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Hydroxide Exchange Membrane Carbon Capture (HEMCC) Using Nickel Hydroxide Batteries and Flow-through Membranes
Proposed is an electrochemical nickel hydroxide based hydroxide exchange membrane carbon capture (HEMCC) device for Direct Air Capture (DAC) of CO2. DAC has been identified as one of the key net negative carbon technologies to achieve net zero carbon emissions. Net negative carbon technologies are required to offset continued emissions from dilute CO2 sources such as agriculture and construction. The majority of current DAC technologies at scale (>1 KT∙yr-1) are adsorbent based technologies with significant energy cost. The traditional DAC energy cost is primarily driven by the temperature swing required to regenerate the sorbent and has been shown to be 1.8 MWh·ton-1 at the system level. Electrochemical pH swing devices are a growing research area for carbon capture devices with the goal of lowering the energy cost required for DAC. A pH gradient is built by generating OH- at the cathode and consuming OH- at the anode. An acid-base equilibrium with CO2 allows for the capture of CO2 at the cathode and release at the anode. This extends from other electrochemical CO2 capture devices based on pKa shifts of an electrochemically active organic species allowing for the capture and release of CO2. Electrochemical CO2 capture is considered promising based on potentially low energy costs to capture CO2 in comparison with current temperature swing adsorption technologies. This work explores Ni(OH)2 electrodes to produce the pH gradient for CO2 capture and release. At the cathode NiOOH is reduced to Ni(OH)2 while at the anode Ni(OH)2 is oxidized to NiOOH. The symmetrical electrodes allow for a low voltage requirement; the thermodynamic potential difference of standard electrochemical reactions is zero. Most of the voltage observed is to produce the pH gradient with the remainder driving the polarization of the electrodes. There is a resistance component as well, but this is small in comparison due to the low current densities used in the device, nominally 2 mA·cm-1. Two similar devices are presented, a traditional MEA (membrane electrode assembly) and a flow-through MEA. The traditional MEA separates the two Ni(OH)2 electrodes with an 80μm Piperion® membrane. While the flow-through membrane separates the electrodes with a three piece membrane consisting of two 80μm Piperion® membranes with a porous membrane between them. In the traditional MEA system air is passed over the cathode for capture, while the flow-through MEA the air is passed through the porous membrane isolated from the electrodes. The traditional MEA has been used to establish a baseline performance of the device and has been shown to capture CO2 at an energy cost of 1 MWh·ton-1 at the device level. An understanding has been built around the components of that energy cost including the relationship of flux to current density, effect of a regeneration process, transient battery behavior, and gas losses coinciding with changing the polarization of the batteries. The flow-through MEA looks to address of transient battery behavior and gas losses. It allows for denser, higher capacity electrodes, which can lean on traditional Ni-MH battery technology used in alkaline batteries used today. The higher capacities, limit the transient battery effect on flux in the device. Gas losses are addressed by having a continuous inlet air stream to the device and continuous outlet product.
Treyson Ricks - Intern Showcase Poster
Quinone-based sorbents offer a tunable, energy-efficient route to electrochemical CO2 capture, but systematic guidance for molecular design is lacking. Here, we report a high-throughput computational workflow that combines density functional theory (DFT) screening with machine-learning (ML) modeling to evaluate CO2 binding thermodynamics across several quinone derivatives, spanning benzoquinones, naphthoquinones, and anthraquinones. In addition to using solvents to stabilize the quinone anion and dianion, we studied the effect of ion-pairing on the reduction potentials and the CO2 binding energy. Automated Python scripts handled geometry optimizations and adduct-formation energies on an HPC cluster, reducing manual effort significantly. This integrated platform can uncover structure–property relationships and enables rapid in silico evaluation of untested candidates. We present one example from our workflow to showcase the capability of using quinones with ion-pairing to effectively capture CO2. Our approach paves the way for the rational selection of optimal quinone sorbents and can be extended with experimental thermochemical and kinetic data, alternative redox cycles, and stability assessments to accelerate development of next-generation electrochemical CO2 capture materials.
Nitrogen–Rich Conjugated Macrocycles: Synthesis, Conductivity, and Application in Electrochemical CO 2 Capture
Here we report a series of nitrogen-rich conjugated macrocycles that mimic the structure and function of semiconducting 2D metal–organic and covalent organic frameworks while providing greater solution processability and surface tunability. Using a new tetraaminotriphenylene building block that is compatible with both coordination chemistry and dynamic covalent chemistry reactions, we have synthesized two distinct macrocyclic cores containing Ni–N and phenazine-based linkages, respectively. The fully conjugated macrocycle cores support strong interlayer stacking and accessible nanochannels. For the metal–organic macrocycles, good out-of-plane charge transport is preserved, with pressed pellet conductivities of 10 –3 S/cm for the nickel variants. Lastly, using electrochemically mediated CO2 capture as an example, we illustrate how colloidal phenazine-based organic macrocycles improve electrical contact and active site electrochemical accessibility relative to bulk covalent organic framework powders. Together, these results highlight how simple macrocycles can enable new synthetic directions as well as new applications by combining the properties of crystalline porous frameworks, the processability of nanomaterials, and the precision of molecular synthesis.
Dissolved CO 2 Modulates the Electrochemical Capacitance on Gold Electrodes
The presence of CO 2 at an electrified interface between an aqueous electrolyte and a metal electrode is the prerequisite for many electrochemical CO 2 capture technologies. To understand the behavior of dissolved CO 2 at an aqueous electrified interface, we characterized the electrochemical interface of planar gold electrodes with cyclic voltammetry, electrochemical impedance spectroscopy (EIS), electrochemical surface plasmon resonance (EC–SPR), and attenuated total reflectance surface-enhanced infrared spectroscopy (ATR–SEIRAS). Under all investigated conditions, we observed a decrease in the electrochemical capacitance upon saturation of the electrolyte with CO 2 , as compared to an electrolyte saturated with Ar. EIS and EC–SPR showed that this capacitance reduction was also potential dependent: it reached a minimum near the point of zero charge and became more significant as the applied potential moved further away from the point of zero charge. Hybrid quantum–classical simulations of the gold/aqueous electrolyte interface indicate that bicarbonate decreases the capacitance and modifies the composition of the electric double layer. In addition to the binding of bicarbonate under positive bias, we propose that molecular CO 2 can be induced by applied potential to concentrate in the diffuse layer of the electric double layer, leading to a reduction in the electrochemical capacitance under both negative and positive bias. Furthermore, this work advances the understanding of non-Faradaic effects of dissolved CO 2 at aqueous electrified interfaces of relevance for electrochemical CO 2 capture.
Oxygen‐Assisted Supercapacitive Swing Adsorption of Carbon Dioxide
We report on the supercapacitive swing adsorption (SSA) of carbon dioxide at different voltage windows in the presence of oxygen using activated carbon electrodes, and deliquescent, aqueous electrolytes. The presence of O 2 in the CO 2 /N 2 gas mixture results in an up to 11 times higher CO 2 adsorption capacity with 3 M MgBr 2 (at 0.6 V) and up to 4–5 times higher adsorption capacity with 3 M MgCl 2 (at 1 V). A tradeoff between high CO 2 adsorption capacities and lower coulombic efficiencies was observed at voltages above 0.6 V. The energetic and adsorptive performance of the electrodes in the presence of oxygen below 0.5 V was similar to the performance with a CO 2 /N 2 mixture without oxygen at 1 V. Cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) of the electrodes demonstrate that the specific capacitance increases while the diffusion resistance decreases in the presence of oxygen. Oxygen concentrations ranging between 5–20 % give similar energetic and adsorptive performance. The electrodes exhibit stable performance for up to 100 cycles of operation.
Direct Air Capture-Compatible Azolate and Amino Acid Ionic Liquids for Electrochemical CO 2 Reduction to CO on a Silver Cathode
Direct air capture (DAC) compatible ionic liquids (ILs) are attractive for integrating CO 2 capture and conversion due to their high CO 2 solubility at low partial pressures, tunable chemisorption mechanisms, low volatility, and wide electrochemical windows. However, very few ILs have high CO 2 uptake at DAC conditions (420 ppm CO 2 ), and even fewer have been evaluated for chemical compatibility and mechanistic continuity for combined capture and electrochemical CO 2 reduction (eCO 2 RR). We demonstrate that two representative DAC-capable ILs, [P 4444 ][Val] (amino acid-based) and [P 66614 ][5-Me-Imd] (azolate-based), exhibit favorable electrochemical reduction behavior. CO and H 2 were the dominant gas-phase products by GC, while 1 H and 13 C NMR confirmed negligible liquid-phase HCOOH. Chronoamperometry at moderate applied potentials (−2.0 to −2.5 V vs Ag/AgCl) in a two-compartment H-cell with a Ag coated carbon paper as the working electrode yielded steady-state current densities of ∼10 mA cm −2 with CO FE of 96% for [P 4444 ][Val] and 95% for [P 66614 ][5-Me-Imd], highlighting the role of viscosity and chemically absorbed CO 2 -IL species to provide highly selective CO formation while suppressing H 2 evolution.
Advanced Alkaline Membrane H 2 /Air Fuel Cell System with Novel Technique for Air CO 2 Removal
Over the course of this project, significant progress was achieved in developing the hydroxide exchange membrane fuel cell (HEMFC) and the electrochemically-driven CO₂ separator (EDCS), with a focus on improving performance, durability, and scalability. Key milestones were met, and the technology demonstrated potential for a wide range of applications, including fuel cell vehicles, direct air capture (DAC), and life support systems.
Enzymes Under Confinement: Materials Interactions and Functionality for CO2 Capture and Conversion
CO2 capture membranes are of interest in industries where large amounts of CO2 waste is produced. Captured CO2 can be electrochemically reduced to CO and recycled for other uses. These capture membranes consist of an alumina substrate with a silicon layer. Enzymes have been used to lower reaction energies on nanoporous silica enabling better CO2 capture, however eliminating the silicon layer would improve manufacturability. We have proposed the use of nanoporous alumina alone, as an alternative.
A direct coupled electrochemical system for capture and conversion of CO2 from oceanwater
Not Available
Enhanced Depolarized Electro-Membrane System (EDEMS) for Direct Capture of Carbon Dioxide from Ambient Air (Final Report)
The goal of this final project report is to summarize the work conducted on project DE-FE0031962. In accordance with the Statement of Project Objectives (SOPO), the University of Kentucky Center for Applied Energy Research (UK CAER) (Recipient) developed an intensified process to capture CO2 from ambient conditions (400 ppm CO2). The process combines low-temperature solvent-aided membrane capture with electrochemically-mediated solvent regeneration to simultaneously capture ambient CO2 while regenerating the solvent. The technology employs only two primary units (regenerator and absorber/contactor) while generating high purity hydrogen as a co-product that can be sold, used for energy storage, or cost-saving depolarization of the direct air capture (DAC) system during the grid peak demand, allowing for flexible operation. When depolarization is employed, the operating voltage is reduced by more than 1 V. Since the technology is powered directly by DC electricity, it can seamlessly tie in with power sources like solar cells without the need for AC/DC converters, therefore allowing for a remote operation to further mitigate greenhouse gas generation toward deploying a negative carbon emissions technology that is completely decoupled from the carbon emissions from the power source for the DAC unit. The project results verified that UK CAER’s integrated approach addressed the complexities of incumbent DAC systems by demonstrating at ambient conditions, including (1) low gas-side pressure-drop facile CO2 capture via a membrane contactor with in-situ generated hydroxide as capture solvent, (2) multi-functional electrochemical regenerator for hydroxide regeneration, CO2 concentration and hydrogen production, and (3) depolarization using cathode-produced hydrogen to reduce energy requirement. The EH&S Assessment of the process did not identify any obvious concern for the bench-scale operation and no apparent barriers to implementing UK CAER’s carbon capture and solvent regeneration system at a larger scale.
A Model of Large Scale Electrochemical Direct Ocean Capture Under Variable Power
Since limiting warming to 1.5 degrees C by 2100 will not only require an energy transition but also billions of tons of carbon dioxide (CO2) removal per year, it is essential to expand these efforts. This can be done offshore via electrochemical direct ocean capture (eChem DOC) which extracts CO2 from seawater that can later be stored underground or converted to products. Deployments of eChem DOC will be powered by renewable energy and therefore need to function with variable power inputs. This project aims to support future large-scale deployments by developing a model of eChem DOC operation, informed by industry and literature, and assessing its performance under variable power and varying designs. Initial analysis suggests that discretizing the eChem system has a higher impact on increasing overall capture than storing the chemical solutions to continue capture during periods of lower power availability, but this is likely situation dependent. Future work will use more realistic power profiles.
Adaptive Laboratory Evolution for Enhanced Performance of Cupriavidus Necator on Formic Acid
The threat of global warming, driven by rising carbon emissions, highlights the need to decarbonize our economy. This requires innovative solutions for managing carbon waste and its effective utilization. One promising method for CO2 capture and sequestration is the electrochemical reduction of CO2 to formic acid, a soluble C1 molecule that can be used to store carbon and energy, and as a feedstock for biological conversion. Cupriavidus necator H16, a soil bacterium capable of consuming and growing on formic acid as its sole carbon and energy source, is well positioned to upgrade CO2-derived formic acid into platform chemicals and fuel precursors. To improve the performance of C. necator on formic acid, adaptive laboratory evolution (ALE), a proven tool for improving microbial fitness, has been conducted using continuous pH-stat bioreactors. The system works on the basis that consumption of formic acid raises the pH and triggers the addition of more formic acid to maintain the pH (in this case 6.7), such that formic acid is provided at the same rate as it is consumed. This system has been coupled with level control to achieve continuous fermentation where cells acquiring mutations that improve growth on formic acid become more abundant in the population, from which they can be isolated and characterized. During developmental experiments it was discovered that formic acid accumulated to inhibitory levels. It was determined that the nitrogen source, ammonium hydroxide, must be tailored to the carbon consumption to avoid formic acid accumulation. The ALE ran in three lineages for approximately 3000 hours and more than 500 generations. Evolved isolates obtained from each lineage demonstrated an increase in growth rate in conjunction with improve formate utilization compared to the parental strain when evaluated in pH-stat bioreactors. The isolates with improved performance were then subjected to whole genome sequencing to identify potentially causative mutations. Mutations in several key genes across different lineages have been found and will be evaluated individually and in combination to identify those that improve growth on formic acid. Incorporating these mutations into production strains has the potential to greatly improve formic acid conversion and further industrial decarbonization.
Direct Air Capture of Carbon Dioxide Using Nickel Hydroxide Batteries in a Membrane Electrode Assembly
Direct air capture (DAC) is a growing field responding to the need to remove carbon dioxide from the atmosphere. Several technologies are being developed today attempting to meet this need. The technology furthest in development are temperature swing adsorption technologies which have recently moved out of the pilot plant scale.1 This presentation looks to present an electrochemical device as alternative to these technologies. The electrochemical device proposed is a pair of nickel hydroxide (Ni(OH)2) battery electrodes which produce hydroxide (OH-). The hydroxide reacts with carbon dioxide (CO2) to create carbonate (CO32-) and bicarbonate (HCO3-). These carbonates can be transported from the cathode across an anion exchange membrane to the anode where they are evolved back into CO2 due to a pH reduction at the anode. This builds on work that optimized a Hydroxide Exchange Membrane Fuel Cell (HEMFC) for CO2 capture, showing the efficacy of an electrochemically mediated pH swing carbon capture device.2,3 The benefit of the nickel hydroxide battery approach is the low energy cost associated with separation. Because a pair of nickel hydroxide batteries undergo the same electrochemical reaction, low potentials, and thus low energy cost is required. Experiments have shown device level energy requirements of less than 1 MWh ton-1CO2. Most of the energy required by the device produces the pH gradient used to capture and release CO2. The biggest hurdle for this electrochemical approach is increasing the flux of CO2 to allow for more compact devices. Strategies for managing the transient charge and discharge behavior of the battery system will be discussed. Focus will be on improving flux to reduce the overall cost of the device.
Integrated Technology for Cost-Effective CO2 Capture and Formic Acid Production: Modeling, Optimization, and Economic Analysis
A novel reactive technology is being investigated that electrochemically converts CO2 into valuable chemicals, particularly formic acid. This work focuses on identifying the optimal design and operation of an integrated membrane-based CO2 capture unit with the electrochemical conversion process. In this setup, the CO2 in the flue gas permeates through a CO2-selective membrane and enters an electrolyzer to produce formic acid, creating an integrated reaction module. To refine the chemical product, gas products from the electrolyzer are directed to a pressure swing adsorption unit, while the liquid product undergoes refinement to achieve commercial-grade formic acid using reactive distillation. A membrane CO2 capture model and an electrochemical conversion model have been developed using the IDAES Integrated Platform (Institute for the Design of Advanced Energy System), facilitating rigorous flowsheet modeling and process design and optimization.
Electrochemically driven carbon dioxide separation
This project explored the viability of a Ni(OH) 2 based hydroxide exchange membrane carbon capture (HEMCC) device for direct air capture. It is built off an H 2 fuel cell based HEMCC previously developed in the Yushan Yan group at University of Delaware. Taking the same membrane-based, electrochemically driven pH gradient concept, similar flux performance was able to be seen in the Ni(OH) 2 system as the H 2 system when using comparable current densities. The project produced two types of membrane electrode assemblies (MEA). The first was a traditional MEA with two electrodes and a membrane, the second was a flow-through membrane MEA. Consistent performance was achieved with the traditional MEA with an energy cost of 1.1 MWh∙ton -1 and flux of 82 kg∙m -2 ∙yr -1 . This was the most stable of the two designs. This project investigated strategies to improve performance with a flow-through membrane design. Two designs were made, one with a cast phase inversion membrane, and one with powdered membrane layer. The template phase inversion membrane achieved low pressure drop but had performance limitations due to a skin layer of membrane limiting CO 2 gas transport. The powdered membrane layer had better performance but higher pressure drop. Finally, using the powdered membrane, commercial battery materials were able to be used in order to achieve higher flux. This showed that the flow through membrane design does have the capability to overcome flux inefficiencies in the traditional MEA. Moreover, the process design of the system is proposed and given in this project. The process mass and energy balances were calculated for a reference plant of 1000 t/yr CO 2 capture, which contains several subsystems, e.g. air processing subsystem, electrical subsystem, and CO 2 purification and compression subsystem is designed and evaluated. Based on our calculation, When the power consumption for stack is 1 MWh t -1 CO 2 , Additional 382 kWh t -1 CO 2 will be consumed by other subsystem of the plant, i.e. The total power consumption of 1.38 MWh t -1 CO 2 , lower than the final milestone of 1.5 MWh t -1 CO 2 in this project.
Direct Measurement of Electrochemical Selectivity Gradients over a 25 cm 2 Copper Gas Diffusion Electrode
Not Available