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Probes for detecting phosphate ions (Pi) are required for environmental monitoring and to protect human health. Here, novel ratiometric luminescent lanthanide coordination polymer nanoparticles (CPNs) were successfully prepared and used to selectively and sensitively detect Pi. The nanoparticles were prepared from adenosine monophosphate (AMP) and Tb 3+ , and lysine (Lys) was used as a sensitizer (through the antenna effect) to switch on Tb 3+ luminescence at 488 and 544 nm while Lys luminescence at 375 nm was quenched because of energy transfer from Lys to Tb 3+ . The complex involved is here labeled AMP-Tb/Lys. Pi destroyed the AMP-Tb/Lys CPNs and therefore decreased the AMP-Tb/Lys luminescence intensity at 544 nm and increased the luminescence intensity at 375 nm at an excitation wavelength of 290 nm, meaning ratiometric luminescence detection was possible. The ratio between the luminescence intensities at 544 and 375 nm ( I 544 / I 375 ) was strongly associated with the Pi concentration between 0.1 and 6.0 μM, and the detection limit was 0.08 μM. The dual-emission reverse-change ratio luminescence sensing method can exclude environmental effects, so the proposed assay was found to be very selective. The method was successfully used to detect Pi in real water samples, and acceptable recoveries were found, suggesting that the method could be used in practice to detect Pi in water samples.

Fluorescent silver coordination polymer nanoparticles (Ag-TPA CPNs) were synthesized using a combination of terephthalic acid (TPA) and silver nitrate via an ultrarapid microwave-assisted strategy within 15 min. The Ag-TPA CPNs displayed a high fluorescent quantum yield (QY = 20.19%) and large Stokes shift (~200 nm), with two emission peaks at 490 nm and 520 nm under an excitation wavelength of 320 nm. A fluorescent “turn-off” method using fluorescent Ag-TPA CPNs was applied to detect the alkaline phosphatase (ALP) activity on the basis of the ALP-catalyzed hydrolysis of ascorbic acid 2-phosphate (AA2P) to ascorbic acid (AA), and the AA product triggered the reduction of Ag+ ions into silver nanoparticles. The fluorescent lifetime of Ag-TPA CPNs decreased from 3.93 ms to 3.80 ms after the addition of ALP, which suggests that this fluorescent “turn-off” detection of ALP activity is a dynamic quenching process. The fluorescent intensity had a linear relationship with the concentration of ALP in the range of 0.2–12 mU/mL (r = 0.991) and with a limit of detection (LOD) of 0.07 mU/mL. It showed high selectivity in ALP detection towards metal ions and amino acids, as well as other enzymes such as horseradish peroxidase, glucose oxidase, tyrosinase, trypsin, lysozyme, and superoxides. When it was applied for the fluorescent “turn-off” detection of ALP activity in serum samples, mean recovery levels ranging from 99.5% to 101.2% were obtained, with relative standard deviations (RSDs) lower than 4% accuracy. Therefore, it is an efficient and accurate tool for analyzing ALP levels in biosamples.

A new method based on coordination polymer nanoparticles (CPNs) derived from nucleotides and Tb 3+ ions (GMP/Tb) for the selective and sensitive determination of aqueous 2,4,6-trinitrophenol (TNP) (picric acid) is established. The fluorescence of GMP/Tb nanoparticles is effectively quenched by TNP via photo-induced charge transfer (PCT), thus achieving its selectivity toward TNP over other nitroaromatic explosives. The decreased fluorescence of GMP/Tb shows a good linear relationship to the concentrations of TNP ranging from 5.0 to 40.0 μM, and the limit of detection is 26.0 nM (5.96 ppb). The proposed GMP/Tb probe also achieves satisfactory results in real samples. The obtained recoveries of this method in river water samples are in the range 93.15–106.10%. The relative standard deviation (RSD) are 0.57 to 1.01% based on three repeated determinations. This fabricated detector provides a feasible path for determination of ppb-level TNP in natural water samples, which can help humans to avoid TNP-contaminated drinking water. Graphical abstract

A fluorometric method is described for the determination of thrombin. Polymer nanoparticles containing the luminol-terbium(III) complex (luminol-Tb) were prepared where luminol acts as the bridging ligand, and Tb(III) acts as the central metal ion. Thrombin possesses a large number of electrons donating groups that coordinate with luminol-Tb. Following coordination, the rigidity of the linker is increased, and this decreases the non-radiative decay rate and induces an increase in fluorescence intensity at 430 nm. Hence, thrombin can be fluorometrically determined. The detection limit of thrombin is as low as 3.5 pM (at an SNR of 3). This is about 10 times lower than assays using an aptamer. The method was applied in the determination of thrombin in human serum via the standard addition method and gave satisfying results. Graphical abstract Schematic representation of the preparation of the luminol-Tb(III) complex in a nanoparticle host by the self-assembly of luminol and Tb(III) ions. Thrombin readily coordinates with the luminol-Tb(III) system, and this results in particle aggregation. The blue fluorescence of luminol increases strongly, and this effect provides the basis for fluorometric determination of thrombin.

BackgroundDrug-resistant bacterial infections in chronic wounds are a persistent issue, as they are resistant to antibiotics and can cause excessive inflammation due to generation of reactive oxygen species (ROS). An effective solution would be to not only combat bacterial infections but also scavenge ROS to relieve inflammation at the wound site. Scaffolds with antioxidant properties are attractive for their ability to scavenge ROS, and there is medical demand in developing antioxidant enzyme-mimicking nanomaterials for wound healing.MethodsIn this study, we fabricated copper-coordination polymer nanoparticles (Cu-CPNs) through a self-assembly process. Furthermore, ε-polylysine (EPL), an antibacterial and cationic polymer, was integrated into the Cu-CPNs structure through a simple one-pot self-assembly process without sacrificing the glutathione peroxidase (GPx) and superoxide dismutase (SOD)-mimicking activity of Cu-CPNs.ResultsThe resulting Cu-CPNs exhibit excellent antioxidant propertiesin mimicking the activity of glutathione peroxidase and superoxide dismutase and allowing them to effectively scavenge harmful ROS produced in wound sites. The in vitro experiments showed that the resulting Cu-CPNs@EPL complex have superior antioxidant properties and antibacterial effects. Bacterial metabolic analysis revealed that the complex mainly affects the cell membrane integrity and nucleic acid synthesis that leads to bacterial death.ConclusionsThe Cu-CPNs@EPL complex has impressive antioxidant properties and antibacterial effects, making it a promising solution for treating drug-resistant bacterial infections in chronic wounds. The complex’s ability to neutralize multiple ROS and reduce ROS-induced inflammation can help relieve inflammation at the wound site.

Acid phosphatase has become a significant indicator of prognostic and medical diagnosis, and its dysfunction may lead to a series of diseases. A novel dual-signal fluorescence method for acid phosphatase detection based on europium polymer (europium-pyridine dicarboxylicacid-adenine) and pyridoxal phosphate (PLP) was proposed. PLP coordinated with europium polymer via Eu3+ and P–O bonds, and the fluorescence of europium polymer was quenched due to the photoinduced electron transfer (PET) effect between aldehyde and europium polymer. Upon addition of acid phosphatase, the PLP was transformed to phosphate (Pi) and pyridoxal (PL). The PL was released from the surface of europium polymer, and the blue emission was enhanced due to the formation of internal hemiacetal, while the fluorescence of europium polymer recovered. The blue (PL) and red emission (Eu3+) were positively correlated with acid phosphatase activity; thus the sensitive assay of acid phosphatase was effectively achieved. The two signals were applied to determine the acid phosphatase with limits of detection (LOD) of 0.04 mU/mL and 0.38 mU/mL, and the linear ranges were 0.13–5.00 mU/mL and 1.25–20.00 mU/mL, respectively. The probe can be used to trace the acid phosphatase in biological systems and holds promise for use in clinical diagnosis and early prevention.

A fluorescence quenching enhanced immunoassay has been developed to achieve ultrasensitive recognition of human epididymal 4 (HE4) modifying the fluorescence quencher. The carboxymethyl cellulose sodium-functionalized Nb 2 C MXene nanocomposite (CMC@MXene) was firstly introduced to quench the fluorescence signal of the luminophore Tb-Norfloxacin coordination polymer nanoparticles (Tb-NFX CPNPs). The Nb 2 C MXene nanocomposite as fluorescent nanoquencher inhibits the electron transfer between Tb and NFX to quench the fluorescent signal by coordinating the strongly electronegative carboxyl group on CMC with Tb (III) of Tb-NFX complex. Simultaneously, due to the superior photothermal conversion capability of CMC@MXene, the fluorescence signal has been further weakened by the photothermal effect driven non-radiative decay of the excited state under near-infrared laser irradiation. The constructed fluorescent biosensor based on CMC@MXene probe finally realized the enhanced fluorescence quenching effect, and achieved ultra-high sensitivity and selective detection of HE4, exhibiting a wide linear relationship with HE4 concentration on the logarithmic axis in the range of 10 −5 to 10 ng/mL and a low detection limit of 3.3 fg/mL (S/N = 3). This work not only provides an enhanced fluorescent signal quenching method for the detection of HE4, but also provides novel insights for the design of fluorescent sensor toward different biomolecules. Graphical Abstract

Green light photoactive Ru-based coordination polymer nanoparticles (CPNs), with chemical formula [[Ru(biqbpy)]1.5(bis)](PF6)3 (biqbpy = 6,6′-bis[N-(isoquinolyl)-1-amino]-2,2′-bipyridine; bis = bis(imidazol-1-yl)-hexane), were obtained through polymerization of the trans-[Ru(biqbpy)(dmso)Cl]Cl complex (Complex 1) and bis bridging ligands. The as-synthesized CPNs (50 ± 12 nm diameter) showed high colloidal and chemical stability in physiological solutions. The axial bis(imidazole) ligands coordinated to the ruthenium center were photosubstituted by water upon light irradiation in aqueous medium to generate the aqueous substituted and active ruthenium complexes. The UV-Vis spectral variations observed for the suspension upon irradiation corroborated the photoactivation of the CPNs, while High Performance Liquid Chromatography (HPLC) of irradiated particles in physiological media allowed for the first time precisely quantifying the amount of photoreleased complex from the polymeric material. In vitro studies with A431 and A549 cancer cell lines revealed an 11-fold increased uptake for the nanoparticles compared to the monomeric complex [Ru(biqbpy)(N-methylimidazole)2](PF6)2 (Complex 2). After irradiation (520 nm, 39.3 J/cm2), the CPNs yielded up to a two-fold increase in cytotoxicity compared to the same CPNs kept in the dark, indicating a selective effect by light irradiation. Meanwhile, the absence of 1O2 production from both nanostructured and monomeric prodrugs concluded that light-induced cell death is not caused by a photodynamic effect but rather by photoactivated chemotherapy.

Advanced colorectal cancer is one of the deadliest cancers, with a 5-year survival rate of only 12% for patients with the metastatic disease. Checkpoint inhibitors, such as the antibodies inhibiting the PD-1/PD-L1 axis, are among the most promising immunotherapies for patients with advanced colon cancer, but their durable response rate remains low. We herein report the use of immunogenic nanoparticles to augment the antitumour efficacy of PD-L1 antibody-mediated cancer immunotherapy. Nanoscale coordination polymer (NCP) core-shell nanoparticles carry oxaliplatin in the core and the photosensitizer pyropheophorbide-lipid conjugate (pyrolipid) in the shell (NCP@pyrolipid) for effective chemotherapy and photodynamic therapy (PDT). Synergy between oxaliplatin and pyrolipid-induced PDT kills tumour cells and provokes an immune response, resulting in calreticulin exposure on the cell surface, antitumour vaccination and an abscopal effect. When combined with anti-PD-L1 therapy, NCP@pyrolipid mediates regression of both light-irradiated primary tumours and non-irradiated distant tumours by inducing a strong tumour-specific immune response. Blockade of PD-L1 is usually not very effective in colon cancer patients. Here, the authors show the efficacy of PD-L1 blockade in combination with coordination polymer nanoparticles carrying oxaliplatin and a photosensitizer to induce anti-tumor immunity in metastatic models of colon cancer.

Radiation therapy can potentially induce immunogenic cell death, thereby priming anti-tumor adaptive immune responses. However, radiation-induced systemic immune responses are very rare and insufficient to meet clinical needs. Here, we demonstrate a synergetic strategy for boosting radiation-induced immunogenic cell death by constructing gadolinium-hemin based nanoscale coordination polymers to simultaneously perform X-ray deposition and glutathione depletion. Subsequently, immunogenic cell death is induced by sensitized radiation to potentiate checkpoint blockade immunotherapies against primary and metastatic tumors. In conclusion, nanoscale coordination polymers-sensitized radiation therapy exhibits biocompatibility and therapeutic efficacy in preclinical cancer models, and has the potential for further application in cancer radio-immunotherapy. Radiotherapy has the potential to induce immunogenic cell death (ICD), however radiation-induced immune responses are often limited. Here the authors design gadolinium-based nanoscale coordination polymers to amplify radiation-mediated oxidative stress, promoting ICD and anti-tumor immune responses.