved through the‘‘memory effect’’of the Ni‐Al hydrotalcite structure,and ICP‐MS confirmed that only0.42wt.%of Mg2+ions were added into the Ni‐Mg/Al catalyst.Although no differences in the Ni particle size and basicity strength were observed,the Ni‐Mg/Al catalyst showed a higher catalytic stability than the Ni/Al catalyst.A series of surface reaction experiments were used and showed that the addition of a MgO promoter with low concentration can promote CO2dissociation to form active surface oxygen arising from the formation of the Ni‐MgO interface sites.Therefore,the carbon‐resistance promotion by nature was suggested to contribute to an oxidative environment around Ni particles,which would increase the conversion of carbon residues from CH4cracking to yield CO on the Ni metal surface.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved.展开更多
In this work, the effects of different methods of activation on CO2 adsorption performance of activated carbon were studied. Activated carbons were prepared from biochar, obtained from fast pyrolysis of white wood, us...In this work, the effects of different methods of activation on CO2 adsorption performance of activated carbon were studied. Activated carbons were prepared from biochar, obtained from fast pyrolysis of white wood, using three different activation methods of steam activation, CO2 activation and Potassium hydroxide(KOH) activation. CO2 adsorption behavior of the produced activated carbons was studied in a fixed-bed reactor set-up at atmospheric pressure, temperature range of 25–65°C and inlet CO2 concentration range of10–30 mol% in He to determine the effects of the surface area, porosity and surface chemistry on adsorption capacity of the samples. Characterization of the micropore and mesopore texture was carried out using N2 and CO2 adsorption at 77 and 273 K, respectively.Central composite design was used to evaluate the combined effects of temperature and concentration of CO2 on the adsorption behavior of the adsorbents. The KOH activated carbon with a total micropore volume of 0.62 cm3/g and surface area of 1400 m2/g had the highest CO2 adsorption capacity of 1.8 mol/kg due to its microporous structure and high surface area under the optimized experimental conditions of 30 mol% CO2 and 25°C. The performance of the adsorbents in multi-cyclic adsorption process was also assessed and the adsorption capacity of KOH and CO2 activated carbons remained remarkably stable after50 cycles with low temperature(160°C) regeneration.展开更多
Variations in soil organic matter accumulation across an elevation can be used to explain the control of substrate supply and variability on soil metabolic activity. We investigated geographic changes in soil organic ...Variations in soil organic matter accumulation across an elevation can be used to explain the control of substrate supply and variability on soil metabolic activity. We investigated geographic changes in soil organic matter and metabolic rates along an elevation gradient(289–2,489 m) in the Santa Rosa Mountains, California, USA from subalpine and montane pine forests through chaparral to desert. From base(289 m) to summit(2,489 m), 24 sites were established for collecting soil samples under canopies and inter-canopy spaces, at 0–5 and 5–15 cm soil depths increments. Soil organic matter(SOM) content was determined using weight loss on ignition at 550°C and soil CO2 efflux(R) was measured at day 5(R5) and day 20(R20) of incubation. Changes in SOM content along the elevation gradient showed a significant relationship(P〈0.05) but R5 and R20 were not related to either elevation or SOM content. However, the ratio of R and SOM(R5/SOM) showed a strong relationship across the mountains at both soil depths. R5/SOM, as an indicator of carbon use efficiency, may be applicable to other semi-arid transects at larger scale modeling of soil metabolic processes.展开更多
The hydrogenation of carbon dioxide(CO2)is one of important processes to effectively convert and utilize CO2,which is also regarded as the key step at the industrial methanol synthesis.Water is likely to play an impor...The hydrogenation of carbon dioxide(CO2)is one of important processes to effectively convert and utilize CO2,which is also regarded as the key step at the industrial methanol synthesis.Water is likely to play an important role in this process,but it still remains elusive.To systematically understand its influence,here we computationally compare the reaction mechanisms of CO2 hydrogenation over the stepped Cu(211)surface between in the absence and presence of water based on microkinetic simulations upon density functional theory(DFT)calculations.The effects of water on each hydrogenation step and the whole activity and selectivity are checked and its physical origin is discussed.It is found that the water could kinetically accelerate the hydrogenation on CO2 to COOH,promoting the reverse water gas shift reaction to produce carbon monoxide(CO).It hardly influences the CO2 hydrogenation to methanol kinetically.In addition,the too high initial partial pressure of water will thermodynamically inhibit the CO2 conversion.展开更多
基金Supported by the National Natural Science Foundation of China(21506194,21676255)the Natural Science Foundation of Zhejiang Province(Y16B070025)the Commission of Science and Technology of Zhejiang Province(2013C03021,2017C33106)
文摘An activated carbon pore-expanding technique was achieved through innovative reactivation by CO_2/microwave.The original and modified activated carbons were characterized by nitrogen adsorption–desorption,scanning electron microscopy,transmission electron microcopy,and Fourier transform infrared spectroscopy.The mesopore volume increased from 0.122 cm^3·g^(-1) to 0.270 cm^3·g^(-1),and a hierarchical pore structure was formed.A gradual decrease in the phenolic hydroxyl and carboxyl groups on the surface of activated carbon enhanced the surface inertia of granular activated carbon(GAC).The toluene desorption rate of the modified sample increased by 8.81% compared with that of the original GAC.Adsorption isotherm fittings revealed that the Langmuir model was applicable for the original and modified activated carbons.The isosteric adsorption heat of toluene on the activated carbon decreased by approximately 50%,which endowed the modified sample with excellent stability in application.The modified samples showed an enhanced desorption performance of toluene,thereby opening a way to extend the cycle life and improve the economic performance of carbon adsorbent in practical engineering applications.
基金supported by the National Natural Science Fundation of China(U1361202,51276120)~~
文摘The CO2reforming of CH4is studied over MgO‐promoted Ni catalysts,which were supported on alumina prepared from hydrotalcite.This presents an improved stability compared with non‐promoted catalysts.The introduction of the MgO promoter was achieved through the‘‘memory effect’’of the Ni‐Al hydrotalcite structure,and ICP‐MS confirmed that only0.42wt.%of Mg2+ions were added into the Ni‐Mg/Al catalyst.Although no differences in the Ni particle size and basicity strength were observed,the Ni‐Mg/Al catalyst showed a higher catalytic stability than the Ni/Al catalyst.A series of surface reaction experiments were used and showed that the addition of a MgO promoter with low concentration can promote CO2dissociation to form active surface oxygen arising from the formation of the Ni‐MgO interface sites.Therefore,the carbon‐resistance promotion by nature was suggested to contribute to an oxidative environment around Ni particles,which would increase the conversion of carbon residues from CH4cracking to yield CO on the Ni metal surface.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved.
基金Funding for this research is provided by Natural Sciences and Engineering Research Council (NSERC) of Canada
文摘In this work, the effects of different methods of activation on CO2 adsorption performance of activated carbon were studied. Activated carbons were prepared from biochar, obtained from fast pyrolysis of white wood, using three different activation methods of steam activation, CO2 activation and Potassium hydroxide(KOH) activation. CO2 adsorption behavior of the produced activated carbons was studied in a fixed-bed reactor set-up at atmospheric pressure, temperature range of 25–65°C and inlet CO2 concentration range of10–30 mol% in He to determine the effects of the surface area, porosity and surface chemistry on adsorption capacity of the samples. Characterization of the micropore and mesopore texture was carried out using N2 and CO2 adsorption at 77 and 273 K, respectively.Central composite design was used to evaluate the combined effects of temperature and concentration of CO2 on the adsorption behavior of the adsorbents. The KOH activated carbon with a total micropore volume of 0.62 cm3/g and surface area of 1400 m2/g had the highest CO2 adsorption capacity of 1.8 mol/kg due to its microporous structure and high surface area under the optimized experimental conditions of 30 mol% CO2 and 25°C. The performance of the adsorbents in multi-cyclic adsorption process was also assessed and the adsorption capacity of KOH and CO2 activated carbons remained remarkably stable after50 cycles with low temperature(160°C) regeneration.
文摘Variations in soil organic matter accumulation across an elevation can be used to explain the control of substrate supply and variability on soil metabolic activity. We investigated geographic changes in soil organic matter and metabolic rates along an elevation gradient(289–2,489 m) in the Santa Rosa Mountains, California, USA from subalpine and montane pine forests through chaparral to desert. From base(289 m) to summit(2,489 m), 24 sites were established for collecting soil samples under canopies and inter-canopy spaces, at 0–5 and 5–15 cm soil depths increments. Soil organic matter(SOM) content was determined using weight loss on ignition at 550°C and soil CO2 efflux(R) was measured at day 5(R5) and day 20(R20) of incubation. Changes in SOM content along the elevation gradient showed a significant relationship(P〈0.05) but R5 and R20 were not related to either elevation or SOM content. However, the ratio of R and SOM(R5/SOM) showed a strong relationship across the mountains at both soil depths. R5/SOM, as an indicator of carbon use efficiency, may be applicable to other semi-arid transects at larger scale modeling of soil metabolic processes.
基金supported by the National Key Research and Development Program of China(2018YFA0208600)the National Natural Science Foundation of China(21673072,21333003,91845111)Program of Shanghai Subject Chief Scientist(17XD1401400)
文摘The hydrogenation of carbon dioxide(CO2)is one of important processes to effectively convert and utilize CO2,which is also regarded as the key step at the industrial methanol synthesis.Water is likely to play an important role in this process,but it still remains elusive.To systematically understand its influence,here we computationally compare the reaction mechanisms of CO2 hydrogenation over the stepped Cu(211)surface between in the absence and presence of water based on microkinetic simulations upon density functional theory(DFT)calculations.The effects of water on each hydrogenation step and the whole activity and selectivity are checked and its physical origin is discussed.It is found that the water could kinetically accelerate the hydrogenation on CO2 to COOH,promoting the reverse water gas shift reaction to produce carbon monoxide(CO).It hardly influences the CO2 hydrogenation to methanol kinetically.In addition,the too high initial partial pressure of water will thermodynamically inhibit the CO2 conversion.