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At least 217 records · Page 12

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DOE OSTI2023

CO 2 adsorption mechanisms at the ZIF-8 interface in a Type 3 porous liquid

Porous liquids (PLs) are an attractive material for gas separation and carbon sequestration due to their permanent internal porosity and high adsorption capacity. PLs that contain zeolitic imidazole frameworks (ZIFs), such as ZIF-8, form PLs through exclusion of aqueous solvents from the framework pore due to its hydrophobicity. The gas adsorption sites in ZIF-8 based PLs are historically unknown; gas molecules could be captured in the ZIF-8 pore or adsorb at the ZIF-8 interface. To address this question, ab initio molecular dynamics was used to predict CO 2 binding sites in a PL composed of a ZIF-8 particle solvated in a water, ethylene glycol, and 2-methylimidazole solvent system. Further, the results show that CO 2 energetically prefers to reside inside the ZIF-8 pore aperture due to strong van der Waals interactions with the terminal imidazoles. However, the CO 2 binding site can be blocked by larger solvent molecules that have greater adsorption interactions. CO 2 molecules were unable to diffuse into the ZIF-8 pore, with CO 2 adsorption occurring due to binding with the ZIF-8 surface. Therefore, future design of ZIF-based PLs for enhanced CO 2 adsorption should be based on the strength of gas binding at the solvated particle surface.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Effect of Zeolitization on Noble Gas Transport in Natural Materials [Poster]

The goal of this project is to quantify the effect of adsorption on noble gas transport though rocks that contain zeolite compared with rocks that don't. Success is defined by developing a coefficient called Retardation that describes the separation effect of zeolites. This coefficient can then be used by gas transport modelers to predict field-scale observations of noble gases released underground in a chemical explosion

36 MATERIALS SCIENCE↗

DOE OSTI2023

Elucidating the Influence of Metal Surface Composition on Organic Adsorbate Binding Using Active Particle Dynamics

The adsorption strengths of organic compounds on metal surfaces are sensitive to the metal composition, and they play a central role in many catalytic reactions, helping to control the coverage of the reactant and altering the overall reaction rate. While adsorption energies are straightforward to measure and calculate in vacuum and gas-phase environments, adsorption energetics can be dramatically altered by the presence of solvent in liquid-phase reactions. However, the effects of metal composition on binding strengths in a liquid environment are less well understood, primarily due to the difficulty of accurate in situ measurements of organic binding on metal surfaces in the liquid phase. Here, we utilize the motion of active particles in water to probe the adsorption energies of an organic adsorbate (furfural) on a range of metal surfaces (pure Pd, pure Pt, and four PdAu alloy compositions) to elucidate the effect of metal composition. Janus particles with catalytic caps of particular metal compositions all exhibited active motion resulting from consumption of H 2 O 2 ; adsorbate binding was inferred through the decrease in the velocity of active motion and was modeled by a Langmuir adsorption isotherm. The measured adsorption affinities were used to extract the adsorption enthalpy of furfural on the different metals. The Pd surface was found to bind furfural more strongly than the Pt surface by some 10 kJ/mol. Furthermore, the adsorption of furfural on the alloys was found to increase monotonically in magnitude with Pd content. As a result, the data reported herein aid the development of accurate understanding of organic adsorption in the presence of solvent and the role of the metal surface in tuning adsorption strengths to optimize catalytic processes in the liquid phase.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Cooperative chemical adsorption of acid gases in functionalized metal-organic frameworks

A system and method for acid gas separations using porous frameworks of metal atoms coordinatively bound to polytopic linkers that are functionalized with basic nitrogen ligands that expose nitrogen atoms to the pore volumes forming adsorption sites. Adjacent basic nitrogen ligands on the metal-organic framework can form an ammonium from one ligand and a carbamate from the other. The formation of one ammonium carbamate pair influences the formation of ammonium carbamate on adjacent adsorption sites. Adsorption of acid gas at the adsorption sites form covalently linked aggregates of more than one ammonium carbamate ion pair. The acid gas adsorption isotherm can be tuned to match the step position with the partial pressure of acid gas in the gas mixture stream through manipulation of the metal-ligand bond strength by selection of the ligand, metal and polytopic linker materials.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Cooperative chemical adsorption of acid gases in functionalized metal-organic frameworks

Long, Jeffrey R.↗

DOE OSTI2020

Effects of natural zeolites on field-scale geologic noble gas transport

Improving predictive models for noble gas transport through natural materials at the field-scale is an essential component of improving US nuclear monitoring capabilities. Several field-scale experiments with a gas transport component have been conducted at the Nevada National Security Site (Non-Proliferation Experiment, Underground Nuclear Explosion Signatures Experiment). However, the models associated with these experiments have not treated zeolite minerals as gas adsorbing phases. This is significant as zeolites are a common alteration mineral with a high abundance at these field sites and are shown here to significantly fractionate noble gases during field-scale transport. This fractionation and associated retardation can complicate gas transport predictions by reducing the signal-to-noise ratio to the detector (e.g. mass spectrometers or radiation detectors) enough to mask the signal or make the data difficult to interpret. Omitting adsorption-related retardation data of noble gases in predictive gas transport models therefore results in systematic errors in model predictions where zeolites are present.Herein is presented noble gas adsorption data collected on zeolitized and non-zeolitized tuff. Experimental results were obtained using a unique piezometric adsorption system designed and built for this study. Data collected were then related to pure-phase mineral analyses conducted on clinoptilolite, mordenite, and quartz. These results quantify the adsorption capacity of materials present in field-scale systems, enabling the modeling of low-permeability rocks as significant sorption reservoirs vital to bulk transport predictions.

58 GEOSCIENCES↗

DOE OSTI2023

Bench-Scale Testing of a High Efficiency, Ultra-Compact Process for Pre-Combustion CO 2 Capture (Final Report)

The overarching objective of this bench-scale study is to field-validate the technical feasibility of a membrane- and adsorption-enhanced water gas shift (WGS) reaction process that employs a carbon molecular sieve (CMS) membrane reactor (MR) followed by an adsorption reactor (AR) for pre-combustion CO 2 capture while demonstrating progress towards achievement of the overall performance goals of CO 2 capture with 95% CO 2 purity at a cost of electricity (COE) of 30% less than the baseline capture approaches. The main goal of this bench-scale project is to advance the proposed MR-AR transformative CO 2 capture technology to a sufficient maturity level so that our present industrial partners (M&PT and Worley) can potentially adapt the technology for further small pilot-scale testing. The project began at TRL 4, as the system prototype had already been validated in the laboratory on simulated syngas (as part of project DE-FE0026423). The project ended at TRL 5, via scaling-up of the prototype system and testing it on actual syngas at a host site (CAER at the University of Kentucky (UKy)). The project was carried-out in two different phases: In Phase I (during BP1 of the project), the team designed, constructed, and assembled the bench-scale experimental MR-AR system, prepared the membranes, adsorbents, and catalysts, tested the bench-scale unit with simulated syngas to validate functionality, and prepared a preliminary TEA of the technology. In Phase II (during BP2 of the project), the team installed the unit at the test site at the UKy site and completed all utility connections and hookups, field-tested the novel MR-AR process in the bench-scale system using real syngas, collected and analyzed experimental data, and completed a detailed TEA of the technology. A key aim of the project was to identify and address the technical and process risks and to generate information to advance the technology to the next stage of development. All project milestones and success criteria were met. Specifically, the team: (i) designed, constructed and assembled a bench scale system that handled 1 – 5 scfm syngas and tested its functionality with simulated syngas; (ii) prepared high performance CMS membrane tubes (ID: 3.5 mm, OD: 5.7 mm, 30” long) that meet the target H 2 permeance ( > 1 m 3 /(m 2 .hr.bar) or (> 370.3 GPU)) and a target H 2 /CO selectivity >80 at the relevant temperature (up to 300oC) and pressure conditions (up to 25 bar) with a <10% decline in performance over each 250 hr. testing period (iii) procured commercial sour-shift catalyst in sufficient quantity and prepared up to 10 kg of pelletized adsorbent for use at relevant conditions (250oC 2.5wt.% and target sorbent attrition rate < 0.2; (iv) installed the bench-scale unit at the test site (UKy) and tested the MR-AR technology using real syngas for over 250 hr. for both static and flow experiments; (v) updated the TEA analysis based on bench-scale data and met CO 2 capture goals of 95% CO 2 purity at a cost of electricity 30% less than baseline capture approaches. The CMS membranes, HTC adsorbents and catalysts employed all exhibited very robust and stable performance during the long-term run (over a >250 hr live syngas run). Furthermore, the proposed MR-AR IGCC system achieved a LCOE with a N 2 sale price of $\$$ 30/ton, with N 2 compression (no N 2 compression) of 101.2 $\$$/MWh (95.3 $\$$/MWh), which represents a 29.8% (33.9%) LCOE reduction in the baseline IGCC with carbon capture of 144.2 $\$$/MWh. The proposed MR-AR IGCC delivers a CO 2 capture cost of 44.8 $\$$/tonne (39.9 $\$$/tonne) vs 98.1 $\$$/tonne of the baseline capture case and a net power production of 586 MWe (623 MWe) vs 556 MWe of the baseline capture case.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2024

Field-Scale Testing of a High-Efficiency Membrane Reactor (MR)—Adsorptive Reactor (AR) Process for H2 Generation and Pre-Combustion CO2 Capture

The study objective was to field-validate the technical feasibility of a membrane- and adsorption-enhanced water gas shift reaction process employing a carbon molecular sieve membrane (CMSM)-based membrane reactor (MR) followed by an adsorptive reactor (AR) for pre-combustion CO2 capture. The project was carried out in two different phases. In Phase I, the field-scale experimental MR-AR system was designed and constructed, the membranes, and adsorbents were prepared, and the unit was tested with simulated syngas to validate functionality. In Phase II, the unit was installed at the test site, field-tested using real syngas, and a technoeconomic analysis (TEA) of the technology was completed. All project milestones were met. Specifically, (i) high-performance CMSMs were prepared meeting the target H2 permeance (>1 m3/(m2.hbar) and H2/CO selectivity of >80 at temperatures of up to 300 °C and pressures of up to 25 bar with a <10% performance decline over the testing period; (ii) pelletized adsorbents were prepared for use in relevant conditions (250 °C < T < 450 °C, pressures up to 25 bar) with a working capacity of >2.5 wt.% and an attrition rate of <0.2; (iii) TEA showed that the MR-AR technology met the CO2 capture goals of 95% CO2 purity at a cost of electricity (COE) 30% less than baseline approaches.

42 ENGINEERING↗

DOE OSTI2022

On multidomain multiscale modeling and simulation of a novel partial pressure and temperature swing adsorptive reactor ($\mathrm{PPTSAR}$) with application to the water gas shift reaction

Here in this work, a dynamic, multidomain, multiscale model of a novel Partial Pressure and Temperature Swing Adsorptive Reactor (PPTSAR) Process is developed and simulated for a Water Gas Shift Reaction (WGSR) application. The proposed model couples the reactor wall, catalyst/adsorbent pellet, and fluid mixture domains at their respective scales to comprehensively model mass, momentum, and energy transport phenomena occurring within each domain. The resulting model elucidates the PPTSAR’s start-up, transient, and long-term, periodic, dynamic behavior, during both adsorption/reaction and desorption operating modes. In the WGSR application considered, the use of two PPTSARs is shown to allow continuous operation that delivers CO conversion greater than 95% with simultaneous complete CO 2 capture.

42 ENGINEERING↗

NASA NTRS2003

The use of rice hulls for sustainable control of NOx emissions in deep space missions

The use of the activated carbon produced from rice hulls to control NOx emissions for future deep space missions has been demonstrated. The optimal carbonization temperature range was found to be between 600 and 750 degrees C. A burnoff of 61.8% was found at 700 degrees C in pyrolysis and 750 degrees C in activation. The BET surface area of the activated carbon from rice hulls was determined to be 172 m2/g when prepared at 700 degrees C. The presence of oxygen in flue gas is essential for effective adsorption of NO by activated carbon. On the contrary, water vapor inhibits the adsorption efficiency of NO. Consequently, water vapor in flue gas should be removed by drying agents before adsorption to ensure high NO adsorption efficiency. All of the NO in the flue gas was removed for more than 1.5 h when 10% oxygen was present and the ratio of the carbon weight to the flue gas flow rate (W/F) was 15.4 g min/L. Reduction of the adsorbed NO to form N2 could be effectively accomplished under anaerobic conditions at 550 degrees C. The adsorption capacity of NO on the activated carbon was found to be 5.02 mg of NO/g of carbon. The loss of carbon mass was determined to be about 0.16% of the activated carbon per cycle of regeneration if the regeneration occurred when the NO in the flue gas after the carbon bed reached 4.8 ppm, the space maximum allowable concentration. The reduction of the adsorbed NO also regenerated the activated carbon, and the regenerated activated carbon exhibited an improved NO adsorption efficiency.

NASA Program Advanced Human Support Technology↗

NASA NTRS1999

Effects of Cabin Upsets on Adsorption Columns for Air Revitalization

The National Aeronautics and Space Administration (NASA) utilizes adsorption technology as part of contaminant removal systems designed for long term missions. A variety of trace contaminants can be effectively removed from gas streams by adsorption onto activated carbon. An activated carbon adsorption column meets NASA's requirements of a lightweight and efficient means of controlling trace contaminant levels aboard spacecraft and space stations. The activated carbon bed is part of the Trace Contaminant Control System (TCCS) which is utilized to purify the cabin atmosphere. TCCS designs oversize the adsorption columns to account for irregular fluctuations in cabin atmospheric conditions. Variations in the cabin atmosphere include changes in contaminant concentrations, temperature, and relative humidity. Excessively large deviations from typical conditions can result from unusual crew activity, equipment malfunctions, or even fires. The research carried out under this award focussed in detail on the effects of cabin upsets on the performance of activated carbon adsorption columns. Both experiments and modeling were performed with an emphasis on the roll of a change in relative humidity on adsorption of trace contaminants. A flow through fixed-bed apparatus was constructed at the NASA Ames Research Center, and experiments were performed there by W. Scot Appel under the direction of Dr. John E. Finn. Modeling work was performed at the University of Virginia and at Vanderbilt University by W. Scot Appel under the direction of M. Douglas LeVan. All three participants collaborated in all of the various phases of the research. The most comprehensive document describing the research is the Ph.D. dissertation of W. Scot Appel. Results have been published in several papers and presented in talks at technical conferences. All documents have been transmitted to Dr. John E. Finn.

LeVan, M. Douglas↗

NASA NTRS1999

Effects of Cabin Upsets on Adsorption Columns for Air Revitalization

The National Aeronautics and Space Administration (NASA) utilizes adsorption technology as part of contaminant removal systems designed for long term missions. A variety of trace contaminants can be effectively removed from gas streams by adsorption onto activated carbon. An activated carbon adsorption column meets NASA's requirements of a lightweight and efficient means of controlling trace contaminant levels aboard spacecraft and space stations. The activated carbon bed is part of the Trace Contaminant Control System (TCCS) which is utilized to purify the cabin atmosphere. TCCS designs oversize the adsorption columns to account for irregular fluctuations in cabin atmospheric conditions. Variations in the cabin atmosphere include changes in contaminant concentrations, temperature, and relative humidity. Excessively large deviations from typical conditions can result from unusual crew activity, equipment malfunctions, or even fires. The research carried out under this award focussed in detail on the effects of cabin upsets on the performance of activated carbon adsorption columns. Both experiments and modeling were performed with an emphasis on the roll of a change in relative humidity on adsorption of trace contaminants. A flow through fixed-bed apparatus was constructed at the NASA Ames Research Center, and experiments were performed there. Modeling work was performed at the University of Virginia.

LeVan, Douglas↗

NASA NTRS2003

Method for the control of NOx emissions in long-range space travel

The wheat straw, an inedible biomass that can be continuously produced in a space vehicle has been used to produce activated carbon for effective control of NOx emissions from the incineration of wastes. The optimal carbonization temperature of wheat straw was found to be around 600 degrees C when a burnoff of 67% was observed. The BET surface area of the activated carbon produced from the wheat straw reached as high as 300 m2/g. The presence of oxygen in flue gas is essential for effective adsorption of NO by activated carbon. On the contrary, water vapor inhibits the adsorption efficiency of NO. Consequently, water vapor in flue gas should be removed by drying agents before adsorption to ensure high NO adsorption efficiency. All of the NO in the flue gas was removed for more than 2 h by the activated carbons when 10% oxygen was present and the ratio of carbon weight to the flue gas flow rate (W/F) was 30 g min/L, with a contact time of 10.2 s. All of NO was reduced to N2 by the activated carbon at 450 degrees C with a W/F ratio of 15 g min/L and a contact time of 5.1 s. Reduction of the adsorbed NO also regenerated the activated carbon, and the regenerated activated carbon exhibited an improved NO adsorption efficiency. However, the reduction of the adsorbed NO resulted in a loss of carbon which was determined to be about 0.99% of the activated carbon per cycle of regeneration. The sufficiency of the amount of wheat straw in providing the activated carbon based on a six-person crew, such as the mission planned for Mars, has been determined. This novel approach for the control of NOx emissions is sustainable in a closed system such as the case in space travel. It is simple to operate and is functional under microgravity environment.

NASA Discipline Life Support Systems↗

DOE OSTI2024

Exploring the Influence of Linker Substitution and Ratios on Cooperative Framework Flexibility through the Mixed-Linker Approach

Cooperatively flexible metal–organic frameworks that exhibit step-shaped, or Type V-like, adsorption–desorption profiles can lower requisite pressure–temperature swings and thus energy input, necessary for an array of gas storage, delivery, and separations applications. However, such benefits are lost if the pressure threshold of the adsorption and desorption steps at a given temperature does not match the conditions dictated by the application, such as H 2 storage and delivery or olefin–paraffin separations. Unfortunately, the discovery of cooperatively flexible frameworks remains wholly serendipitous and de novo design remains impossible. Accordingly, there is a great need to further our understanding of flexibility such that we can intuitively derivatize known frameworks and, ultimately, design entirely new ones to meet the requisite conditions of energy-consumptive processes. In this work, we demonstrate that the mixed-linker, or multivariate, approach is a powerful tool for the derivation of a known flexible framework, with variances in linker substitution and ratio giving rise to a family wherein significant changes to the step-shaped adsorption–desorption profiles for multiple adsorbates are observed. Specifically, we report 12 isostructural mixed-linker derivatives of CdIF-13 (sod–Cd(benzimidazolate) 2 ) with six point-modified benzimidazole linkers spontaneously synthesized through prototypical solvothermal conditions. Furthermore, each is shown by PXRD to exhibit similar reversible flexibility to CdIF-13 and by TGA and DSC to be similarly thermally stable. Isothermal gas adsorption measurements with N 2 at 77 K, CO 2 at 195 K, and propane at 298 K demonstrate the wide-ranging, adsorbate-dependent effects of linker substitution and ratio, including dramatic reductions in the adsorption threshold pressure, evolution of multiple steps, and complete absence of observable adsorption. Aided by prior crystallographic characterization of CdIF-13, the observed trends were analyzed in an attempt to resolve the influence of linker substitution and ratios on structural behavior. In total, this work illustrates how the mixed-linker approach enables the synthesis and study of a large catalog of functionally modified frameworks, which can help identify the variables that influence flexibility and sorption behavior.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

A Numerical Study on the Energy Performance of a Novel Furnace With Acidic Gas Trap Absorbers

Natural gas furnaces are widely used in US residential and commercial building markets. An important issue for natural gas furnaces is serious corrosion and fouling problems caused by acidic gas, such as SOx. An advanced adsorption technology based on acidic gas trap (AGT) absorbers offers the possibility to remove SOx acidic gas from natural gas furnaces with high efficiency and low cost, thereby enabling the development of condensing furnaces without the use of expensive corrosion resistant materials in the heat exchanger. A three-dimensional (3D) computational fluid dynamics (CFD) model has been developed to evaluate the heat transfer performance of a furnace with AGT absorbers and to compare it with a baseline conventional furnace without the AGT. Moreover, an axisymmetric model has been built focusing on the absorbing process in the AGT. The baseline conventional furnace used for the study is a commercial condensing furnace (Rheem 92% AFUE 84,000 BTU Multi-Position Gas Furnace). This furnace was completely disassembled, and the dimensions of each part were carefully measured and used to build a detailed CFD model. A model representing the new furnace, incorporating the AGT absorbers, was developed by adding the AGT system to the conventional furnace model. For the CFD analysis, a mixture model was employed to characterize the heat and mass transfer during the condensing process in the furnace while considering three components—air, water vapor and liquid water. Condensation takes place in the condensing heat exchanger, where water vapor changes phase to liquid water, and the latent heat is thus used in the furnace for useful heating. The simulation results characterize the energy performance of both the conventional furnace and the novel furnace with AGT absorbers, as well as the reactive processing in the AGT. These results provide insightful guidance for the development of the AGT absorber-based furnace from the perspective of its energy performance and will be used to further optimize this novel furnace design.

Laclair, Tim↗

DOE OSTI2025

Isopotential Electron Titration of Ammonia Charge Transfer on Metal Catalysts

Electron transfer between adsorbates and surfaces determines the binding strength and reactivity of chemical moieties on materials designed for separations and catalysis. To quantify electron exchange, the extent of charge transfer resulting from ammonia adsorption on a Ru surface was measured by isopotential electron titration (IET) on a Ru catalytic condenser, where isopotential conditions were maintained between Ru and silicon separated by an insulating HfO 2 layer during gas phase ammonia adsorption. Charge transfer upon ammonia adsorption on a Ru catalytic condenser increased from 40 to 1200 nC/cm 2 at 75 and 225 °C, respectively. Charge transfer measurements provided a direct estimate of ammonia adsorption thermodynamics on Ru without knowing surface coverages a priori, revealing an adsorption enthalpy of −53 ± 10 kJ/mol and entropy of −61 ± 26 J/mol·K. Combining experimentally-measured charge transfer with kinetic Monte Carlo simulations informed adsorbate surface coverages determined that 0.058 electrons were transferred to the Ru surface for each molecular ammonia adsorption event (δ NH 3 = 0.058 ± 0.005 e – /NH 3 *), consistent with calculated Bader charges. The ability to measure the extent of charge transfer for adsorbed species provides a fundamental descriptor to understand existing and new chemically functional surfaces, providing a foundational method for the emerging field of thermochemical surface coulometry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Porous ceramic supports for resistively heated hybrid gas sorbents

A porous sorbent ceramic product includes a three-dimensional structure having an electrically conductive ceramic material, wherein the conductive ceramic material has an open cell structure with a plurality of intra-material pores, a sorbent additive primarily present in the intra-material pores of the conductive ceramic material for adsorption of a gas, and at least two electrodes in electrical communication with the conductive ceramic material.

Ellebracht, Nathan C.↗

DOE OSTI2021

Simulation of 12-bed vacuum pressure-swing adsorption for hydrogen separation from methanol-steam reforming off-gas

This study focuses on analysis of a 12-bed vacuum pressure-swing adsorption (VPSA) process capable of purifying hydrogen from a ternary mixture (H 2 /CO 2 /CO 75/24/1 mol%) derived from methanol-steam reforming. The process produces 9 kmol H 2 /h with less than 2 ppm and 0.2 ppm of CO2 and CO, respectively, to supply a polymer electrolyte membrane fuel cell. The process model is developed in Aspen Adsorption® using the “uni-bed” approach. A parametric study of H 2 purity and recovery with respect to adsorption pressure, adsorbent height, activated carbon:zeolite ratio, feed composition, and number of beds is performed. Results show 12-bed VPSA can meet the H 2 purity goals, with H 2 recovery as high as 75.75%. Adsorption occurs at 7 bar, the column height is 1.2 m, and the adsorbent ratio is 70%:30%. Furthermore, a 4-bed VPSA can achieve the same purity goals as the 12-bed process, but H 2 recovery decreases to 61.34%.

03 NATURAL GAS↗