Resultados de investigación

No

82 pages. -- S1. Materials.-- S2. Synthetic procedures . -- S2.1. Synthesis of 5-((triisopropylsilyl)ethynyl)isophthalic acid, H2btc-TIPS. -- S2.2 Synthesis of alkyne-protected Rh(II)-MOP. -- S2.3 Deprotection procedure of alkyne-protected Rh(II)-MOP. Synthesis of BCN-23. -- S2.4 Copper-catalyzed azide-alkyne cycloaddition (CuAAC) on RhMOPs. -- S2.4.1 General CuAAC protocol for RhMOPs. -- S2.4.1.1 Bz-BCN-23.-- S2.4.1.2 Polymeric ligands. -- S2.4.2 Introducing coordinating groups. -- S2.4.2.1 Introducing free carboxylic acid groups. -- S2.4.2.2 Introducing free phosphonic acid groups. -- S2.4.3 Water-soluble COONa- and Na2PO3-functionalized MOPs. -- S2.4.4 Acid digestion of RhMOP. -- S2.4.4 Biotinylation of RhMOPs. -- S2.5 Competitive HABA-Avidin assay. -- S3. Computational Methods. -- S4. Characterization. -- S.4.1. Alkyne-protected RhMOP. -- S.4.2 BCN-23. -- S.4.3 Bz-BCN-23. -- S.4.4 mPEG42-BCN-23. -- S.4.5 COOH-bz-BCN-23. -- S.4.6 COOH-PEG3-BCN-23. -- S.4.7 COOH-C5-BCN-23 . -- S.4.8 H2PO3-BCN-23. -- S.4.9 Biotin-PEG5-BCN-23. -- S.5 Porosity of acidic Rh-MOPs. -- S.6 Biorecognition. Competitive HABA-Avidin assay. -- S7. Bibliography., Peer reviewed

20 pages. -- I. Growth methods. -- II. Er deposition and X-ray photoemission spectroscopy (XPS) coverage calibration. -- III. Er/Bi2Se2Te extended ARPES and XPS data. -- IV. Dy/Bi2Se2Te extended ARPES and XPS data. -- V. Theoretical model. -- VI. Theoretical prove of the Fermi velocity anisotropy upon Er doping. -- VII. MDCs and EDCs fittings: band dispersion and gap opening. -- VIII. Structural characterization: LEED patters., Magnetic topological insulators constitute a novel class of materials whose topological surface states (TSSs) coexist with long-range ferromagnetic order, eventually breaking time-reversal symmetry. The subsequent bandgap opening is predicted to co-occur with a distortion of the TSS warped shape from hexagonal to trigonal. We demonstrate such a transition by means of angle-resolved photoemission spectroscopy on the magnetically rare-earth (Er and Dy) surface-doped topological insulator Bi2Se2Te. Signatures of the gap opening are also observed. Moreover, increasing the dopant coverage results in a tunable p-type doping of the TSS, thereby allowing for a gradual tuning of the Fermi level toward the magnetically induced bandgap. A theoretical model where a magnetic Zeeman out-of-plane term is introduced in the Hamiltonian governing the TSS rationalizes these experimental results. Our findings offer new strategies to control magnetic interactions with TSSs and open up viable routes for the realization of the quantum anomalous Hall effect., Peer reviewed

17 pages. -- Table S1. Quantification of CuO, Cu2O and Cu from the XRD of all the compared blends. -- Table S2. Productivity comparison of the synthesised blends with respect to weight of Cu. -- Table S3. Comparison of Elemental composition from EDX analysis of as-prepared samples. -- Figures S1-S17., Peer reviewed

13 pages. -- Figures S1-S16. -- Table S1. Comparison of the HER performance in 0.5 M H2SO4 of FeP electrodes synthesized by growth or deposition of the electrocatalyst on the conductive support without the use of binders, in chronological order. NaH2PO2 was used as a phosphorous source in all cases unless otherwise stated. -- Table S2. Comparison of the HER performance in 1 M KOH of FeP electrodes synthesized by growth or deposition of the electrocatalyst on the conductive support without the use of binders, in chronological order. NaH2PO2 was used as a phosphorous source in all cases unless otherwise stated., Peer reviewed

41 pages. -- Materials and methods. -- Reagents. -- Instruments. -- Microwave reaction conditions. -- Synthesis of (Hf)PCN-224(Ni,Cu,Zn). -- Results and discussion. -- Synthesis and characterization- -- Optimization of synthetic protocol. -- Structure resolution. -- Physicochemical characterization. -- Catalysis. -- Selection of optimal conditions for CO2 cycloaddition. -- Catalytic performance. -- 1H-NMR., Peer reviewed

15 pages. -- SI-1 Discussion of spin states in the {M4} complex. -- SI-2 DFT calculations of {Mn4} and {Co4} complex grafted to the carbon nanotube. -- SI-3 Raman spectrum of the {Mn4} functionalised CNT device. -- SI-4 Histogram of the derivative of the original data. -- SI-5 Theoretical models and results. -- References., Peer reviewed

26 pages. -- S1. Materials and experimental methods. -- S1.1 Materials and characterization techniques. -- S1.2 Synthesis of COOHRhMOP and Rh2(BDC)4 cluster. -- S1.3 Fabrication and functionalization of the BiMW sensor. -- S1.4 Coordination capabilities of COOHRhMOP in aqueous solutions. -- S2. Characterization. -- S2.1 Model amide coupling between COOHRhMOP and propylamine. -- S2.2 Coordination capabilities of COOHRhMOP in aqueous solutions. -- S2.3 BiMW sensor surface characterization. -- S2.4 Characterization of the analytical performance of the Rh(II)-functionalized BiMW sensor surface. -- S3. Data analysis., The grave health and environmental consequences of water pollution demand new tools, including new sensing technologies, for the immediate detection of contaminants in situ. Herein, we report the integration of metal–organic cages or polyhedra (MOCs/MOPs) within a nanophotonic sensor for the rapid, direct, and real-time detection of small (<500 Da) pollutant molecules in water. The sensor, a bimodal waveguide silicon interferometer incorporating Rh(II)-based MOPs as specific chemical receptors, does not require sample pretreatment and enables minimal expenditure of time and reagents. We validated our sensor for the detection of two common pollutants: the industrial corrosion inhibitor 1,2,3-benzotriazole (BTA) and the systemic insecticide imidacloprid (IMD). The sensor offers a fast time-to-result response (15 min), high sensitivity, and high accuracy. The limit of detection (LOD) in tap water for BTA is 0.068 μg/mL and for IMD, 0.107 μg/mL, both of which are below the corresponding toxicity thresholds defined by the European Chemicals Agency (ECHA). By combining innovative chemical molecular receptors such as MOPs with state-of-the-art photonic sensing technologies, our research opens the path to implement competitive sensor devices for in situ environmental monitoring., Peer reviewed

4 pages. -- The Supplemental Information contains the following sections: Derivation of the mechanical susceptibilities. -- Geometrical parameters of the designed device. -- Determination of the lasing thresholds. -- Thermo-optic effect and free-carrier absorption. -- Intermodulation of MHz and GHz modes. -- Self-pulsing and other multimode lasing regimes. -- Numerical simulation details., Peer reviewed

46 pages. -- Section S1. General Methods and Materials. -- S1.1 Chemicals and reagents. -- S1.2 Instruments. -- Section S2. Synthetic Procedures. -- S2.1 Synthesis of 4,4′,4′′-s-triazine-2,4,6-triyl-tribenzoic acid (H3TATB). -- S2.2 Synthesis of (In)BCN-20B. -- S2.3 Synthesis of (Sc)BCN-20C. -- Section S3. (In)BCN-20B. -- Section S4. (In)BCN-20B’. -- Section S5. (In)BCN-20A. -- Section S6. Structural Evolution from (Sc)BCN-20C to (Sc)BCN-20A. -- References., Isoreticular chemistry, in which the organic or inorganic moieties of reticular materials can be replaced without destroying their underlying nets, is a key concept for synthesizing new porous molecular materials and for tuning or functionalization of their pores. Here, we report that the rational cleavage of covalent bonds in a metal–organic framework (MOF) can trigger their isoreticular contraction, without the need for any additional organic linkers. We began by synthesizing two novel MOFs based on the MIL-142 family, (In)­BCN-20B and (Sc)­BCN-20C, which include cleavable as well as noncleavable organic linkers. Next, we selectively and quantitatively broke their cleavable linkers, demonstrating that various dynamic chemical and structural processes occur within these structures to drive the formation of isoreticular contracted MOFs. Thus, the contraction involves breaking of a covalent bond, subsequent breaking of a coordination bond, and finally, formation of a new coordination bond supported by structural behavior. Remarkably, given that the single-crystal character of the parent MOF is retained throughout the entire transformation, we were able to monitor the contraction by single-crystal X-ray diffraction., Peer reviewed