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Journal articleLi L, Lu X, He Q, et al., 2025,
NADPH-Independent Fluorescent Probe for Live-Cell Imaging of Heme Oxygenase-1.
, ACS Sens, Vol: 10, Pages: 499-506Heme oxygenase-1 (HO-1) catalyzes heme degradation on the consumption of NADPH and molecular oxygen. As an inducible enzyme, HO-1 is highly induced in various disease states, including cancer. Currently, two fluorescent probes for HO-1 have been designed based on the catalytic activity of HO-1, in which the probes serve as a substrate, so NADPH is required to enable the detection. Probes functioning in a NADPH-dependent way may influence other NADPH-consuming pathways, as all these pathways share a common NADPH pool. Here, we report the peptide-based fluorescent probe NBD-P5 as a simple alternative approach for HO-1 sensing. The designed probe NBD-P5 functions independently of the catalytic activity of HO-1, therefore enabling fast and sensitive detection of HO-1 with no requirements of other substances, including NADPH and biliverdin reductase. Moreover, it overcomes the need for a large substrate amount and long incubation time during the detection. NBD-P5 can be quickly taken up by cells, demonstrates an excellent colocalization with the endoplasmic reticulum (where HO-1 is mainly located), and is shown to be reliable in reporting changes in HO-1 levels in live cells. This work provides a simple alternative approach for designing HO-1 fluorescent probes, and we expect it will act as a practical tool for further studying HO-1 biology.
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Journal articleWoolley B, Wu Y, Xiong L, et al., 2025,
Lanthanide-tetrazine probes for bio-imaging and click chemistry.
, Chem Sci, ISSN: 2041-6520The blood-brain-barrier prevents many imaging agents and therapeutics from being delivered to the brain that could fight central nervous system diseases such as Alzheimer's disease and strokes. However, techniques such as the use of stapled peptides or peptide shuttles may allow payloads through, with bioconjugation achieved via bio-orthogonal tetrazine/norbornene click chemistry. A series of lanthanide-tetrazine probes have been synthesised herein which could be utilised in bio-orthogonal click chemistry with peptide-based delivery systems to deliver MRI agents through the blood-brain-barrier. The Gd complexes show higher relaxivities than the clinical standard of Gd(DOTA) at 1.4 T and phosphorescence is observed from the Eu and Tb complexes via tetrazine sensitization, with supporting in vitro cytotoxicity and cell imaging. A bio-orthogonal click reaction between a Gd-tetrazine complex and a cyclic-RGD-norbornene conjugate was successful and the resulting clicked probe demonstrated enhanced relaxivity and could potentially act as a peptide shuttle for the Gd MRI agent.
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Journal articleVanin F, Tremlett WDJ, Gao D, et al., 2025,
Modulating Perovskite Surface Energetics Through Tuneable Ferrocene Interlayers for High-Performance Perovskite Solar Cells.
, Angew Chem Int Ed EnglAchieving rational control over chemical and energetic properties at the perovskite/electron transport layer (ETL) interface is crucial for realizing highly efficient and stable next-generation inverted perovskite solar cells (PSCs). To address this, we developed multifunctional ferrocene (Fc)-based interlayers engineered to exhibit adjustable passivating and electrochemical characteristics. These interlayers are designed to reduce non-radiative recombination, and to modulate the work function (WF) and uniformity of the perovskite surface, thereby enhancing device performance. The key role played by the highest occupied molecular orbital energies (EHOMO) of the Fc compounds relative to the perovskite valance band maximum (EVBM) is revealed. This relationship is pivotal in controlling band bending and optimizing charge extraction. Notably, the conformationally flexible and more easily oxidized ferrocenyl-bis-furyl-2-carboxylate (2) is found to more effectively bind with undercoordinated Pb2+ surface sites and modulate interfacial energetics, resulting in inverted PSCs achieving champion efficiencies of 25.16 %. These cells also displayed excellent stability, retaining >92 % of the initial efficiency after 1,000 h of maximum power point operation at 65 °C. By correlating the broadly tunable Fc-EHOMO with a decreased and homogenized perovskite surface WF, our work advances our understanding of Fc-based interlayers and opens new pathways for their application in high-efficiency solar technologies.
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Journal articleYeung YH, Lam PL, Thor W, et al., 2025,
An Efficient Solid-Phase Synthetic Approach to Prepare TACN-Functionalized Peptides
, Chemistry-Methods1,4,7-triazacyclononane (TACN) derivatives play important roles in various metal-based biomedical applications. However, the unmanageable functionalization of TACN remains a long-standing challenge to yield useful partially substituted building blocks. Herein, by utilizing nitrobenzoxadiazole (NBD) as a thiol-liable protecting group for secondary amines, a bis-NBD-substituted TACN was obtained as the first example in the preparation of partially substituted TACN without strict stoichiometric control and column chromatography. Upon facile deprotection of NBD using solid-phase synthesis, a series of TACN-peptide conjugates with different bioactive peptides and chelating units were derivatized from the TACN building block, demonstrating the potential widespread application of this work.
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Journal articleYue TTC, Teh JH, Aboagye E, et al., 2024,
Site-specific π-clamp-mediated radiosynthesis of <SUP>68</SUP>Ga and <SUP>18</SUP>F PET radiopharmaceuticals
, CHEMICAL COMMUNICATIONS, ISSN: 1359-7345 -
Journal articleWilson LE, Yue TTC, Inkpen MS, et al., 2024,
Controlling quantum interference patterns in redox-active rings
, JOURNAL OF ORGANOMETALLIC CHEMISTRY, Vol: 1022, ISSN: 0022-328X -
Journal articleWalter ERH, Leung PK-K, Lee LC-C, et al., 2024,
Potent BODIPY-based photosensitisers for selective mitochondrial dysfunction and effective photodynamic therapy
, JOURNAL OF MATERIALS CHEMISTRY B, Vol: 12, Pages: 10409-10415, ISSN: 2050-750X -
Journal articleGao D, Li B, Liu Q, et al., 2024,
Long-term stability in perovskite solar cells through atomic layer deposition of tin oxide.
, Science, Vol: 386, Pages: 187-192Robust contact schemes that boost stability and simplify the production process are needed for perovskite solar cells (PSCs). We codeposited perovskite and hole-selective contact while protecting the perovskite to enable deposition of SnOx/Ag without the use of a fullerene. The SnOx, prepared through atomic layer deposition, serves as a durable inorganic electron transport layer. Tailoring the oxygen vacancy defects in the SnOx layer led to power conversion efficiencies (PCEs) of >25%. Our devices exhibit superior stability over conventional p-i-n PSCs, successfully meeting several benchmark stability tests. They retained >95% PCE after 2000 hours of continuous operation at their maximum power point under simulated AM1.5 illumination at 65°C. Additionally, they boast a certified T97 lifetime exceeding 1000 hours.
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Journal articleXie C, Li X, Zhang L, et al., 2024,
Bimetallic porphyrin PET radiotracers for Low-Dose MRI contrast enhancement
, CHEMICAL ENGINEERING JOURNAL, Vol: 495, ISSN: 1385-8947 -
Journal articleMann P, Fairclough SM, Bourke S, et al., 2024,
Interface Engineering of Water-Dispersible Near-Infrared-Emitting CuInZnS/ZnSe/ZnS Quantum Dots
, CRYSTAL GROWTH & DESIGN, Vol: 24, Pages: 6275-6283, ISSN: 1528-7483 -
Journal articleLi B, Gao D, Sheppard SA, et al., 2024,
Highly efficient and scalable p-i-n perovskite solar cells enabled by poly-metallocene interfaces
, Journal of the American Chemical Society, Vol: 146, Pages: 13391-13398, ISSN: 0002-7863Inverted p-i-n perovskite solar cells (PSCs) are easy to process but need improved interface characteristics with reduced energy loss to prevent efficiency drops when increasing the active photovoltaic area. Here, we report a series of poly ferrocenyl molecules that can modulate the perovskite surface enabling the construction of small- and large-area PSCs. We found that the perovskite-ferrocenyl interaction forms a hybrid complex with enhanced surface coordination strength and activated electronic states, leading to lower interfacial nonradiative recombination and charge transport resistance losses. The resulting PSCs achieve an enhanced efficiency of up to 26.08% for small-area devices and 24.51% for large-area devices (1.0208 cm2). Moreover, the large-area PSCs maintain >92% of the initial efficiency after 2000 h of continuous operation at the maximum power point under 1-sun illumination and 65 °C.
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Journal articleWalter ERH, Lee LC-C, Leung PK-K, et al., 2024,
Mitochondria-targeting biocompatible fluorescent BODIPY probes
, Chemical Science, Vol: 15, Pages: 4846-4852, ISSN: 2041-6520An increase in the mitochondrial membrane potential (MMP) is a characteristic feature of cancer and cardiovascular disease. Therefore, it remains of crucial importance to develop new and improved fluorescent probes that are sensitive to the MMP, to report on mitochondrial health and function. Reported here are the design, synthesis, photophysical properties and biological characterisation of a series of BODIPY dyes, BODIPY-Mito-n, for mitochondria-targeted fluorescence imaging applications. Six BODIPY-Mito-n analogues were synthesised under mild conditions, and displayed excellent fluorescence quantum yields of between 0.59 and 0.72 in aqueous environments at physiological pH (pH = 7.4). The incorporation of poly(ethylene glycol) (PEG) chains to the triarylphosphonium cation moiety significantly improved the biocompatibility of the probes (BODIPY-Mito-6, IC50 > 50 μM). All BODIPY-Mito-n compounds demonstrated a high MMP-sensitive localisation in the mitochondria, with Pearson's correlation coefficients (PCC) of between 0.76 and 0.96. Compounds BODIPY-Mito-2 and BODIPY-Mito-6 revealed the highest sensitivity to the MMP, with a decrease in the emission intensity of 62% and 75%, respectively following MMP depolarisation. It is anticipated that the highest MMP sensitivity and enhanced biocompatibility of BODIPY-Mito-6 could lead to the development of new probes for mitochondrial imaging in the future.
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Journal articleBennett TLR, Long NJ, 2023,
A convenient synthesis of ferrocene-(ethynylphenyl)thioacetates
, DALTON TRANSACTIONS, Vol: 52, Pages: 16465-16471, ISSN: 1477-9226 -
Journal articleYue TTC, Ge Y, Aprile FA, et al., 2023,
Site-Specific <SUP>68</SUP>Ga Radiolabeling of Trastuzumab Fab via Methionine for ImmunoPET Imaging
, BIOCONJUGATE CHEMISTRY, ISSN: 1043-1802 -
Journal articleAboagye E, Teh JH, Amgheib A, et al., 2023,
Evaluation of [18F]AlF-EMP-105 for molecular imaging of 2 C-Met
, Pharmaceutics, Vol: 15, Pages: 1-13, ISSN: 1999-4923C-Met is a receptor tyrosine kinase that is overexpressed in a range of different cancer types, and has been identified as a potential biomarker for cancer imaging and therapy. Previously, a 68Ga-labelled peptide, [68Ga]Ga-EMP-100, has shown promise for imaging c-Met in renal cell carcinoma in humans. Herein, we report the synthesis and preliminary biological evaluation of an [18F]AlF-labelled analogue, [18F]AlF-EMP-105, for c-Met imaging by positron emission tomography. EMP-105 was radiolabelled using the aluminium-[18F]fluoride method with 46 ± 2% RCY and >95% RCP in 35–40 min. In vitro evaluation showed that [18F]AlF-EMP-105 has a high specificity for c-Met-expressing cells. Radioactive metabolite analysis at 5 and 30 min post-injection revealed that [18F]AlF-EMP-105 has good blood stability, but undergoes transformation—transchelation, defluorination or demetallation—in the liver and kidneys. PET imaging in non-tumour-bearing mice showed high radioactive accumulation in the kidneys, bladder and urine, demonstrating that the tracer is cleared predominantly as [18F]fluoride by the renal system. With its high specificity for c-Met expressing cells, [18F]AlF-EMP-105 shows promise as a potential diagnostic tool for imaging cancer.
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Contact
Professor Nick Long
Email: n.long@imperial.ac.uk
Telephone: +44 (0)20 7594 5781
Location
501J
Molecular Sciences Research Hub
White City Campus