arXiv subjects

Vladislav Ivanistsev

Publications and source records attributed to Vladislav Ivanistsev.

2 recordsLinked to original sources

arXiv2026

Demonstrating Electrochemical CO$_2$ Capture on Redox-Active Metal-Organic Frameworks

Addressing climate change calls for action to control CO$_2$ pollution. Direct air and ocean capture offer a solution to this challenge. Making carbon capture competitive with alternatives, such as forestation and mineralisation, requires fundamentally novel approaches and ideas. One such approach is electrosorption, which is currently limited by the availability of suitable electrosorbents. In this work, we introduce a metal-organic copper-2,3,6,7,10,11-hexahydroxytriphenylene (Cu$_3$(HHTP)$_2$) metal-organic framework (MOF) that can act as electrosorbent for CO$_2$ capture, thereby expanding the palette of materials that can be used for this process. Cu$_3$(HHTP)$_2$ is the first MOF to switch its ability to capture and release CO$_2$ in aqueous electrolytes. By using cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), galvanostatic charge-discharge (GCD) analysis, and differential electrochemical mass spectrometry (DEMS), we demonstrate reversible CO$_2$ electrosorption. Based on density functional theory (DFT) calculations, we provide atomistic insights into the mechanism of electrosorption and conclude that efficient CO$_2$ capture is facilitated by a combination of redox-active copper atom and aromatic HHTP ligand within Cu3(HHTP)2. By showcasing the applicability of Cu$_3$(HHTP)$_2$ -- with a CO$_2$ capacity of 2 mmol g$^{-1}$ and an adsorption enthalpy of -20 kJ mol$^{-1}$ - this study encourages further exploration of conductive redox-active MOFs in the search for superior CO$_2$ electrosorbents.

cond-mat.mtrl-sci↗

arXiv2024

Accounting for the Quantum Capacitance of Graphite in Constant Potential Molecular Dynamics Simulations

Molecular dynamics simulations at a constant electric potential are an essential tool to study electrochemical processes, providing microscopic information on the structural, thermodynamic, and dynamical properties. Despite the numerous advances in the simulation of electrodes, they fail to accurately represent the electronic structure of materials such as graphite. In this work, we introduce a simple parameterization method that allows to tune the metallicity of the electrode based on a quantum chemistry calculation of the density of states. As a first illustration, we study the interface between graphite electrodes and two different liquid electrolytes, an aqueous solution of NaCl and a pure ionic liquid, at different applied potentials. We show that the simulations reproduce qualitatively the experimentally-measured capacitance; in particular, they yield a minimum of capacitance at the point of zero charge, which is due to the quantum capacitance contribution. An analysis of the structure of the adsorbed liquids allows to understand why the ionic liquid displays a lower capacitance despite its large ionic concentration. In addition to its relevance for the important class of carbonaceous electrodes, this method can be applied to any electrode materials (e.g. 2D materials, conducting polymers, etc), thus enabling molecular simulation studies of complex electrochemical devices in the future.

cond-mat.mtrl-sci↗