Two-Dimensional MoS Nanosheets Derived from Cathodic Exfoliation for Lithium Storage Applications.

The preparation of 2H-phase MoS thin nanosheets by electrochemical delamination remains a challenge, despite numerous efforts in this direction. In this work, by choosing appropriate intercalating cations for cathodic delamination, the insertion process was facilitated, leading to a higher degree of exfoliation while maintaining the original 2H-phase of the starting bulk MoS material. Specifically, trimethylalkylammonium cations were tested as electrolytes, outperforming their bulkier tetraalkylammonium counterparts, which have been the focus of past studies.

Cation desolvation-induced capacitance enhancement in reduced graphene oxide (rGO).

Understanding the local electrochemical processes is of key importance for efficient energy storage applications, including electrochemical double layer capacitors. In this work, we studied the charge storage mechanism of a model material - reduced graphene oxide (rGO) - in aqueous electrolyte using the combination of cavity micro-electrode, operando electrochemical quartz crystal microbalance (EQCM) and operando electrochemical dilatometry (ECD) tools. We evidence two regions with different charge storage mechanisms, depending on the cation-carbon interaction.

Role of Surface Terminations for Charge Storage of TiCT MXene Electrodes in Aqueous Acidic Electrolyte.

In this study, we used 2-Dimmensionnal TiC MXene as model materials to understand how the surface groups affect their electrochemical performance. By adjusting the nature of the surface terminations (Cl-, N/O-, and O-) of TiC MXene through a molten salt approach, we could change the spacing between MXene layers and the level of water confinement, resulting in significant modifications of the electrochemical performance in acidic electrolyte. Using a combination of techniques including in-operando X-ray diffraction and electrochemical quartz crystal microbalance (EQCM) techniques, we found that the presence of confined water results in a drastic transition from an almost electrochemically inactive behavior for Cl-terminated TiC to an ideally fast pseudocapacitive signature for N,O-terminated TiC MXene.

NbSe Nanosheets/Nanorolls Obtained via Fast and Direct Aqueous Electrochemical Exfoliation for High-Capacity Lithium Storage.

Layered transition-metal dichalcogenides (LTMDs) in two-dimensional (2D) form are attractive for electrochemical energy storage, but research efforts in this realm have so far largely focused on the best-known members of such a family of materials, mainly MoS, MoSe, and WS. To exploit the potential of further, currently less-studied 2D LTMDs, targeted methods for their production, preferably by cost-effective and sustainable means, as well as control over their nanomorphology, are highly desirable. Here, we report a quick and straightforward route for the preparation of 2D NbSe and other metallic 2D LTMDs that relies on delaminating their bulk parent solid under aqueous cathodic conditions.

Exploring the Carbon/Electrolyte Interface in Supercapacitors Operating in Highly Concentrated Aqueous Electrolytes.

The development of superconcentrated or water-in-salt electrolytes (WISEs) has paved a new way toward realizing environmentally friendly, nonflammable batteries and supercapacitors based on aqueous electrolytes. The development of new electrolytes, such as WISEs, needs to be accompanied by further studies of the charging mechanism. This is essential to guide the choice of the electrode/electrolyte pairs for optimizing the performance of WISE-based supercapacitors.

Magnetic Resonance Imaging of a Complete Supercapacitor Giving Additional Insight on the Role of Nanopores.

Nuclear magnetic resonance is one of the rare techniques able to probe selectively the ions inside the nanoporous network in supercapacitor devices. With a magnetic resonance imaging method able to detect all ions (adsorbed and nonadsorbed), we record one-dimensional concentration profiles of the active ions in supercapacitors with an electrode configuration close to that used in industry. Larger anionic concentration changes are probed upon charge and discharge in a carbide-derived carbon (CDC) with micropores smaller than 1 nm compared to a conventional nanoporous carbon (CC) with a larger distribution of pore sizes, up to 2 nm.

Pulsed Electrochemical Mass Spectrometry for Operando Tracking of Interfacial Processes in Small-Time-Constant Electrochemical Devices such as Supercapacitors.

A more detailed understanding of the electrode/electrolyte interface degradation during the charging cycle in supercapacitors is of great interest for exploring the voltage stability range and therefore the extractable energy. The evaluation of the gas evolution during the charging, discharging, and aging processes is a powerful tool toward determining the stability and energy capacity of supercapacitors. Here, we attempt to fit the gas analysis resolution to the time response of a low-gas-generation power device by adopting a modified pulsed electrochemical mass spectrometry (PEMS) method.

The effect of hydrazine intercalation on the structure and capacitance of 2D titanium carbide (MXene).

Herein we show that hydrazine intercalation into 2D titanium carbide (Ti3C2-based MXene) results in changes in its surface chemistry by decreasing the amounts of fluorine, OH surface groups and intercalated water. It also creates a pillaring effect between Ti3C2Tx layers pre-opening the structure and improving the accessability to active sites. The hydrazine treated material has demonstrated a greatly improved capacitance of 250 F g(-1) in acidic electrolytes with an excellent cycling ability for electrodes as thick as 75 μm.

Exploring electrolyte organization in supercapacitor electrodes with solid-state NMR.

Supercapacitors are electrochemical energy-storage devices that exploit the electrostatic interaction between high-surface-area nanoporous electrodes and electrolyte ions. Insight into the molecular mechanisms at work inside supercapacitor carbon electrodes is obtained with (13)C and (11)B ex situ magic-angle spinning nuclear magnetic resonance (MAS-NMR). In activated carbons soaked with an electrolyte solution, two distinct adsorption sites are detected by NMR, both undergoing chemical exchange with the free electrolyte molecules.

A solid-state NMR study of C(70): a model molecule for amorphous carbons.

We show that natural abundance, solid-state MAS-NMR (13)C INADEQUATE spectra can be recorded for crystallized C(70), using the through-bond J-coupling for the magnetization transfer. The effect of strong J-coupling can be lessened at high magnetic fields, allowing the observation of cross-peaks between close resonances. DFT calculations of the chemical shifts show an excellent agreement with the experimental values.

Carbon nanotubes as nanotexturing agents for high power supercapacitors based on seaweed carbons.

The advantages provided by multiwalled carbon nanotubes (CNTs) as backbones for composite supercapacitor electrodes are discussed. This paper particularly highlights the electrochemical properties of carbon composites obtained by pyrolysis of seaweed/CNTs blends. Due to the nanotexturing effect of CNTs, supercapacitors fabricated with electrodes from these composites exhibit enhanced electrochemical performances compared with CNT-free carbons.