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  • Journal article
    Cooper SM, White AJP, Eykyn TR, Ma MT, Miller PW, Long NJet al., 2022,

    N-centered tripodal phosphine Re(V) and Tc(V) oxo complexes: revisiting a [3+2] mixed-ligand approach

    , Inorganic Chemistry: including bioinorganic chemistry, Vol: 61, Pages: 8000-8014, ISSN: 0020-1669

    N-Triphos derivatives (NP3R, R = alkyl, aryl) and asymmetric variants (NP2RXR′, R′ = alkyl, aryl, X = OH, NR2, NRR′) are an underexplored class of tuneable, tripodal ligands in relation to the coordination chemistry of Re and Tc for biomedical applications. Mixed-ligand approaches are a flexible synthetic route to obtain Tc complexes of differing core structures and physicochemical properties. Reaction of the NP3Ph ligand with the Re(V) oxo precursor [ReOCl3(PPh3)2] generated the bidentate complex [ReOCl3(κ2-NP2PhOHAr)], which possesses an unusual AA’BB’XX’ spin system with a characteristic second-order NMR lineshape that is sensitive to the bi- or tridentate nature of the coordinating diphosphine unit. The use of the asymmetric NP2PhOHAr ligand resulted in the formation of both bidentate and tridentate products depending on the presence of base. The tridentate Re(V) complex [ReOCl2(κ3-NP2PhOAr)] has provided the basis of a new reactive “metal-fragment” for further functionalization in [3 + 2] mixed-ligand complexes. The synthesis of [3 + 2] complexes with catechol-based π-donors could also be achieved under one-pot, single-step conditions from Re(V) oxo precursors. Analogous complexes can also be synthesized from suitable 99Tc(V) precursors, and these complexes have been shown to exhibit highly similar structural properties through spectroscopic and chromatographic analysis. However, a tendency for the {MVO}3+ core to undergo hydrolysis to the {MVO2}+ core has been observed both in the case of M = Re and markedly for M = 99Tc complexes. It is likely that controlling this pathway will be critical to the generation of further stable Tc(V) derivatives.
  • Journal article
    Bennett TLR, Alshammari M, Au-Yong S, Almutlg A, Wang X, Wilkinson LA, Albrecht T, Jarvis SP, Cohen LF, Ismael A, Lambert CJ, Robinson BJ, Long NJet al., 2022,

    Multi-component self-assembled molecular-electronic films: towards new high-performance thermoelectric systems

    , Chemical Science, Vol: 13, Pages: 5176-5185, ISSN: 2041-6520

    The thermoelectric properties of parallel arrays of organic molecules on a surface offer the potential for large-area, flexible, solution processed, energy harvesting thin-films, whose room-temperature transport properties are controlled by quantum interference (QI). Recently, it has been demonstrated that constructive QI (CQI) can be translated from single molecules to self-assembled monolayers (SAMs), boosting both electrical conductivities and Seebeck coefficients. However, these CQI-enhanced systems are limited by rigid coupling of the component molecules to metallic electrodes, preventing the introduction of additional layers which would be advantageous for their further development. These rigid couplings also limit our ability to suppress the transport of phonons through these systems, which could act to boost their thermoelectric output, without comprising on their impressive electronic features. Here, through a combined experimental and theoretical study, we show that cross-plane thermoelectricity in SAMs can be enhanced by incorporating extra molecular layers. We utilize a bottom-up approach to assemble multi-component thin-films that combine a rigid, highly conductive ‘sticky’-linker, formed from alkynyl-functionalised anthracenes, and a ‘slippery’-linker consisting of a functionalized metalloporphyrin. Starting from an anthracene-based SAM, we demonstrate that subsequent addition of either a porphyrin layer or a graphene layer increases the Seebeck coefficient, and addition of both porphyrin and graphene leads to a further boost in their Seebeck coefficients. This demonstration of Seebeck-enhanced multi-component SAMs is the first of its kind and presents a new strategy towards the design of thin-film thermoelectric materials.
  • Journal article
    Sheppard SA, Bennett TLR, Long NJ, 2022,

    Development and Characterisation of Highly Conjugated Functionalised Ferrocenylene Macrocycles

    , EUROPEAN JOURNAL OF INORGANIC CHEMISTRY, Vol: 2022, ISSN: 1434-1948
  • Journal article
    Li Z, Li B, Wu X, Sheppard SA, Zhang S, Gao D, Long NJ, Zhu Zet al., 2022,

    Organometallic-functionalized interfaces for highly efficient inverted perovskite solar cells

    , SCIENCE, Vol: 376, Pages: 416-+, ISSN: 0036-8075
  • Journal article
    Baker CA, Romain C, Long NJ, 2021,

    Cation-π interactions enabling hard/soft Ti/Ag heterobimetallic cooperativity in lactide ring-opening polymerisation

    , CHEMICAL COMMUNICATIONS, Vol: 57, Pages: 12524-12527, ISSN: 1359-7345
  • Journal article
    Braga M, Leow CH, Gil JH, Teh JH, Carroll L, Long NJ, Tang M-X, Aboagye EOet al., 2021,

    Investigating CXCR4 expression of tumor cells and the vascular compartment: A multimodal approach

    , PLoS One, Vol: 16, Pages: 1-21, ISSN: 1932-6203

    The C-X-C chemokine receptor 4 (CXCR4) is G protein-coupled receptor that upon binding to its cognate ligand, can lead to tumor progression. Several CXCR4-targeted therapies are currently under investigation, and with it comes the need for imaging agents capable of accurate depiction of CXCR4 for therapeutic stratification and monitoring. PET agents enjoy the most success, but more cost-effective and radiation-free approaches such as ultrasound (US) imaging could represent an attractive alternative. In this work, we developed a targeted microbubble (MB) for imaging of vascular CXCR4 expression in cancer. A CXCR4-targeted MB was developed through incorporation of the T140 peptide into the MB shell. Binding properties of the T140-MB and control, non-targeted MB (NT-MB) were evaluated in MDA-MB-231 cells where CXCR4 expression was knocked-down (via shRNA) through optical imaging, and in the lymphoma tumor models U2932 and SuDHL8 (high and low CXCR4 expression, respectively) by US imaging. PET imaging of [18F]MCFB, a tumor-penetrating CXCR4-targeted small molecule, was used to provide whole-tumor CXCR4 readouts. CXCR4 expression and microvessel density were performed by immunohistochemistry analysis and western blot. T140-MB were formed with similar properties to NT-MB and accumulated sensitively and specifically in cells according to their CXCR4 expression. In NOD SCID mice, T140-MB persisted longer in tumors than NT-MB, indicative of target interaction, but showed no difference between U2932 and SuDHL8. In contrast, PET imaging with [18F]MCFB showed a marked difference in tumor uptake at 40–60 min post-injection between the two tumor models (p<0.05). Ex vivo analysis revealed that the large differences in CXCR4 expression between the two models are not reflected in the vascular compartment, where the MB are restricted; in fact, microvessel density and CXCR4 expression in the vasculature was comparable between U2932 and SuDHL8 tumors. In conclusion, we success
  • Journal article
    Osborne BE, Yue TTC, Waters ECT, Baark F, Southworth R, Long NJet al., 2021,

    Synthesis and <i>ex vivo</i> biological evaluation of gallium-68 labelled NODAGA chelates assessing cardiac uptake and retention

    , DALTON TRANSACTIONS, Vol: 50, Pages: 14695-14705, ISSN: 1477-9226
  • Journal article
    Teh JH, Braga M, Allott L, Barnes C, Hernandez-Gil J, Tang M-X, Aboagye EO, Long NJet al., 2021,

    A kit-based aluminium-[F-18]fluoride approach to radiolabelled microbubbles

    , Chemical Communications, Vol: 57, Pages: 11677-11680, ISSN: 1359-7345

    The production of 18F-labelled microbubbles (MBs) via the aluminium-[18F]fluoride ([18F]AlF) radiolabelling method and facile inverse-electron-demand Diels–Alder (IEDDA) ‘click’ chemistry is reported. An [18F]AlF-NODA-labelled tetrazine was synthesised in excellent radiochemical yield (>95% RCY) and efficiently conjugated to a trans-cyclooctene (TCO) functionalised phospholipid (40–50% RCY), which was incorporated into MBs (40–50% RCY). To demonstrate the potential of producing 18F-labelled MBs for clinical studies, we also describe a kit-based approach which is amenable for use in a hospital radiopharmacy setting.
  • Journal article
    Walter ERH, Cooper SM, Boyle JJ, Long NJet al., 2021,

    Enzyme-activated probes in optical imaging: a focus on atherosclerosis

    , DALTON TRANSACTIONS, Vol: 50, Pages: 14486-14497, ISSN: 1477-9226
  • Journal article
    Wu Y, Chau H, Thor W, Chan KHY, Ma X, Chan W, Long NJ, Wong Ket al., 2021,

    Solid‐Phase Peptide Macrocyclization and Multifunctionalization via Dipyrrin Construction

    , Angewandte Chemie, Vol: 133, Pages: 20463-20469, ISSN: 0044-8249

    <jats:title>Abstract</jats:title><jats:p>We introduce a new and highly efficient synthetic protocol towards multifunctional fluorescent cyclopeptides by solid‐phase peptide macrocyclization via dipyrrin construction, with full scope of proteinogenic amino acids and different ring sizes. Various bicyclic peptides can be created by dipyrrin‐based crosslinking and double dipyrrin‐ring formation. The embedded dipyrrin can be either transformed to fluorescent BODIPY and then utilized as cancer‐selective targeted protein imaging probe in vitro, or directly employed as a selective metal sensor in aqueous media. This work provides a valuable addition to the peptide macrocyclization toolbox, and a blueprint for the development of multifunctional dipyrrin linkers in cyclopeptides for a wide range of potential bioapplications.</jats:p>
  • Journal article
    Wu Y, Chau H-F, Thor W, Chan KHY, Ma X, Chan W-L, Long NJ, Wong K-Let al., 2021,

    Solid-phase peptide macrocyclization and multifunctionalization via dipyrrin construction

    , Angewandte Chemie International Edition, Vol: 60, Pages: 20301-20307, ISSN: 1433-7851

    We introduce a new and highly efficient synthetic protocol towards multifunctional fluorescent cyclopeptides by solid-phase peptide macrocyclization via dipyrrin construction, with full scope of proteinogenic amino acids and different ring sizes. Various bicyclic peptides can be created by dipyrrin-based crosslinking and double dipyrrin-ring formation. The embedded dipyrrin can be either transformed to fluorescent BODIPY and then utilized as cancer-selective targeted protein imaging probe in vitro, or directly employed as a selective metal sensor in aqueous media. This work provides a valuable addition to the peptide macrocyclization toolbox, and a blueprint for the development of multifunctional dipyrrin linkers in cyclopeptides for a wide range of potential bioapplications.
  • Journal article
    Jiang L, Mak H-N, Walter ERH, Wong W-T, Wong K-L, Long NJet al., 2021,

    A fluorescent probe for the discrimination of oxidation states of palladium

    , CHEMICAL SCIENCE, Vol: 12, Pages: 9977-9982, ISSN: 2041-6520
  • Journal article
    Chau H-F, Wu Y, Fok W-Y, Thor W, Cho WC-S, Ma P, Lin J, Mak N-K, Bunzli J-CG, Jiang L, Long NJ, Lung HL, Wong K-Let al., 2021,

    Lanthanide-Based Peptide-Directed Visible/Near-Infrared Imaging and Inhibition of LMP1

    , JACS AU, Vol: 1, Pages: 1034-1043
  • Journal article
    Farleigh M, Pham TT, Yu Z, Kim J, Sunassee K, Firth G, Forte N, Chudasama V, Baker JR, Long NJ, Rivas C, Ma MTet al., 2021,

    New Bifunctional Chelators Incorporating Dibromomaleimide Groups for Radiolabeling of Antibodies with Positron Emission Tomography Imaging Radioisotopes

    , BIOCONJUGATE CHEMISTRY, Vol: 32, Pages: 1214-1222, ISSN: 1043-1802
  • Journal article
    Boltersdorf T, Gavins FNE, Long NJ, 2021,

    Long-lived lanthanide emission <i>via</i> a pH-sensitive and switchable LRET complex

    , CHEMICAL SCIENCE, ISSN: 2041-6520

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Professor Nick Long
Email: n.long@imperial.ac.uk
Telephone: +44 (0)20 7594 5781

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501J
Molecular Sciences Research Hub
White City Campus

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