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- ItemA Two-Dimensional Polyimide-Graphene Heterostructure with Ultra-fast Interlayer Charge Transfer(Weinheim : Wiley-VCH, 2021) Liu, Kejun; Li, Jiang; Qi, Haoyuan; Hambsch, Mike; Rawle, Jonathan; Vázquez, Adrián Romaní; Nia, Ali Shaygan; Pashkin, Alexej; Schneider, Harald; Polozij, Mirosllav; Heine, Thomas; Helm, Manfred; Mannsfeld, Stefan C.B.; Kaiser, Ute; Dong, Renhao; Feng, XinliangTwo-dimensional polymers (2DPs) are a class of atomically/molecularly thin crystalline organic 2D materials. They are intriguing candidates for the development of unprecedented organic–inorganic 2D van der Waals heterostructures (vdWHs) with exotic physicochemical properties. In this work, we demonstrate the on-water surface synthesis of large-area (cm2), monolayer 2D polyimide (2DPI) with 3.1-nm lattice. Such 2DPI comprises metal-free porphyrin and perylene units linked by imide bonds. We further achieve a scalable synthesis of 2DPI-graphene (2DPI-G) vdWHs via a face-to-face co-assembly of graphene and 2DPI on the water surface. Remarkably, femtosecond transient absorption spectroscopy reveals an ultra-fast interlayer charge transfer (ca. 60 fs) in the resultant 2DPI-G vdWH upon protonation by acid, which is equivalent to that of the fastest reports among inorganic 2D vdWHs. Such large interlayer electronic coupling is ascribed to the interlayer cation–π interaction between 2DP and graphene. © 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH
- ItemHighly Crystalline and Semiconducting Imine-Based Two-Dimensional Polymers Enabled by Interfacial Synthesis(Weinheim : Wiley-VCH, 2020) Sahabudeen, Hafeesudeen; Qi, Haoyuan; Ballabio, Marco; Položij, Miroslav; Olthof, Selina; Shivhare, Rishi; Jing, Yu; Park, SangWook; Liu, Kejun; Zhang, Tao; Ma, Ji; Rellinghaus, Bernd; Mannsfeld, Stefan; Heine, Thomas; Bonn, Mischa; Cánovas, Enrique; Zheng, Zhikun; Kaiser, Ute; Dong, Renhao; Feng, XinliangSingle-layer and multi-layer 2D polyimine films have been achieved through interfacial synthesis methods. However, it remains a great challenge to achieve the maximum degree of crystallinity in the 2D polyimines, which largely limits the long-range transport properties. Here we employ a surfactant-monolayer-assisted interfacial synthesis (SMAIS) method for the successful preparation of porphyrin and triazine containing polyimine-based 2D polymer (PI-2DP) films with square and hexagonal lattices, respectively. The synthetic PI-2DP films are featured with polycrystalline multilayers with tunable thickness from 6 to 200 nm and large crystalline domains (100–150 nm in size). Intrigued by high crystallinity and the presence of electroactive porphyrin moieties, the optoelectronic properties of PI-2DP are investigated by time-resolved terahertz spectroscopy. Typically, the porphyrin-based PI-2DP 1 film exhibits a p-type semiconductor behavior with a band gap of 1.38 eV and hole mobility as high as 0.01 cm2 V−1 s−1, superior to the previously reported polyimine based materials. © 2020 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
- ItemUltrathin two-dimensional conjugated metal– organic framework single-crystalline nanosheets enabled by surfactant-assisted synthesis(Cambridge : RSC, 2020) Wang, Zhonghao; Wang, Gang; Qi, Haoyuan; Wang, Mao; Wang, Mingchao; Park, SangWook; Wang, Huaping; Yu, Minghao; Kaiser, Ute; Fery, Andreas; Zhou, Shengqiang; Dong, Renhao; Feng, XinliangTwo-dimensional conjugated metal-organic frameworks (2D c-MOFs) have recently emerged for potential applications in (opto-)electronics, chemiresistive sensing, and energy storage and conversion, due to their excellent electrical conductivity, abundant active sites, and intrinsic porous structures. However, developing ultrathin 2D c-MOF nanosheets (NSs) for facile solution processing and integration into devices remains a great challenge, mostly due to unscalable synthesis, low yield, limited lateral size and low crystallinity. Here, we report a surfactant-assisted solution synthesis toward ultrathin 2D c-MOF NSs, including HHB-Cu (HHB = hexahydroxybenzene), HHB-Ni and HHTP-Cu (HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene). For the first time, we achieve single-crystalline HHB-Cu(Ni) NSs featured with a thickness of 4-5 nm (∼8-10 layers) and a lateral size of 0.25-0.65 μm2, as well as single-crystalline HHTP-Cu NSs with a thickness of ∼5.1 ± 2.6 nm (∼10 layers) and a lateral size of 0.002-0.02 μm2. Benefiting from the ultrathin feature, the synthetic NSs allow fast ion diffusion and high utilization of active sites. As a proof of concept, when serving as a cathode material for Li-ion storage, HHB-Cu NSs deliver a remarkable rate capability (charge within 3 min) and long-term cycling stability (90% capacity retention after 1000 cycles), superior to the corresponding bulk materials and other reported MOF cathodes. This journal is © The Royal Society of Chemistry.
- ItemControlled growth of transition metal dichalcogenide monolayers using Knudsen-type effusion cells for the precursors(Bristol : IOP Publishing, 2019) George, Antony; Neumann, Christof; Kaiser, David; Mupparapu, Rajeshkumar; Lehnert, Tibor; Hübner, Uwe; Tang, Zian; Winter, Andreas; Kaiser, Ute; Staude, Isabelle; Turchanin, AndreyControlling the flow rate of precursors is essential for the growth of high quality monolayer single crystals of transition metal dichalcogenides (TMDs) by chemical vapor deposition. Thus, introduction of an excess amount of the precursors affects reproducibility of the growth process and results in the formation of TMD multilayers and other unwanted deposits. Here we present a simple method for controlling the precursor flow rates using the Knudsen-type effusion cells. This method results in a highly reproducible growth of large area and high density TMD monolayers. The size of the grown crystals can be adjusted between 10 and 200 μm. We characterized the grown MoS2 and WS2 monolayers by optical, atomic force and transmission electron microscopies as well as by x-ray photoelectron, Raman and photoluminescence spectroscopies, and by electrical transport measurements showing their high optical and electronic quality based on the single crystalline nature.
- ItemWafer-sized multifunctional polyimine-based two-dimensional conjugated polymers with high mechanical stiffness([London] : Nature Publishing Group UK, 2016) Sahabudeen, Hafeesudeen; Qi, Haoyuan; Glatz, Bernhard Alexander; Tranca, Diana; Dong, Renhao; Hou, Yang; Zhang, Tao; Kuttner, Christian; Lehnert, Tibor; Seifert, Gotthard; Kaiser, Ute; Fery, Andreas; Zheng, Zhikun; Feng, XinliangOne of the key challenges in two-dimensional (2D) materials is to go beyond graphene, a prototype 2D polymer (2DP), and to synthesize its organic analogues with structural control at the atomic- or molecular-level. Here we show the successful preparation of porphyrin-containing monolayer and multilayer 2DPs through Schiff-base polycondensation reaction at an air-water and liquid-liquid interface, respectively. Both the monolayer and multilayer 2DPs have crystalline structures as indicated by selected area electron diffraction. The monolayer 2DP has a thickness of∼0.7 nm with a lateral size of 4-inch wafer, and it has a Young's modulus of 267±30 GPa. Notably, the monolayer 2DP functions as an active semiconducting layer in a thin film transistor, while the multilayer 2DP from cobalt-porphyrin monomer efficiently catalyses hydrogen generation from water. This work presents an advance in the synthesis of novel 2D materials for electronics and energy-related applications.
- ItemTwo-Dimensional Boronate Ester Covalent Organic Framework Thin Films with Large Single Crystalline Domains for a Neuromorphic Memory Device(Weinheim : Wiley-VCH, 2020) Park, SangWook; Liao, Zhongquan; Ibarlucea, Bergoi; Qi, Haoyuan; Lin, Hung-Hsuan; Becker, Daniel; Melidonie, Jason; Zhang, Tao; Sahabudeen, Hafeesudeen; Baraban, Larysa; Baek, Chang-Ki; Zheng, Zhikun; Zschech, Ehrenfried; Fery, Andreas; Heine, Thomas; Kaiser, Ute; Cuniberti, Gianaurelio; Dong, Renhao; Feng, XinliangDespite the recent progress in the synthesis of crystalline boronate ester covalent organic frameworks (BECOFs) in powder and thin-film through solvothermal method and on-solid-surface synthesis, respectively, their applications in electronics, remain less explored due to the challenges in thin-film processability and device integration associated with the control of film thickness, layer orientation, stability and crystallinity. Moreover, although the crystalline domain sizes of the powder samples can reach micrometer scale (up to ≈1.5 μm), the reported thin-film samples have so far rather small crystalline domains up to 100 nm. Here we demonstrate a general and efficient synthesis of crystalline two-dimensional (2D) BECOF films composed of porphyrin macrocycles and phenyl or naphthyl linkers (named as 2D BECOF-PP or 2D BECOF-PN) by employing a surfactant-monolayer-assisted interfacial synthesis (SMAIS) on the water surface. The achieved 2D BECOF-PP is featured as free-standing thin film with large single-crystalline domains up to ≈60 μm2 and tunable thickness from 6 to 16 nm. A hybrid memory device composed of 2D BECOF-PP film on silicon nanowire-based field-effect transistor is demonstrated as a bio-inspired system to mimic neuronal synapses, displaying a learning–erasing–forgetting memory process. © 2020 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
- ItemWater-Soluble Polymeric Carbon Nitride Colloidal Nanoparticles for Highly Selective Quasi-Homogeneous Photocatalysis(Weinheim : Wiley-VCH, 2019) Krivtsov, Igor; Mitoraj, Dariusz; Adler, Christiane; Ilkaeva, Marina; Sardo, Mariana; Mafra, Luis; Neumann, Christof; Turchanin, Andrey; Li, Chunyu; Dietzek, Benjamin; Leiter, Robert; Biskupek, Johannes; Kaiser, Ute; Im, Changbin; Kirchhoff, Björn; Jacob, Timo; Beranek, RadimHeptazine-based polymeric carbon nitrides (PCN) are promising photocatalysts for light-driven redox transformations. However, their activity is hampered by low surface area resulting in low concentration of accessible active sites. Herein, we report a bottom-up preparation of PCN nanoparticles with a narrow size distribution (ca. 10±3 nm), which are fully soluble in water showing no gelation or precipitation over several months. They allow photocatalysis to be carried out under quasi-homogeneous conditions. The superior performance of water-soluble PCN, compared to conventional solid PCN, is shown in photocatalytic H2O2 production via reduction of oxygen accompanied by highly selective photooxidation of 4-methoxybenzyl alcohol and benzyl alcohol or lignocellulose-derived feedstock (ethanol, glycerol, glucose). The dissolved photocatalyst can be easily recovered and re-dissolved by simple modulation of the ionic strength of the medium, without any loss of activity and selectivity. © 2019 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
- Item1D p–n Junction Electronic and Optoelectronic Devices from Transition Metal Dichalcogenide Lateral Heterostructures Grown by One-Pot Chemical Vapor Deposition Synthesis(Weinheim : Wiley-VCH, 2021) Najafidehaghani, Emad; Gan, Ziyang; George, Antony; Lehnert, Tibor; Ngo, Gia Quyet; Neumann, Christof; Bucher, Tobias; Staude, Isabelle; Kaiser, David; Vogl, Tobias; Hübner, Uwe; Kaiser, Ute; Eilenberger, Falk; Turchanin, AndreyLateral heterostructures of dissimilar monolayer transition metal dichalcogenides provide great opportunities to build 1D in-plane p–n junctions for sub-nanometer thin low-power electronic, optoelectronic, optical, and sensing devices. Electronic and optoelectronic applications of such p–n junction devices fabricated using a scalable one-pot chemical vapor deposition process yielding MoSe2-WSe2 lateral heterostructures are reported here. The growth of the monolayer lateral heterostructures is achieved by in situ controlling the partial pressures of the oxide precursors by a two-step heating protocol. The grown lateral heterostructures are characterized structurally and optically using optical microscopy, Raman spectroscopy/microscopy, and photoluminescence spectroscopy/microscopy. High-resolution transmission electron microscopy further confirms the high-quality 1D boundary between MoSe2 and WSe2 in the lateral heterostructure. p–n junction devices are fabricated from these lateral heterostructures and their applicability as rectifiers, solar cells, self-powered photovoltaic photodetectors, ambipolar transistors, and electroluminescent light emitters are demonstrated. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH