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Instruments / Technical Area	Publication Details	Published	Actions
I09-Surface and Interface Structural Analysis	On the use of Ti3C2Tx MXene as a negative electrode material for lithium-ion batteries Tatiana Koriukina , Antonia Kotronia , Joseph Halim , Maria Hahlin , Johanna Rosen , Kristina Edström , Leif Nyholm Acs Omega DOI: 10.1021/acsomega.2c05785 Diamond Proposal Number(s): [23159, 26551] Open Access Show Abstract ▼ Abstract: The pursuit of new and better battery materials has given rise to numerous studies of the possibilities to use two-dimensional negative electrode materials, such as MXenes, in lithium-ion batteries. Nevertheless, both the origin of the capacity and the reasons for significant variations in the capacity seen for different MXene electrodes still remain unclear, even for the most studied MXene: Ti3C2Tx. Herein, freestanding Ti3C2Tx MXene films, composed only of Ti3C2Tx MXene flakes, are studied as additive-free negative lithium-ion battery electrodes, employing lithium metal half-cells and a combination of chronopotentiometry, cyclic voltammetry, X-ray photoelectron spectroscopy, hard X-ray photoelectron spectroscopy, and X-ray absorption spectroscopy experiments. The aim of this study is to identify the redox reactions responsible for the observed reversible and irreversible capacities of Ti3C2Tx-based lithium-ion batteries as well as the reasons for the significant capacity variation seen in the literature. The results demonstrate that the reversible capacity mainly stems from redox reactions involving the Tx–Ti–C titanium species situated on the surfaces of the MXene flakes, whereas the Ti–C titanium present in the core of the flakes remains electro-inactive. While a relatively low reversible capacity is obtained for electrodes composed of pristine Ti3C2Tx MXene flakes, significantly higher capacities are seen after having exposed the flakes to water and air prior to the manufacturing of the electrodes. This is ascribed to a change in the titanium oxidation state at the surfaces of the MXene flakes, resulting in increased concentrations of Ti(II), Ti(III), and Ti(IV) in the Tx–Ti–C surface species. The significant irreversible capacity seen in the first cycles is mainly attributed to the presence of residual water in the Ti3C2Tx electrodes. As the capacities of Ti3C2Tx MXene negative electrodes depend on the concentration of Ti(II), Ti(III), and Ti(IV) in the Tx–Ti–C surface species and the water content, different capacities can be expected when using different manufacturing, pretreatment, and drying procedures.	Nov 2022
I09-Surface and Interface Structural Analysis	Strategies of mitigating dissolution of solid electrolyte interphases in sodium‐ion batteries Le Anh Ma , Andrew J. Naylor , Leif Nyholm , Reza Younesi Angewandte Chemie International Edition DOI: 10.1002/anie.202013803 Diamond Proposal Number(s): [23159] Open Access Show Abstract ▼ Abstract: With emerging interest in sodium‐ion battery (SIB) technology due to its cost effectiveness and high earth abundance of sodium, the search for an optimised SIB system becomes more and more crucial. It is well known that the formation of a stable solid electrolyte interphase (SEI) at the anode in Na‐based systems is a challenge due to the higher solubility of the SEI components compared to in the lithium‐ion battery case. Our knowledge about the formation and dissolution of the SEI in SIBs is so far based on limited experimental data. The aim of the present research is therefore to enhance the understanding of the behaviour of the SEI in SIBs and shed more light on the influence of the electrolyte chemistry on the dissolution of the SEI. By conducting electrochemical tests including extended open circuit pauses, we study the SEI dissolution in different time domains. With this, it is possible to determine the extent of self‐discharge due to SEI dissolution during a specific time. Instead of using a conventional separator, β‐alumina is employed as a Na‐conductive membrane to avoid crosstalk between the working electrode and Na‐metal counter electrode. The SEI composition is monitored using synchrotron‐based soft X‐ray photoelectron spectroscopy (SOXPES). The electrochemical and XPS results show that the SEIs formed in the studied electrolyte systems have different stabilities. The relative capacity loss after a 50‐hour pause in the tested electrolyte systems can be up to 30%. Among three carbonate‐based solvent systems, NaPF 6 in ethylene carbonate: diethyl carbonate exhibits the most stable SEI. The addition of electrolyte additives improves the SEI stability in PC. The electrolyte is saturated with typical SEI species, NaF and Na 2 CO 3 , in order to oppose the dissolution of the SEI. Furthermore, the solubilities of the latter additives in the different solvent systems are determined by inductively coupled plasma – optical emission spectrometry.	Nov 2020

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