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Owing to an expanding economy and growing population, there is increasing consumer demand for freshwater. However, with global climate change and water pollution issues, there is rising water stress in many countries worldwide. Electrochemical water desalination technologies such as capacitive deionization (CDI) utilize electrical energy to store ions in porous materials and provide energy-efficient water desalination. However, due to the cation and anion exchange process during the charging and discharging processes, CDI is considered suitable for low salinity water desalination (salinity of 1-10 g/L). This dissertation explores novel approaches to next-generation CDI for better desalination performances and water desalination at high ionic strength. In particular, the ability of sub-nanometer carbon pores (ultramicropores) to enable highly efficient CDI even at seawater salinity is demonstrated based on unexpected simulation predictions. This unique ability originates from the energy barrier of ion solvation for pores smaller than the solvation shell. Consequently, uncharged carbon ultramicropores behave ionophobic and overcome the limitation of CDI only to be suitable for remediation of brackish water. Ultramicropores also provide novel perspectives for ion separation via the interplay of intrinsic and kinetic ion selectivity. This work also establishes electrocatalytic fuel cell desalination, whereby conventional fuel cell technology can easily be adapted to generate electricity, heat, and desalinated water concurrently.
Supercapacitors are fast-charging energy storage devices of great importance for developing robust and climate-friendly energy infrastructures for the future. Research in this field has seen rapid growth in recent years, therefore consistent reporting practices must be implemented to enable reliable comparison of device performance. Although several studies have highlighted the best practices for analysing and reporting data from such energy storage devices, there is yet to be an empirical study investigating whether researchers in the field are correctly implementing these recommendations, and which assesses the variation in reporting between different laboratories. Here we address this deficit by carrying out the first interlaboratory study of the analysis of supercapacitor electrochemistry data. We find that the use of incorrect formulae and researchers having different interpretations of key terminologies are major causes of variability in data reporting. Furthermore we highlight the more significant variation in reported results for electrochemical profiles showing non-ideal capacitive behaviour. From the insights gained through this study, we make additional recommendations to the community to help ensure consistent reporting of performance metrics moving forward.
Summary Electrochemical seawater desalination has drawn significant attention as an energy-efficient technique to address the global issue of water remediation. Microporous carbons, that is, carbons with pore sizes smaller than 2 nm, are commonly used for capacitive deionization. However, micropores are ineffective for capacitive deionization at high molar strength because of their inability to permselectively uptake ions. In our work, we combine experimental work with molecular dynamics simulation and reveal the ability of sub-nanometer pores (ultramicropores) to effectively desalinate aqueous media at seawater-like molar strength. This is done without any ion-exchange membrane. The desalination capacity in 600 mM reaches 12 mg/g, with a charge efficiency of 94% and high cycling stability over 200 cycles (97% of charge efficiency retention). Using molecular dynamic simulations and providing experimental data, our work makes it possible both to understand and to calculate desalination capacity and charge efficiency at high molar strength as a function of pore size.
Electrochemical ion separation is a promising technology to recover valuable ionic species from water. Pseudocapacitive materials, especially 2D materials, are up-and-coming electrodes for electrochemical ion separation. For implementation, it is essential to understand the interplay of the intrinsic preference of a specific ion (by charge/size), kinetic ion preference (by mobility), and crystal structure changes. Ti3C2Tz MXene is chosen here to investigate its selective behavior toward alkali and alkaline earth cations. Utilizing an online inductively coupled plasma system, it is found that Ti3C2Tz shows a time-dependent selectivity feature. In the early stage of charging (up to about 50 min), K+ is preferred, while ultimately Ca2+ and Mg2+ uptake dominate; this unique phenomenon is related to dehydration energy barriers and the ion exchange effect between divalent and monovalent cations. Given the wide variety of MXenes, this work opens the door to a new avenue where selective ion-separation with MXene can be further engineered and optimized.
Energy-efficient technologies for the remediation of water and generation of drinking water is a key towards sustainable technologies. Electrochemical desalination technologies are promising alternatives towards established methods, such as reverse osmosis or nanofiltration. In the last few years, hydrogen-driven electrochemical water purification has emerged. This review article explores the concept of desalination fuel cells and capacitive-Faradaic fuel cells for ion separation.
Advanced hydrogen technologies contribute essentially to the decarbonization of our industrialized world. Large-scale hydrogen production would benefit from using the abundantly available water reservoir of our planet’s oceans. Current seawater-desalination technologies suffer from high energy consumption, high cost, or low performance. Here, we report technology for water desalination at seawater molarity, based on a polymer ion-exchange membrane fuel cell. By continuously supplying hydrogen and oxygen to the cell, a 160-mM concentration decrease from an initial value of 600 mM is accomplished within 40 h for a 55-mL reservoir. This device’s desalination rate in 600 mM NaCl and substitute ocean water are 18 g/m2/h and 16 g/m2/h, respectively. In addition, by removing 1 g of NaCl, 67 mWh of electric energy is generated. This proof-of-concept work shows the high application potential for sustainable fuel-cell desalination (FCD) using hydrogen as an energy carrier.
Electrochemical desalination shows promise for ion-selective, energy-efficient water desalination. This work reviews performance metrics commonly used for electrochemical desalination. We provide a step-by-step guide on acquiring, processing, and calculating raw desalination data, emphasizing informative and reliable figures of merit. A typical experiment uses calibrated conductivity probes to relate measured conductivity to concentration. Using a standard electrochemical desalination cell with activated carbon electrodes, we demonstrate the calculation of desalination capacity, charge efficiency, energy consumption, and ion selectivity metrics. We address potential pitfalls in performance metric calculations, including leakage current (charge) considerations and aging of conductivity probes, which can lead to inaccurate results. The relationships between pH, temperature, and conductivity are explored, highlighting their influence on final concentrations. Finally, we provide a checklist for calculating performance metrics and planning electrochemical desalination tests to ensure accuracy and reliability. Additionally, we offer simplified spreadsheet tools to aid data processing, system design, estimations, and upscaling.
