Abstract:Abstract:The polymerization of CO 2 by Lewis basic moieties has been recently proposed to account for the high adsorption ability of N and S-doped porous carbon materials formed from the pyrolysis of sulfur or nitrogen containing polymers in the presence of KOH. Ab initio calculations performed on the ideal CO 2 tetramer complex LB-(CO 2 ) 4 (LB = NH 3 , H 2 O, H 2 S) showed no propensity for stabilization. A weak association is observed using Lewis acid species bound to oxygen (LA = H + , AlF 3 , AlH 3 , B 4 … Show more
“…To date, a common approach is to synthesize PC via the KOH activation of carbon rich precursors such as polymers and bio‐sourced materials . It has been traditional thought that the presence of nitrogen or sulfur enhanced the uptake, however, recent work has shown that this is not true, and that the oxygen (or total heteroatom content) is more important ,. In fact, the carbon content may be used as a quick guide to uptake efficiency.…”
The reproducible synthesis is reported for oxygen containing porous carbons (OPC) by the KOH activation at 500–800 °C of two oxygen containing precursor polymers: polyfurfuryl alcohol (PFFA) and polyanisyl alcohol (PAA) yielding FFA‐OPC and AA‐OPC, respectively. Both OPCs exhibits good thermal stability and reproducible gas uptake properties over multiple cycles. The surface area and pore volumes of the OPC are independent of the precursor identity, but controlled by the activation temperature. Similarly, the uptake of CO2 is determined by the physical properties of the OPC: activation at 750 °C results in uptake that equals or out‐performs existing PCs for high pressure uptake (30 bar) at 24.0 °C (FFA‐OPC750: 117 wt%; AA‐OPC750: 115 wt%). The high uptake is related to a high relative percentage of pores <2 nm. The uptake of CH4 for both OPCs is greatest for samples activation at 750 °C, FFA‐OPC750 shows enhanced uptake compared to AA‐OPC750, 15.5 wt% versus 13.7 wt%, respectively. Uptake for CH4 appears to relate to a high relative percentage of pores 1–2 nm, which is observed for AA‐OPC750. As a consequence, AA‐OPC750 demonstrates superior selectivity for CO2 capture over CH4 uptake (AA‐OPC750: Vmass(CO2/CH4)=8.37 at 30 bar) as compared to reported PCs. A higher value for the isosteric heat of adsorption of CO2 (33 kJ mol−1) versus CH4 (11 kJ mol−1) suggests a new temperature dependent strategy for removing CO2 from natural gas via selective adsorption and desorption cycles.
“…To date, a common approach is to synthesize PC via the KOH activation of carbon rich precursors such as polymers and bio‐sourced materials . It has been traditional thought that the presence of nitrogen or sulfur enhanced the uptake, however, recent work has shown that this is not true, and that the oxygen (or total heteroatom content) is more important ,. In fact, the carbon content may be used as a quick guide to uptake efficiency.…”
The reproducible synthesis is reported for oxygen containing porous carbons (OPC) by the KOH activation at 500–800 °C of two oxygen containing precursor polymers: polyfurfuryl alcohol (PFFA) and polyanisyl alcohol (PAA) yielding FFA‐OPC and AA‐OPC, respectively. Both OPCs exhibits good thermal stability and reproducible gas uptake properties over multiple cycles. The surface area and pore volumes of the OPC are independent of the precursor identity, but controlled by the activation temperature. Similarly, the uptake of CO2 is determined by the physical properties of the OPC: activation at 750 °C results in uptake that equals or out‐performs existing PCs for high pressure uptake (30 bar) at 24.0 °C (FFA‐OPC750: 117 wt%; AA‐OPC750: 115 wt%). The high uptake is related to a high relative percentage of pores <2 nm. The uptake of CH4 for both OPCs is greatest for samples activation at 750 °C, FFA‐OPC750 shows enhanced uptake compared to AA‐OPC750, 15.5 wt% versus 13.7 wt%, respectively. Uptake for CH4 appears to relate to a high relative percentage of pores 1–2 nm, which is observed for AA‐OPC750. As a consequence, AA‐OPC750 demonstrates superior selectivity for CO2 capture over CH4 uptake (AA‐OPC750: Vmass(CO2/CH4)=8.37 at 30 bar) as compared to reported PCs. A higher value for the isosteric heat of adsorption of CO2 (33 kJ mol−1) versus CH4 (11 kJ mol−1) suggests a new temperature dependent strategy for removing CO2 from natural gas via selective adsorption and desorption cycles.
“…Contrary to some recent claims [17], it has been shown in multiple studies that the presence of nitrogen-or sulfur-doping in PC materials does not enhance the uptake of CO 2 or the selectivity [18][19][20]. Instead, the presence of N, S, and O are more to do with the generation of the optimum pore size and distribution [16].…”
The expansion product from the sulfuric acid dehydration of para-nitroaniline has been characterized and studied for CO 2 adsorption. The X-ray photoelectron spectroscopy (XPS) characterization of the foam indicates that both N and S contents (15 and 9 wt%, respectively) are comparable to those separately reported for nitrogen-or sulfur-containing porous carbon materials. The analysis of the XPS signals of C1s, O1s, N1s, and S2p reveals the presence of a large number of functional groups and chemical species. The CO 2 adsorption capacity of the foam is 7.9 wt% (1.79 mmol/g) at 24.5 • C and 1 atm in 30 min, while the integral molar heat of adsorption is 113.6 kJ/mol, indicative of the fact that chemical reactions characteristic of amine sorbents are observed for this type of carbon foam. The kinetics of adsorption is of pseudo-first-order with an extrapolated activation energy of 18.3 kJ/mol comparable to that of amine-modified nanocarbons. The richness in functionalities of H 2 SO 4-expanded foams represents a valuable and further pursuable approach to porous carbons alternative to KOH-derived activated carbons.
“…All the Coulomb interaction terms in direct and exchange channels are calculated exactly to find the Born-Oppenheimer (BO) matrix elements [2] that acts as input to find the unknown SEM amplitude, following a coupled-channel methodology introduced by Calcutta Group [3]. The detailed of the theory is available in the literature [1][2][3][4][5][6][7][8][9]. Here Lippman-Schwinger type coupled integral equation in momentum space formalism [3] is used.…”
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confidence: 99%
“…The detailed of the theory is available in the literature [1][2][3][4][5][6][7][8][9]. Here Lippman-Schwinger type coupled integral equation in momentum space formalism [3] is used. The formally exact Lippman-Schwinger type coupled integral equation for the scattering amplitude in momentum space is given by [3]:…”
mentioning
confidence: 99%
“…when W C is the van der Waals coefficient [10] and 0 R is the minimum value of the interatomic distance. The s-wave elastic triplet phase shift and the corresponding scattering length are calculated following the standard procedure described in references [1][2][3][4][5][6][7][8][9].…”
The static-exchange model (SEM) and the modified static-exchange model (MSEM) recently introduced by Ray [1] is applied to study the elastic collision between two hydrogen-like atoms when both are in ground states considering the system as a four-body Coulomb problem in the center of mass frame, in which all the Coulomb interaction terms in direct and exchange channels are treated exactly. The SEM includes the non-adiabatic short-range effect due to electron-exchange. The MSEM added in it, the long-range effect due to induced dynamic dipole polarizabilities between the atoms e.g. the Van der Waals interaction. Applying the SEM code in different H-like two-atomic systems, a reduced mass ( ) dependence on scattering length is observed. Again applying the MSEM code on H(1s)-H(1s) elastic scattering and varying the minimum values of interatomic distance 0 R , the dependence of scattering length on the effective interatomic potential consistent with the existing physics are observed. Both these basic findings in low and cold energy atomic collision physics are quite useful and are being reported for the first time.
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