New paper published in Advanced Materials Interfaces on SnO2/MXene batteries

New paper published on “Unraveling the Electrochemical Mechanism in Tin Oxide/MXene Nanocomposites as Highly Reversible Negative Electrodes for Lithium-Ion Batteries” in Advanced Materials Interfaces.

As the demand for power and energy storage continues to grow, we researchers are constantly exploring new ways to improve battery performance. One promising approach involves using conversion/alloying materials, such as tin oxide, to design high-performance lithium-ion batteries. While these materials show excellent performance and ease of preparation, they often suffer from mechanical instabilities during cycling that limits their usefulness. This issue can be addressed (and overcome) by combining tin oxide with MXene.

In this study, we prepared a 50/50 (by mass) tin oxide / Ti-MXene (SnO2/Ti3C2Tz) nanocomposite and optimized it as a negative electrode for lithium-ion batteries. The result? A nanocomposite that delivers over 500 mAh/g for 700 cycles at 0.1 A/g and demonstrates excellent rate capability, with 340 mAh/g at 8 A/g.

The success of this nanocomposite lies in the synergistic behavior of its two components, which we confirmed through ex situ chemical, structural, and morphological analyses. Not only does this knowledge allow us to formulate a reaction mechanism with lithium-ions that provides partial reversibility of the conversion reaction, but it also opens up new possibilities for designing high-performance lithium-ion batteries.

Thanks to our great team of collaborators:

Team Ricerca sul Sistema Energetico – RSE SpA & Università degli Studi di Milano-Bicocca:
Antonio Gentile
Chiara Ferrara
Stefano Marchionna
Riccardo Ruffo

Team INM-Leibniz Institute for New Materials:
Stefanie Arnold
Volker Presser

Team Karlsruhe Institute of Technology (KIT)
Yushu Tang
Julia Maibach
Christian Kübel

New article published in ChemSusChem on degradation of dye pollutants via Sb-SnO2 nanodesigned materials

Our research team has published an article in ChemSusChem on the promising use of stable and efficient SnO2 electrodes for degrading refractory organic pollutants in wastewater treatment. Our approach involved the preparation of Ti3+ self-doped urchin-like rutile TiO2 nanoclusters (TiO2-xNCs) on a Ti mesh substrate using hydrothermal and electroreduction methods, which served as an interlayer for the deposition of Sb-SnO2. Our TiO2-xNCs/Sb-SnO2 anode exhibited a high oxygen evolution potential and strong *OH generation ability, resulting in improved degradation performance for rhodamine B, methylene blue, alizarin yellow R, and methyl orange. Our unique rutile interlayer also extended the anode lifetime sixfold due to its good lattice match with SnO2 and three-dimensional concave-convex structure. Overall, our work highlights the importance of designing interlayer crystal forms and structures for achieving efficient and stable SnO2 electrodes in addressing dye wastewater problems. This work was done in collaboration with our colleagues from Chongqing University.

New paper published in the Journal of Industrial and Engineering Chemistry on TMAH recovery

New paper published in the Journal of Industrial and Engineering Chemistry. In cooperation with former group member Choonsoo Kim (now at Kongju University, Korea), we have used redox flow desalination for the valorization of tetramethylammonium hydroxide as a value-added organic compounds from wastewater which is widely being used as an etching solvent, photoresist developer, and surfactant
in semiconductor and display industries. By applying a low cell voltage (<1.2 V), a reversible redox
reaction allowed a continuous removal of TMAH from the wastewater stream and a simultaneous recovery for reuse as a form of tetramethylammonium cation. The TMAH removal rate was approximately
4.3 mM/g/h with a 40% recovery ratio.

New paper published in Communications Materials on 2D high entropy materials

New perspective paper published in Communications Materials. The high entropy concept is ideally suited for MXenes but also capable to be a unique tool to tailor and improve electrochemical properties in other materials.

Multiple principal element or high-entropy materials have recently been studied in the two-dimensional (2D) materials phase space. These promising classes of materials combine the unique behavior of solid-solution and entropy-stabilized systems with high aspect ratios and atomically thin characteristics of 2D materials. The current experimental space of these materials includes 2D transition metal oxides, carbides/carbonitrides/nitrides (MXenes), dichalcogenides, and hydrotalcites. However, high-entropy 2D materials have the potential to expand into other types, such as 2D metal-organic frameworks, 2D transition metal carbo-chalcogenides, and 2D transition metal borides (MBenes).

So, what is our perspective article about? We discuss the entropy stabilization from bulk to 2D systems, the effects of disordered multi-valent elements on lattice distortion and local electronic structures and elucidate how these local changes influence the catalytic and electrochemical behavior of these 2D high-entropy materials. We also provide a perspective on 2D high-entropy materials research and its challenges and discuss the importance of this emerging field of nanomaterials in designing tunable compositions with unique electronic structures for energy, catalytic, electronic, and structural applications.

This perspective paper has been the result of our collaboration with my dear friend Babak Anasori (with his team: Kartik Nemani and Brian Wyatt) from Purdue University and our team (including Mohammad Torkamanzadeh).

New paper published on solid lubrication of carbon nanotubes in ACS Applied Nano Materials

New paper published in ACS Applied Nano Materials. Rolling bearings need lubrication to operate smoothly, but when traditional methods fail, multiwall carbon nanotubes (MWCNT) can come to the rescue. To understand how MWCNTs lubricate highly loaded contacts, we combined experimentation and large-scale molecular dynamics simulations. We applied tribometry to iron plates coated with different types of MWCNTs, discovering that both resulted in a steady-state coefficient of friction of 0.18. Wear tracks and tribolayers revealed a transformation process, resulting in layers of MWCNT fragments, iron oxide, and iron carbide nanoparticles embedded in an amorphous carbon matrix. We also found that MWCNTs slide against the ball interface to provide low carbon transfer to the counter body. Molecular dynamics simulations predicted a low-load regime that keeps MWCNTs intact, and a high-load regime that partially collapses the tube structure, forming a-C regions. We confirmed the results through transmission electron microscopy, and formulated a multistep lubrication mechanism for MWCNT coatings rubbing against alumina on an iron substrate. This work was done in collaboration with the teams of Frank Mücklich and Michael Moseler.

New paper published in Journal of the American Ceramic Society on oxide/carbon hybrid electrodes for Lithium-ion batteries

New paper published in the Journal of the American Ceramic Society on the synthesis of new hybrid electrode materials for Li-ion batteries (LIBs). Through controlled oxidation of layered Ti2SnC, we were able to obtain TiO2-SnO2-C/carbide hybrid materials using two different methods: partial oxidation in an open-air furnace (OAF) and rapid thermal annealing (RTA). The resulting carbide phase included both residual Ti2SnC and TiC as a reaction product. In testing, we found that the sample oxidized in the OAF at 700°C for 1 hour had the highest initial lithiation capacity of 838 mAh/g at 100 mA/g. However, its delithiation capacity decreased to 427 mAh/g over cycling. In contrast, the RTA sample treated at 800°C for 30 seconds demonstrated the most efficient performance, with a reversible capacity of approximately 270 mAh/g after 150 cycles and a specific capacity of about 150 mAh/g under high cycling rate (2000 mA/g). Our findings suggest that this processing method could have wide-ranging applications in energy storage, particularly for other members of the MAX family. This work was the latest product of collaboration with the team of Michael Naguib (Tulane University, USA).

New paper published in Carbon on photocatalytic use of TiO2 loaded carbon spherogels

New paper published in Carbon. This is our latest work from our collaboration with our Austrian partners now being published in the January issue of Carbon. Combining the expertise in catalysis of the Eder group (TU Vienna) with the innovative carbon spherogel material developed by Michael Elsaesser from the Hüsing Group (Paris Lodron Universität Salzburg) makes up for an interesting system. Spherogels are hollow carbon spheres which, as shown by this work, can be conveniently loaded with electrocatalytically active species, such as titania. In our case, we studied the photocatalytic hydrogen evolution.

New paper published in ACS Omega on Cu-Fe sulfides for lithium-ion batteries

New paper published in ACS Omega. Batteries employing transition-metal sulfides enable high-charge storage capacities, but polysulfide shuttling and volume expansion cause structural disintegration and early capacity fading. The design of heterostructures combining metal sulfides and carbon with an optimized morphology can effectively address these issues. Our work introduces dopamine-coated copper Prussian blue (CuPB) analogue as a template to prepare nanostructured mixed copper–iron sulfide electrodes. The material was prepared by coprecipitation of CuPB with in situ dopamine polymerization, followed by thermal sulfidation. Dopamine controls the particle size and favors K-rich CuPB due to its polymerization mechanism. While the presence of the coating prevents particle agglomeration during thermal sulfidation, its thickness demonstrates a key effect on the electrochemical performance of the derived sulfides. After a two-step activation process during cycling, the C-coated KCuFeS2 electrodes showed capacities up to 800 mAh/g at 10 mA/g with nearly 100% capacity recovery after rate handling and a capacity of 380 mAh/g at 250 mA/g after 500 cycles.

New paper published in Electrochimica Acta on Ni-decorated AgAu alloy graphene/cobalt hydroxide electrodes for flexible micro-supercapacitors

New paper published in Electrochimica Acta on Ni-decorated AgAu alloy graphene/cobalt hydroxide electrodes for micro-supercapacitors to obtain high-performance micro-supercapacitors. A nanocomposite of graphene, cobalt hydroxide and nickel can was obtained from using gold-silver alloy lines. Using a two-step electrodeposition method, the scaly morphology is pre-deposited on a Ni film, followed by the interconnecting corrugated graphene/cobalt hydroxide composite nanomaterial. The resulting device, a graphene/cobalt hydroxide/Ni//activated carbon flexible micro-supercapacitor (MSC), was assembled by gel KOH-PVA electrolyte, graphene/cobalt hydroxide/Ni (positive electrode), and activated carbon (negative electrode). When testing, we obtained a volumetric energy of about 19 mWh/cm3 and the devices retained over 94% capacitance after 10,000 cycles. After 1,000 continuous bending/unbending cycles at a 180° bending angle with the frequency of 100 mHz, the capacitance retention of MSC is still maintained at 97% of the initial value.

New paper published in ACS Energy Letters on continuous Li-ion harvesting from seawater

new paper published in ACS Energy Letters on continuous electrochemical lithium-ion extraction. We used a redox electrolyte “engine” to drive the ion transfer (in our case: potassium ferricyanide). Employing a pair of ceramic lithium superionic conductor (LISICON) membranes meant that only Lithium ions were accessible to the redox electrolyte for charge compensation. And to complement the design, we used an anion exchange membrane to separate the inflow (e.g., seawater) from a recovery solution. By this way, we obtained an electrochemical system for the continuous extraction of Lithium ions. This sets this technology apart from earlier works (including our contributions) that relied on a cyclic operation to obtain ion separation. Yet, this is just one of many more steps towards seeing such technology toward application; future research must critically address cell design, optimization of the Li-membranes, and investigating the robustness and durability of continuous operation.

This work was the result of the collaboration of our Ph.D. students Lei Wang, Stefanie Arnold, Panyu Ren, and our former Postdoc (now group leader at Bavarian Center for Battery Technology (BayBatt)Qingsong Wang, as well as our Chinese collaborators Jun Jin and Zahoyin Wen (Chinese Academy of Sciences).