Abstract This work introduces the facile and scalable two‐step synthesis of Ti2Nb10O29 (TNO)/carbon hybrid material as a promising anode for lithium‐ion batteries (LIBs). The first step consisted of a mechanically induced self‐sustaining reaction via ball‐milling at room temperature to produce titanium niobium carbide with a Ti and Nb stoichiometric ratio of 1 to 5. The second step involved the oxidation of as‐synthesized titanium niobium carbide to produce TNO. Synthetic air yielded fully oxidized TNO, while annealing in CO2 resulted in TNO/carbon hybrids. The electrochemical performance for the hybrid and non‐hybrid electrodes was surveyed in a narrow potential window (1.0–2.5 V vs. Li/Li+) and a large potential window (0.05–2.5 V vs. Li/Li+). The best hybrid material displayed a specific capacity of 350 mAh g−1 at a rate of 0.01 A g−1 (144 mAh g−1 at 1 A g−1) in the large potential window regime. The electrochemical performance of hybrid materials was superior compared to non‐hybrid materials for operation within the large potential window. Due to the advantage of carbon in hybrid material, the rate handling was faster than that of the non‐hybrid one. The hybrid materials displayed robust cycling stability and maintained ca. 70 % of their initial capacities after 500 cycles. In contrast, only ca. 26 % of the initial capacity was maintained after the first 40 cycles for non‐hybrid materials. We also applied our hybrid material as an anode in a full‐cell lithium‐ion battery by coupling it with commercial LiMn2O4.

In their initial manuscript, an incorrect dataset was plotted in Figure 5b for the 4000 ppm data line. The incorrect version can be seen here: A corrected version of Fig. 5b is shown below. Figure 5 …(b) corresponding salt concentration variation in the diluted stream at 0.25 mA cm−2 current density. The correct version shown below. Figure 5 …(b) corresponding salt concentration variation in the diluted stream at 0.25 mA cm−2 current density. This correction has no influence on the scientific content. The authors apologize for this oversight and for any inconvenience caused.

The reason for the capacity fading of LiFePO4 in lithium recovery is explored. And two approaches, reducing the content of oxygen and carbon coating, are put forward, and the mechanism of them are studied.

Owing to high electrical conductivity and ability to reversibly host a variety of inserted ions, 2D metallic molybdenum disulfide（1 T-MoS 2 ） has demonstrated promising energy storage performance when used as a supercapacitor electrode. However, its charge storage mechanism is still not fully understood,in particular, how the interlayer spacing of 1 T-MoS 2 would affect its capacitive performance. In this work, molecular dynamics simulations of 1 T-Mo S 2 with interlayer spacing ranging from 0.615 to 1.615 nm have been performed to investigate the resulting charge storage capacity in ionic liquids. Simulations reveal a camel-like capacitance-potential relation, and MoS 2 with an interlayer spacing of 1.115 nm has the highest volumetric and gravimetric capacitance of118 F cm -3 and 42 F g -1 , respectively. Although ions in MoS 2 with an interlayer spacing of 1.115 nm diffuse much faster than with interlayer spacings of 1.365 and 1.615 nm, the MoS 2 with larger interlayer spacing has a much faster-charging process. Our analyses reveal that the ion number density and its charging speed, as well as ion motion paths, have significant impacts on the charging response. This work helps to understand how the interlayer spacing affects the interlayer ion structures and the capacitive performance of MoS 2 , which is important for revealing the charge storage mechanism and designing MoS 2 supercapacitor.

The high sodium uptake capacity of antimony can be used for high performance water desalination by using a ceramic ion-exchange membrane.

This study demonstrates the hybridization of Li4Ti5O12 (LTO) with different types of carbon onions synthesized from nanodiamonds. The carbon onions mixed with a Li4Ti5Ox precursor for sol–gel synthesis. These hybrid materials are tested as anodes for both lithium‐ion battery (LIB) and sodium‐ion battery (SIB). Electrochemical characterization for LIB application is carried out using 1 m LiPF6 in a 1:1 (by volume) ethylene carbonate and dimethyl carbonate as the electrolyte. For lithium‐ion intercalation, LTO hybridized with carbon onions from the inert‐gas route achieves an excellent electrochemical performance of 188 mAh g−1 at 10 mA g−1, which maintains 100 mAh g−1 at 1 A g−1 and has a cycling stability of 96% of initial capacity after 400 cycles, thereby outperforming both neat LTO and LTO with onions obtained via vacuum treatment. The performance of the best‐performing hybrid material (LTO with carbon onions from argon annealing) in an SIB is tested, using 1 m NaClO4 in ethylene/dimethyl/fluoroethylene carbonate (19:19:2 by mass) as the electrolyte. A maximum capacity of 102 mAh g−1 for the SIB system is obtained, with a capacity retention of 96% after 500 cycles.

The freshwater scarcity and increasing energy demand are two challenging global issues. Herein, we propose a new route for desalination, self-sustained visible-light-driven electrochemical redox desalination. We propose a novel device architecture involving internal integration of a quasi-solid-state dye-sensitized solar cell and continuous redox-flow desalination units with a bifunctional platinized-graphite-paper electrode. Both the solar cell and redox-flow desalination units are integrated using the bifunctional electrode with one side facing the solar cell operating as a positive electrode and the other side facing the redox-flow desalination unit operating as a negative electrode. The solar cell contains a gel-based tri-iodide/iodide redox couple sandwiched between an N719 dye-modified photoanode and cathode. In contrast, the redox-flow desalination consists of re-circulating ferro/ferricyanide redox couple sandwiched between the anode and cathode with two salt streams located between these electrodes. The performances of bifunctional electrodes in both redox couples were thoroughly investigated by electrochemical characterization. The brackish feed can be continuously desalted to the freshwater level by utilizing visible light illumination. As a device, this architecture combines energy conversion and water desalination. This concept bypasses the need for electrical energy consumption for desalination, which provides a novel structural design using photodesalination to facilitate the development of self-sustained solar desalination technologies.

In this work, carbon electrode modified polymer membrane and free-standing polymer membranes are applied for desalination via capacitive deionization with microporous activated carbon. The desalination performance under different concentrations (20 mM and 600 mM) of feed water and different voltage operation mode (zero volt and voltage-reversal operation). For the ion exchange membrane coating under 20 mM NaCl solution at a cell voltage of 0/+1 V, the desalination capacity reached 22.7 mg/g at the charge efficiency of 142.1%. In the case of the free-standing membrane, under 600 mM NaCl solution at a voltage range of -1/+1 V, the desalination capacity reached 26.0 mg/g with a charge efficiency of 61.5%. These results not only show the possibility of membrane capacitive deionization (MCDI) application in seawater desalination but also reveals different ion transport mechanisms of the coated membrane and free-standing membranes under different molar strength of feed water.

Electrochemical processes enable a new generation of energy-efficient desalination technologies. While ion electrosorption via capacitive deionization is only suitable for brackish water with low molar strength, the use of Faradaic materials capable of reversible ion intercalation or conversion reactions allows energy-efficient removal of ions from seawater. However, the limited charge transfer/storage capacity of Faradaic materials indicates an upper limit for their desalination applications. Therefore, a new electrochemical concept must be explored to exceed the current state-of-the-art results and to push the desalination capacity beyond 100–200 mgNaCl/gelectrode. In this proof-of-concept work, we introduce the new concept of using metal–air battery technology for desalination. We do so by presenting performance data for zinc–air desalination (ZAD) in 600 mM NaCl. The ZAD cell provides a desalination capacity of 0.9–1.0 mgNaCl/cm2 (normalized to the membrane area; corresponding to 1300 mgNaCl/gZn) with a charge efficiency of 70% when charging/discharging the cell at 1 mA/cm2. The energy consumption of ZAD is 68–92 kJ/mol.

Continuous and low-energy desalination technologies are in high demand to enable sustainable water remediation. Our work introduces a continuous desalination process based on the redox reaction of a dual-zinc electrode. The system consists of two zinc foils as redox electrodes with flowing ZnCl2 electrolyte, concentrated and diluted salt streams with three anion- and cation-exchange membranes (AEM and CEM) separated configuration (AEM|CEM|AEM). If a constant current is applied, the negative zinc electrode is oxidized, and electrons are released to the external circuit, whereas the positive zinc electrode is reduced, causing salt removal in the dilution stream. The results showed that brackish water can be directly desalted to 380.6 ppm during a continuous batch-mode process. The energy consumption can be as low as 35.30 kJ mol(-1) at a current density of 0.25 mA cm(-2), which is comparable to reverse osmosis. In addition, the dual-zinc electrode electrochemical desalination demonstrates excellent rate performance, reversibility, and batch cyclability through electrode exchange regeneration. Our research provides a route for continuous low-energy desalination based on metal redox mediators.

Reversible electrochemical processes are a promising technology for energy-efficient water treatment. Electrochemical desalination is based on the compensation of electric charge by ionic species, through which the ions are immobilized and, thereby, removed from a feed-water stream flowing through a desalination cell. For decades, electrochemical desalination has focused on the use of carbon electrodes, but their salt-removal ability is limited by the mechanism of ion electrosorption at low molar concentrations and low charge-storage capacity. Recently, charge-transfer materials, often found in batteries, have demonstrated much larger charge-storage capacities and energy-efficient desalination at both low and high molar strengths. In this Review, we assess electrochemical-desalination mechanisms and materials, including ion electrosorption and charge-transfer processes, namely, ion binding with redox-active polymers, ion insertion, conversion reactions and redox-active electrolytes. Furthermore, we discuss performance metrics and cell architectures, which we decouple from the nature of the electrode material and the underlying mechanism to show the versatility of cell-design concepts. These charge-transfer processes enable a wealth of environmental applications, ranging from potable-water generation and industrial-water remediation to lithium recovery and heavy-metal-ion removal. Electrochemical processes enable energy-efficient desalination of water and the separation and recovery of elements. In this Review, we discuss the mechanisms and materials of this emerging generation of water-remediation technology.

Electrolyte-filled subnanometre pores exhibit exciting physics and play an increasingly important role in science and technology. In supercapacitors, for instance, ultranarrow pores provide excellent capacitive characteristics. However, ions experience difficulties in entering and leaving such pores, which slows down charging and discharging processes. In an earlier work we showed for a simple model that a slow voltage sweep charges ultranarrow pores quicker than an abrupt voltage step. A slowly applied voltage avoids ionic clogging and co-ion trapping-a problem known to occur when the applied potential is varied too quickly-causing sluggish dynamics. Herein, we verify this finding experimentally. Guided by theoretical considerations, we also develop a non-linear voltage sweep and demonstrate, with molecular dynamics simulations, that it can charge a nanopore even faster than the corresponding optimized linear sweep. For discharging we find, with simulations and in experiments, that if we reverse the applied potential and then sweep it to zero, the pores lose their charge much quicker than they do for a short-circuited discharge over their internal resistance. Our findings open up opportunities to greatly accelerate charging and discharging of subnanometre pores without compromising the capacitive characteristics, improving their importance for energy storage, capacitive deionization, and electrochemical heat harvesting.

Two-dimensional, layered transition metal carbides (MXenes) are an intriguing class of intercalation-type electrodes for electrochemical applications. The ability for preferred counterion uptake qualifies MXenes as an attractive material for electrochemical desalination. Our work explores Ti3C2Tx-MXene paired with activated carbon in such a way that both electrodes operate in an optimized potential range. This is accomplished by electrode mass balancing and control over the cell voltage. Thereby, we enable effective remediation of saline media with low (brackish) and high (seawater-like) ionic strength by using 20 and 600 mM aqueous NaCl solutions. It is shown that MXene/activated-carbon asymmetric cell design capitalizes on the permselective behavior of MXene in sodium removal, which in turn forces carbon to mirror the same behavior in the removal of chloride ions. This has minimized the notorious co-ion desorption of carbon in highly saline media (600 mM NaCl) and boosted the charge efficiency from 4% in a symmetric activated-carbon/activated-carbon cell to 85% in a membrane-less asymmetric MXene/activated-carbon cell. Stable electrochemical performance for up to 100 cycles is demonstrated, yielding average desalination capacities of 8 and 12 mg/g, respectively, for membrane-less MXene/activated-carbon cells in NaCl solutions of 600 mM (seawater-level) and 20 mM (brackish-water-level). In the case of the 20 mM NaCl solutions, surprising charge efficiency values of over 100% have been obtained, which is attributed to the role of MXene interlayer surface charges.

In nanoconfinement, the reversible electrochemisorption of hydrogen extends the voltage window of aqueous electrolytes. This process has been well studied for different aqueous electrolytes but not compared to the performance of heavy water. Herein, we study hydrogen and deuterium electrosorption on a porous carbon electrode under negative polarization using sodium chloride as the salt. As electrodes, we use microporous carbons with an average pore size in the sub-nanometer range and, for comparison, mesoporous carbon nanotube bucky paper. We show that the hydrogen electrochemisorption and gas evolution processes are more pronounced than for deuterium while the same potential is applied. Our data confirm lower ion mobility of D2O compared to H2O, and a shift of the reversible charging and discharging process toward more negative potentials. (C) 2019 The Electrochemical Society.

Over recent decades, a new type of electric energy storage system has emerged with the principle that the electric charge can be stored not only at the interface between the electrode and the electrolyte but also in the bulk electrolyte by redox activities of the electrolyte itself. Those redox electrolytes are promising for non-flow hybrid energy storage systems, or redox electrolyte-aided hybrid energy storage (REHES) systems; particularly, when they are combined with highly porous carbon electrodes. In this review paper, critical design considerations for the REHES systems are discussed as well as the effective electrochemical characterization techniques. Appropriate evaluation of the electrochemical performance is discussed thoroughly, including advanced analytical techniques for the determination of the electrochemical stability of the redox electrolytes and self-discharge rate. Additionally, critical summary tables for the recent progress on REHES systems are provided. Furthermore, the unique synergistic combination of porous carbon materials and redox electrolytes is introduced in terms of the diffusion, adsorption, and electrochemical kinetics modulating energy storage in REHES systems.

In recent years, a wealth of new desalination technologies based on reversible electrochemical redox reactions has emerged. Among them, the use of redox-active electrolytes is highly attractive due to the high production rate and energy efficiency. Yet, these technologies suffer from the imperfect permselectivity of polymer membranes. Our present work demonstrates the promising desalination performance of a sodium superionic conductor (NASICON) for selective removal of sodium against iodide in a half-cell configuration consisting of an activated carbon electrode in aqueous 600 mM NaI solution. For feedwater with aqueous 600 mM NaCl, the desalination cell exhibited a stable performance over a month with more than 400 operation cycles with the aid of high sodium permselectivity of the NASICON membrane against iodide (99.9-100%). The cell exhibited a maximum sodium removal capacity of 69 +/- 4 mg/g (equivalent to the NaCl salt uptake capacity of 87 +/- 4 mg/g) with a charge efficiency of 81 +/- 3%.

The silver/silver chloride conversion reaction allows for a high desalination capacity of saline media with high molar strength.

Hydrated vanadyl phosphate is a promising electrode material for electrochemical water desalinationviareversible ion intercalation.

We present a facile two-step synthesis of vanadium (III) oxide/carbon core/shell hybrid material for application as lithium-ion battery electrode. The first step is a thermal treatment of a mixture of vanadium carbide (VC) and NiCl2 center dot 6H(2)O at 700 degrees C in an inert gas atmosphere. Elemental nickel obtained from decomposing NiCl2 center dot 6H(2)O served as a catalyst to trigger the local formation of graphitic carbon. In a second step, residual nickel was removed by washing the material in aqueous HCl. By replacing NiCl2 center dot 6H(2)O with anhydrous NiCl2, we obtained a hybrid material of vanadium carbide-derived carbon and a vanadium carbide core. Material characterization revealed a needle-like morphology of the rhombohedral V2O3 along with two carbon species with a different degree of graphitic ordering. We varied the NiCl2 center dot 6H(2)O-to-VC ratio, and the optimized material yielded a capacity of 110 mAh.g(-1) at 2.5 A.g(-1) which increased to 225 mAh.g(-1) at 0.1 A.g(-1) after 500 cycles in the potential range of 0.01-3.00 V vs. Li/Li+. This enhanced performance is in stark contrast to the loss of lithium uptake capacity when using commercially available V2O3 mixed with carbon black, where 93% of the initial capacity was lost after 50 cycles.