Recent Submissions

  • Influence of the anionic ligands on properties and reactivity of Hoveyda-Grubbs catalysts

    Albalawi, Mona O.; Falivene, Laura; Jedidi, Abdesslem; Osman, Osman I.; Elroby, Shaaban A.; Cavallo, Luigi (Molecular Catalysis, Elsevier BV, 2021-06-26) [Article]
    Ruthenium based catalysts remain among the more successful complexes used in the catalysis of metathesis processes for the synthesis of new carbon-carbon bonds. The investigation of the influence of the different system moieties on its catalytic performance has led to important improvements in the field. To this extent, density functional theory (DFT) calculations have contributed significantly providing fundamental understandings to develop new catalysts. With this aim, we presented here a detailed computational study of how the nature of the anion ligand binding to the metal affects the global properties and reactivity of the catalyst. Geometric, energetic and electronic analysis have been performed to reach the key insights necessary to build structure-performance correlations.
  • Tumor-Associated-Macrophage-Membrane-Coated Nanoparticles for Improved Photodynamic Immunotherapy

    Chen, Cailing; Song, Meiyu; Du, Yangyang; Yu, Ying; Li, Chunguang; Han, Yu; Yan, Fei; Shi, Zhan; Feng, Shouhua (Nano Letters, American Chemical Society (ACS), 2021-06-16) [Article]
    Cell-membrane-coated nanoparticles have emerged as a promising antitumor therapeutic strategy. However, the immunologic mechanism remains elusive, and there are still crucial issues to be addressed including tumor-homing capacity, immune incompatibility, and immunogenicity. Here, we reported a tumor-associated macrophage membrane (TAMM) derived from the primary tumor with unique antigen-homing affinity capacity and immune compatibility. TAMM could deplete the CSF1 secreted by tumor cells in the tumor microenvironment (TME), blocking the interaction between TAM and cancer cells. Especially, after coating TAMM to upconversion nanoparticle with conjugated photosensitizer (NPR@TAMM), NPR@TAMM-mediated photodynamic immunotherapy switched the activation of macrophages from an immunosuppressive M2-like phenotype to a more inflammatory M1-like state, induced immunogenic cell death, and consequently enhanced the antitumor immunity efficiency via activation of antigen-presenting cells to stimulate the production of tumor-specific effector T cells in metastatic tumors. This TAM-membrane-based photodynamic immunotherapy approach offers a new strategy for personalized tumor therapy.
  • Concurrent cationic and anionic perovskite defect passivation enables 27.4% perovskite/silicon tandems with suppression of halide segregation

    Isikgor, Furkan Halis; Furlan, Francesco; Liu, Jiang; Ugur, Esma; Eswaran, Mathan Kumar; Subbiah, Anand Selvin; Yengel, Emre; de Bastiani, Michele; Harrison, George T.; Zhumagali, Shynggys; Howells, Calvyn Travis; Aydin, Erkan; Wang, Mingcong; Gasparini, Nicola; Allen, Thomas; Rehman, Atteq Ur; Van Kerschaver, Emmanuel; Baran, Derya; McCulloch, Iain; Anthopoulos, Thomas D.; Schwingenschlögl, Udo; Laquai, Frédéric; De Wolf, Stefaan (Joule, Elsevier BV, 2021-06-16) [Article]
    Stable and efficient perovskite/silicon tandem solar cells require defect passivation and suppression of light-induced phase segregation of the wide-band-gap perovskite. Here, we report how molecules containing both electron-rich and electron-poor moieties, such as phenformin hydrochloride (PhenHCl), can satisfy both requirements, independent of the perovskite’s surface chemical composition and its grain boundaries and interfaces. PhenHClpassivated wide-band-gap ( 1.68 eV) perovskite p-i-n single-junction solar cells deliver an open-circuit voltage (VOC) 100 mV higher than control devices, resulting in power conversion efficiencies (PCEs) up to 20.5%. These devices do not show any VOC losses after more than 3,000 h of thermal stress at 85C in a nitrogen ambient. Moreover, PhenHCl passivation improves the PCE of textured perovskite/silicon tandem solar cells from 25.4% to 27.4%. Our findings provide critical insights for improved passivation of metal halide perovskite surfaces and the fabrication of highly efficient and stable perovskite-based single-junction and tandem solar cells.
  • n-Type organic semiconducting polymers: stability limitations, design considerations and applications

    Griggs, Sophie; Marks, Adam; Bristow, Helen; McCulloch, Iain (Journal of Materials Chemistry C, Royal Society of Chemistry (RSC), 2021-06-15) [Article]
    This review outlines the design strategies which aim to develop high performing n-type materials in the fields of organic thin film transistors (OTFT), organic electrochemical transistors (OECT) and organic thermoelectrics (OTE). Figures of merit for each application and the limitations in obtaining these are set out, and the challenges with achieving consistent and comparable measurements are addressed. We present a thorough discussion of the limitations of n-type materials, particularly their ambient operational instability, and suggest synthetic methods to overcome these. This instability originates from the oxidation of the negative polaron of the organic semiconductor (OSC) by water and oxygen, the potentials of which commonly fall within the electrochemical window of n-type OSCs, and consequently require a LUMO level deeper than ∼−4 eV for a material with ambient stability. Recent high performing n-type materials are detailed for each application and their design principles are discussed to explain how synthetic modifications can enhance performance. This can be achieved through a number of strategies, including utilising an electron deficient acceptor–acceptor backbone repeat unit motif, introducing electron-withdrawing groups or heteroatoms, rigidification and planarisation of the polymer backbone and through increasing the conjugation length. By studying the fundamental synthetic design principles which have been employed to date, this review highlights a path to the development of promising polymers for n-type OSC applications in the future.
  • Redox-Neutral Cross-Coupling Amination with Weak N-Nucleophiles: Arylation of Anilines, Sulfonamides, Sulfoximines, Carbamates, and Imines via Nickelaelectrocatalysis

    Zhu, Chen; Kale, Ajit Prabhakar; Yue, Huifeng; Rueping, Magnus (JACS Au, American Chemical Society (ACS), 2021-06-15) [Article]
    A nickel-catalyzed cross-coupling amination with weak nitrogen nucleophiles is described. Aryl halides as well as aryl tosylates can be efficiently coupled with a series of weak N-nucleophiles, including anilines, sulfonamides, sulfoximines, carbamates, and imines via concerted paired electrolysis. Notably, electron-deficient anilines and sulfonamides are also suitable substrates. Interestingly, when benzophenone imine is applied in the arylation, the product selectivity toward the formation of amine and imine product can be addressed by a base switch. In addition, the alternating current mode can be successfully applied. DFT calculations support a facilitated reductive elimination pathway.
  • Magnesium complexes in hydroelementation and reduction catalysis: Opportunities and Challenges

    Magre, Marc; Szewczyk, Marcin; Rueping, Magnus (Current Opinion in Green and Sustainable Chemistry, Elsevier BV, 2021-06-10) [Article]
    The addition of a Y-H (Y= B, Si, Sn, N, P and O) bonds and H2 to unsaturated bonds is a powerful and atom economic method for the synthesis of fine chemicals. In the recent years, magnesium-based organometallic complexes have appeared as an alternative to transition metal catalysts for the hydrofunctionalization and hydrogenation of unsaturated systems. This review focuses on the progress of magnesium catalysis for the hydrofunctionalization and hydrogenation of unsaturated bonds, provides a critical assessment of the state-of-the-art research, highlights the major developments achieved in the past three years and provides an overview of the challenges and opportunities.
  • Insights into the Enhancement of MOF/Polymer Adhesion in Mixed-Matrix Membranes via Polymer Functionalization

    Carja, Ionela-Daniela; Tavares, Sergio Rodrigues; Shekhah, Osama; Ozcan, Aydin; Semino, Rocio; Kale, Vinayak Swamirao; Eddaoudi, Mohamed; Maurin, Guillaume (ACS Applied Materials & Interfaces, American Chemical Society (ACS), 2021-06-09) [Article]
    MOF-based mixed-matrix membranes (MMMs) prepared using standard routes often exhibit poor adhesion between polymers and MOFs. Herein, we report an unprecedented systematic exploration on polymer functionalization as the key to achieving defect-free MMMs. As a case study, we explored computationally MMMs based on the combination of the prototypical UiO-66(Zr) MOF with polymer of intrinsic porosity-1 (PIM-1) functionalized with various groups including amidoxime, tetrazole, and N-((2-ethanolamino)ethyl)carboxamide. Distinctly, the amidoxime-derivative PIM-1/UiO-66(Zr) MMM was predicted to express the desired enhanced MOF/polymer interfacial interactions and thus subsequently prepared and evaluated experimentally. Prominently, high-resolution transmission electron microscopy confirmed optimal adhesion between the two components in contrast to the nanometer-sized voids/defects shown by the pristine PIM-1/UiO-66(Zr) MMM. Notably, single-gas permeation measurements further corroborated the need of optimal MOF/polymer adhesion in order to effectively enable the MOF to play a role in the gas transport of the resulting MMM.
  • Engineering the Coordination Sphere of Isolated Active Sites to Explore the Intrinsic Activity in Single-Atom Catalysts

    Wu, Xin; Zhang, Huabin; Zuo, Shouwei; Dong, Juncai; Li, Yang; Zhang, Jian; Han, Yu (Nano-Micro Letters, Springer Science and Business Media LLC, 2021-06-07) [Article]
    AbstractReducing the dimensions of metallic nanoparticles to isolated, single atom has attracted considerable attention in heterogeneous catalysis, because it significantly improves atomic utilization and often leads to distinct catalytic performance. Through extensive research, it has been recognized that the local coordination environment of single atoms has an important influence on their electronic structures and catalytic behaviors. In this review, we summarize a series of representative systems of single-atom catalysts, discussing their preparation, characterization, and structure–property relationship, with an emphasis on the correlation between the coordination spheres of isolated reactive centers and their intrinsic catalytic activities. We also share our perspectives on the current challenges and future research promises in the development of single-atom catalysis. With this article, we aim to highlight the possibility of finely tuning the catalytic performances by engineering the coordination spheres of single-atom sites and provide new insights into the further development for this emerging research field.
  • Characterization of Silica-Supported Tungsten Bis- and Tris-hydrides by Advanced Solid-State NMR

    Wackerow, Wiebke; Thiam, Zeynabou; Abou-Hamad, Edy; Almaksoud, Walid; Hedhili, Mohamed N.; Basset, Jean-Marie (The Journal of Physical Chemistry C, American Chemical Society (ACS), 2021-06-03) [Article]
    Tungsten-hydrides supported on oxide supports are unique catalysts regarding the direct transformation of ethylene to propylene, alkane metathesis, and the low-temperature hydrogenolysis of waxes to lower molecular paraffins. The number of hydrides coordinated to the tungsten center and their structure on the siliceous support with very high surface silica (KCC-1) is unknown. KCC-1(700) silica of extremely high surface area allows for a high tungsten metal loading of 14 wt %. We show here the full characterization of supported tungsten bis- and tris-hydrides, which, after reaction with N2O gas, yield well-defined tungsten bis- and tris-hydroxide species on KCC-1(700). The obtained tungsten-hydroxide species are perfectly suitable for a detailed NMR study. The obtained tungsten hydroxo complexes are proven to be a tungsten bis-hydroxo and tungsten tris-hydroxo species. This analysis supports the conclusion that supported tungsten-hydride complexes coexist on the support as bis-hydride and tris-hydride species. They are, respectively, in close proximity to the silicon bis-hydride and the silicon mono-hydride. This proximity is explained by the mechanism of the formation of tungsten-hydride on the silica surface.
  • The Deuterated “Magic Methyl“ Group - A Guide for Site-selective Trideuteromethyl Incorporation and Labeling using CD3-reagents

    Steverlynck, Joost Andre; Sitdikov, Ruzal; Rueping, Magnus (Chemistry – A European Journal, Wiley, 2021-06-02) [Article]
    In the field of medicinal chemistry the precise installation of a trideuteromethyl group is gaining ever-increasing attention. Site-selective incorporation of the deuterated “magic methyl” group can provide profound pharmacological benefits and can be considered as an important tool for drug optimization and development. This review provides a structured overview, according to the trideuteromethylation reagent, of currently established methods for site-selective trideuteromethylations of carbon atoms. Selective introduction of CD2H and CDH2 groups, in addition to CD3, is also considered. For all methods, the corresponding mechanism and scope are discussed whenever reported. As such, this review can be a starting point for synthetic chemists to further advance trideuteromethylation methodologies. At the same time, this review aims to be a guide for medicinal chemists, offering them the available C-CD3 formation strategies for the preparation of new or modified drugs.
  • Efficiency Limits in Wide-Bandgap Ge-Containing Donor Polymer:Non-Fullerene Acceptor Bulk Heterojunction Solar Cells

    Khan, Jafar Iqbal; Alsaggaf, Sarah; Ashraf, Raja; Purushothaman, Balaji; Chaturvedi, Neha; McCulloch, Iain; Laquai, Frédéric (physica status solidi (RRL) – Rapid Research Letters, Wiley, 2021-06-02) [Article]
    A precise picture of the photophysics that determine the efficiency of non-fullerene acceptor (NFA) bulk heterojunction (BHJ) organic solar cells is still missing, yet needed to mitigate the remaining loss channels. Here, we investigate charge carrier generation and recombination dynamics in blends of a novel wide-bandgap germanium-containing donor polymer, namely PEHGeNDT-BT, paired with either O-IDTBR or O-IDTBCN as non-fullerene acceptor in BHJ solar cells by (ultrafast) transient spectroscopy and time-delayed collection field (TDCF) experiments. Photovoltaic devices yield moderate power conversion efficiencies (PCEs) of 5.3% when using O-IDTBCN as acceptor, and only about 2% when using O-IDTBR as acceptor, the latter severely limited by its low photocurrent and moderate fill factor (FF) of ∽43%. Time-resolved photoluminescence experiments reveal limited exciton quenching as one loss channel in O-IDTBR based blends, accompanied by significant geminate recombination further reducing the photocurrent, while field-dependent charge generation is identified as the origin of the low FF. Geminate recombination is less in the O-IDTBCN blend and charge generation is field-independent, leading to improved photocurrent and FF. Carrier drift-diffusion simulations of the devices’ current-voltage (J-V) characteristics confirm that the experimentally-determined kinetic parameters and process yields can reproduce the measured J-V curves under steady-state solar illumination.
  • Simple Synthetic Routes to Carbene-M-Amido (M = Cu, Ag, Au) Complexes for Luminescence and Photocatalysis Applications

    Nolan, Steven Patrick; Tzouras, Nikolaos V.; Martynova, Ekaterina A.; Ma, Xinyuan; Scattolin, Thomas; Hupp, Benjamin; Busen, Hendrik; Saab, Marina; Zhang, Ziyun; Falivene, Laura; Pisanò, Gianmarco; Van Hecke, Kristof; Cavallo, Luigi; Cazin, Catherine S. J.; Steffen, Andreas (Chemistry – A European Journal, Wiley, 2021-05-26) [Article]
    The development of novel and operationally simple synthetic routes to Carbene-Metal-Amido (CMA) complexes of copper, silver and gold relevant for photonic applications are reported. A mild base and sustainable solvents allow all operations to be conducted in air and at room temperature, leading to high yields of the targeted compounds even on multigram scales. The effect of various mild bases on the N-H metallation was studied in silico and experimentally, while a mechanochemical, solvent-free synthetic approach was also developed. Our photophysical studies on [M(NHC)(Cbz)] indicate that the occurrence of fluorescent or phosphorescent states is determined primarily by the metal, providing control over the excited state properties. Consequently, we demonstrate the potential of the new CMAs beyond luminescence applications by employing a selected CMA as a photocatalyst. The exemplified synthetic ease is expected to accelerate the applications of CMAs in photocatalysis and materials chemistry.
  • Shining Light on the Structure of Lead Halide Perovskite Nanocrystals

    Chen, Jia-Kai; Zhao, Qing; Shirahata, Naoto; Yin, Jun; Bakr, Osman; Mohammed, Omar F.; Sun, Hong-Tao (ACS Materials Letters, American Chemical Society (ACS), 2021-05-24) [Article]
    Lead halide perovskite nanocrystals (NCs) have attracted great attention owing to the simplicity of their synthesis and excellent defect-tolerance nature. They not only demonstrate outstanding optical and electronic properties, but also hold substantially ionic lattices with some counterintuitive structural features that are significantly different from conventional colloidal semiconductor NCs such as CdSe and InP. In this Review, we summarize and assess the recent advances in the understanding of structural characteristics of lead halide perovskite NCs. We specifically focus on the role of intrinsic defects, NC size, dopants, alloying, and external stimuli in affecting their structure. Moreover, we highlight the use of atomic resolution imaging technique in investigating their microstructural characteristics. Finally, we discuss open questions and present our perspectives on future research directions in the exciting field of science
  • Rapid single-molecule detection of COVID-19 and MERS antigens via nanobody-functionalized organic electrochemical transistors

    Guo, Keying; Wustoni, Shofarul; Koklu, Anil; Díaz-Galicia, Escarlet; Moser, Maximilian; Hama, Adel; Alqahtani, Ahmed A.; Ahmad, Adeel Nazir; Alhamlan, Fatimah Saeed; Shuaib, Muhammad; Pain, Arnab; McCulloch, Iain; Arold, Stefan T.; Grunberg, Raik; Inal, Sahika (Nature Biomedical Engineering, Springer Science and Business Media LLC, 2021-05-24) [Article]
    The coronavirus disease 2019 (COVID-19) pandemic has highlighted the need for rapid and sensitive protein detection and quantification in simple and robust formats for widespread point-of-care applications. Here, we report on nanobody-functionalized organic electrochemical transistors with a modular architecture for the rapid quantification of single-molecule-to-nanomolar levels of specific antigens in complex bodily fluids. The sensors combine a solution-processable conjugated polymer in the transistor channel and high-density and orientation-controlled bioconjugation of nanobody–SpyCatcher fusion proteins on disposable gate electrodes. The devices provide results after 10 min of exposure to 5 μl of unprocessed samples, maintain high specificity and single-molecule sensitivity in human saliva and serum, and can be reprogrammed to detect any protein antigen if a corresponding specific nanobody is available. We used the sensors to detect green fluorescent protein, and severe acute respiratory syndrome coronavirus-2 (SARS-CoV-2) and Middle East respiratory syndrome coronavirus (MERS-CoV) spike proteins, and for the COVID-19 screening of unprocessed clinical nasopharyngeal swab and saliva samples with a wide range of viral loads.
  • Impact of Acceptor Quadrupole Moment on Charge Generation and Recombination in Blends of IDT-Based Non-Fullerene Acceptors with PCE10 as Donor Polymer

    Khan, Jafar Iqbal; Alamoudi, Maha A; Chaturvedi, Neha; Ashraf, Raja; Nabi, Mohammed N.; Markina, Anastasia; Liu, Wenlan; Dela Peña, Top Archie; Zhang, Weimin; Alévêque, Olivier; Harrison, George T.; Alsufyani, Wejdan; Levillain, Eric; De Wolf, Stefaan; Andrienko, Denis; McCulloch, Iain; Laquai, Frédéric (Advanced Energy Materials, Wiley, 2021-05-24) [Article]
    Advancing non-fullerene acceptor (NFA) organic photovoltaics requires the mitigation of the efficiency-limiting processes. Acceptor end-group and side-chain engineering are two handles to tune properties, and a better understanding of their specific impact on the photophysics could facilitate a more guided acceptor design. Here, the device performance, energetic landscape, and photophysics of rhodanine and dicyanovinyl end-capped IDT-based NFAs, namely, O-IDTBR and O-IDTBCN, in PCE10-based solar cells are compared by transient optical and electro-optical spectroscopy techniques and density functional theory calculations. It is revealed how the acceptors’ quadrupole moments affect the interfacial energetic landscape, in turn causing differences in exciton quenching, charge dissociation efficiencies, and geminate versus non-geminate recombination losses. More precisely, it is found that the open circuit voltage (VOC) is controlled by the acceptors’ electron affinity (EA), while geminate and non-geminate recombination, and the field dependence of charge generation, rely on the acceptors’ quadrupole moments. The kinetic parameters and yields of all processes are determined, and it is demonstrated that they can reproduce the performance differences of the devices’ current–voltage characteristics in carrier drift-diffusion simulations. The results provide insight into the impact of the energetic landscape, specifically the role of the quadrupole moment of the acceptor, beyond trivial considerations of the donor–acceptor energy offsets.
  • Operando Elucidation on the Working State of Immobilized Fluorinated Iron Porphyrin for Selective Aqueous Electroreduction of CO2 to CO

    Lu, Xiaofei; Ait Ahsaine, Hassan; Dereli, Busra; Garcia Esparza, Angel T.; Reinhard, Marco; Shinagawa, Tatsuya; Li, Duanxing; Adil, Karim; Tchalala, Mohammed; Kroll, Thomas; Eddaoudi, Mohamed; Sokaras, Dimosthenis; Cavallo, Luigi; Takanabe, Kazuhiro (ACS Catalysis, American Chemical Society (ACS), 2021-05-19) [Article]
    Iron porphyrin-based molecular catalysts can electrocatalyze CO2 reduction to CO at nearly 100% selectivity in water. Nevertheless, the associated active sites and reaction mechanisms remain debatable, impeding the establishment of design guidelines for effective catalysts. This study reports coupling in operando experiments and theoretical calculations for immobilized 5,10,15,20-tetrakis(pentafluorophenyl) porphyrin Fe(III) chloride (FeF20TPP) for electrocatalytic CO2 reduction in an aqueous phase. In operando UV–vis and X-ray absorption near-edge structure spectra indicated the persisting presence of Fe(II) species during the cathodic reaction, acting as catalytic sites that accommodate CO as Fe(II)–CO adducts. Consistently, the density functional calculations pointed out that the ligand-reduced state with oxidized Fe, namely, [Fe(II)F20(TPP•)]−, prevails in the catalytic cycle prior to the rate-controlling step. This work provides the conclusive representation related to the working states of Fe-based molecular catalysts under reaction conditions.
  • Directional Exciton Migration in Benzoimidazole-Based Metal–Organic Frameworks

    Gutierrez Arzaluz, Luis; Jia, Jiangtao; Gu, Chun; Czaban-Jozwiak, Justyna; Yin, Jun; Shekhah, Osama; Bakr, Osman; Eddaoudi, Mohamed; Mohammed, Omar F. (The Journal of Physical Chemistry Letters, American Chemical Society (ACS), 2021-05-19) [Article]
    Highly luminescent metal-organic frameworks (MOFs) have recently received great attention due to their potential applications as sensors and light-emitting devices. In these MOFs, the highly ordered fluorescent organic linkers positioning prevents excited-state self-quenching and rotational motion, enhancing their light-harvesting properties. Here, the exciton migration between the organic linkers with the same chemical structure but different protonation degrees in Zr-based MOFs was explored and deciphered using ultrafast laser spectroscopy and density functional theory calculations. First, we clearly demonstrate how hydrogen-bonding interactions between free linkers and solvents affect the twisting changes, internal conversion processes, and luminescent behavior of a benzoimidazole-based linker. Second, we provide clear evidence of an ultrafast energy transfer between well-aligned adjacent linkers with different protonation states inside the MOF. These findings provide a new fundamental photophysical insight into the exciton migration dynamics between linkers with different protonation states coexisting at different locations in MOFs and serve as a benchmark for improving light-harvesting MOF architectures.
  • Electrolyte Chemistry in 3D Metal Oxide Nanorod Arrays Deciphers Lithium Dendrite-Free Plating/Stripping Behaviors for High-Performance Lithium Batteries

    Li, Qian; Cao, Zhen; Liu, Gang; Cheng, Haoran; Wu, Yingqiang; Ming, Hai; Park, Geon-Tae; Yin, Dongming; Wang, Limin; Cavallo, Luigi; Sun, Yang-Kook; Ming, Jun (The Journal of Physical Chemistry Letters, American Chemical Society (ACS), 2021-05-18) [Article]
    Lithium dendrite-free deposition is crucial to stabilizing lithium batteries, where the three-dimensional (3D) metal oxide nanoarrays demonstrate an impressive capability to suppress dendrite due to the spatial effect. Herein, we introduce a new insight into the ameliorated lithium plating process on 3D nanoarrays. As a paradigm, novel 3D Cu<sub>2</sub>O and Cu nanorod arrays were <i>in situ</i> designed on copper foil. We find that the dendrite and electrolyte decomposition can be mitigated effectively by Cu<sub>2</sub>O nanoarrays, while the battery failed fast when the Cu nanoarrays were used. We show that Li<sub>2</sub>O (i.e., formed in the lithiation of Cu<sub>2</sub>O) is critical to stabilizing the electrolyte; otherwise, the electrolyte would be decomposed seriously. Our viewpoint is further proved when we revisit the metal (oxide) nanoarrays reported before. Thus, we discovered the importance of electrolyte stability as a precondition for nanoarrays to suppress dendrite and/or achieve a reversible lithium plating/stripping for high-performance lithium batteries.
  • Surface organometallic chemistry: A sustainable approach in modern catalysis

    Samantaray, Manoja; Mishra, Sandeep K.; Saidi, Aya; Basset, Jean-Marie (Journal of Organometallic Chemistry, Elsevier BV, 2021-05-14) [Article]
    Surface organometallic chemistry (SOMC) is an established concept, associated with specific tools for the characterization of a well-defined single-site catalysts. Primarily, chemical industry preferred heterogeneous catalyst over homogeneous catalyst for various reasons. But the difficulty in development of a well-defined heterogeneous catalyst stalled by the presence of various kinds of active sites as well as their low concentration on surfaces. To develop a well-defined heterogeneous catalyst which can possess hundred percent active sites like that of homogeneous catalyst a new branch was developed called surface organometallic catalyst (SOMCcat). This is a well-proven concept where a homogeneous catalyst could graft on an oxide support to form SOMCcat. These surface species can be well-characterized by modern NMR techniques apart from EXAFS, IR, and gas quantification methods. In this review the application of SOMC strategy for the design and preparation of catalyst for industrial relevant processes are discussed.
  • Inkjet Printed Circuits with 2D Semiconductor Inks for High-Performance Electronics

    Carey, Tian; Arbab, Adrees; Anzi, Luca; Bristow, Helen; Hui, Fei; Bohm, Sivasambu; Wyatt-Moon, Gwenhivir; Flewitt, Andrew; Wadsworth, Andrew; Gasparini, Nicola; Kim, Jong M.; Lanza, Mario; McCulloch, Iain; Sordan, Roman; Torrisi, Felice (Advanced Electronic Materials, Wiley, 2021-05-13) [Article]
    Air-stable semiconducting inks suitable for complementary logic are key to create low-power printed integrated circuits (ICs). High-performance printable electronic inks with 2D materials have the potential to enable the next generation of high performance low-cost printed digital electronics. Here, the authors demonstrate air-stable, low voltage (<5 V) operation of inkjet-printed n-type molybdenum disulfide (MoS2), and p-type indacenodithiophene-co-benzothiadiazole (IDT-BT) field-effect transistors (FETs), estimating an average switching time of τMoS2 ≈ 4.1 μs for the MoS2 FETs. They achieve this by engineering high-quality MoS2 and air-stable IDT-BT inks suitable for inkjet-printing complementary pairs of n-type MoS2 and p-type IDT-BT FETs. They then integrate MoS2 and IDT-BT FETs to realize inkjet-printed complementary logic inverters with a voltage gain |Av| ≈ 4 when in resistive load configuration and |Av| ≈ 1.4 in complementary configuration. These results represent a key enabling step towards ubiquitous long-term stable, low-cost printed digital ICs.

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