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1.
This study reports an improved method for activating asphalt to produce ultra‐high surface area porous carbons. Pretreatment of asphalt (untreated Gilsonite, uGil ) at 400 °C for 3 h removes the more volatile organic compounds to form pretreated asphalt ( uGil‐P ) material with a larger fraction of higher molecular weight π‐conjugated asphaltenes. Subsequent activation of uGil‐P at 900 °C gives an ultra‐high surface area (4200 m2 g?1) porous carbon material ( uGil‐900 ) with a mixed micro and mesoporous structure. uGil‐900 shows enhanced room temperature CO2 uptake capacity at 54 bar of 154 wt% (35 mmol g?1). The CH4 uptake capacity is 37.5 wt% (24 mmol g?1) at 300 bar. These are relevant pressures in natural gas production. The room temperature working CO2 uptake capacity for uGil‐900 is 19.1 mmol g?1 (84 wt%) at 20 bar and 32.6 mmol g?1 (143 wt%) at 50 bar. In order to further assess the reliability of uGil‐900 for CO2 capture at elevated pressures, the authors study competitive sorption of CO2 and CH4 on uGil‐900 at pressures from 1 to 20 bar at 25 °C. CO2/CH4 displacement constants are measured at 2 to 40 bar, and found to increase significantly with pressure and surface area.  相似文献   

2.
Natural gas is the cleanest fossil fuel source. However, natural gas wells typically contain considerable amounts of CO2, with on‐site CO2 capture necessary. Solid sorbents are advantageous over traditional amine scrubbing due to their relatively low regeneration energies and non‐corrosive nature. However, it remains a challenge to improve the sorbent's CO2 capacity at elevated pressures relevant to natural gas purification. Here, the synthesis of porous carbons derived from a 3D hierarchical nanostructured polymer hydrogel, with simple and effective tunability over the pore size distribution is reported. The optimized surface area reaches 4196 m2 g?1, which is among the highest of carbon‐based materials, with abundant micro‐ and narrow mesopores (2.03 cm3 g?1 with d < 4 nm). This carbon exhibits a record‐high CO2 capacity among reported carbons at elevated pressure (i.e., 28.3 mmol g?1 total adsorption at 25 °C and 30 bar). This carbon also shows good CO2/CH4 selectivity and excellent cyclability. Molecular simulations suggest increased CO2 density in micro‐ and narrow mesopores at high pressures. This is consistent with the observation that these pores are mainly responsible for the material's high‐pressure CO2 capacity. This work provides insights into material design and further development for CO2 capture from natural gas.  相似文献   

3.
Active carbons have unique physicochemical properties, but their conductivities and surface to weight ratios are much poorer than graphene. A unique and facile method is innovated to chemically process biomass by “drilling” holes with H2O2 and exfoliating into graphene‐like nanosheets with HAc, followed by carbonization at a high temperature for highly graphitized activated carbon with greatly enhanced porosity, unique pore structure, high conductivity, and large surface area. This graphene‐like carbon exhibits extremely high specific capacitance (340 F g?1 at 0.5 A g?1) and high specific energy density (23.33 to 16.67 W h kg?1) with excellent rate capability and long cycling stability (remains 98% after 10 000 cycles), which is much superior to all reported carbons including graphene. Synthesis mechanism for deriving biomass into porous graphene‐like carbons is discussed in detail. The enhancement mechanism for the porous graphene‐like carbon electrode reveals that rationally designed meso‐ and macropores are very critical in porous electrode performance, which can network micropores for diffusion freeways, high conductivity, and high utilization. This work has universal significance in producing highly porous and conductive carbons from biomass including biowastes for various energy storage/conversion applications.  相似文献   

4.
Nanoporous carbons (NPCs) with engineered specific pore sizes and sufficiently high porosities (both specific surface area and pore volume) are necessary for storing energy in the form of electric charges and molecules. Herein, NPCs, derived from biomass pine‐cones, coffee‐grounds, graphene‐oxide and metal‐organic frameworks, with systematically increased pore width (<1.0 nm to a few nm), micropore volume (0.2–0.9 cm3 g?1) and specific surface area (800–2800 m2 g?1) are presented. Superior CO2, H2, and H2O uptakes of 35.0 wt% (≈7.9 mmol g?1 at 273 K), 3.0 wt% (at 77 K) and 85.0 wt% (at 298 K), respectively at 1 bar, are achieved. At controlled microporosity, supercapacitors deliver impressive performance with a capacity of 320 and 230 F g?1 at 500 mA g?1, in aqueous and organic electrolytes, respectively. Excellent areal capacitance and energy density (>50 Wh kg?1 at high power density, 1000 W kg?1) are achieved to form the highest reported values among the range of carbons in the literature. The noteworthy energy storage performance of the NPCs for all five cases (CO2, H2, H2O, and capacitance in aqueous and organic electrolytes) is highlighted by direct comparison to numerous existing porous solids. A further analysis on the specific pore type governed physisorption capacities is presented.  相似文献   

5.
Zeolite‐templated, high‐surface‐area, microporous, N‐doped carbons exhibit the highest CO2 uptake capacity recorded to date for any carbon material and one of the highest for any inorganic or organic porous material of up to 6.9 mmol g?1 at 273 K and ambient pressure and 4.4 mmol g?1 at ambient temperature and pressure, along with an initial CO2 adsorption energy of 36 kJ mol?1 at lower coverage and 20 kJ mol?1 at higher CO2 coverage. Combined with their ease of preparation, excellent recyclability and regeneration stability, and high selectivity for CO2, the N‐doped zeolite‐templated carbons are amongst the most promising solid‐state absorbents reported so far for CO2 capture and storage.  相似文献   

6.
Fullerenes are of tremendous interest from fundamental researches to applied perspectives in the past decades. However, their application in supercapacitors has been underdeveloped for a long time. Here, the KOH activation of C70 microtubes is reported at high temperatures, which provides activated samples exhibiting excellent capacitive properties. The improved capacitive performance can be attributed to three aspects: the generation of macropores and micropores, the introduction of oxygen functionalities, and the formation of graphitic carbons from ellipsoidal fullerenes. The optimum activated state for supercapacitor application is achieved at 600 °C, at which the product exhibits the best electrochemical behavior with a gravimetric capacitance of 362.0 F g?1 at 0.1 A g?1 and excellent cycling stability with capacitance retention of 92.5% over 5000 cycles at 1 A g?1.  相似文献   

7.
The natural abundance of 15N in plant biomass has been used to infer how N dynamics change with elevated atmospheric CO2 and changing water availability. However, it remains unclear if atmospheric CO2 effects on plant biomass 15N are driven by CO2-induced changes in soil moisture. We tested whether 15N abundance (expressed as δ15N) in plant biomass would increase with increasing soil moisture content at two atmospheric CO2 levels. In a greenhouse experiment we grew sunflower (Helianthus annuus) at ambient and elevated CO2 (760 ppm) with three soil moisture levels maintained at 45, 65, and 85% of field capacity, thereby eliminating potential CO2-induced soil moisture effects. The δ15N value of total plant biomass increased significantly with increased soil moisture content at both CO2 levels, possibly due to increased uptake of 15N-rich organic N. Although not adequately replicated, plant biomass δ15N was lower under elevated than under ambient CO2 after adjusting for plant N uptake effects. Thus, increases in soil moisture can increase plant biomass δ15N, while elevated CO2 can decrease plant biomass δ15N other than by modifying soil moisture.  相似文献   

8.
In the present study, granular activated carbons were prepared from agricultural waste corn cob by chemical activation with potassium salts and/or physical activation with CO2. Under the experimental conditions investigated, potassium hydroxide (KOH) and potassium carbonate (K2CO3) were effective activating agents for chemical activation during a ramping period of 10 degrees C/min and subsequent gasification (i.e., physical activation) at a soaking period of 800 degrees C. Large BET surface areas (>1,600 m2/g) of activated carbons were thus obtained by the combined activation. In addition, this study clearly showed that the porosity created in the acid-unwashed carbon products is substantially lower than that of acid-washed carbon products due to potassium salts left in the pore structure.  相似文献   

9.
Projected depletions in the stratospheric ozone layer will result in increases in solar ultraviolet-B radiation (290–320 nm) reaching the earth's surface, These increases will likely occur in concert with other environmental changes such as increases in atmospheric carbon dioxide concentrations. Currently very little information is available on the effectiveness of UV-B radiation within a CO2-enriched atmosphere, and this is especially true for trees. Loblolly pine (Pinus taeda L.) seedlings were grown in a factorial experiment at the Duke University Phytotron with either 0, 8.8 or 13.8 kJ m−2 of biologically effective UV-B radiation (UV-BBE). The CO2 concentrations used were 350 and 650 μmol mol−1. Measurements of chlorophyll fluorescence were made at 5-week intervals and photosynthetic oxygen evolution and leaf pigments were measured after 22 weeks, prior to harvest. The results of this study demonstrated a clear growth response to CO2 enrichment but neither photosynthetic capacity nor quantum efficiency were altered by CO2. The higher UV-B irradiance reduced total biomass by about 12% at both CO2 levels but biomass partitioning was altered by the interaction of CO2 and UV-B radiation. Dry matter was preferentially allocated to shoot components by UV-B radiation at 350 μmol mol−1 CO2 and towards root components at 650 μmol mol−1 CO2. These subtle effects on biomass allocation could be important in the future to seedling establishment and competitive interactions in natural as well as agricultural communities.  相似文献   

10.
Several Nocardia and Pseudomonas spp., as well as some unidentified bacteria, isolated from lake water containing high loads of waste lignin, were tested for their capacity to release 14CO2 from specifically 14C-labelled dehydropolymer of coniferyl alcohol (DHP) or corn stalk lignins. The bacteria were selected according to their ability to degrade phenolic compounds. However, only some of them could release significant amounts of 14CO2 from the labelled lignin. The tested Nocardia spp. were more active than the Pseudomonas spp. and the unidentified bacteria. The most active strains belonged to N. autotrophica. These strains released CO2 significantly from the methoxyl group and transformed the other carbons from the phenylpropane skeleton of lignin also into CO2. Other less demethylating strains also released little CO2 from the other carbons of the lignin molecule. From corn stalk materials which were specifically labelled in the lignin part only small amounts of labelled CO2 were released.Non-Common-Abbreviation Used DHP dehydropolymers of coniferyl alcohol  相似文献   

11.
In many coastal areas of South-East Asia, attempts have been made to revive coastal ecosystem by initiating projects that encourage planting of mangrove trees. Compared to the terrestrial trees, mangrove trees possess a higher carbon fixation capacity. It becomes a very significant option for clean development mechanism (CDM) program. However, a reliable method to estimate CO2 fixation capacity of mangrove trees has not been established. Acknowledging the above fact, we decided to set up an estimation method for the CDM program, using gas exchange analysis to estimate mangrove productivity, we put into consideration the net CO2 fixation of reforested Kandelia candel (5-, 10-, and 15-year-old stand). This was estimated by gas exchange analysis and growth curve analysis. In growth curve analysis, we drew a growth curve of a single stand using data of above- and below-ground biomass. In the gas exchange analysis, we calculated CO2 fixation capacity by (1) measuring respiration rate of each organ of stand and calculating respiratory CO2 emission from above- to below-ground biomass. (2) Measuring the single-leaf photosynthetic rate in response to light intensity and calculating the photosynthetic CO2 absorption. (3) We also developed a model for the diurnal changes in temperature, and monthly averages based on one-day estimation of CO2 absorption and emission, which we corrected by this model in order to estimate the net CO2 fixation capacity in response to temperature. Comparing the biomass accumulation of the two methods constructed for the same forest, the above-ground biomass accumulation of 10-year-old forest (34.3 ton ha−1 yr−1) estimated by gas exchange analysis was closely compared to those of growth curve analysis (26.6 ton ha−1 yr−1), suggesting that the gas exchange analysis was capable of estimating mangrove productivity. The validity of the estimated CO2 fixation capacity by the gas exchange analysis and the growth curve analysis was also discussed.  相似文献   

12.
The long-term interaction between elevated CO2 and soil water deficit was analysed in N2-fixing alfalfa plants in order to assess the possible drought tolerance effect of CO2. Elevated CO2 could delay the onset of drought stress by decreasing transpiration rates, but this effect was avoided by subjecting plants to the same soil water content. Nodulated alfalfa plants subjected to ambient (400 μmol mol?1) or elevated (700 μmol mol?1) CO2 were either well watered or partially watered by restricting water to obtain 30% of the water content at field capacity (ampproximately 0.55 g water cm?3). The negative effects of soil water deficit on plant growth were counterbalanced by elevated CO2. In droughted plants, elevated CO2 stimulated carbon fixation and, as a result, biomass production was even greater than in well-watered plants grown in ambient CO2. Below-ground production was preferentially stimulated by elevated CO2 in droughted plants, increasing nodule biomass production and the availability of photosynthates to the nodules. As a result, total nitrogen content in droughted plants was higher than in well-watered plants grown in ambient CO2. The beneficial effect of elevated CO2 was not correlated with a better plant water status. It is concluded that elevated CO2 enhances growth of droughted plants by stimulating carbon fixation, preferentially increasing the availability of photosynthates to below-ground production (roots and nodules) without improving water status. This means that elevated CO2 enhances the ability to produce more biomass in N2-fixing alfalfa under given soil water stress, improving drought tolerance.  相似文献   

13.
Lolium temulentum L. Ba 3081 was grown hydroponically in air (350 μmol mol−1 CO2) and elevated CO2 (700 μmol mol−1 CO2) at two irradiances (150 and 500 μmol m−2 s−1) for 35 days at which point the plants were harvested. Elevated CO2 did not modify relative growth rate or biomass at either irradiance. Foliar carbon-to-nitrogen ratios were decreased at elevated CO2 and plants had a greater number of shorter tillers, particularly at the lower growth irradiance. Both light-limited and light-saturated rates of photosynthesis were stimulated. The amount of ribulose-1,5-bisphosphate carboxylase-oxygenase (Rubisco) protein was increased at elevated CO2, but maximum extractable Rubisco activities were not significantly increased. A pronounced decrease in the Rubisco activation state was found with CO2 enrichment, particularly at the higher growth irradiance. Elevated-CO2-induced changes in leaf carbohydrate composition were small in comparison to those caused by changes in irradiance. No CO2-dependent effects on fructan biosynthesis were observed. Leaf respiration rates were increased by 68% in plants grown with CO2 enrichment and low light. We conclude that high CO2 will only result in increased biomass if total light input favourably increases the photosynthesis-to-respiration ratio. At low irradiances, biomass is more limited by increased rates of respiration than by CO2-induced enhancement of photosynthesis. Received: 23 February 1999 / Accepted: 15 June 1999  相似文献   

14.
Conservation agriculture in its version of permanent raised bed planting with crop residue retention increases yields and improves soil characteristics, e.g. aggregate distribution, organic matter content, so it remained to be seen how greenhouse gas emissions and dynamics of C and N might be altered. The objective of this study was to investigate how conservation agriculture with permanent raised beds, tied ridges, i.e. dykes within the furrows to prevent water run-off, and residue retention affected greenhouse gas emissions. A field experiment was started in 1999 comparing permanent and conventionally tilled raised beds with different residue management under rain fed conditions. Soil was characterized and emissions of CH4, N2O and CO2 and dynamics of NH4 +, NO2 ? and NO3 ? were monitored in a laboratory experiment. The crop and tied ridges had no effect on soil characteristics and dynamics of C and N. Tilled beds reduced the water holding capacity (WHC) 1.1 times and increased conductivity 1.3 times compared to soil under nontilled beds with retention of all crop residues. The WHC, organic C, soil microbial biomass and total N were ≥1.1 larger in soil from nontilled beds where the crop residue was retained compared to where it was removed after only 6 years. The emission of CO2 was 1.2 times and production of NO3 ? 1.8 times larger in nontilled beds where the crop residue was retained compared to where it was removed. The CO2 emission was 1.2 times and the emission of N2O after 1 day 2.3 times larger in soil under tilled beds compared to nontilled beds with full residue retention, while the increase in concentration of NO3 ? was 0.05 mg N kg?1 soil in the former and 2.38 in the latter. We found that permanent raised bed planting with crop residue retention decreased emissions of N2O and CO2 compared to soil under conventionally tilled raised beds. Production of NO3 ? is larger in soil with permanent raised bed planting with crop residue retention compared to conventionally tilled raised beds.  相似文献   

15.
Bioenergy with carbon capture and storage (BECCS) is recognized as a potential negative emission technology, needed to keep global warming within safe limits. With current technologies, large-scale implementation of BECCS would compromise food production. Bioenergy derived from phototrophic microorganisms, with direct capture of CO2 from air, could overcome this challenge and become a sustainable way to realize BECCS. Here we present an alkaline capture and conversion system that combines high atmospheric CO2 transfer rates with high and robust phototrophic biomass productivity (15.2 ± 1.0 g/m 2/d). The system is based on a cyanobacterial consortium, that grows at high alkalinity (0.5 mol/L) and a pH swing between 10.4 and 11.2 during growth and harvest cycles.  相似文献   

16.
Olive husk was used for the preparation of activated carbon by chemical activation with KOH. The effects of carbonization and activation time on carbon properties were evaluated. The surface area of the produced carbons was measured by means of N(2) adsorption at 77K. The carbons with the highest surface area were further characterized by means of elemental analysis, particle size measurement, Boehm titration, zeta potential measurement, and temperature programmed desorption (TPD). Subsequently they were used for adsorption of a mixture of polyphenols consisting of caffeic acid, vanillin, vanillic acid, pi-hydroxybenzoic acid and gallic acid at two temperatures, and their adsorptive capacity was compared to a commercial carbon Acticarbon CX and found to be higher enough. The role of the porosity and surface groups are discussed in relation to the adsorption forces and the properties of the adsorbed substances. A thermodynamic interpretation of the results is also attempted.  相似文献   

17.
As a means to improve carbon uptake in the cyanobacterium Synechocystis sp. strain PCC6803, we engineered strains to contain additional inducible copies of the endogenous bicarbonate transporter BicA, an essential component of the CO2-concentrating mechanism in cyanobacteria. When cultured under atmospheric CO2 pressure, the strain expressing extra BicA transporters (BicA+ strain) grew almost twice as fast and accumulated almost twice as much biomass as the control strain. When enriched with 0.5% or 5% CO2, the BicA+ strain grew slower than the control but still showed a superior biomass production. Introducing a point mutation in the large C-terminal cytosolic domain of the inserted BicA, at a site implicated in allosteric regulation of transport activity, resulted in a strain (BicA+(T485G) strain) that exhibited pronounced cell aggregation and failed to grow at 5% CO2. However, the bicarbonate uptake capacity of the induced BicA+(T485G) was twice higher than for the wild-type strain. Metabolic analyses, including phenotyping by synchrotron-radiation Fourier transform Infrared spectromicroscopy, scanning electron microscopy, and lectin staining, suggest that the excess assimilated carbon in BicA+ and BicA+(T485G) cells was directed into production of saccharide-rich exopolymeric substances. We propose that the increased capacity for CO2 uptake in the BicA+ strain can be capitalized on by re-directing carbon flux from exopolymeric substances to other end products such as fuels or high-value chemicals.  相似文献   

18.
Summary Gas exchange characteristics in leaves of the sclerophyll shrub Quercus coccifera were studied in the natural habitat in Portugal during spring and during the summer dry period. Compared to other sclerophyll species growing at the same site, photosynthesis in leaves of Quercus coccifera was less affected by water stress. Moderate water stress after six weeks of drought led to large decreases in stomatal conductance but no change in mesophyll photosynthetic capacity as compared to late spring. Leaf internal CO2 pressure remained near 220 bar during diurnal courses in the spring. On midsummer days, leaf internal CO2 decreased from a late morning value of 200 bar to a late afternoon value of approximately 150 bar. In contrast to Quercus suber (Tenhunen et al. 1984), restriction of CO2 supply due to stomatal closure reduced net CO2 uptake at midday and in the afternoon during midsummer. A decrease in leaf carboxylation efficiency and an increase in CO2 compensation point at midday also played an important role in determining the diurnal course of net photosynthesis. During the late stages of drought in September, severe water stress led to reduction in mesophyll photosynthetic capacity and further reduction in leaf conductance. The observed decrease in mesophyll photosynthetic capacity was correlated with decrease in the daily minimum leaf water potential to greater negative values than-30 bar. At this time, CO2 saturated photosynthetic rates decreased as much as 50% over the course of a day when measured at constant saturating light, 32° C leaf temperature, and a water vapor mole fraction difference between leaf and air of 30 mbar bar-1.  相似文献   

19.
The effects of long‐term (4 year) CO2 enrichment (70 Pa versus 35 Pa) and nitrogen nutrition (8 mm versus 1 mm NO3) on biomass accumulation and the development of photosynthetic capacity in leaves of cork oak (Quercus suber L., a Mediterranean evergreen tree) were studied. The evolution of photosynthetic parameters with leaf development was estimated by fitting the biochemical model of Farquhar et al. (Planta 149, 78–90, 1980) with modifications by Sharkey (Botanical Review 78, 71–75, 1985) to ACi response curves. CO2 enrichment had a small reduction effect on the development of the maximum CO2 fixation capacity by Rubisco (VCmax), and no effect over maximum electron transport capacity (Jmax), day‐time respiration (Rd) and Triose‐P utilization (TPU). However, there was a statistically significant effect of N fertilization and the interaction CO2 × N over the evolution of VCmax, Jmax and TPU. Relative stomatal limitation (estimated from ACi curves) was higher (+20%) for plants grown under ambient CO2 than for plants grown under elevated CO2. There was a significant effect of CO2 and N fertilization over total biomass accumulation as well as leaf area. Plants grown at elevated CO2 had 27% more biomass than plants grown at ambient CO2 when given high N. However, for plants grown under low N there was no significant effect of CO2 enrichment on biomass accumulation. Plants grown under low N also had significantly higher root : shoot ratios whereas there were no differences between CO2 treatments. The larger biomass accumulation of Q. suber under elevated CO2 is attributable to a higher availability of CO2 coupled to a larger leaf area, with no significant decrease in photosynthetic capacity under CO2 enrichment and elevated N fertilization. For low N fertilization, the effects of CO2 enrichment over leaf area and biomass accumulation are lost, suggesting that in native ecosystems with low N availability, the effects of CO2 enrichment may be insignificant.  相似文献   

20.
One cultivar each of spring wheat (Triticum aestivum L. cv. Arkas), oat (Avena sativa L. cv. Lorenz), and barley (Hordeum vulgare L. cv. Aramir) was chosen in order to study the relative contributions of individual bracts to the gas exchange of whole ears. The distribution and frequency of the stomata on the bracts were examined. Gas exchange was measured at normal atmospheric CO2 (330 bar) and at high CO2 (2000 bar) on intact ears and on ears from which glumes or lemmas and pleae (wheat and oat) or awns (barley) had been removed.The relative contribution to the gas exchange of the whole organ is highest for the awns of barley ears. In wheat, the contribution of the glumes is slightly higher than that of the inner bracts before anthesis. Two weeks after anthesis the inner bracts contribute more than the glumes. This tendency of increasing importance of the inner bracts is also found in oat ears, but the relative amount of CO2 uptake by the glumes is higher than in wheat. These changes during ontogeny result from the better supply of light to the inner bracts caused by opening of the ears' structures during grain filling, which in part compensates for the decreasing photosynthetic capacity.The ratio of the photosynthesis rate at high CO2 to that at normal CO2 is lower for the glumes of oat and for the awns of barley than for the other bracts.Abbreviations A330, A2000 net photosynthesis rate, A330 at normal atmospheric CO2 (330 bar), A2000 at high CO2 (2000 bar) - PPFD photosynthetic photon flux density - pc intercellular partial pressure of CO2  相似文献   

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