Highlight Publications 2018

Red-Light-Controlled Release of Drug–Ru Complex Conjugates from Metallopolymer Micelles for Phototherapy in Hypoxic Tumor Environments
Wen Sun, Yan Wen, Raweewan Thiramanas, Mingjia Chen, Jianxiong Han, Ningqiang Gong, Manfred Wagner, Shuai Jiang, Michael S. Meijer, Sylvestre Bonnet, Hans-Jürgen Butt, Volker Mailänder, Xing-Jie Liang, and Si Wu
Red-Light-Controlled Release of Drug–Ru Complex Conjugates from Metallopolymer Micelles for Phototherapy in Hypoxic Tumor Environments
Amphiphilic metallopolymers, which contain photocleavable drug-Ru complex conjugates, self-assemble into micelles. The micelles are biocompatible and carry the conjugates into tumor cells. Subsequent red light irradiation induces intracellular release of the drug-Ru complex conjugates. Because the photoinduced release is oxygen-independent, the novel metallopolymer provides a new platform for phototherapy against hypoxic tumors in vivo.
© Wiley (2018)
Layered Thiadiazoloquinoxaline Containing Long Pyrene‐fused N‐Heteroacenes
Ben-Lin Hu, Ke Zhang, Cunbin An, Dieter Schollmeyer, Wojciech Pisula, and Martin Baumgarten
Layered Thiadiazoloquinoxaline Containing Long Pyrene‐fused N‐Heteroacenes
Three thiadiazoloquinoxaline containing long pyrene-fused N-heteroacenes with 8, 13 and 18 rings were designed and synthesized, which show high electron affinities (EAs) of ~4.1 eV derived from the onset of reductive peaks in cyclic voltammetry. Crystal structure analysis demonstrated in-plane extension through close contacts of thiadiazoles and layered packing enabling in-plane and interlayer electron transport. Organic field-effect transistor devices provided electron mobilities, which supplies a potential way to enhance the charge transport in long N-heteroacenes.
© Wiley VCH (2018)
Efficient Hot Electron Transfer in Quantum Dot-Sensitized Mesoporous Oxides at Room Temperature
Hai I. Wang, Ivan Infante, Stephanie ten Brinck, Enrique Cánovas, and Mischa Bonn
Efficient Hot Electron Transfer in Quantum Dot-Sensitized Mesoporous Oxides at Room Temperature
The efficiency of a single bandgap solar cell, such as silicon, is limited to ~31%. This limit is primarily the result of very rapid relaxation of electrons, once they are generated by a photon. For photons that have energies exceeding the bandgap energy, this excess energy is lost in this relaxation process. In order to circumvent such losses, and increase solar cell efficiency, the extraction of hot carriers towards selective contacts is required to be faster than thermalization in the absorber. Quantum dot (QD)-sensitized oxides have long been proposed as an appealing system to harvest hot carriers for solar energy conversion. Previous work has demonstrated the possibility of hot electron extraction in quantum dot (QD)-sensitized systems, but only at low temperatures (e.g. 77 Kelvin). Here, we demonstrate a room-temperature hot electron transfer with unity quantum efficiency in strongly coupled PbS quantum dot-sensitized mesoporous oxide. Such achievement is realized by enhancing the electronic coupling between QDs and oxides, which ensures an ultrafast hot electron transfer process (sub-100 fs) that can effectively compete with the hot carrier thermalization processes. These results provide new insights into circumventing thermal losses in sensitized systems, with potential relevance for low-cost solar energy conversion schemes.
© ACS (2018)
Room-temperature hot electron transfer with unity quantum efficiency in strongly coupled PbS quantum dot-sensitized mesoporous oxide
Detaching microparticles from a liquid surface
Frank Schellenberger, Periklis Papadopoulos, Michael Kappl, Stefan A.L. Weber, Doris Vollmer, Hans-Jürgen Butt
Detaching microparticles from a liquid surface
The work required to detach microparticles from fluid interfaces depends on the shape of the liquid meniscus. However, measuring the capillary force on a single microparticle and simultaneously imaging the shape of the liquid meniscus has not yet been accomplished. To correlate force and shape, we combined a laser scanning confocal microscope with a colloidal probe setup. While moving a hydrophobic microsphere (radius 5-10 µm) in and out of a 2-5 µm thick glycerol film, we simultaneously measured the force and imaged the shape of the liquid meniscus. In this way we verified the fundamental equations (D.F. James, J. Fluid Mech. 63, 657 (1974); A.D. Scheludko, A.D. Nikolov, Colloid Polymer Sci. 253, 396 (1975)) which describe the adhesion of particles in flotation, deinking of paper, the stability of Pickering emulsions and particle-stabilized-foams. Comparing experimental results with theory showed, however, that the receding contact angle has to be applied, which can be much lower than the static contact angle obtained right after jump-in of the particle.
© MPI-P (2018)
Macroscopic and microscopic particle withdrawn from a liquid. The microsphere was imaged with a confocal microscope while simultaneously the force was measured.
Asymmetric Covalent Triazine Framework for Enhanced Visible Light Photoredox Catalysis via Energy Transfer Cascade
Wei Huang, Jeehye Byun, Irina Rörich, Charusheela Ramanan, Paul W. M. Blom, Hao Lu, Di Wang, Lucas Caire da Silva, Run Li, Lei Wang, Katharina Landfester, Kai A. I. Zhang
Asymmetric Covalent Triazine Framework for Enhanced Visible Light Photoredox Catalysis via Energy Transfer Cascade
Complex multiple‐component semiconductor photocatalysts can be constructed that display enhanced catalytic efficiency via multiple charge and energy transfer, mimicking photosystems in nature. In contrast, the efficiency of single‐component semiconductor photocatalysts is usually limited due to the fast recombination of the photogenerated excitons. Here, we report the design of an asymmetric covalent triazine framework as an efficient organic single‐component semiconductor photocatalyst. Four different molecular donor–acceptor domains are obtained within the network, leading to enhanced photogenerated charge separation via an intramolecular energy transfer cascade. The photocatalytic efficiency of the asymmetric covalent triazine framework is superior to that of its symmetric counterparts; this was demonstrated by the visible‐light‐driven formation of benzophosphole oxides from diphenylphosphine oxide and diphenylacetylene.
© Wiley VCH (2018)
Asymmetric Covalent Triazine Framework for Enhanced Visible Light Photoredox Catalysis via Energy Transfer Cascade
Bottom-Up Synthesis of Heteroatom-Doped Chiral Graphene Nanoribbons
Wang, Xiao-Ye; Urgel, José I.; Barin, Gabriela Borin; Eimre, Kristjan; Di Giovannantonio, Marco; Milani, Alberto; Tommasini, Matteo; Pignedoli, Carlo A.; Ruffieux, Pascal; Feng, Xinliang; Fasel, Roman; Müllen, Klaus; Narita, Akimitsu
Bottom-Up Synthesis of Heteroatom-Doped Chiral Graphene Nanoribbons
Bottom-up synthesis of graphene nanoribbons (GNRs) has significantly advanced during the past decade, providing various GNR structures with tunable properties. The synthesis of chiral GNRs, however, has been underexplored and only limited to (3,1)-GNRs. We report herein the surface-assisted synthesis of the first heteroatom-doped chiral (4,1)-GNRs from the rationally designed precursor 6,16-dibromo-9,10,19,20-tetraoxa-9a,19a-diboratetrabenzo[a,f,j,o]perylene. The structure of the chiral GNRs has been verified by scanning tunneling microscopy, noncontact atomic force microscopy, and Raman spectroscopy in combination with theoretical modeling. Due to the presence of oxygen–boron–oxygen (OBO) segments on the edges, lateral self-assembly of the GNRs has been observed, realizing well-aligned GNR arrays with different modes of homochiral and heterochiral inter-ribbon assemblies.
© JACS (2018)
Bottom-Up Synthesis of Heteroatom-Doped Chiral Graphene Nanoribbons
 
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