Editorial Material
Chemistry, Multidisciplinary
Linfang Lu, Baizeng Fang
Summary: Scientists have reported an efficient catalyst that can produce cyclohexanone oxime with high selectivity (>95%) through in-situ generated H2O2, comparable to the current industrial route. The use of in-situ generated H2O2 can achieve significant cost savings in current oxime production and is believed to have promising prospects in other industrial chemical reactions requiring H2O2.
Article
Multidisciplinary Sciences
Jiwon Kim, Jae Hyung Kim, Cheoulwoo Oh, Hyewon Yun, Eunchong Lee, Hyung-Suk Oh, Jong Hyeok Park, Yun Jeong Hwang
Summary: An electro-assisted approach using acid-treated carbon electrocatalyst and in-situ cathodically generated reactive oxygen species is proposed for the partial oxidation of methane at ambient temperature and pressure. Reactive oxygen species activate methane and methanol, leading to selective methane partial oxidation. This study presents a method for the electrochemically assisted partial oxidation of methane to produce liquid oxygenate, HCOOH, selectively.
NATURE COMMUNICATIONS
(2023)
Article
Materials Science, Ceramics
Siqiao Teng, Wen Xie, Dong Zhang, Junyi Yang, Bin Quan, Xiaochi Lu
Summary: The development of dielectric microwave absorbing materials with broad electromagnetic response is a significant project in the field. In this work, thermal-assisted in-situ bonding technology was used to fabricate the composite absorbing materials. The resulting aerogel showed strong interface contacting, good mechanical stability, and ultra-broad effective bandwidth, making it suitable for large-scale production of microwave absorbing devices.
CERAMICS INTERNATIONAL
(2023)
Article
Environmental Sciences
Emily Summers, Jiabi Du, Kyeong Park, Karl Kaiser
Summary: Much remains unknown about the transport behavior of microplastic pollutants in marine environments, specifically in smaller coastal systems like estuaries. Using a combination of a Lagrangian particle-tracking model and a validated 3D hydrodynamic model, this study investigated the transport, pathway, and fate of microplastic particles in an idealized estuary and Galveston Bay, Texas. The study focused on differences due to settling behavior, diffusion processes, and release location. The results showed that settling behavior significantly influenced the transport pathway and retention time of microplastic particles, with negatively buoyant particles being retained longer and dispersing in a different direction compared to neutrally buoyant particles. The study emphasized the need to quantify the specific settling velocities of plastic pollutants in coastal estuarine systems.
SCIENCE OF THE TOTAL ENVIRONMENT
(2023)
Article
Chemistry, Physical
Xiangyao Gu, Min Yu, Siqi Chen, Xueqin Mu, Zihan Xu, Wenqian Shao, Jinjing Zhu, Changyun Chen, Suli Liu, Shichun Mu
Summary: Seawater electrolysis holds promise for renewable production of green hydrogen, but its hydrogen evolution reaction (HER) faces difficulties due to electrode corrosion and undesirable side reactions. This study reveals that replacing some Ru atoms with atomically dispersed non-stoichiometric CdySex can optimize the catalyst's activity, resulting in higher activity and lower overpotential in seawater.
Article
Materials Science, Ceramics
Yurun Feng, Xue Guo, Junbin Lu, Jie Liu, Guantong Wang, Hongyu Gong
Summary: SiCN(Fe) fibers with excellent one-dimensional microstructure and EMW absorption performance were synthesized using PDCs method and electrospinning. The in-situ generation of Fe3Si and CNTs by adding FA effectively improved the properties of the fibers. The EMW absorption of SiCN(Fe) fibers mainly relies on dipole polarization loss, interface polarization loss, and eddy current loss.
CERAMICS INTERNATIONAL
(2021)
Article
Engineering, Environmental
Ruby Pyke, Nathalie Fortin, Jessica Wasserscheid, Julien Tremblay, Lars Schreiber, Marie-Josee Levesque, Stephanie Messina-Pacheco, Lyle Whyte, Feiyue Wang, Kenneth Lee, David Cooper, Charles W. Greer
Summary: The microbial response and biodegradability of residues from in-situ burning were studied using microcosms. The results showed that the concentrations of hydrocarbons and polycyclic aromatic hydrocarbons (PAHs) in the residues decreased, especially in residues generated from burning weathered diesel.
JOURNAL OF HAZARDOUS MATERIALS
(2023)
Article
Chemistry, Organic
Linqing Wang, Dongxu Yang
Summary: The paper reviews the progress in the development of in situ generated magnesium catalysts for asymmetric synthesis, presenting a concise classification of different modes and discussing representative mechanisms. It predicts the future development of more innovative and creatively structured magnesium catalysts to overcome challenges in enantioselective reactions.
Article
Chemistry, Inorganic & Nuclear
Luisa Kaufmann, Steffen A. Foehrenbacher, Michael C. Krummer, Burkhard Butschke
Summary: The novel bidentate PP and PN ligands, L-PP and L-PN, have been designed for the stabilization of heterodinuclear complexes. The synthesis of heterodinuclear complexes with L-PP is straightforward and shows high selectivity. While similar experiments with L-PN have not been successful, it can still serve as a ditopic ligand.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2023)
Article
Multidisciplinary Sciences
Zhangyan Mu, Na Han, Dan Xu, Bailin Tian, Fangyuan Wang, Yiqi Wang, Yamei Sun, Cheng Liu, Panke Zhang, Xuejun Wu, Yanguang Li, Mengning Ding
Summary: In this study, the surface adsorption and sub-surface absorption of hydrogen on Pd and its alloy nanocatalysts are quantified under operando electrocatalytic conditions. The competitive relationship between electrochemical CO2 reduction and hydrogen sorption kinetics is investigated. The results reveal the key impacts of proton donors on the hydrogen sorption kinetics during CO2 reduction.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Analytical
Timothy Ronald Holbrook, Doriane Gallot-Duval, Thorsten Reemtsma, Stephan Wagner
Summary: A new method using laser ablation time-of-flight mass spectrometry was developed to directly analyze multi-elemental particles in sediment samples. The comparison between different techniques showed that laser ablation time-of-flight mass spectrometry is well-suited for measuring low abundant elements in unextracted sediment samples.
JOURNAL OF ANALYTICAL ATOMIC SPECTROMETRY
(2021)
Article
Chemistry, Multidisciplinary
Xuemei Zhou, George E. Sterbinsky, Eman Wasim, Linxiao Chen, Steven L. Tait
Summary: This study investigated the impact of the choice of organic ligand on the activity and stability of TiO2-supported single-atom Pt-ligand catalysts for ethylene hydrogenation. The results showed that the activity of these catalysts significantly depended on the coordination number of the ligand, with the lowest coordination number ligand showing the highest reaction rate. Through in-situ X-ray absorption spectroscopy experiments, it was found that the activity correlated with good heterolytic dissociation of hydrogen, and the ligand-coordinated catalysts showed excellent stability against structural and chemical change, suggesting potential new applications at high temperatures.
Article
Multidisciplinary Sciences
Xiaozhi Su, Zhuoli Jiang, Jing Zhou, Hengjie Liu, Danni Zhou, Huishan Shang, Xingming Ni, Zheng Peng, Fan Yang, Wenxing Chen, Zeming Qi, Dingsheng Wang, Yu Wang
Summary: This article investigates the activity and selectivity issues of copper-based materials in converting carbon dioxide into multi-carbon products, and reports a high-performance CO2RR catalyst. Through in-situ experiments and computational methods, the authors demonstrate the atomic structure-activity relationship of the catalyst and reveal the potential-dependent transformation of Cu-2-CuN3 clusters and the role of charge-asymmetric sites in efficient ethanol formation.
NATURE COMMUNICATIONS
(2022)
Article
Engineering, Chemical
Julia Szabadi, Joerg Meyer, Achim Dittler
Summary: The morphology of particle deposits on filter fibers was studied for gas-cleaning filter design. Polydisperse particulate material was used to generate particle structures through diffusion or interception and inertia. The structures were compared quantitatively to those of monodisperse material, showing similarities. In situ investigation was shown to provide artifact-free results for dendritic particle structures of Carbon Black. The characteristics of particle structures at different Peclet numbers were evaluated.
JOURNAL OF AEROSOL SCIENCE
(2023)
Article
Chemistry, Physical
Bing Hu, Bapurao Bharate, Juan D. Jimenez, Jochen Lauterbach, Naoto Todoroki, Toshimasa Wadayama, Kotaro Higashi, Tomoya Uruga, Yasuhiro Iwasawa, Hiroko Ariga-Miwa, Satoru Takakusagi, Kiyotaka Asakura
Summary: The difference in Pt-Pt bond distance between PtAu nanoparticles and Pt overlayer on Au(111) is revealed. The abnormal bond lengths are attributed to the surface tension and lattice distortion relaxation. The surface tension results in a decrease in Pt-Pt bond length in PtAu nanoparticles, while lattice distortion between Pt overlayer and substrate is the driving force for the expansion of Pt-Pt bond length on flat Au surfaces.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Swen Zerebecki, Soma Salamon, Joachim Landers, Yuke Yang, Yujin Tong, Eko Budiyanto, Daniel Waffel, Maik Dreyer, Sascha Saddeler, Tim Kox, Stephane Kenmoe, Eckhard Spohr, Stephan Schulz, Malte Behrens, Martin Muhler, Harun Tueysuez, R. Kramer Campen, Heiko Wende, Sven Reichenberger, Stephan Barcikowski
Summary: This study investigates the effects of cation occupancy on oxidation catalysis by utilizing pulsed laser defect engineering. By gradually altering the cation occupancy and studying its impact on the oxidation reaction of cinnamyl alcohol, the importance of octahedral Co3+ sites and the feasibility of pulsed laser processing in changing cation occupancy and crystallographic defect density are demonstrated.
Article
Materials Science, Multidisciplinary
Friedrich Waag, Wessam I. M. A. Fares, Yao Li, Corina Andronescu, Bilal Gokce, Stephan Barcikowski
Summary: Alloy nanoparticles offer the possibility to tune functional properties of nanoscale structures. This study experimentally contributes to the understanding of mixing processes during laser-based synthesis of alloy nanoparticles and highlights the benefits of well pre-mixed ablation targets and longer laser pulse durations.
JOURNAL OF MATERIALS SCIENCE
(2022)
Article
Electrochemistry
Vaijayanthi Ramesh, Brian Giera, John J. Karnes, Nadine Stratmann, Viktor Schaufler, Yao Li, Christoph Rehbock, Stephan Barcikowski
Summary: This study demonstrates the beneficial effects of using ethanol-water mixtures as a solvent for electrophoretic deposition of platinum nanoparticles (PtNPs) on neural electrodes. The deposition process enhances the electrode's electrical performance by increasing the active surface area and reducing impedance.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Sandra Zwiehoff, Jacob Johny, Carina Behrends, Alina Landmann, Florian Mentzel, Christian Baeumer, Kevin Kroeninger, Christoph Rehbock, Beate Timmermann, Stephan Barcikowski
Summary: Proton irradiation-induced ROS generation sensitized by noble metal nanoparticles is driven by the total available particle surface area rather than particle size or mass. A distinctive material effect with platinum being more active than gold is observed, indicating that the chemical reactivity of the nanoparticle surface is a main contributor to ROS generation upon proton irradiation.
Article
Chemistry, Physical
Anna R. Ziefuss, Michael Willeke, Matthias Miertz, Alexander Heinemann, Christoph Rehbock, Stephan Barcikowski
Summary: Noble metal alloy nanoclusters (NCs) are intriguing systems that combine the properties of two or more elements, resulting in interesting fluorescence phenomena. Previous studies have focused on ligand-capped NCs from wet chemical synthesis, making it difficult to determine the extent to which fluorescence is affected by ligand-induced effects or the elemental composition of the metal core. This study used laser fragmentation in liquids (LFL) to create ligand-free gold-rich bi-metallic AuPt NCs and demonstrated the effectiveness of this technique in producing a series of 1nm alloy NCs with varying molar fractions. The research found that ligand-free NCs exhibit photoluminescence beyond just gold, but the presence of even small amounts of Pt atoms in the AuPt NCs leads to quenching and red-shift of the fluorescence, potentially due to changes in surface charge density.
Article
Engineering, Biomedical
Yaya Li, Vaijayanthi Ramesh, Faina Bider, Nathan Bradshaw, Christoph Rehbock, Aldo R. Boccaccini, Stephan Barcikowski
Summary: In this study, nanosized bioactive glass (BG) was produced using the reactive laser fragmentation in liquids method. The doped nanoscopic BG samples showed promising potential for angiogenesis or bone regeneration, with adjustable doping levels and good cytocompatibility.
JOURNAL OF BIOMEDICAL MATERIALS RESEARCH PART A
(2022)
Article
Optics
Maximilian Spellauge, Carlos Donate-Buendia, Stephan Barcikowski, Bilal Goekce, Heinz P. Huber
Summary: Laser ablation in liquids is an interdisciplinary method that can generate surfactant-free and stable nanoparticles from almost any material. Ablation dynamics occurring on a sub-nanosecond timescale are essential for nanoparticle generation. This study visualizes the complete spatiotemporal picosecond laser-induced ablation dynamics of gold in air and water, revealing the significant influence of the water confinement layer on the entire investigated timescale from picoseconds to microseconds.
LIGHT-SCIENCE & APPLICATIONS
(2022)
Article
Chemistry, Physical
Frederic Stein, Sebastian Kohsakowski, Ricardo Martinez-Hincapie, Sven Reichenberger, Christoph Rehbock, Viktor Colic, Daniel Guay, Stephan Barcikowski
Summary: The catalytic activity and toxicity of mixed-metal nanoparticles depend on their surface composition. This study analyzed the electrochemical properties and redox chemistry of different gold-silver alloy nanoparticles with varying gold content. The results showed that the surface gold content influenced the oxygen reduction reaction and the stability of the particles. XPS analysis revealed the accumulation of the minor constituent on the surface of the alloy nanoparticles. The equimolar Au50Ag50 composition exhibited particularly low reactivity and high chemical stability.
FARADAY DISCUSSIONS
(2023)
Article
Mechanics
Alexander Bussmann, Farbod Riahi, Bilal Goekce, Stefan Adami, Stephan Barcikowski, Nikolaus A. Adams
Summary: This study investigates the dynamics of a single cavitation bubble near a horizontal wall during expansion and collapse using a sharp-interface level-set method. A finite-volume formulation with low-dissipation high-order reconstruction schemes is utilized, considering viscosity and surface tension. The simulations are conducted in three-dimensional axi-symmetric space and cover a wide range of initial bubble wall standoff distances. The focus is primarily on the near-wall region.
Article
Chemistry, Multidisciplinary
Maximilian Spellauge, Meike Tack, Rene Streubel, Matthias Miertz, Kai Steffen Exner, Sven Reichenberger, Stephan Barcikowski, Heinz Paul Huber, Anna Rosa Ziefuss
Summary: Pulsed laser fragmentation of microparticles is a synthesis method for producing high-purity nanoparticles from any material. By studying the fragmentation mechanism of single IrO2 microparticles in water, the contribution of stress-mediated processes is highlighted. The synthesis of nanoclusters from multiparticle fragmentation achieved high efficiency and catalytic activity, making them promising candidates in electrocatalytic sensing. These insights pave the way for laser fragmentation of microparticles to become a versatile and scalable technique for nanomaterial design and development.
Article
Chemistry, Physical
Theo Fromme, Lucie K. Tintrop, Sven Reichenberger, Torsten C. Schmidt, Stephan Barcikowski
Summary: Laser ablation in liquids is a scalable method for preparing nanoparticles and suppressing oxidation. The related chemical processes resulting from laser-induced decomposition reactions of organic solvents remain uncertain. This study investigates the solvent-dependent influence on gas formation rates, nanoparticle productivity, and gas composition during nanosecond laser ablation of gold.
Article
Physics, Applied
C. Donate-Buendia, M. Spellauge, R. Streubel, F. Riahi, S. Barcikowski, H. P. Huber, B. Goekce
Summary: Nanoparticles (NPs) are widely used in various fields, and developing NP production methods with material and solvent versatility, high purity, and size control is crucial. Pulsed laser ablation in liquids (PLAL) is a promising technique, but controlling NP size remains challenging. To address this, a double pulse configuration with specific inter-pulse delays is proposed, allowing for better control over NP size distribution. Experimental results demonstrate a significant reduction in the large NP fraction by 9 +/- 1 wt% at a pulse delay of 600 ps, suggesting the potential of modifying NP size distribution in PLAL through temporal pulse shaping.
JOURNAL OF PHYSICS D-APPLIED PHYSICS
(2023)
Article
Chemistry, Physical
Simon Siebeneicher, Sven Reichenberger, Christoph Hengst, Franz Dornhaus, Bernd Wittek, Stephan Barcikowski
Summary: Commercial diesel oxidation catalysis mainly uses Pt-Pd-based catalysts, but systematic alloying with different elements has rarely been studied. In this study, 45 binary alloys of platinum and selected transition metals were synthesized and their catalytic performance was evaluated for diesel oxidation and ammonia-slip environments. The results showed that the alloy with similar adsorption enthalpy of molecular oxygen to Pt exhibited the highest activity. The durability of the alloy catalysts also increased with the melting point of the second element alloyed with Pt. Synergies beyond binary systems were observed, suggesting the potential for further improvements using ternary or multinary alloys accessible via laser synthesis.
Article
Chemistry, Physical
Tina Friedenauer, Kim Buck, Maike Eberwein, Anna-Lena Buente, Christoph Rehbock, Stephan Barcikowski
Summary: In this study, the picosecond-pulsed laser fragmentation in liquids (LFL) technique was used to comminute drug particles in a liquid-jet passage reactor. The results show that the LFL technique significantly increases the fraction of submicrometer particles (SMP) of the drugs, leading to enhanced solubility and minimal chemical degradation.
PARTICLE & PARTICLE SYSTEMS CHARACTERIZATION
(2023)
Article
Materials Science, Multidisciplinary
Pichaporn Sutthavas, Matthias Schumacher, Martyna Nikody, Vaijayanthi Ramesh, Jurij Jakobi, Elizabeth R. R. Balmayor, Pamela Habibovic, Christoph Rehbock, Stephan Barcikowski, Sabine van Rijt
Summary: Bioactive glass nanoparticles (nBGs) have been successfully doped with iron, strontium, and/or copper ions using pulsed laser techniques. The laser-doped nBGs maintained their morphology and showed biocompatibility. Furthermore, the presence of specific ions in the nBGs enhanced bone repair and vessel formation.
MATERIALS ADVANCES
(2023)