Defining graphenic crystallites in disordered carbon: Moving beyond the platelet model

J., Putman, Kate; Rowles, Matthew R.; Marks, Nigel A.; Tomás, Carla de; Martin, Jacob W.; Suarez-Martinez, Irène

doi:10.1016/j.carbon.2023.03.040

Cited by 26 publications

(6 citation statements)

References 32 publications

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“…For these materials, the L a parameter quantifies how defective the individual sheets of turbostratic carbon are; larger L a values correspond to, on average, less defective sheets with larger coherent domains. [ 39 ] These defects could include pores, heteroatoms, and/or structure terminations that cause deviation in the hexagonal structure of the typical C 6 ring. In fact, the L a parameter is directly related to the commonly reported I D / I G ratio from Raman analysis of carbon materials.…”

Section: Resultsmentioning

confidence: 99%

A Data‐Driven Approach to Molten Salt Synthesis of N‐Rich Carbon Adsorbents for Selective CO₂ Capture

Burrow,

Eichler,

Martinez

et al. 2023

Advanced Materials

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Applying a design of experiments methodology to molten salt synthesis of nanoporous carbons enables inverse design and optimization of N‐rich carbon adsorbents with excellent CO2/N2 selectivity and appreciable CO2 capacity for carbon capture via swing adsorption from dilute gas mixtures, such as natural gas combined cycle flue gas. This data‐driven study reveals fundamental relationships between the synthesis conditions, physicochemical properties, and achievable selective adsorption performance of N‐rich nanoporous carbons derived from molten salt synthesis for CO2 capture. Taking advantage of size‐sieving separation of CO2 (3.30 Å) from N2 (3.64 Å) within the turbostratic nanostructure of these N‐rich carbons, while limiting deleterious N2 adsorption in a weaker adsorption site that harms selectivity, enables a large low‐pressure CO2 capacity (0.73 mmol/g at 30.4 Torr and 30°C) with noteworthy concurrent CO2/N2 selectivity (SIAST = 246, adsorbed phase purity = 91%) from a simulated gas stream with only 4% CO2. This study reveals general structure‐function relationships of selective CO2 adsorption by nanoporous carbon adsorbents. Optimized N‐rich porous carbons, with good physicochemical stability, low cost, and moderate regeneration energy, can achieve performance for selective CO2 adsorption that competes with other classes of advanced porous materials, such as chemisorbing zeolites and functionalized metal‐organic frameworks.This article is protected by copyright. All rights reserved

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Section: Resultsmentioning

confidence: 99%

A Data‐Driven Approach to Molten Salt Synthesis of N‐Rich Carbon Adsorbents for Selective CO₂ Capture

Burrow,

Eichler,

Martinez

et al. 2023

Advanced Materials

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“…The slit pore model also lacks any defects or functional groups, meaning that an uncharged CO 2 model can be used that does not account for the quadrupole moment. It is our aim to extend this DFT method for calculations in functionalized 3D structures and to simulate adsorption-induced deformation in atomistic 3D carbon models. , …”

Section: Discussionmentioning

confidence: 99%

“…It is our aim to extend this DFT method for calculations in functionalized 3D structures 46 and to simulate adsorption-induced deformation in atomistic 3D carbon models. 47…”

Section: Discussionmentioning

confidence: 99%

Deformation of Nanoporous Carbons Induced By Multicomponent Adsorption: Insight from the SAFT-DFT Model

Corrente,

Hinks,

Kasera

et al. 2024

J. Phys. Chem. C

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Deformation of nanoporous materials during gas adsorption has been attracting considerable attention due to various applications, including energy and gas storage, carbon capture, and separation. While most practical applications involve multicomponent mixtures, most experimental and theoretical works deal with single-component adsorption. Here, we study the specifics of adsorption-induced deformation during the displacement of methane by carbon dioxide from carbon nanopores, a process of paramount importance for secondary gas recovery and carbon sequestration in shale and coal formations. Density functional theory calculations augmented by the perturbed-chain statistical associating fluid theory (SAFT-DFT) and grand canonical Monte Carlo (GCMC) simulations are employed to model the adsorption of CH 4 −CO 2 mixtures on carbon slit nanopores of various sizes. We found a nonmonotonic behavior of adsorption deformation with increasing pressure and varying mixture composition that is explained by the peculiarities of molecule packings confined in nanoscale pores. The SAFT-DFT method is shown to produce results in agreement with atomistic GCMC simulations at a fraction of the computational cost. The SAFT-DFT method can be extended to study the adsorption selectivity and deformation effects for complex mixtures, including hydrocarbons and CO 2 .

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“…This adjustment better reflects the structure of biochar. 215 However, the nonhexagonal ring inclusion impacts the true density of the molecular structure, 167 porosity, and hence also reactivity. Simulated HRTEM and experimental micrographs were compared to validate the structural order.…”

Section: Biochar Model Generation and Advanced Atomistic Representationmentioning

confidence: 99%

“…Moreover, in the scenario where the model consisted exclusively of hexagonal rings, the resulting biochar would display a greater abundance of graphitic or crystalline formations, typically absent in conventional biochar structures. , Therefore, the model was modified by integrating nonhexagonal rings, which introduced curvature and generated amorphous regions or sections with reduced order. This adjustment better reflects the structure of biochar . However, the nonhexagonal ring inclusion impacts the true density of the molecular structure, porosity, and hence also reactivity.…”

Section: Biochar Model Generation and Advanced Atomistic Representationmentioning

confidence: 99%

Atomistic Modeling of Lignocellulosic and Carbonaceous Fuels and Their Pyrolysis Reactions: A Review

Sierra-Jimenez,

Mathews,

Chejne

et al. 2023

Energy Fuels

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This paper explores the utility of large-scale atomistic models to examine the complex relationship between biochar behavior, its structural characteristics, and the reactions involved in its formation. Pyrolysis kinetic models primarily focus on explaining the formation of small volatiles and aromatic structures without fully understanding the carbonization process. To gain a deeper understanding of carbonization and move beyond unrealistic structures resembling levoglucosan, it is necessary to examine the transformation of the lignocellulosic macromolecules into carbonaceous structures from a molecular-level perspective. This includes exploring structural transitions and large-scale reactive dynamics. Furthermore, incorporating atomistic representations derived from experimental data and theoretical modeling can help overcome the limitations of relying solely on empirical and density functional theory approaches due to the need for scale to capture biochar properties. Additionally, by considering structural transitions on a large scale, we can effectively capture the complexity of biomass pyrolysis, the interaction of free radicals, and the pore size distribution, all essential for comprehending biochar reactivity and utility.

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Defining graphenic crystallites in disordered carbon: Moving beyond the platelet model

Cited by 26 publications

References 32 publications

A Data‐Driven Approach to Molten Salt Synthesis of N‐Rich Carbon Adsorbents for Selective CO₂ Capture

A Data‐Driven Approach to Molten Salt Synthesis of N‐Rich Carbon Adsorbents for Selective CO₂ Capture

Deformation of Nanoporous Carbons Induced By Multicomponent Adsorption: Insight from the SAFT-DFT Model

Atomistic Modeling of Lignocellulosic and Carbonaceous Fuels and Their Pyrolysis Reactions: A Review

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Defining graphenic crystallites in disordered carbon: Moving beyond the platelet model

Cited by 26 publications

References 32 publications

A Data‐Driven Approach to Molten Salt Synthesis of N‐Rich Carbon Adsorbents for Selective CO2 Capture

A Data‐Driven Approach to Molten Salt Synthesis of N‐Rich Carbon Adsorbents for Selective CO2 Capture

Deformation of Nanoporous Carbons Induced By Multicomponent Adsorption: Insight from the SAFT-DFT Model

Atomistic Modeling of Lignocellulosic and Carbonaceous Fuels and Their Pyrolysis Reactions: A Review

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A Data‐Driven Approach to Molten Salt Synthesis of N‐Rich Carbon Adsorbents for Selective CO₂ Capture

A Data‐Driven Approach to Molten Salt Synthesis of N‐Rich Carbon Adsorbents for Selective CO₂ Capture