Abstract:Amine-containing adsorbents have been extensively investigated for post-combustion carbon dioxide capture due to their ability to chemisorb low-concentration carbon dioxide from a wet flue gas. However, earlier studies have focused primarily on the carbon dioxide uptake of adsorbents, and have not demonstrated effective adsorbent regeneration and long-term stability under such conditions. Here, we report the versatile and scalable synthesis of a functionalized-polyethyleneimine (PEI)/silica adsorbent which sim… Show more
“…S35 †). 4,5,7,8,10,11,[13][14][15][20][21][22][23][24][25][26][27][28][29][30][31][32][33] Here, it is worth noting that the pore volume of our exfGO samples is much higher than those reported in the literature for amine impregnation.…”
Section: 7813-1521-28mentioning
confidence: 58%
“…5b). 4,7,8,[13][14][15][21][22][23][24][25][26][27][28]32,33 Here it is worth noting that the capacity loss of z21% in our TEPA@exfGO sample is arguably smaller than the z40% capacity loss from TEPA@mesoporous silica capsules, under similar synthetic and experimental conditions.…”
Section: 7813-1521-28mentioning
confidence: 58%
“…Due to their ultrahigh pore volume, exfGO-D samples can accept a record high TETA loading of z10 g g À1 of sample, without any sign of surface wetting (Table S6 †). 4,7,8,[13][14][15][21][22][23][24][25][26][27][28] Indeed, SEM micrographs still show void spaces for a TETA loading as high as 7.0 g g À1 in the exfGO-D sample (Fig. S26 †).…”
Section: 7813-1521-28mentioning
confidence: 99%
“…4c, S30, Tables S6 and S8 †). 4,5,7,8,10,11,[13][14][15][20][21][22][23][24][25][26][27][28][29][30][31][32][33] These uptake capacities are further conrmed under a simulated ue-gas stream of z100 ml min À1 , consisting of only 15% of CO 2 in N 2 , bubbled through water. A CO 2 capture of 35-40 wt% from the ue-gas is attained at 75 C ( Fig.…”
We demonstrate a simple and fully scalable method for obtaining hierarchical hyperporous graphene networks of ultrahigh total pore volume by thermal-shock exfoliation of graphene-oxide (exfGO) at a relatively mild temperature of 300 C. Such pore volume per unit mass has not previously been achieved in any type of porous solid. We find that the amount of oxidation of starting graphene-oxide is the key factor that determines the pore volume and surface area of the final material after thermal shock. Specifically, we emphasize that the development of the hyperporosity is directly proportional to the enhanced oxidation of sp 2 C]C to form C]O/COO. Using our method, we reproducibly synthesized remarkable meso-/macroporous graphene networks with exceptionally high total pore volumes, exceeding 6 cm 3 g
À1. This is a step change compared to #3 cm 3 g À1 in conventional GO under similar synthetic conditions.Moreover, a record high amine impregnation of >6 g g À1 is readily attained in exfGO samples (solid-amine@exfGO), where amine loading is directly controlled by the pore-structure and volume of the host materials. Such solid-amine@exfGO samples exhibit an ultrahigh selective flue-gas CO 2 capture of 30-40 wt% at 75 C with a working capacity of z25 wt% and a very long cycling stability under simulated flue-gas stream conditions. To the best of our knowledge, this is the first report where a graphene-oxide based hyperporous carbon network is used to host amines for carbon capture application with exceptionally high storage capacity and stability.The widespread implementation of clean energy technologies, such as CCS (carbon capture and sequestration), fuel cells, batteries, supercapacitors, water electrolysers, and/or molecular storage and transport, is critical to tackle climate change and energy security issues. [1][2][3][4][5] In this regard, nanoporous carbons, metal-organic frameworks (MOFs), polymers and zeolites have gained tremendous attention as storage, transport and conversion media.2-7 Considerable performance improvements have been achieved by synthesizing and manipulating their functional features and porous structures.6 In the case of CO 2 capture, obtaining high enough CO 2 uptake capacities by using sorbent based materials under ue-gas conditions is still a challenging task. Many sorbent materials show good CO 2 uptake capacities but only at 0 C or 25 C and for 100% dry CO 2 .Porous sorbents including zeolites, activated carbons and MOFs do not show desirable selective CO 2 uptake under humid conditions and/or at >50 C. 8 This is a major setback for the implementation of CCS. The recent efforts on the introduction of CO 2 -philic amine groups into nanoporous structures have led to a large enhancement in selective carbon (CO 2 ) capture and effluent ue-gas tolerance. 4,7,8 However, the practical feasibility of these materials for CO 2 capture is compromised by the lack of a simple and large-scale synthesis method. Substantial improvements in both the structural stability and scalable synthesis of these...
“…S35 †). 4,5,7,8,10,11,[13][14][15][20][21][22][23][24][25][26][27][28][29][30][31][32][33] Here, it is worth noting that the pore volume of our exfGO samples is much higher than those reported in the literature for amine impregnation.…”
Section: 7813-1521-28mentioning
confidence: 58%
“…5b). 4,7,8,[13][14][15][21][22][23][24][25][26][27][28]32,33 Here it is worth noting that the capacity loss of z21% in our TEPA@exfGO sample is arguably smaller than the z40% capacity loss from TEPA@mesoporous silica capsules, under similar synthetic and experimental conditions.…”
Section: 7813-1521-28mentioning
confidence: 58%
“…Due to their ultrahigh pore volume, exfGO-D samples can accept a record high TETA loading of z10 g g À1 of sample, without any sign of surface wetting (Table S6 †). 4,7,8,[13][14][15][21][22][23][24][25][26][27][28] Indeed, SEM micrographs still show void spaces for a TETA loading as high as 7.0 g g À1 in the exfGO-D sample (Fig. S26 †).…”
Section: 7813-1521-28mentioning
confidence: 99%
“…4c, S30, Tables S6 and S8 †). 4,5,7,8,10,11,[13][14][15][20][21][22][23][24][25][26][27][28][29][30][31][32][33] These uptake capacities are further conrmed under a simulated ue-gas stream of z100 ml min À1 , consisting of only 15% of CO 2 in N 2 , bubbled through water. A CO 2 capture of 35-40 wt% from the ue-gas is attained at 75 C ( Fig.…”
We demonstrate a simple and fully scalable method for obtaining hierarchical hyperporous graphene networks of ultrahigh total pore volume by thermal-shock exfoliation of graphene-oxide (exfGO) at a relatively mild temperature of 300 C. Such pore volume per unit mass has not previously been achieved in any type of porous solid. We find that the amount of oxidation of starting graphene-oxide is the key factor that determines the pore volume and surface area of the final material after thermal shock. Specifically, we emphasize that the development of the hyperporosity is directly proportional to the enhanced oxidation of sp 2 C]C to form C]O/COO. Using our method, we reproducibly synthesized remarkable meso-/macroporous graphene networks with exceptionally high total pore volumes, exceeding 6 cm 3 g
À1. This is a step change compared to #3 cm 3 g À1 in conventional GO under similar synthetic conditions.Moreover, a record high amine impregnation of >6 g g À1 is readily attained in exfGO samples (solid-amine@exfGO), where amine loading is directly controlled by the pore-structure and volume of the host materials. Such solid-amine@exfGO samples exhibit an ultrahigh selective flue-gas CO 2 capture of 30-40 wt% at 75 C with a working capacity of z25 wt% and a very long cycling stability under simulated flue-gas stream conditions. To the best of our knowledge, this is the first report where a graphene-oxide based hyperporous carbon network is used to host amines for carbon capture application with exceptionally high storage capacity and stability.The widespread implementation of clean energy technologies, such as CCS (carbon capture and sequestration), fuel cells, batteries, supercapacitors, water electrolysers, and/or molecular storage and transport, is critical to tackle climate change and energy security issues. [1][2][3][4][5] In this regard, nanoporous carbons, metal-organic frameworks (MOFs), polymers and zeolites have gained tremendous attention as storage, transport and conversion media.2-7 Considerable performance improvements have been achieved by synthesizing and manipulating their functional features and porous structures.6 In the case of CO 2 capture, obtaining high enough CO 2 uptake capacities by using sorbent based materials under ue-gas conditions is still a challenging task. Many sorbent materials show good CO 2 uptake capacities but only at 0 C or 25 C and for 100% dry CO 2 .Porous sorbents including zeolites, activated carbons and MOFs do not show desirable selective CO 2 uptake under humid conditions and/or at >50 C. 8 This is a major setback for the implementation of CCS. The recent efforts on the introduction of CO 2 -philic amine groups into nanoporous structures have led to a large enhancement in selective carbon (CO 2 ) capture and effluent ue-gas tolerance. 4,7,8 However, the practical feasibility of these materials for CO 2 capture is compromised by the lack of a simple and large-scale synthesis method. Substantial improvements in both the structural stability and scalable synthesis of these...
“…The basic chemistry of CO 2 adsorption on immobilized amines is very similar to amine scrubbing (typical chemisorption), which is responsible for its high CO 2 uptake in PCC conditions. Deactivation is a concern for amine‐based adsorbents, which can be alleviated by controlled regeneration or modification of the amines Metal‐organic frameworks (MOFs).…”
The application of characterization methods with high spatial resolution to the analysis of buried coating/metal interfaces requires the design and use of model systems. Herein, an epoxy‐like thin film is used as a model coating resembling the epoxy‐based coatings and adhesives widely used in technical applications. Spin coating is used for the deposition of a 30 nm‐thin bilayer (BL) composed of poly‐(ethylenimine) (PEI) and poly[(o‐cresyl glycidyl ether)‐co‐formaldehyde] (CNER). Fourier‐transform infrared spectroscopy (FTIR) results confirm that the exposure of coated AA2024‐T3 (AA) samples to the corrosive electrolyte solution does not cause the degradation of the polymer layer. In situ atomic force microscopy (AFM) studies are performed to monitor local corrosion processes at the buried interface of the epoxy‐like film and the AA2024‐T3 aluminum alloy surface in an aqueous electrolyte solution. Hydrogen evolution due to the reduction of water as the cathodic corrosion reaction leads to local blister formation. Based on the results of the complementary energy‐dispersive X‐ray spectroscopy (EDX) analysis performed at the same region of interest, most of the hydrogen evolved originates at the vicinity of Mg‐containing intermetallic particles.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.