TY - JOUR AU - Tapio, Kosti AU - Kielar, Charlotte AU - Parikka, Johannes M. AU - Keller, Adrian AU - Järvinen, Heini AU - Fahmy, Karim AU - Toppari, J. Jussi ID - 42517 JF - Chemistry of Materials KW - Materials Chemistry KW - General Chemical Engineering KW - General Chemistry SN - 0897-4756 TI - Large-Scale Formation of DNA Origami Lattices on Silicon VL - 35 ER - TY - JOUR AB - Understanding high-temperature unconventional superconductivity has become a long-lasting problem in which the cuprates stand as central reference materials. Given this impasse, the recent discovery of superconductivity in analogous nickelate thin films represents a fundamental breakthrough calling for the identification of additional materials in this class. In particular, thermodynamically more robust systems are required to “upgrade” nickelate superconductors from thin films to bulk samples. Here, we contribute in this direction by reporting the synthesis of the new single-layer T′ Pr2NiO3F compound, assessing this synthesis in relation to the only previous T′ nickelate La2NiO3F, and analyzing the electronic properties across the R2NiO3F series (R = La–Lu) via first-principles calculations. We find that these mixed anion systems have a comparatively high degree of stability and their synthesis enables a fine-tuning of their composition as inferred from their characterization. Furthermore, we find that these unprecedented square-planar nickelates hold great promise as prospective superconductors due to their exceptional electronic structure. AU - Wissel, Kerstin AU - Bernardini, Fabio AU - Oh, Heesu AU - Vasala, Sami AU - Schoch, Roland AU - Blaschkowski, Björn AU - Glatzel, Pieter AU - Bauer, Matthias AU - Clemens, Oliver AU - Cano, Andrés ID - 40993 IS - 16 JF - Chemistry of Materials KW - Materials Chemistry KW - General Chemical Engineering KW - General Chemistry SN - 0897-4756 TI - Single-Layer T′ Nickelates: Synthesis of the La and Pr Members and Electronic Properties across the Rare-Earth Series VL - 34 ER - TY - JOUR AU - Geise, Natalie R. AU - Kasse, Robert M. AU - Nelson Weker, Johanna AU - Steinrück, Hans-Georg AU - Toney, Michael F. ID - 25183 JF - Chemistry of Materials SN - 0897-4756 TI - Quantification of Efficiency in Lithium Metal Negative Electrodes via Operando X-ray Diffraction VL - 33 ER - TY - JOUR AU - Cao, Chuntian AU - Pollard, Travis P. AU - Borodin, Oleg AU - Mars, Julian E. AU - Tsao, Yuchi AU - Lukatskaya, Maria R. AU - Kasse, Robert M. AU - Schroeder, Marshall A. AU - Xu, Kang AU - Toney, Michael F. AU - Steinrück, Hans-Georg ID - 25184 JF - Chemistry of Materials SN - 0897-4756 TI - Toward Unraveling the Origin of Lithium Fluoride in the Solid Electrolyte Interphase VL - 33 ER - TY - JOUR AB - Within this article, it is shown that an electrochemical defluorination and additional fluorination of Ruddlesden–Popper-type La2NiO3F2 is possible within all-solid-state fluoride-ion batteries. Structural changes within the reduced and oxidized phases have been examined by X-ray diffraction studies at different states of charging and discharging. The synthesis of the oxidized phase La2NiO3F2+x proved to be successful by structural analysis using both X-ray powder diffraction and automated electron diffraction tomography techniques. The structural reversibility on re-fluorinating and re-defluorinating is also demonstrated. Moreover, the influence of different sequences of consecutive reduction and oxidation steps on the formed phases has been investigated. The observed structural changes have been compared to changes in phases obtained via other topochemical modification approaches such as hydride-based reduction and oxidative fluorination using F2 gas, highlighting the potential of such electrochemical reactions as alternative synthesis routes. Furthermore, the electrochemical routes represent safe and controllable synthesis approaches for novel phases, which cannot be synthesized via other topochemical methods. Additionally, side reactions, occurring alongside the desired electrochemical reactions, have been addressed and the cycling performance has been studied. AU - Wissel, Kerstin AU - Schoch, Roland AU - Vogel, Tobias AU - Donzelli, Manuel AU - Matveeva, Galina AU - Kolb, Ute AU - Bauer, Matthias AU - Slater, Peter R. AU - Clemens, Oliver ID - 41013 IS - 2 JF - Chemistry of Materials KW - Materials Chemistry KW - General Chemical Engineering KW - General Chemistry SN - 0897-4756 TI - Electrochemical Reduction and Oxidation of Ruddlesden–Popper-Type La2NiO3F2 within Fluoride-Ion Batteries VL - 33 ER - TY - JOUR AU - Huang, Tzu-Yen AU - Larrain, Felipe A. AU - Borca, Carlos H. AU - Fuentes-Hernandez, Canek AU - Yan, Hongping AU - Schneider, Sebastian Alexander AU - Chou, Wen-Fang AU - Rodriguez-Toro, Victor A. AU - Steinrück, Hans-Georg AU - Cao, Chuntian AU - Sherrill, C. David AU - Kippelen, Bernard AU - Toney, Michael F. ID - 23621 JF - Chemistry of Materials SN - 0897-4756 TI - Morphology of Organic Semiconductors Electrically Doped from Solution Using Phosphomolybdic Acid VL - 31 ER - TY - JOUR AU - Clemens, Oliver AU - Bauer, Matthias AU - Haberkorn, Robert AU - Springborg, Michael AU - Beck, Horst Philipp ID - 41239 IS - 24 JF - Chemistry of Materials KW - Materials Chemistry KW - General Chemical Engineering KW - General Chemistry SN - 0897-4756 TI - Synthesis and Characterization of Vanadium-Doped LiMnPO4-Compounds: LiMn(PO4)x(VO4)1–x (0.8 ≤ x ≤ 1.0) VL - 24 ER - TY - JOUR AU - Thiede, Tobias B. AU - Krasnopolski, Michael AU - Milanov, Andrian P. AU - de los Arcos de Pedro, Maria Teresa AU - Ney, Andreas AU - Becker, Hans-Werner AU - Rogalla, Detlef AU - Winter, Jörg AU - Devi, Anjana AU - Fischer, Roland A. ID - 22608 JF - Chemistry of Materials SN - 0897-4756 TI - Evaluation of Homoleptic Guanidinate and Amidinate Complexes of Gadolinium and Dysprosium for MOCVD of Rare-Earth Nitride Thin Films ER - TY - JOUR AU - Cravillon, Janosch AU - Nayuk, Roman AU - Springer, Sergej AU - Feldhoff, Armin AU - Huber, Klaus AU - Wiebcke, Michael ID - 41990 IS - 8 JF - Chemistry of Materials KW - Materials Chemistry KW - General Chemical Engineering KW - General Chemistry SN - 0897-4756 TI - Controlling Zeolitic Imidazolate Framework Nano- and Microcrystal Formation: Insight into Crystal Growth by Time-Resolved In Situ Static Light Scattering VL - 23 ER - TY - JOUR AU - Cravillon, Janosch AU - Münzer, Simon AU - Lohmeier, Sven-Jare AU - Feldhoff, Armin AU - Huber, Klaus AU - Wiebcke, Michael ID - 41997 IS - 8 JF - Chemistry of Materials KW - Materials Chemistry KW - General Chemical Engineering KW - General Chemistry SN - 0897-4756 TI - Rapid Room-Temperature Synthesis and Characterization of Nanocrystals of a Prototypical Zeolitic Imidazolate Framework VL - 21 ER - TY - JOUR AB - In recent years, a lot of research activity has focused on the synthesis of new ordered porous materials by utilization of porous matrices as templates. Since the matrices are themselves created by templating procedures, the entire process can be envisaged as “repeated templating”. This review describes recent conceptual developments in the field of structure replication and summarizes the large number of publications on new functional materials prepared by this method. AU - Tiemann, Michael ID - 25978 JF - Chemistry of Materials SN - 0897-4756 TI - Repeated Templating ER - TY - JOUR AB - Periodically ordered mesoporous magnesium oxide was synthesized in a double replication procedure. Mesoporous SBA-15 silica and CMK-3 carbon were successively used as hard structure matrixes. The carbon pore system was infiltrated with Mg(NO3)2, which was then converted to MgO at 573 K; the carbon matrix was finally removed by thermal combustion. The structure of the mesoporous MgO corresponds to that of the original SBA-15 silica. The products consist of hexagonally arranged cylindrical mesopores and crystalline pore walls. The efficiency of the replication series was studied by variation of the infiltration method and comprehensive pore size analysis of all involved mesoporous materials. The in situ formation of MgO inside the CMK-3 carbon pore system was monitored by thermal analysis. Postsynthetic treatment of the products at 823 K in a vacuum prior to removal of the carbon matrix was found to improve the crystallinity but to diminish the periodic order of the pore system. AU - Roggenbuck, Jan AU - Koch, Günter AU - Tiemann, Michael ID - 25991 JF - Chemistry of Materials SN - 0897-4756 TI - Synthesis of Mesoporous Magnesium Oxide by CMK-3 Carbon Structure Replication ER - TY - JOUR AB - In situ Synchrotron SAXS/XRD Study on the Formation of Ordered Mesoscopic Hybrid Materials with Crystal-Like Walls... AU - Morell, Jürgen AU - Teixeira, Cilaine V. AU - Cornelius, Maximilian AU - Rebbin, Vivian AU - Tiemann, Michael AU - Amenitsch, Heinz AU - Fröba, Michael AU - Lindén, Mika ID - 25996 JF - Chemistry of Materials SN - 0897-4756 TI - In situ Synchrotron SAXS/XRD Study on the Formation of Ordered Mesoscopic Hybrid Materials with Crystal-Like Walls ER - TY - JOUR AB - Long-chain n-alkylamine surfactants have been used as structure-directing agents in the synthesis of mesoporous aluminophosphates by a highly cooperative formation mechanism in an alcoholic system. Small amounts of water in the synthesis mixture play a significant role in the hydrolysis of the aluminum precursor (Al[OiPr]3) and are important for the quality of the mesostructured products. The materials exhibit disordered mesostructures, the stability and structural order of which can be improved by a postsynthetic thermal treatment. The products are then stable enough for the removal of the surfactant molecules by acidic solvent extraction, yielding surface areas up to 690 m2/g. AU - Tiemann, Michael AU - Schulz, Marcus AU - Jäger, Christian AU - Fröba, Michael ID - 26003 JF - Chemistry of Materials SN - 0897-4756 TI - Mesoporous Aluminophosphate Molecular Sieves Synthesized under Nonaqueous Conditions ER - TY - JOUR AB - Over the past few years a growing number of scientists have dedicated their attention to the synthesis of mesostructured aluminophosphates following the concept of supramolecular structure direction. Their research has produced a large variety of synthetic approaches and yielded materials with various structural properties. Today a substantial number of publications have accumulated; this short review provides a general summary of the literature with the aim to display the opportunities for future work. AU - Tiemann, Michael AU - Fröba, Michael ID - 26002 JF - Chemistry of Materials SN - 0897-4756 TI - Mesostructured Aluminophosphates Synthesized with Supramolecular Structure Directors ER - TY - JOUR AB - Mesostructured aluminophosphate/dodecyl phosphate composite materials were synthesized under aqueous and alcoholic conditions. The syntheses were monitored by temperature- and time-resolved in-situ small-angle X-ray scattering (SAXS). In the aqueous synthesis, a lamellar mesostructure is formed within the first few minutes of the reaction; this structure maintains a constant d spacing independent of the reaction time and temperature. The alcoholic synthesis at low temperature yields a mixture of a lamellar and a supposedly inverted hexagonal mesostructure. SAXS investigations show that these two phases evolve competitively. The lamellar structure is favored by higher temperatures and/or longer synthesis times; above ∼70 °C it is formed exclusively. Mixtures of both phases can be isolated as solid materials, but thermal analysis shows that the inverted hexagonal product transforms into the lamellar phase at ∼35−43 °C. The alcoholic synthesis is a highly cooperative reaction; the pure surfactant/alcohol systems are not lyotropic as long as the inorganic reactants are absent. In comparison, the surfactant/water system with the same surfactant concentrations as employed for the aqueous syntheses is lyotropic with a lamellar structure. AU - Tiemann, Michael AU - Fröba, M. AU - Rapp, G. AU - Funari, S. S. ID - 26005 JF - Chemistry of Materials SN - 0897-4756 TI - Nonaqueous Synthesis of Mesostructured Aluminophosphate/Surfactant Composites:  Synthesis, Characterization, and In-Situ SAXS Studies ER - TY - JOUR AB - Lamellar mesostructured aluminophosphates were synthesized from aluminum triisopropoxide and phosphoric acid; monododecyl phosphate surfactant was used as structure-directing template. Depending on the relative Al/P ratio in the samples, variable relative amounts of tetrahedrally and octahedrally coordinated Al are found, indicating that both aluminophosphate and aluminum oxide species (as thermodynamically favored) are being formed in the syntheses. This is investigated quantitatively by Al K-edge XANES spectroscopy. The same syntheses were carried out without phosphoric acid, resulting in similar lamellar structures. The inorganic lamellae of these products consist to a significant extent of aluminophosphate rather than exclusively of aluminum oxide, which means that the phosphate headgroups of the surfactant molecules become incorporated into the inorganic network. Thus, for the first time, the surfactant serves as both template and reactant. AU - Fröba, Michael AU - Tiemann, Michael ID - 26009 JF - Chemistry of Materials SN - 0897-4756 TI - A New Role of the Surfactant in the Synthesis of Mesostructured Phases:  Dodecyl Phosphate as Template and Reactant for Aluminophosphates ER - TY - JOUR AU - Buey, Julio AU - Díez, Laura AU - Espinet, Pablo AU - Kitzerow, Heinz-Siegfried AU - Miguel, Jesús A. ID - 40301 IS - 9 JF - Chemistry of Materials KW - Materials Chemistry KW - General Chemical Engineering KW - General Chemistry SN - 0897-4756 TI - Platinum Orthometalated Liquid Crystals Compared with Their Palladium Analogues. First Optical Storage Effect in an Organometallic Liquid Crystal VL - 8 ER -