Effects of energetic heterogeneity on gas adsorption and gas storage in geologic shale systems

AbstractHigh-resolution gas adsorption techniques were used to analyse the evolution of the aspect ratio and adsorption energy distribution on synthetic saponite samples with increasing layer charge. Using Ar as a gaseous probe, the aspect ratio of the saponite particles can be determined easily by decomposing the derivative adsorption isotherms and taking into account high-energy sites which can be assigned to talc-like ditrigonal cavities. Changes in the shape of the elementary particles are observed for layer charges above 1.30, i.e. when all the ditrigonal cavities contain at least one Al atom substituting for Si. When N2 is used as a probe, high-energy sites that could be wrongly interpreted as micropores on the basis of classical t-plot treatments are observed whatever the layer charge. Using the information obtained from both Ar and N2, schemes for describing adsorption can be proposed for all layer charges and suggest complex adsorption mechanisms for charged clay minerals.

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A heterometallic metal–organic framework based on multi-nuclear clusters exhibiting high stability and selective gas adsorption

Dalton Transactions ◽

10.1039/c8dt03826k ◽

2019 ◽

Vol 48 (1) ◽

pp. 278-284 ◽

Cited By ~ 12

Author(s):

Dongmei Wang ◽

Zihua Liu ◽

Lili Xu ◽

Chunxia Li ◽

Dian Zhao ◽

...

Keyword(s):

Chemical Stability ◽

High Performance ◽

High Stability ◽

Gas Adsorption ◽

Metal Organic Framework ◽

Gas Storage ◽

Nuclear Clusters ◽

Metal Organic ◽

Thermal And Chemical Stability ◽

Organic Framework

Porous In/Tb-CBDA has been successfully synthesized in the light of the heterometallic cooperative crystallization (HCC) approach. In/Tb-CBDA with high thermal and chemical stability exhibited high performance for gas storage and separation.

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Efficiently mapping structure–property relationships of gas adsorption in porous materials: application to Xe adsorption

Faraday Discussions ◽

10.1039/c7fd00038c ◽

2017 ◽

Vol 201 ◽

pp. 221-232 ◽

Cited By ~ 4

Author(s):

A. R. Kaija ◽

C. E. Wilmer

Keyword(s):

Porous Materials ◽

Void Fraction ◽

Large Scale ◽

Gas Adsorption ◽

Structural Characteristics ◽

Gas Storage ◽

Computational Method ◽

Structure Property ◽

Structure Property Relationships ◽

Computational Screening

Designing better porous materials for gas storage or separations applications frequently leverages known structure–property relationships. Reliable structure–property relationships, however, only reveal themselves when adsorption data on many porous materials are aggregated and compared. Gathering enough data experimentally is prohibitively time consuming, and even approaches based on large-scale computer simulations face challenges. Brute force computational screening approaches that do not efficiently sample the space of porous materials may be ineffective when the number of possible materials is too large. Here we describe a general and efficient computational method for mapping structure–property spaces of porous materials that can be useful for adsorption related applications. We describe an algorithm that generates random porous “pseudomaterials”, for which we calculate structural characteristics (e.g., surface area, pore size and void fraction) and also gas adsorption properties via molecular simulations. Here we chose to focus on void fraction and Xe adsorption at 1 bar, 5 bar, and 10 bar. The algorithm then identifies pseudomaterials with rare combinations of void fraction and Xe adsorption and mutates them to generate new pseudomaterials, thereby selectively adding data only to those parts of the structure–property map that are the least explored. Use of this method can help guide the design of new porous materials for gas storage and separations applications in the future.

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Gas adsorption in the topologically disordered Fe-BTC framework

Journal of Materials Chemistry A ◽

10.1039/d1ta08449f ◽

2021 ◽

Author(s):

Adam Sapnik ◽

Christopher W. Ashling ◽

Lauren Macreadie ◽

Seok J. Lee ◽

Timothy Johnson ◽

...

Keyword(s):

Gas Adsorption ◽

Metal Organic Frameworks ◽

Functional Materials ◽

Gas Storage ◽

Metal Organic

Disordered metal–organic frameworks are emerging as an attractive class of functional materials, however their applications in gas storage and separation have yet to be fully explored. Here, we investigate gas...

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The Role of Molecular Modeling & Simulation in the Discovery and Deployment of Metal-Organic Frameworks for Gas Storage and Separation

10.26434/chemrxiv.7854980.v1 ◽

2019 ◽

Author(s):

Arni Sturluson ◽

Melanie T. Huynh ◽

Alec Kaija ◽

Caleb Laird ◽

Sunghyun Yoon ◽

...

Keyword(s):

Gas Adsorption ◽

Metal Organic Frameworks ◽

Gas Storage ◽

Chemical Warfare Agent ◽

Nanoporous Materials ◽

Oxygen Storage ◽

Metal Organic ◽

Computational Materials ◽

Computational Discovery

Metal-organic frameworks (MOFs) are highly tunable, extended-network, crystalline, nanoporous materials with applications in gas storage, separations, and sensing. We review how molecular models and simulations of gas adsorption in MOFs have lucidly impacted the discovery of performant MOFs for methane, hydrogen, and oxygen storage, xenon, carbon dioxide, and chemical warfare agent capture, and xylene enrichment. Particularly, we highlight how large, open databases of MOF crystal structures, post-processed for molecular simulations, are a platform for computational materials discovery. We pontificate how to orient research efforts to routinize the computational discovery of MOFs for adsorption-based engineering applications.

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Predicting the Features of Methane Adsorption in Large Pore Metal-Organic Frameworks for Energy Storage

Nanomaterials ◽

10.3390/nano8100818 ◽

2018 ◽

Vol 8 (10) ◽

pp. 818 ◽

Cited By ~ 7

Author(s):

George Manos ◽

Lawrence Dunne

Keyword(s):

Gas Adsorption ◽

Metal Organic Frameworks ◽

Gas Storage ◽

Methane Adsorption ◽

Energy Applications ◽

Adsorbed Gas ◽

Theoretical Approaches ◽

Large Pore ◽

Metal Organic ◽

Computer Simulation Studies

Currently, metal-organic frameworks (MOFs) are receiving significant attention as part of an international push to use their special properties in an extensive variety of energy applications. In particular, MOFs have exceptional potential for gas storage especially for methane and hydrogen for automobiles. However, using theoretical approaches to investigate this important problem presents various difficulties. Here we present the outcomes of a basic theoretical investigation into methane adsorption in large pore MOFs with the aim of capturing the unique features of this phenomenon. We have developed a pseudo one-dimensional statistical mechanical theory of adsorption of gas in a MOF with both narrow and large pores, which is solved exactly using a transfer matrix technique in the Osmotic Ensemble (OE). The theory effectively describes the distinctive features of adsorption of gas isotherms in MOFs. The characteristic forms of adsorption isotherms in MOFs reflect changes in structure caused by adsorption of gas and compressive stress. Of extraordinary importance for gas storage for energy applications, we find two regimes of Negative gas adsorption (NGA) where gas pressure causes the MOF to transform from the large pore to the narrow pore structure. These transformations can be induced by mechanical compression and conceivably used in an engine to discharge adsorbed gas from the MOF. The elements which govern NGA in MOFs with large pores are identified. Our study may help guide the difficult program of work for computer simulation studies of gas storage in MOFs with large pores.

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Strain-tunable CO2 storage by black phosphorene and α-PC from combined first principles and molecular dynamics studies

Physical Chemistry Chemical Physics ◽

10.1039/c9cp03676h ◽

2019 ◽

Vol 21 (36) ◽

pp. 20107-20117 ◽

Cited By ~ 3

Author(s):

Xiaohan Song ◽

Yang Liu ◽

Yanmei Yang ◽

Weifeng Li ◽

Mingwen Zhao

Keyword(s):

Molecular Dynamics ◽

Structural Stability ◽

First Principles ◽

Gas Adsorption ◽

Co2 Storage ◽

Layered Materials ◽

Gas Storage ◽

Surface Areas ◽

2D Layered Materials ◽

Black Phosphorene

2D layered materials with puckered structure are promising mediums for gas storage because of their strain-tunable large surface areas and structural stability. The gas adsorption and desorption can be well controlled with strain.

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Influence of Energetic Heterogeneity and Lateral Interactions between Adsorbed Molecules on the Kinetics of Gas Adsorption

Industrial & Engineering Chemistry Research ◽

10.1021/ie101340z ◽

2011 ◽

Vol 50 (6) ◽

pp. 3078-3088 ◽

Cited By ~ 6

Author(s):

Krzysztof Nieszporek ◽

Tomasz Banach

Keyword(s):

Gas Adsorption ◽

Lateral Interactions ◽

Adsorbed Molecules ◽

Energetic Heterogeneity ◽

Kinetics Of

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Application of NRTL activity coefficient model to describe the kinetics of gas adsorption

Open Chemistry ◽

10.2478/s11532-013-0367-4 ◽

2014 ◽

Vol 12 (2) ◽

pp. 185-193

Author(s):

Krzysztof Nieszporek ◽

Tomasz Banach ◽

Przemywslaw Podkościelny

Keyword(s):

Activity Coefficient ◽

Gas Adsorption ◽

Solid Surfaces ◽

Rate Theory ◽

Statistical Rate Theory ◽

Activity Coefficient Model ◽

Energetic Heterogeneity ◽

Adsorption Energy Distribution ◽

Kinetics Of ◽

Heterogeneous Solid

AbstractThe Non-Random Two-Liquid activity coefficient model is applied to describe the kinetics of pure gas adsorption on energetically heterogeneous solid surfaces. The surface energetic heterogeneity has been represented by the Gaussian-like function of the adsorption energy distribution. Two different kinetic isotherms have been presented. One of them, determined by using the statistical rate theory, has been critically discussed. The applicability of the presented approach has been demonstrated by a quantitative analysis of two sets of experimental data previously reported in the literature.

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