Article
Chemistry, Multidisciplinary
Yang Qiao, Jin Zhao, Haodong Sun, Zhitang Song, Yuan Xue, Jiao Li, Sannian Song
Summary: Thermal stability and operation speed are the bottlenecks in the development of phase change memory. This paper explores the use of platinum doping to improve PCM performance, resulting in higher data retention temperature and operation speed through reduced grain size and density change rate.
Article
Chemistry, Physical
Peng Chai, Zongfang Wu, Longxia Wu, Haocheng Wang, Cong Fu, Weixin Huang
Summary: In this study, the moisture effect on low-temperature CO oxidation on Pt(111) under near ambient pressure conditions was investigated using operando techniques. The results showed that moisture enhanced the CO oxidation rate on Pt(111) and the enhancement effect varied with reaction temperature. Characterization results provided evidence for the formation of reversibly adsorbed OH species and irreversibly adsorbed COOH species as the key surface intermediates resulting from water activation on Pt(111) at temperatures around 300 K. These findings contribute to the understanding of water-enhanced low-temperature CO oxidation on Pt(111) under near ambient pressure conditions.
Article
Chemistry, Physical
Peng Chai, Zongfang Wu, Longxia Wu, Haocheng Wang, Cong Fu, Weixin Huang
Summary: Fundamental studies of catalytic reaction mechanisms of working catalysts are important. In this study, an operando method was used to investigate the moisture effect on low-temperature CO oxidation on Pt(111). Experimental evidence shows that moisture can enhance the CO oxidation rate on Pt(111), and the enhancement effect varies with reaction temperature.
Article
Chemistry, Multidisciplinary
Lihao Guan, Frank Palmino, Jean-Christophe Lacroix, Frederic Cherioux, Xiaonan Sun
Summary: Polymers obtained through on-surface chemistry have shown promise as a new class of materials. In this study, we propose a novel strategy for the self-assembly of one-dimensional polymers using photochemical [2+2] cyclo-addition or mild thermal annealing. We characterized all nanostructures using scanning tunneling microscopy on a graphite surface under ambient conditions. Our results demonstrate that the nature of the stimulus significantly affects the quality of the resulting polymers in terms of length and defects. This new approach provides an efficient method for on-surface self-assembly of one-dimensional polymers.
Article
Green & Sustainable Science & Technology
Wenping Li, Mingyuan Cao, Shijun Meng, Zhaofei Li, Hao Xu, Lijia Liu, Hua Song
Summary: The catalyst role in performance improvement in hydrogen production by water splitting using catalytic non-thermal plasma (NTP) reactors was explored. An optimized catalyst, 0.2 wt.% Au/(10 wt.% TiO2/SBA-15), achieved a high hydrogen production rate of 1.03 mL min-1 and a water conversion of 36.9%, which is 245% higher than the NTP reactor without catalyst packing. Surface properties of the catalysts, such as specific surface area, pore volume, and water adsorption amount, were investigated and correlated with the catalyst performance. A hypothetical reaction mechanism and a catalyst design principle were proposed based on these findings.
JOURNAL OF CLEANER PRODUCTION
(2023)
Article
Chemistry, Physical
Shijun Meng, Wenping Li, Hao Xu, Zhaofei Li, Yimeng Li, Jack Jarvis, Hua Song
Summary: A novel method of non-thermal plasma assisted catalytic reforming of naphtha at near ambient conditions is introduced, replacing expensive hydrogen with cheaper methane. The non-thermal plasma effectively converts methane and naphtha to high-quality fuel. The produced liquid product has higher iso-paraffin content and well-controlled levels of coke deposition, olefins, and aromatics, offering a cost-effective and environmental-friendly route for naphtha reforming.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Multidisciplinary Sciences
Tao Wang, Frank Abild-Pedersen
Summary: By modifying energy-scaling relationships and utilizing a confined dual site, low-temperature and -pressure ammonia synthesis can be achieved, with an ammonia synthesis rate two to three orders of magnitude higher than the commercial Ru catalyst under the same reaction conditions.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Chemistry, Physical
Meena Said, Amy E. Hixon
Summary: Characterization of plutonium dioxide (PuO2) and thorium dioxide (ThO2) aging under different temperature and relative humidity conditions revealed significant stability differences between actinide oxides, providing important insights for nuclear forensic applications and fundamental safety and storage concerns. The study used a variety of techniques, including scanning electron microscopy and X-ray diffraction, to analyze the morphological and phase changes in the materials, highlighting the need for further research on the chemical and physical properties of actinide compounds near ambient temperatures and humidities.
JOURNAL OF ALLOYS AND COMPOUNDS
(2021)
Article
Multidisciplinary Sciences
Anna L. Eichhorn, Christian Dietz
Summary: Combined in-plane and out-of-plane multifrequency atomic force microscopy techniques have been used to analyze the spatial differences of sample surfaces at the atomic scale. The lateral eigenmode provides information on the shear modulus, while the torsional eigenmode reveals local friction forces between the tip and the sample. The full set of elastic constants of graphite can be determined from combined in-plane and out-of-plane multifrequency atomic force microscopy.
SCIENTIFIC REPORTS
(2022)
Article
Chemistry, Physical
Philip Petzoldt, Moritz Eder, Sonia Mackewicz, Monika Blum, Tim Kratky, Sebastian Guenther, Martin Tschurl, Ueli Heiz, Barbara A. J. Lechner
Summary: The study shows that O-2 and H-2 have a significant impact on the SMSI state of Pt/TiO2 catalysts, with encapsulating oxide layer forming more rapidly at low O-2 pressures, but less effectively at higher pressures. The oxidation/reduction of Pt particles is reversible, but once encapsulated, they remain embedded in the support.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Michal Marszewski, Sophia C. King, Tiphaine Galy, Glareh N. Kashanchi, Ali Dashti, Yan Yan, Man Li, Danielle M. Butts, Patricia E. McNeil, Esther Lan, Bruce Dunn, Yongjie Hu, Sarah H. Tolbert, Laurent Pilon
Summary: This paper introduces a novel sol-gel method for synthesizing large and thick silica aerogel monoliths at near ambient conditions using commercial colloidal silica nanoparticles as building blocks. By combining specific strategies, such as synthesis on omniphobic liquid substrates, aging at elevated temperatures, and solvent exchange prior to drying, the method produces aerogels with high transmittance and low thermal conductivity.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2022)
Review
Chemistry, Multidisciplinary
Erik Vesselli
Summary: Advancements in surface science methods have partially bridged the pressure gap between ultra-high vacuum and practical conditions, allowing for better characterization of catalytic systems and tetrapyrroles. The investigation of small ligands at single-metal atom reaction sites has gained attention, particularly in biomimetic 2D metalorganic frameworks. The study of tetrapyrroles at surfaces has opened potential applications in light harvesting, catalysts, chemical sensing, and spintronics.
NANOSCALE ADVANCES
(2021)
Article
Chemistry, Multidisciplinary
Wei Yan, Guang Li, Shuangshuang Cui, Gyeong-Su Park, Rena Oh, Weixin Chen, Xiaoyang Cheng, Jun-Ming Zhang, Weize Li, Li-Fei Ji, Ouardia Akdim, Xiaoyang Huang, Haixin Lin, Jian Yang, Yan-Xia Jiang, Shi-Gang Sun
Summary: This study reports a Pt3Ga/C electrocatalyst that efficiently produces CO2 through direct and sustainable oxidation of C2 intermediate species (acetaldehyde). The atomic interval structure between Pt and Ga prevents the formation of poisonous species and increases the available sites for interaction with C2 intermediates. The high hydrophilicity of Ga facilitates the dissociation of H2O, promoting the deep oxidation of C2 intermediates. This research represents a rare EOR process that produces CO2 without observing kinetic limitations under medium potential conditions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Tianyuan Xiao, Yasutaka Nagaoka, Xirui Wang, Tian Jiang, Derek LaMontagne, Qiang Zhang, Can Cao, Xizheng Diao, Jiahua Qiu, Yiruo Lu, Zhongwu Wang, Y. Charles Cao
Summary: This study investigates the ambient metastability of the rock-salt phase in well-defined nanocrystal systems and proposes general rules for transformation-barrier engineering, which are important for the rational design of next-generation materials.
Article
Green & Sustainable Science & Technology
Miqdam T. Chaichan, Maytham T. Mahdi, Hussein A. Kazem, Ali H. A. Al-Waeli, Mohammed A. Fayad, Ahmed A. Al-Amiery, Wan Nor Roslam Wan Isahak, Abdul Amir H. Kadhum, Mohd S. Takriff
Summary: The development of modern photovoltaic thermal systems is crucial for utilizing solar energy efficiently. Adding nanoparticles to phase change materials can significantly improve the low thermal conductivity of these materials. Experimental results demonstrate that adding nano-iron oxide to paraffin wax enhances its thermal conductivity, viscosity, and density, while maintaining thermal stability.
Article
Chemistry, Physical
Daniel Hemmeter, Ulrike Paap, Nicola Taccardi, Julian Mehler, Peter S. Schulz, Peter Wasserscheid, Florian Maier, Hans-Peter Steinruck
Summary: This study investigated the formation and surface behavior of Pt(II) and Pd(II) complexes with ligand systems derived from nitrile-functionalized ionic liquids (ILs) using ARXPS. The results showed that these ligand systems enabled a high solubility of the metal complexes in IL solutions, and the formed complexes showed a homogeneous distribution at the surface.
Article
Chemistry, Multidisciplinary
Andre Hofer, Nicola Taccardi, Michael Moritz, Christoph Wichmann, Sabine Huebner, Dominik Drobek, Matthias Engelhardt, Georg Papastavrou, Erdmann Spiecker, Christian Papp, Peter Wasserscheid, Julien Bachmann
Summary: This study establishes a preparative route towards a model system for supported catalytically active liquid metal solutions (SCALMS) on nanostructured substrates. The model is characterized by a precise control of the gallium particle size distribution. The system involves spin-coating a gallium-containing precursor on nanostructured aluminum substrates and functionalizing the substrates with distinct oxide coatings. The model system can be functionalized with a dissolved noble metal catalyst for specific applications.
Article
Chemistry, Physical
Valentin Schwaab, Felix Hemauer, Eva Marie Freiberger, Natalie J. Waleska-Wellnhofer, Hans-Peter Steinrueck, Christian Papp
Summary: The molecular pair of 1-cyclohexylethanol and acetophenone is an interesting system for chemical hydrogen storage, as it combines different classes of liquid organic hydrogen carriers. The dehydrogenation reaction of 1-cyclohexylethanol to acetophenone was investigated on a Pt(111) catalyst. The reaction occurs in two steps, yielding 1-cyclohexylethanone and an acetophenone-like species. The system shows good thermal robustness.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Evanie Franz, Jannis Jung, Anne Kunz, Hermann A. Wegner, Olaf Brummel, Doreen Mollenhauer, Joerg Libuda
Summary: Molecular solar-thermal (MOST) systems combine solar energy conversion, storage, and release within one molecule. In this study, the catalytic activity and selectivity of three different surfaces (graphite(0001), Pt(111), and Au(111)) for energy release from the MOST system were investigated. Graphite(0001) showed the weakest reactant-surface interaction and was suitable for electrochemical triggering. Pt(111) had strong reactant-surface interactions, moderate catalytic activity, and partial decomposition, limiting its applicability. Au(111) exhibited high catalytic activity and selectivity (>99%), attributed to moderate reactant surface interaction facilitating energy release.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Editorial Material
Chemistry, Physical
Joerg Libuda, Andreas Goerling
Article
Chemistry, Physical
Daniel Hemmeter, Ulrike Paap, Nicolas Wellnhofer, Afra Gezmis, Daniel Kremitzl, Peter Wasserscheid, Hans-Peter Steinrueck, Florian Maier
Summary: We have demonstrated that Pt catalyst complexes can be enriched at the surface of an ionic liquid by introducing perfluorinated substituents, which act as buoys to drag the metal complex towards the surface. Our study shows that the enrichment is most pronounced at a concentration of 1 %mol and is temperature-dependent. The enrichment of Pt complexes at the surface is reflected by the decrease in surface tension with increasing catalyst concentration. The results are important for the design of catalyst systems with large contact areas, such as supported ionic liquid phase (SILP) catalysis.
Editorial Material
Chemistry, Physical
Rajan Adhikari, Jan Brox, Stephen Massicot, Michael Ruppel, Norbert Jux, Hubertus Marbach, Hans-Peter Steinrueck
Summary: This research investigates the self-assembly behavior of 2H-diTTBP(x)BPs molecules on Ag(111), Cu(111), and Cu(110) surfaces to understand the fundamental aspects of this process. The study reveals a novel and peculiar long-range-ordered quadratic arrangement of crown-shaped molecules on Ag(111) and Cu(111) surfaces.
Article
Chemistry, Physical
Eva Marie Freiberger, Julien Steffen, Natalie J. Waleska-Wellnhofer, Anton Harrer, Felix Hemauer, Valentin Schwaab, Andreas Gorling, Hans-Peter Steinruck, Christian Papp
Summary: This study investigates the adsorption and thermal stability of bromine on Rh(111) using synchrotron radiation-based XPS, LEED and DFT. Depending on the coverage, four different superstructures are observed. At low coverages, bromine occupies fcc hollow sites while, at higher coverages, a compression of the overlayer leads to bridge-bound bromine atoms. Br/Rh(111) shows a high thermal stability, implying strong covalent bonding.
Article
Chemistry, Physical
Natalie J. Waleska-Wellnhofer, Eva Marie Freiberger, Felix Hemauer, Valentin Schwaab, Christian Papp
Summary: In this work, nano-strong metal-support interaction is observed for bimetallic FePt nanoclusters on graphene/Rh(111) substrate. The encapsulation of Pt with an Fe oxide layer and the formation of an FePt alloy were found at elevated temperature.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Tzung-En Hsieh, Sven Maisel, Haiko Wittkaemper, Johannes Frisch, Julien Steffen, Regan G. Wilks, Christian Papp, Andreas Goerling, Marcus Baer
Summary: This study reports the electronic and chemical structure of supported GaRh alloys as model systems for the active phase in supported catalytically active liquid metal solutions. Through photoemission spectroscopy, ab initio calculations, and electron microscopy, the characteristic shifts and narrowing of Rh core levels and derived bands are observed, which can be explained by the coexistence of isolated Rh atoms in random GaRh alloys and GaRh intermetallic compounds.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Olaf Brummel, Leon Jacobse, Alexander Simanenko, Xin Deng, Simon Geile, Olof Gutowski, Vedran Vonk, Yaroslava Lykhach, Andreas Stierle, Jorg Libuda
Summary: New diagnostic approaches are needed in the field of electrocatalysis. A versatile experimental setup combining two complementary in-situ techniques has been developed for simultaneous chemical and structural analysis of planar electrodes. The setup has been tested with a model study and shows a high potential for application in energy conversion and storage.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Chemistry, Physical
Alexander Simanenko, Maximilian Kastenmeier, Lesia Piliai, Yuliia Kosto, Tomas Skala, Nataliya Tsud, Sascha Mehl, Mykhailo Vorokhta, Iva Matolinova, Yaroslava Lykhach, Joerg Libuda
Summary: The redox capacity of Pt-CeO2 catalysts for low-temperature CO oxidation was investigated using various spectroscopy methods. Different Pt species were prepared and their oxidation states were monitored upon CO exposure. Metallic Pt-0 nanoparticles, ultra-small Pt*/PtOx clusters, and Pt4+ species were found to serve as CO adsorption sites at low temperature. The redox pathway for low-temperature CO oxidation involved CO spillover and the formation of bidentate carbonate species, while above 400 K, the Mars-van Krevelen mechanism was observed.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Nanoscience & Nanotechnology
Elif Bilgilisoy, Ali Kamali, Thomas Xaver Gentner, Gerd Ballmann, Sjoerd Harder, Hans-Peter Steinrueck, Hubertus Marbach, Oddur Ingolfsson
Summary: Motivated by the potential application of focused-electron-beam-induced deposition (FEBID) in plasmonic and detector technology, this study comprehensively investigated [Au(CH3)2Cl]2 as a potential precursor. The dissociation processes and composition of FEBID deposits were studied under single collision conditions and in an ultrahigh-vacuum (UHV) chamber. The results showed significant carbon loss and chlorine removal in the gas phase, while quantitative chlorine loss and desorption were observed in the UHV setup. The precursor was found stable at ambient conditions and suitable for use in HV instruments, producing deposits with high gold content.
BEILSTEIN JOURNAL OF NANOTECHNOLOGY
(2023)
Article
Chemistry, Physical
Lukas Fusek, Pankaj Kumar Samal, Jiri Kerestes, Ivan Khalakhan, Viktor Johanek, Yaroslava Lykhach, Joerg Libuda, Olaf Brummel, Josef Myslivecek
Summary: This study investigates the electrochemical properties of CeO2 nanoislands on Pt in alkaline electrolyte. The size and preparation of the nanoislands are found to affect the redox behavior of CeO2 and its moderation of the hydrogen evolution reaction on Pt.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)