Discrete Heteropolynuclear Yb/Er Assemblies: Switching on Molecular Upconversion Under Mild Conditions DOI
Jie Wang, Yue Jiang,

Jiao‐Yang Liu

и другие.

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(41), С. 22368 - 22375

Опубликована: Авг. 12, 2021

Abstract The salts {[Ln 2 Ln*(Hhmq) 3 (OAc) (hfac) ] + [Ln*(hfac) (OAc)(MeOH)] − } (Hhmq=2‐methanolquinolin‐8‐oxide, hfac=hexafluoroacetylacetonate; Ln, Ln*=Er, Gd, Yb) feature a discrete heteronuclear cation consisting of two types lanthanide atoms. quinolinoxy O‐atom serves as μ ‐bridge to Ln atoms and all three atoms, with metal⋅⋅⋅metal distances being around 3.7 Å. For 1 ( [Yb Er] ), near‐infrared downshifted luminescence is switched competitive upconversion upon irradiation by 980 nm laser under an extremely low excitation power (0.288 W cm −2 ) through introduction fluoride ions. stability after addition was confirmed powder X‐ray diffraction multistage mass spectrometry, associated the H NMR 6 [La Eu] ). More importantly, at least 20‐fold enhancement quantum yield in non‐deuterated solvents room temperature densities (2 highest among few molecular examples reported.

Язык: Английский

Supramolecular cancer nanotheranostics DOI
Jiong Zhou, Lang Rao, Guocan Yu

и другие.

Chemical Society Reviews, Год журнала: 2021, Номер 50(4), С. 2839 - 2891

Опубликована: Янв. 1, 2021

Supramolecular cancer nanotheranostics have shown promising potentials in early-stage diagnosis and personal therapy. Herein, we summarize the progress of supramolecular provide guidance for designing new targeted theranostic agents.

Язык: Английский

Процитировано

348

Recent progress on molecularly near-infrared fluorescent probes for chemotherapy and phototherapy DOI
Chenxu Yan, Yutao Zhang,

Zhiqian Guo

и другие.

Coordination Chemistry Reviews, Год журнала: 2020, Номер 427, С. 213556 - 213556

Опубликована: Сен. 16, 2020

Язык: Английский

Процитировано

148

An Activatable Phototheranostic Probe for Anti‐hypoxic Type I Photodynamic‐ and Immuno‐Therapy of Cancer DOI Open Access
Min Zhao, Yuyang Zhang,

Jia Miao

и другие.

Advanced Materials, Год журнала: 2023, Номер 36(4)

Опубликована: Авг. 29, 2023

Photodynamic therapy (PDT), which utilizes type I photoreactions, has great potential as an effective cancer treatment because of its hypoxia-tolerant superiority over the commonly used II pathway. A few photosensitizers are exploited; however, they majorly induce cytotoxicity and possess poor tumor specificity low-efficient theranostics. To resolve this issue, herein aminopeptidase N (APN)-activated phototheranostic probe (CyA) is reported for anti-hypoxic PDT in conjunction with immunotherapy treatment. CyA can specifically activate near-infrared fluorescence, photoacoustic signals, phototoxicity following APN-induced substrate cleavage subsequent generation active molecules (such CyBr). endows specific imaging capabilities toward cells overexpressing APN under both normoxia hypoxia. In addition, locally activatable induces systemic antitumor immune responses. More importantly, integration localized activated evokes enhanced therapeutic effects improved inhibition efficiency live mice compared individual treatments. This study aims to present combination therapy.

Язык: Английский

Процитировано

65

De Novo Designed Ru(II) Metallacycle as a Microenvironment‐Adaptive Sonosensitizer and Sonocatalyst for Multidrug‐Resistant Biofilms Eradication DOI
Yuling Xu,

Yida Pang,

Lishi Luo

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(15)

Опубликована: Фев. 8, 2024

Abstract Albeit sonodynamic therapy (SDT) has achieved encouraging progress in microbial sterilization, the scarcity of guidelines for designing highly effective sonosensitizers and intricate biofilm microenvironment (BME), substantially hamper therapeutic efficacy against infections. To address bottlenecks, we innovatively design a Ru(II) metallacycle‐based sonosensitizer/sonocatalyst (named Ru‐A3‐TTD ) to enhance potency sonotherapy by employing molecular engineering strategies tailored BME. Our approach involves augmenting ’s production ultrasonic‐triggered reactive oxygen species (ROS), surpassing performance commercial sonosensitizers, through straightforward but potent π‐expansion approach. Within BME, synergistically amplifies sonotherapeutic via triple‐modulated approaches: (i) alleviation hypoxia, leading increased ROS generation, (ii) disruption antioxidant defense system, which shields from glutathione consumption, (iii) enhanced penetration, enabling deep sites. Notably, sono‐catalytically oxidizes NADPH, critical coenzyme involved defenses. Consequently, demonstrates superior eradication multidrug‐resistant Escherichia coli compared conventional clinical antibiotics, both vitro vivo. our knowledge, this study represents pioneering instance supramolecular sonosensitizer/sonocatalyst. It provides valuable insights into structure‐activity relationship paves promising pathway treatment

Язык: Английский

Процитировано

34

A Metal–Organic Framework Based on a Nickel Bis(dithiolene) Connector: Synthesis, Crystal Structure, and Application as an Electrochemical Glucose Sensor DOI
Yan Zhou, Qin Hu, Fei Yu

и другие.

Journal of the American Chemical Society, Год журнала: 2020, Номер 142(48), С. 20313 - 20317

Опубликована: Ноя. 13, 2020

Functionalizing the redox-active tetrathiafulvalene (TTF) core with groups capable of coordination to metals provides new perspectives on modulation architectures and electronic properties organic–inorganic hybrid materials. With a view extending this concept, we have now synthesized nickel bis(dithiolene-dibenzoic acid), [Ni(C2S2(C6H4COOH)2)2], which can be considered as inorganic analogue organic tetrathiafulvalene-tetrabenzoic acid (H4TTFTB). Likewise, [Ni(C2S2(C6H4COOH)2)2] is linker for functional metal–organic frameworks, demonstrated here synthesis [Mn2{Ni(C2S2(C6H4COO)2)2}(H2O)2]·2DMF, (1, DMF = N,N-dimethylformamide). 1 isomorphic reported [Mn2(TTFTB)(H2O)2] (2) but better electrochemical glucose sensor due multiple oxidation–reduction states [NiS4] core, allow oxidized glucolactone by high oxidation state center. As non-enzymatic sensor, Cu foam (CF), 1-CF, was one-step hydrothermal method exhibited an excellent performance. The fabricated 1-CF electrode offers sensitivity 27.9 A M–1 cm–2, wide linear detection range from 2.0 × 10–6 10–3 M, low limit 1.0 10–7 M (signal/noise 3), satisfactory stability reproducibility.

Язык: Английский

Процитировано

116

Coordination-Assembled Water-Soluble Anionic Lanthanide Organic Polyhedra for Luminescent Labeling and Magnetic Resonance Imaging DOI
Zhuo Wang, Lizhen He, Bingqing Liu

и другие.

Journal of the American Chemical Society, Год журнала: 2020, Номер 142(38), С. 16409 - 16419

Опубликована: Сен. 3, 2020

Lanthanide-containing functional complexes have found a variety of applications in materials science and biomedicine because their unique electroptical magnetic properties. However, the poor stability solubility water multicomponent lanthanide organic assemblies significantly limit practical applications. We report here series water-stable anionic Ln2nL3n-type (n = 2, 3, 4, 5) polyhedra (LOPs) constructed by deprotonation self-assembly three fully conjugated ligands (H4L1 H4L2a/b) featuring 2,6-pyridine bitetrazolate chelating moiety. The outcomes LOPs formation reactions were to be very sensitive toward reaction conditions including base, metal source, solvents, concentrations as characterized combination NMR, high-resolution ESI-MS X-ray crystallography. Ligands H4L2a/b manifested an excellent sensitization ions (Ln EuIII TbIII), with high luminescent quantum yields for Tb8L2a12 (Φ 11.2% water) Eu8L2b12 76.8% DMSO) measured polar solvents. Furthermore, due giant molecular weight rigidity polyhedral skeleton, Gd8L2b12 showed longitudinal relaxivity (r1) 400.53 mM-1S-1. performance potential resonance imaging contrast agents (CAs) vivo was evaluated much longer retention time tumor sites compared commercial GdIII-based CAs. Dual-modal has also been demonstrated mixed Eu/Gd LOPs. Our results not only provide new design route multinuclear but offer candidates supramolecular-edifices bioimaging drug delivery.

Язык: Английский

Процитировано

104

Single-atom replacement as a general approach towards visible-light/near-infrared heavy-atom-free photosensitizers for photodynamic therapy DOI Creative Commons
Juan Tang, Lushun Wang, Axel Loredo

и другие.

Chemical Science, Год журнала: 2020, Номер 11(26), С. 6701 - 6708

Опубликована: Янв. 1, 2020

Photodynamic therapy has become an emerging strategy for the treatment of cancer. This technology relies on development photosensitizers (PSs) that convert molecular oxygen to cytotoxic reactive species upon exposure light. In this study, we have developed a facile and general obtaining visible light/near-infrared-absorbing PSs by performing simple sulfur-for-oxygen replacement within existing fluorophores. Thionation carbonyl groups fluorophore cores leads improvement singlet quantum yield molar absorption coefficient at longer wavelengths (deep 600-800 nm). Additionally, these thio-based lack dark cytotoxicity but exhibit significant phototoxicity against monolayer cancer cells 3D multicellular tumor spheroids with IC50 in micromolar range. To achieve tumor-specific delivery, conjugated antibody demonstrated their therapeutic activity.

Язык: Английский

Процитировано

98

Metal Modulation: An Easy-to-Implement Tactic for Tuning Lanthanide Phototheranostics DOI
Mengliang Zhu, Hang Zhang, Guangliu Ran

и другие.

Journal of the American Chemical Society, Год журнала: 2021, Номер 143(19), С. 7541 - 7552

Опубликована: Май 11, 2021

Phototheranostics constitute an emerging cancer treatment wherein the core diagnostic and therapeutic functions are integrated into a single photosensitizer (PS). Achieving full potential of this modality requires being able to tune photosensitizing properties PS in question. Structural modification organic framework represents time-honored strategy for tuning photophysical features given system. Here we report easy-to-implement metal selection approach that allows fine-tuning excited-state energy dissipation phototheranostics as exemplified by set lanthanide (Ln = Gd, Yb, Er) carbazole-containing porphyrinoid complexes. Femto- nanosecond time-resolved spectroscopic studies, conjunction with density functional theory calculations, revealed pathways PSs highly dependent on gap between lowest triplet excited state ligand states coordinated Ln ions. The Yb complex displayed balance deactivation mechanisms made it attractive combined photoacoustic imaging photothermal/photodynamic therapy agent. It was encapsulated mesoporous silica nanoparticles (MSN) provide biocompatible construct, YbL@MSN, which displays high photothermal conversion efficiency (η 45%) decent singlet oxygen quantum yield (ΦΔ 31%). Mouse model studies YbL@MSN both synergistic photothermal- photodynamic-therapy-based tumor reduction vivo. Our results lead us suggest promising phototheranostics.

Язык: Английский

Процитировано

65

Lanthanide porphyrinoids as molecular theranostics DOI
Guoqing Jin, Calvin V. Chau, Jonathan F. Arambula

и другие.

Chemical Society Reviews, Год журнала: 2022, Номер 51(14), С. 6177 - 6209

Опубликована: Янв. 1, 2022

This Review summarises the history and ‘state-of-the-art’ development of lanthanide (Ln) porphyrinoids as theranostic agents. Applications such near-infrared (NIR) fluorescence imaging (FL), magnetic resonance (MRI), radiotherapy, chemotherapy phototheranostics will be discussed.

Язык: Английский

Процитировано

63

Photoresponsive Covalent Organic Frameworks with Diarylethene Switch for Tunable Singlet Oxygen Generation DOI

Nana Sun,

Yucheng Jin, Hailong Wang

и другие.

Chemistry of Materials, Год журнала: 2022, Номер 34(4), С. 1956 - 1964

Опубликована: Фев. 12, 2022

Incorporation of molecular switches with light, heat, and electricity responsibility into artificial solids has been developed as a successful strategy to construct stimuli-responsive functional materials. However, precise manipulation their geometries electronic structures control the properties macroscopic materials still remains fundamental challenge. Herein, photoresponsive covalent organic framework (o-COF) square lattice was fabricated from dynamic chemistry reaction ring-open dithienylethene–dialdehyde 5,10,15,20-tetrakis(4-aminophenyl)porphyrin (H2TAPP). UV irradiation dithienylethene-based units in o-COF afforded its reversible photoisomer (c-COF) ring-closed form. In addition range diffraction, microscopic, gas physical sorption characterizations, spectroscopic investigations help theoretical simulations revealed different photocatalytic activities toward evolution singlet oxygen corresponding oxidation amines due energy transfer pathways porphyrin unit BBTP photoisomers these two COFs. Most interestingly, such behaviors for COFs could be easily tuned manner by adjusting ring-closed/open form dithienylethene means visible light.

Язык: Английский

Процитировано

58