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Jacek Jagiello

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Senior Scientist at Micromeritics Instrument Corporation, Norcross, GA, USA.Interested in the development of methods for interpretation and modeling of adsorption measurements. Research interests focused on adsorption properties of non-porous and porous materials. Application of the density functional theory (DFT) for the characterization of porous materials. Recent development: extension of the standard one dimensional NLDFT treatment of confined fluids to two dimensions.

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Papers by Jacek Jagiello

CCDC 1970612: Experimental Crystal Structure Determination

Improved DFT Methods for Micropore Size Characterization of Activated Carbons: Role of Pore Wall Heterogeneity

The density functional theory (DFT) based method for the calculation of pore size distribution (P... more

Low temperature double-layer capacitors with improved energy density: an overview of recent development efforts

Electrochemical double-layer capacitors are finding increased use in a wide range of energy stora... more Electrochemical double-layer capacitors are finding increased use in a wide range of energy storage applications, particularly where high pulse power capabilities are required. Double-layer capacitors store charge at a liquid/solid interface, making them ideal for low temperature power applications, due to the facile kinetic processes associated with the rearrangement of the electrochemical double-layer at these temperatures. Potential low temperature applications include hybrid and electric vehicles, operations in polar regions, high altitude aircraft and aerospace avionics, and distributed environmental and structural health monitoring. State-ofthe-art capacitors can typically operate to -40°C, with a subsequent degradation in power performance below room temperature. However, recent efforts focused on advanced electrolyte and electrode systems can enable operation to temperatures as low as -70°C, with capacities similar to room temperature values accompanied by reasonably low equ...

Crystallizing Atomic Xenon in a Flexible MOF to Probe and Understand Its Temperature-Dependent Breathing Behavior and Unusual Gas Adsorption Phenomenon

Journal of the American Chemical Society

Flexible metal-organic frameworks (MOFs) hold great promise as smart materials for specific appli... more Flexible metal-organic frameworks (MOFs) hold great promise as smart materials for specific applications such as gas separation. These materials undergo interesting structural changes in response to guest molecules, which is often associated with unique adsorption behavior not possible for rigid MOFs. Understanding the dynamic behavior of flexible MOFs is crucial yet challenging as it involves weak host-guest interactions and subtle structural transformation not only at the atomic/molecular level but also in a nonsteady state. We report here an in-depth study on the adsorbate- and temperature-dependent adsorption in a flexible MOF by crystallizing atomic gases into its pores. Mn(ina)2 shows an interesting temperature-dependent response toward noble gases. Its nonmonotonic, temperature-dependent adsorption profile results in an uptake maximum at a temperature threshold, a phenomenon that is unusual. Full characterization of Xe-loaded MOF structures is performed by in situ single-crystal and synchrotron X-ray diffraction, IR spectroscopy, and molecular modeling. The X-ray diffraction analysis offers a detailed explanation into the dynamic structural transformation and provides a convincing rationalization of the unique adsorption behavior at the molecular scale. The guest and temperature dependence of the structural breathing gives rise to an intriguing reverse of Xe/Kr adsorption selectivity as a function of temperature. The presented work may provide further understanding of the adsorption behavior of noble gases in flexible MOF structures.

Exploiting the adsorption of simple gases O2 and H2 with minimal quadrupole moments for the dual gas characterization of nanoporous carbons using 2D-NLDFT models

Carbon

Exploiting the adsorption of simple gases O 2 and H 2 with minimal quadrupole moments for the dua... more

Enhanced resolution of ultra micropore size determination of biochars and activated carbons by dual gas analysis using N2 and CO2 with 2D-NLDFT adsorption models

Carbon

Exploring the effect of ultramicropore distribution on gravimetric capacitance of nanoporous carbons

Electrochimica Acta

Abstract The capacitive performance of activated carbons of similar volume of ultramicropores but... more Abstract The capacitive performance of activated carbons of similar volume of ultramicropores but of marked differences in their pore size distributions was tested in aqueous electrolytes. Dramatic differences in the capacitive behavior were measured in H2SO4, KOH, or in Na2SO4. In the case of the carbon activated with CO2, the sterical hindrances limited the access of Na+ ions to pores resulting in a small capacitance. The results indicated that even though the high volume of micropores is required for a good capacitive behavior, it is not a sufficient condition for granting a high capacitance. It was found that even subtle differences in the ultramicropore distribution can affect dramatically the capacitive behavior and, for a given carbon, the electrolyte type needs be adjusted, if the optimum performance is targeted. That adjustment should be made based on the size of the large ion and its compatibility/similarity with/to the predominant ultramicropore size. Carbon surface chemistry does not play a marked role for carbons with a high degree of microporosity when used as supercapacitor electrodes. Since the size of pores are critical for ion accessibility, it is suggested that enhanced adsorption potential in small pore might also contribute to the high capacitive performance in pores similar in size to ions.

Hierarchically Engineered Mesoporous Metal-Organic Frameworks toward Cell-free Immobilized Enzyme Systems

Chem

Farha and colleagues have developed a strategy for expanding the pore apertures of csq-net Zr-bas... more Farha and colleagues have developed a strategy for expanding the pore apertures of csq-net Zr-based MOFs to obtain an isoreticular series of MOF structures with pore apertures ranging from 3.3 to 6.7 nm. Enzymes immobilized in the MOF are accessible to coenzymes and show higher activity than that of the free enzymes.

A Simple Approach to the 2D Mobile Adsorption of Gases on Heterogeneous Solid Surfaces Exhibiting Random Surface Topography

Adsorption Science & Technology

Based on a summation to infinity of the virial expansion for the 2D compressibility factor, simpl... more Based on a summation to infinity of the virial expansion for the 2D compressibility factor, simple equations have been developed for adsorption isotherms, and heats of adsorption, of 2D dense mobile films adsorbed on solid surfaces. They have subsequently been generalized for the presence of an external, randomly varying potential field, created by the random surface topography exhibited by heterogeneous solid surfaces.

Testing the feasibility of using the density functional theory route for pore size distribution calculations of ordered microporous carbons

Molecular Simulation

ABSTRACT The pore size distribution (PSD) characterization of microporous carbon materials is tra... more ABSTRACT The pore size distribution (PSD) characterization of microporous carbon materials is traditionally obtained from the analysis of N2 adsorption isotherms at 77 K. In this work, we aim at testing the feasibility of using the density functional theory (DFT) route for PSD calculations of interconnected carbon pore structures. The first step of this study was to generate using an atomistic simulation approach, an ordered porous carbon material with well-defined porosity using NaY zeolite as a templating matrix. For this purpose, we used the grand canonical Monte-Carlo (GCMC) technique in which the carbon–carbon interactions were described within the frame of a newly developed tight binding approach and the carbon–zeolite interactions assumed to be characteristic of physisorption. We calculated the PSD of such a carbon porous material. At a second stage, we calculated nitrogen adsorption isotherms at different temperatures. These data were subsequently used as inputs for DFT calculation to obtain the PSD. Comparisons between DFT–PSD and MC–PSD are made. In particular, we show that with an appropriate wall thickness of two graphene layers, the PSD obtained from DFT calculation agrees well with that from direct analysis of the simulated structure.

Hierarchical Structures: Quantifying the Complex Pore Architecture of Hierarchical Faujasite Zeolites and the Impact on Diffusion (Adv. Funct. Mater. 31/2016)

Advanced Functional Materials, 2016

Method for reducing emissions from evaporative emissions control systems

상기 다중 레이어 또는 스테이지의 흡착제를 이용하여 차량용 증발가스 배출 억제 시스템의 일주 온도변화 손실 배출을 현저히 줄이는 방법이다. 바람직하게는 증발가스 배출 억제 시... more 상기 다중 레이어 또는 스테이지의 흡착제를 이용하여 차량용 증발가스 배출 억제 시스템의 일주 온도변화 손실 배출을 현저히 줄이는 방법이다. 바람직하게는 증발가스 배출 억제 시스템의 연료 소스측의 제1 캐니스터(흡수) 영역에 높은 작용용량의 흡착제가 있다. 배출구측의 제 2 캐니스터 영역(들)에 바람직한 흡착제는 상기 연료 소스 측 흡착제와 비교 했을 때, 체적 베이스에서 평평한 또는 평평하게된 등온 흡착곡선 특성을 갖으며, 고농도의 증발가스에 대해서 비교적 낮은 용량을 나타낸다. 상기한 배출구측 캐니스터 영역을 위한 상기한 바람직한 특성을 얻기 위해 여러 가지 방안 설명된다. 제1 방안은 충전재 및/또는 공극을 체적 확산제로 사용하여 등온 흡착곡선을 평평하게 하는 것이다. 제2 방안은 필요 등온 흡착 특성을 갖는 흡착제를 채택하고 희석을 위한 특별한 대처가 요구될 필요가 없게 상기 흡착제를 적합한 형상 또는 형태로 만드는 것이다. 높은 작용용량의 흡착제를 연료 소스측에 그리고 바람직한 낮은 작용용량의 흡착제를 배출구측에 두는 개선된 조합으로, 차량용 증발가스 배출 억제 시스템 캐니스터에서 사용되는 알려진 흡착제와 비교하여 상당히 낮은 일조 온도변화 손실 배출을 제공한다. 연료 증발가스, 캐니스터, 활성탄 흡착제

Quantifying the Complex Pore Architecture of Hierarchical Faujasite Zeolites and the Impact on Diffusion

Advanced Functional Materials, 2016

An exact knowledge of the architecture of complex pore networks and the impact on transport proce... more An exact knowledge of the architecture of complex pore networks and the impact on transport processes is critical to understand and optimize their integration in many functional solids. Here, a robust and versatile approach is demonstrated to quantitatively map pore constrictions within hierarchical faujasite-type (Y and USY) zeolites, the most widely applied zeolitic materials in industry. Differential hysteresis scanning measurements by high-resolution argon sorption coupled with an advanced modeling framework enable the derivation of the amount and size of pyramidal, constricted, and occluded mesopores. This yields unprecedented insight into the impact of widely practiced demetallation treatments on the porosity evolution and clearly highlights the interplay between the geometry of mesopores developed by a given treatment and those introduced by previously applied postsynthetic modifications. Based on the findings, the dynamic assessment by positron annihilation spectroscopy confirms the effectiveness of each mesopore type at enhancing the diffusion of ortho-positronium within the crystal. The quantitative descriptors attained by these complementary techniques can revolutionize the design of porous materials for a wide range of applications.

Method, System and Canister for Reducing Emissions from Evaporative Emissions Control Systems

Composite microporous carbons for fuel gas storage

Direct Structural Evidence of Commensurate-to-Incommensurate Transition of Hydrocarbon Adsorption in a Microporous Metal Organic Framework

Chem. Sci., 2015

Structural evidence of commensurate-to-incommensurate transition of linear hydrocarbon molecules ... more

The first example of commensurate adsorption of atomic gas in a MOF and effective separation of xenon from other noble gases

Chem. Sci., 2014

Enhanced reactive adsorption of H 2 S on Cu–BTC/ S- and N-doped GO composites

J. Mater. Chem. A, 2015

New composites containing Cu–BTC and S- and N-doped graphite oxides (GOs) were synthesized.

Relationship between energetic and structural heterogeneity of microporous carbons determined on the basis of adsorption potentials in model micropores

Langmuir, 1993

... We have chosen these data to study the effect of different adsorbates on calculated adsorptio... more

Adsorption energy and structural heterogeneity of activated carbons

Studies in Surface Science and Catalysis, 1994

Abstract Gas adsorption on activated carbons at supercritical temperatures takes place mainly in ... more Abstract Gas adsorption on activated carbons at supercritical temperatures takes place mainly in micropores of molecular dimensions due to the enhanced adsorption potential in such pores. Relationship between adsorption energy and pore sizes is used to analyze methane adsorption isotherms in order to obtain micropore size distribution. Isosteric heats of adsorption which are related to the adsorption temperature dependence are considered as additional information about the adsorption process and can be used for the verification of the model assumed. Adsorption isotherms of three carbon samples are analyzed, results of the two of them are consistent with the model of slit pores whereas in the case of the third carbon it seems that some other pore model should be considered. Gas chromatographic methods are also applied. In this method alkane molecular probes of different kinetic diameters are used to study the pore structure of these carbons.

CCDC 1970612: Experimental Crystal Structure Determination

Improved DFT Methods for Micropore Size Characterization of Activated Carbons: Role of Pore Wall Heterogeneity

The density functional theory (DFT) based method for the calculation of pore size distribution (P... more

Low temperature double-layer capacitors with improved energy density: an overview of recent development efforts

Electrochemical double-layer capacitors are finding increased use in a wide range of energy stora... more Electrochemical double-layer capacitors are finding increased use in a wide range of energy storage applications, particularly where high pulse power capabilities are required. Double-layer capacitors store charge at a liquid/solid interface, making them ideal for low temperature power applications, due to the facile kinetic processes associated with the rearrangement of the electrochemical double-layer at these temperatures. Potential low temperature applications include hybrid and electric vehicles, operations in polar regions, high altitude aircraft and aerospace avionics, and distributed environmental and structural health monitoring. State-ofthe-art capacitors can typically operate to -40°C, with a subsequent degradation in power performance below room temperature. However, recent efforts focused on advanced electrolyte and electrode systems can enable operation to temperatures as low as -70°C, with capacities similar to room temperature values accompanied by reasonably low equ...

Crystallizing Atomic Xenon in a Flexible MOF to Probe and Understand Its Temperature-Dependent Breathing Behavior and Unusual Gas Adsorption Phenomenon

Journal of the American Chemical Society

Flexible metal-organic frameworks (MOFs) hold great promise as smart materials for specific appli... more Flexible metal-organic frameworks (MOFs) hold great promise as smart materials for specific applications such as gas separation. These materials undergo interesting structural changes in response to guest molecules, which is often associated with unique adsorption behavior not possible for rigid MOFs. Understanding the dynamic behavior of flexible MOFs is crucial yet challenging as it involves weak host-guest interactions and subtle structural transformation not only at the atomic/molecular level but also in a nonsteady state. We report here an in-depth study on the adsorbate- and temperature-dependent adsorption in a flexible MOF by crystallizing atomic gases into its pores. Mn(ina)2 shows an interesting temperature-dependent response toward noble gases. Its nonmonotonic, temperature-dependent adsorption profile results in an uptake maximum at a temperature threshold, a phenomenon that is unusual. Full characterization of Xe-loaded MOF structures is performed by in situ single-crystal and synchrotron X-ray diffraction, IR spectroscopy, and molecular modeling. The X-ray diffraction analysis offers a detailed explanation into the dynamic structural transformation and provides a convincing rationalization of the unique adsorption behavior at the molecular scale. The guest and temperature dependence of the structural breathing gives rise to an intriguing reverse of Xe/Kr adsorption selectivity as a function of temperature. The presented work may provide further understanding of the adsorption behavior of noble gases in flexible MOF structures.

Exploiting the adsorption of simple gases O2 and H2 with minimal quadrupole moments for the dual gas characterization of nanoporous carbons using 2D-NLDFT models

Carbon

Exploiting the adsorption of simple gases O 2 and H 2 with minimal quadrupole moments for the dua... more

Enhanced resolution of ultra micropore size determination of biochars and activated carbons by dual gas analysis using N2 and CO2 with 2D-NLDFT adsorption models

Carbon

Exploring the effect of ultramicropore distribution on gravimetric capacitance of nanoporous carbons

Electrochimica Acta

Abstract The capacitive performance of activated carbons of similar volume of ultramicropores but... more Abstract The capacitive performance of activated carbons of similar volume of ultramicropores but of marked differences in their pore size distributions was tested in aqueous electrolytes. Dramatic differences in the capacitive behavior were measured in H2SO4, KOH, or in Na2SO4. In the case of the carbon activated with CO2, the sterical hindrances limited the access of Na+ ions to pores resulting in a small capacitance. The results indicated that even though the high volume of micropores is required for a good capacitive behavior, it is not a sufficient condition for granting a high capacitance. It was found that even subtle differences in the ultramicropore distribution can affect dramatically the capacitive behavior and, for a given carbon, the electrolyte type needs be adjusted, if the optimum performance is targeted. That adjustment should be made based on the size of the large ion and its compatibility/similarity with/to the predominant ultramicropore size. Carbon surface chemistry does not play a marked role for carbons with a high degree of microporosity when used as supercapacitor electrodes. Since the size of pores are critical for ion accessibility, it is suggested that enhanced adsorption potential in small pore might also contribute to the high capacitive performance in pores similar in size to ions.

Hierarchically Engineered Mesoporous Metal-Organic Frameworks toward Cell-free Immobilized Enzyme Systems

Chem

Farha and colleagues have developed a strategy for expanding the pore apertures of csq-net Zr-bas... more Farha and colleagues have developed a strategy for expanding the pore apertures of csq-net Zr-based MOFs to obtain an isoreticular series of MOF structures with pore apertures ranging from 3.3 to 6.7 nm. Enzymes immobilized in the MOF are accessible to coenzymes and show higher activity than that of the free enzymes.

A Simple Approach to the 2D Mobile Adsorption of Gases on Heterogeneous Solid Surfaces Exhibiting Random Surface Topography

Adsorption Science & Technology

Based on a summation to infinity of the virial expansion for the 2D compressibility factor, simpl... more Based on a summation to infinity of the virial expansion for the 2D compressibility factor, simple equations have been developed for adsorption isotherms, and heats of adsorption, of 2D dense mobile films adsorbed on solid surfaces. They have subsequently been generalized for the presence of an external, randomly varying potential field, created by the random surface topography exhibited by heterogeneous solid surfaces.

Testing the feasibility of using the density functional theory route for pore size distribution calculations of ordered microporous carbons

Molecular Simulation

ABSTRACT The pore size distribution (PSD) characterization of microporous carbon materials is tra... more ABSTRACT The pore size distribution (PSD) characterization of microporous carbon materials is traditionally obtained from the analysis of N2 adsorption isotherms at 77 K. In this work, we aim at testing the feasibility of using the density functional theory (DFT) route for PSD calculations of interconnected carbon pore structures. The first step of this study was to generate using an atomistic simulation approach, an ordered porous carbon material with well-defined porosity using NaY zeolite as a templating matrix. For this purpose, we used the grand canonical Monte-Carlo (GCMC) technique in which the carbon–carbon interactions were described within the frame of a newly developed tight binding approach and the carbon–zeolite interactions assumed to be characteristic of physisorption. We calculated the PSD of such a carbon porous material. At a second stage, we calculated nitrogen adsorption isotherms at different temperatures. These data were subsequently used as inputs for DFT calculation to obtain the PSD. Comparisons between DFT–PSD and MC–PSD are made. In particular, we show that with an appropriate wall thickness of two graphene layers, the PSD obtained from DFT calculation agrees well with that from direct analysis of the simulated structure.

Hierarchical Structures: Quantifying the Complex Pore Architecture of Hierarchical Faujasite Zeolites and the Impact on Diffusion (Adv. Funct. Mater. 31/2016)

Advanced Functional Materials, 2016

Method for reducing emissions from evaporative emissions control systems

상기 다중 레이어 또는 스테이지의 흡착제를 이용하여 차량용 증발가스 배출 억제 시스템의 일주 온도변화 손실 배출을 현저히 줄이는 방법이다. 바람직하게는 증발가스 배출 억제 시... more 상기 다중 레이어 또는 스테이지의 흡착제를 이용하여 차량용 증발가스 배출 억제 시스템의 일주 온도변화 손실 배출을 현저히 줄이는 방법이다. 바람직하게는 증발가스 배출 억제 시스템의 연료 소스측의 제1 캐니스터(흡수) 영역에 높은 작용용량의 흡착제가 있다. 배출구측의 제 2 캐니스터 영역(들)에 바람직한 흡착제는 상기 연료 소스 측 흡착제와 비교 했을 때, 체적 베이스에서 평평한 또는 평평하게된 등온 흡착곡선 특성을 갖으며, 고농도의 증발가스에 대해서 비교적 낮은 용량을 나타낸다. 상기한 배출구측 캐니스터 영역을 위한 상기한 바람직한 특성을 얻기 위해 여러 가지 방안 설명된다. 제1 방안은 충전재 및/또는 공극을 체적 확산제로 사용하여 등온 흡착곡선을 평평하게 하는 것이다. 제2 방안은 필요 등온 흡착 특성을 갖는 흡착제를 채택하고 희석을 위한 특별한 대처가 요구될 필요가 없게 상기 흡착제를 적합한 형상 또는 형태로 만드는 것이다. 높은 작용용량의 흡착제를 연료 소스측에 그리고 바람직한 낮은 작용용량의 흡착제를 배출구측에 두는 개선된 조합으로, 차량용 증발가스 배출 억제 시스템 캐니스터에서 사용되는 알려진 흡착제와 비교하여 상당히 낮은 일조 온도변화 손실 배출을 제공한다. 연료 증발가스, 캐니스터, 활성탄 흡착제

Quantifying the Complex Pore Architecture of Hierarchical Faujasite Zeolites and the Impact on Diffusion

Advanced Functional Materials, 2016

An exact knowledge of the architecture of complex pore networks and the impact on transport proce... more An exact knowledge of the architecture of complex pore networks and the impact on transport processes is critical to understand and optimize their integration in many functional solids. Here, a robust and versatile approach is demonstrated to quantitatively map pore constrictions within hierarchical faujasite-type (Y and USY) zeolites, the most widely applied zeolitic materials in industry. Differential hysteresis scanning measurements by high-resolution argon sorption coupled with an advanced modeling framework enable the derivation of the amount and size of pyramidal, constricted, and occluded mesopores. This yields unprecedented insight into the impact of widely practiced demetallation treatments on the porosity evolution and clearly highlights the interplay between the geometry of mesopores developed by a given treatment and those introduced by previously applied postsynthetic modifications. Based on the findings, the dynamic assessment by positron annihilation spectroscopy confirms the effectiveness of each mesopore type at enhancing the diffusion of ortho-positronium within the crystal. The quantitative descriptors attained by these complementary techniques can revolutionize the design of porous materials for a wide range of applications.

Method, System and Canister for Reducing Emissions from Evaporative Emissions Control Systems

Composite microporous carbons for fuel gas storage

Direct Structural Evidence of Commensurate-to-Incommensurate Transition of Hydrocarbon Adsorption in a Microporous Metal Organic Framework

Chem. Sci., 2015

Structural evidence of commensurate-to-incommensurate transition of linear hydrocarbon molecules ... more

The first example of commensurate adsorption of atomic gas in a MOF and effective separation of xenon from other noble gases

Chem. Sci., 2014

Enhanced reactive adsorption of H 2 S on Cu–BTC/ S- and N-doped GO composites

J. Mater. Chem. A, 2015

New composites containing Cu–BTC and S- and N-doped graphite oxides (GOs) were synthesized.

Relationship between energetic and structural heterogeneity of microporous carbons determined on the basis of adsorption potentials in model micropores

Langmuir, 1993

... We have chosen these data to study the effect of different adsorbates on calculated adsorptio... more

Adsorption energy and structural heterogeneity of activated carbons

Studies in Surface Science and Catalysis, 1994

Abstract Gas adsorption on activated carbons at supercritical temperatures takes place mainly in ... more Abstract Gas adsorption on activated carbons at supercritical temperatures takes place mainly in micropores of molecular dimensions due to the enhanced adsorption potential in such pores. Relationship between adsorption energy and pore sizes is used to analyze methane adsorption isotherms in order to obtain micropore size distribution. Isosteric heats of adsorption which are related to the adsorption temperature dependence are considered as additional information about the adsorption process and can be used for the verification of the model assumed. Adsorption isotherms of three carbon samples are analyzed, results of the two of them are consistent with the model of slit pores whereas in the case of the third carbon it seems that some other pore model should be considered. Gas chromatographic methods are also applied. In this method alkane molecular probes of different kinetic diameters are used to study the pore structure of these carbons.