Prof. Dr. Volker Presser

Prof. Dr. Volker Presser

Leiter Energie-Materialien

Publikationen

2023
Polyacrylonitrile-containing amphiphilic block copolymers: self-assembly and porous membrane formation

Gemmer, Lea | Niebuur, Bart-Jan | Dietz, christian | Rauber, Daniel | Plank, Martina | Frieß, Florian V. | Presser, Volker | Stark, Robert W. | Kraus, Tobias | Gallei, Markus

DOI:

The development of hierarchically porous block copolymer (BCP) membranes via the application of the self-assembly and non-solvent induced phase separation (SNIPS) process is one important achievement in BCP science in the last decades. In this work, we present the synthesis of polyacrylonitrile-containing amphiphilic BCPs and their unique microphase separation capability, as well as their applicability for the SNIPS process leading to isoporous integral asymmetric membranes. Poly(styrene-co-acrylonitrile)-b-poly(2-hydroxyethyl methacrylate)s (PSAN-b-PHEMA) are synthesized via a two-step atom transfer radical polymerization (ATRP) procedure rendering PSAN copolymers and BCPs with overall molar masses of up to 82 kDa while maintaining low dispersity index values in the range of Đ = 1.13–1.25. The polymers are characterized using size-exclusion chromatography (SEC) and NMR spectroscopy. Self-assembly capabilities in the bulk state are examined using transmission electron microscopy (TEM) and small-angle X-ray scattering (SAXS) measurements. The fabrication of isoporous integral asymmetric membranes is investigated, and membranes are examined by scanning electron microscopy (SEM). The introduction of acrylonitrile moieties within the membrane matrix could improve the membranes’ mechanical properties, which was confirmed by nanomechanical analysis using atomic force microscopy (AFM).

DOI:

Polymer Chemistry ,
2023, 14 (42), 4825-4837.

OPEN ACCESS
Continuous wet chemical synthesis of Mo(C,N,O)x as anode materials for Li-ion batteries†

Abdirahman Mohamed, Mana | Arnold, Stefanie | Janka, Oliver | Quade, Antje | Schmauch, Jörg | Presser, Volker | Kickelbick, Guido

DOI:

Molybdenum carbides, oxides, and mixed anionic carbide–nitride–oxides Mo(C,N,O)x are potential anode materials for lithium-ion batteries. Here we present the preparation of hybrid inorganic–organic precursors by a precipitation reaction of ammonium heptamolybdate ((NH4)6Mo7O24) with para-phenylenediamine in a continuous wet chemical process known as a microjet reactor. The mixing ratio of the two components has a crucial influence on the chemical composition of the obtained material. Pyrolysis of the precipitated precursor compounds preserved the size and morphology of the micro- to nanometer-sized starting materials. Changes in pyrolysis conditions such as temperature and time resulted in variations of the final compositions of the products, which consisted of mixtures of Mo(C,N,O)x, MoO2, Mo2C, Mo2N, and Mo. We optimized the reaction conditions to obtain carbide-rich phases. When evaluated as an anode material for application in lithium-ion battery half-cells, one of the optimized materials shows a remarkably high capacity of 933 mA h g−1 after 500 cycles. The maximum capacity is reached after an activation process caused by various conversion reactions with lithium.

DOI:

Journal of Materials Chemistry A ,
2023, 23 (11), 19936-19954.

OPEN ACCESS
Redox flow desalination for tetramethylammonium hydroxide removal and recovery from semiconductor wastewater

Ahn, Dayoung | Kim, Seonghwan | Ren, Panyu | Presser, Volker | Kim, Choonsoo

DOI:

As part of humankind’s path towards more sustainable water technologies, redox flow desalination (RFD) has emerged as a promising technology due to its high energy efficiency and easy operation. So far, RFD research has focused on removing and recovering inorganic salts such as lithium-ions, heavy metal ions, or phosphate and nitrate ions. Thus, the potential of RFD in water desalination and resource recovery processes has not been fully demonstrated. Therefore, this study aimed to assess RFD for the valorization of tetramethylammonium hydroxide (TMAH) as value-added organic compounds from wastewater beyond inorganic elements, 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. With various operational conditions (i.e., TMAH concentration, cell voltage, and flow rate), our system exhibited a high potential for the valorization of TMAH with 60% reduction in capital cost compared to conventional desalination processes.

DOI:

Journal of Industrial and Engineering Chemistry ,
2023, 118 147-154.

Mechanically Stable, Binder-Free, and Free-Standing Vanadium Trioxide/Carbon Hybrid Fiber Electrodes for Lithium-Ion Batteries

Bornamehr, Behnoosh | Gallei, Markus | Husmann, Samantha | Presser, Volker

DOI:

Abstract Binder is a crucial component in present-day battery electrodes but commonly contains fluorine and requires coating processing using organic (often toxic) solvents. Preparing binder-free electrodes is an attractive strategy to make battery electrode production and its end-of-use waste greener and safer. Here, electrospinning is employed to prepare binder-free and self-standing electrodes. Such electrodes often suffer from low flexibility, and the correlation between performance and flexibility is usually overlooked. Processing parameters affect the mechanical properties of the electrodes, and for the first time it is reported that mechanical flexibility directly influences the electrochemical performance of the electrode. The importance is highlighted when processing parameters advantageous to powder materials, such as a higher heat treatment temperature, harm self-standing electrodes due to deterioration of fiber flexibility. Other strategies, such as conductive carbon addition, can be employed to improve the cell performance, but their effect on the mechanical properties of the electrodes must be considered. Rapid heat treatment achieves self-standing V2O3 with a capacity of 250 mAh g−1 at 250 mA g−1 and 390 mAh g−1 at 10 mA g−1

DOI:

Advanced Sustainable Systems ,
2023, 7 (2), 2200373.

OPEN ACCESS
Prussian blue and its analogues as functional template materials: control of derived structure compositions and morphologies

Bornamehr, Behnoosh | Presser, Volker | Zarbin, Aldo J.G. | Yamauchi, Yusuke | Husmann, Samantha

DOI:

Hexacyanometallates, known as Prussian blue (PB) and its analogues (PBAs), are a class of coordination
compounds with a regular and porous open structure. The PBAs are formed by the self-assembly of
metallic species and cyanide groups. A uniform distribution of each element makes the PBAs robust
templates to prepare hollow and highly porous (hetero)nanostructures of metal oxides, sulfides, carbides,
nitrides, phosphides, and (N-doped) carbon, among other compositions. In this review, we examine
methods to derive materials from PBAs focusing on the correlation between synthesis steps and
derivative morphologies and composition. Insights into catalytic and electrochemical properties resulting
from different derivatization strategies are also presented. We discuss challenges in manipulating the
derivatives' properties, give perspectives of synthetic approaches for the target applications and present
an outlook on less investigated grounds in Prussian blue derivatives

DOI:

Journal of Materials Chemistry A ,
2023, 11 10473-10492.

OPEN ACCESS
Wet-Chemical Etching and Delamination of MoAlB into MBene and Its Outstanding Photocatalytic Performance

Bury, Dominika | Jakubcza, Michal | Purbayanto, Muhammad A. K. | Birowska, Magdalena | Wójcik, Anna | Moszczynska, Dorota | Eisawi, Karamullah | Prenger, Kaitlyn | Presser, Volker | Naguib, Michael | Jastrzebska, Agnieszka M.

DOI:

MBenes are post-MXene materials that contain boron in their structure instead of carbon and nitrogen. This unique composition offers an opportunity to explore the role of boron in the performance of 2D materials. However, wet-chemical etching and delamination of the starting MoAlB phase are challenging due to the persistent bonding of aluminum atoms with their neighboring elements. Herein, it is overcome by processing MoAlB for 24, 48, and 72 h with an aqueous HCl/H2O2 solution. The time-wise etching and delamination delivers individual single-to-few layered 48-MBene flakes. The theoretical-to-experimental XRD analysis revealed the best-delaminated 48-MBene having Mo2B2 orthorhombic lattice arrangement. The presence of Mo oxide allows direct 1.2 eV and indirect 0.2 eV optical band gaps and outstanding photocatalytic activity in decomposing methylene blue as a model organic contaminant. The 48-MBene photocatalyst achieves about 90% of MB decomposition under ultraviolet and simulated white light irradiation with three times faster kinetics outperforming even hybridized MXenes. In addition, 48-MBene appeared best suited to utilize the full spectrum of visible light into reactive oxygen species. Conversely, 24-MBene and 72-MBene shows incomplete delamination or oxidation, hampering their photocatalytic activity. The obtained results open an experimental pathway to apply MBenes in environmental remediation.

DOI:

Advanced Functional Materials ,
2023, 33 2308156.

Hydrogel-Based Flexible Energy Storage Using Electrodes Based on Polypyrrole and Carbon Threads

de Andrade Ruthes, Jean G. | Deller, Andrei E. | Pameté, Emmanuel | Riegel-Vidotti, Izabel C. | Presser, Volker | Vidotti, Marcio

DOI:

Developing new flexible and electroactive materials is a significant challenge to producing safe, reliable, and environmentally friendly energy storage devices. This study introduces a promising electrolyte system that fulfills these requirements. First, polypyrrole (PPy) nanotubes are electropolymerized in graphite-thread electrodes using methyl orange (MO) templates in an acidic medium. The modification increases the conductivity and does not compromise the flexibility of the electrodes. Next, flexible supercapacitors are built using hydrogel prepared from poly(vinyl alcohol) (PVA)/sodium alginate (SA) obtained by freeze–thawing and swollen with ionic solutions as an electrolyte. The material exhibits a homogenous and porous hydrogel matrix allowing a high conductivity of 3.6 mS cm−1 as-prepared while displaying great versatility, changing its electrochemical and mechanical properties depending on the swollen electrolyte. Therefore, it allows its combination with modified graphite-thread electrodes into a quasi-solid electrochemical energy storage device, achieving a specific capacitance (Cs) value of 66 F g−1 at 0.5 A g−1. Finally, the flexible device exhibits specific energy and power values of 19.9 W kg−1 and 3.0 Wh kg−1, relying on the liquid phase in the hydrogel matrix produced from biodegradable polymers. This study shows an environment friendly, flexible, and tunable quasi-solid electrolyte, depending on a simple swell experiment to shape its properties according to its application.

DOI:

Advanced Materials Interfaces ,
2023, 10 (27), 2300373.

OPEN ACCESS
Interlaboratory study assessing the analysis of supercapacitor electrochemistry data

Gittins, Jamie W. | Chen, Yuan | Arnold, Stefanie | Augustyn, Veronica | Balducci, Andrea | Brousse, Thierry | Frackowiak, Elzbieta | Gómez-Romero, Pedro | Kanwade, Archana | Köps, Lukas | Kumar Jha, Plawan | Lyu, Dongxun | Meo, Michele | Pandey, Deepak | Pang, Le | Presser, Volker | Rapisarda, Mario | Rueda-García, Daniel | Saeed, Saeed | Shirage, Parasharam M. | Forse, Alexander C.

DOI:

Supercapacitors are fast-charging energy storage devices of great importance for developing robust and climate-friendly energy infrastructures for the future. Research in this field has seen rapid growth in recent years, therefore consistent reporting practices must be implemented to enable reliable comparison of device performance. Although several studies have highlighted the best practices for analysing and reporting data from such energy storage devices, there is yet to be an empirical study investigating whether researchers in the field are correctly implementing these recommendations, and which assesses the variation in reporting between different laboratories. Here we address this deficit by carrying out the first interlaboratory study of the analysis of supercapacitor electrochemistry data. We find that the use of incorrect formulae and researchers having different interpretations of key terminologies are major causes of variability in data reporting. Furthermore we highlight the more significant variation in reported results for electrochemical profiles showing non-ideal capacitive behaviour. From the insights gained through this study, we make additional recommendations to the community to help ensure consistent reporting of performance metrics moving forward.

DOI:

Journal of Power Sources ,
2023, 585 233637.

OPEN ACCESS
Growth of titania and tin oxide from Ti2SnC via rapid thermal oxidation in air for lithium-ion battery application

Jolly, Shae | Husmann, Samantha | Presser, Volker | Naguib, Michael

DOI:

Herein, we report the synthesis of TiO2–SnO2–C/carbide hybrid electrode materials for Li-ion batteries (LIBs) via two different methods of controlled oxidation of layered Ti2SnC. The material was partially oxidized in an open-air furnace (OAF) or using a rapid thermal annealing (RTA) approach to obtain the desired TiO2–SnO2–C/carbide hybrid material; the carbide phase encompassed both residual Ti2SnC and TiC as a reaction product. We tested the oxidized materials as an anode in a half cell to investigate their electrochemical performance in LIBs. Analysis of the various oxidation conditions indicated the highest initial lithiation capacity of 838 mAh/g at 100 mA/g for the sample oxidized in the OAF at 700°C for 1 h. Still, the delithiation capacity dropped to 427 mAh/g and faded over cycling. Long-term cycling demonstrated that the RTA sample treated at 800°C for 30 s was the most efficient, as it demonstrated a reversible capacity of around 270 mAh/g after 150 cycles, as well as a specific capacity of about 150 mAh/g under high cycling rate (2000 mA/g). Given the materials’ promising performance, this processing method could likely be applied to many other members of the MAX family, with a wide range of energy storage applications.

DOI:

Journal of the American Ceramic Society ,
2023, 106 (5), 3261-3271.

OPEN ACCESS
Recycling and second life of MXene electrodes for lithium-ion batteries and sodium-ion batteries

Li, Yunjie | Arnold, Stefanie | Husmann, Samantha | Presser, Volker

DOI:

The fast growth of electric vehicles and electronic devices produces a mounting number of spent batteries which have reached their end of life. Therefore, it is essential to find a sustainable and efficient approach to battery recycling. Conventional recycling via high-temperature decomposition of the active components in the electrode material into elements level has the disadvantages of cumbersome operation, environmentally unfriendly, and high cost. Herein, one type of MXene material, annealed delaminated Ti3C2Tz (AD-Ti3C2Tz) electrodes, obtained by vacuum-assisted filtration and annealing processes, was directly used as free-standing anodes for both lithium-ion batteries and sodium-ion batteries without the use of binder or carbon additives. Electrochemical analysis showed that the non-diffusion-controlled redox reaction dominates the electrochemical behavior of the AD-Ti3C2Tz electrode. Furthermore, the AD-Ti3C2Tz electrode exhibits good electrochemical performance without adding conductive carbon in lithium-ion and sodium-ion batteries. For example, the lithium storage capacity was 89 mAh g−1 after 2000 cycles at a specific current of 1 A g−1. The sodium storage capacity is 108 mAh g−1 and 71 mAh g−1 at 0.02 A g−1 and 2 A g−1, respectively. After AD-Ti3C2Tz electrodes reach the end of their battery life, facile direct recycling processes were employed to recover the electrodes and the capacity recovery rate is above 90 %. Besides, the cycled MXene electrodes can be easily oxidized into TiO2/C hybrids with adjustable carbon content by changing the heat-treatment temperature in CO2 flow. The obtained TiO2/C could be widely applied in batteries and the electrocatalysis field, which realizes the second life of cycled MXene.

DOI:

Journal of Energy Storage ,
2023, 60 106625.