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A succession of erbium single-doped and erbium/ytterbium co-doped SrF2 nanoparticles (NPs) were fabricated via a hydrothermal synthesis technique followed by high-temperature calcination. Structural, morphology, and element information of SrF2 NPs were explored using X-ray diffraction (XRD), scanning electron microscopy (SEM) and energy dispersive X-ray spectroscopy (EDX) instruments. Under near-infrared (NIR) excitation, the SrF2:Er3+ NPs exhibit a prominent red emission peak (at 670 nm) as well as two oppositely faint green emission peaks (at 525 nm and 548 nm). The probable mechanism of the dominant red up-conversion luminescence (UCL) emission was systematically studied by UC emission spectroscopy, Raman spectroscopy, Fourier transform-infrared spectroscopy (FT-IR) and diffuse reflectance spectrum analyses. We used the energy gap law to estimate the probability of electronic transition, which determines the UCL emission route. The behavior of the R/G value (emission intensity of red to green ratio) and the slope n (the number of photons absorbed during the excitation process) reflected the existence of a highly efficient cross-relaxation (CR) effect during the UC process in the SrF2 system, so we can infer that the prominent red UCL emission is due to the CR effect among adjacent erbium atoms. After co-doping with ytterbium ions, the red UCL emission intensity is further enhanced. By comparing 2 mol% Er3+,5 mol% Yb3+ co-doped SrF2 samples with a similar composition without ytterbium doping, a red UCL emission intensity enhancement of about 200 times was observed. This increase is ascribed to the existence of effective energy transfer up-conversion (ETUC) from ytterbium to erbium, and the presence of a large absorption peak of ytterbium in the range of 830–1060 nm was observed in the diffuse reflectance spectrum, indicating that ytterbium's ability to absorb 980 nm photon energy is significantly stronger than erbium's. The strong red radiation obtained for erbium/ytterbium co-doped SrF2 NPs is expected to have potential application prospects in in vivo bio-imaging and photodynamic therapy.
Ultrathin two-dimensional (2D) nanosheets (NSs) have been widely explored as nanoagents for multimodal cancer therapies, such as photothermal therapy (PTT) combined with chemodynamic therapy (CDT). However, it is still a challenge to prepare 2D NSs with good performance in both CDT and NIR-II PTT. Here, we report the preparation of ultrathin 2D CuFe 2 S 3 NSs as an efficient nanoagent for synergistic CDT and NIR-II PTT to ablate cancer cells/tumors. Ultrathin 2D CuFe 2 S 3 NSs are first prepared by sulfurization of ultrathin CuFe-LDH NSs via a simple hydrothermal treatment. After modification with polyethylene glycol (PEG), the PEG-modified CuFe 2 S 3 NSs (CuFe 2 S 3 -PEG) show broadband NIR-II absorption and excellent photothermal conversion efficiency (~55.86%) at 1064 nm. Moreover, the overproduced glutathione in the tumor microenvironment can react with CuFe 2 S 3 -PEG NSs to release Fe 2+ and Cu + , thus activating Fenton reaction to efficiently produce hydroxyl radicals (·OH). Importantly, the photothermal effect of CuFe 2 S 3 -PEG could further synergistically improve the Fenton reaction by increasing the local temperature. In vitro and in vivo results reveal that the CuFe 2 S 3 -PEG has remarkable synergistic CDT/PTT antitumor activity. This study has proven that the metal chalcogenide NSs of CuFe 2 S 3 -PEG can be used as an efficient nanoagent for multimodal cancer therapies, which could also be promising in other applications like biosensors, drug delivery and antibacterial.
Exploring a combined phototherapeutic strategy to overcome the limitations of a single mode therapy and inducing high anticancer efficiency is highly promising for precision cancer nanomedicine. However, a single-wavelength laser activates dual photothermal/photodynamic therapy (PTT/PDT) treatment is still a formidable challenge. Herein, we strategically design and fabricate a multifunctional theranostic nanosystem based on chlorin e6-functionalized polydopamine (PDA) coated prussian blue/manganese dioxide nanoparticles (PB-MnO2@PDA-Ce6 NPs). Interestingly, the obtained PB-MnO2@PDA NPs not only offer an effective delivery system for Ce6 but also provide strong optical absorption in the near-infrared range, endowing high antitumor efficacy of PTT. More importantly, the as-prepared PB-MnO2@PDA-Ce6 nanoagents exhibit an effective oxygen generation, superior reactive oxygen species (ROS), and outstanding photothermal conversion ability to greatly improve PTT and PDT treatments. As a result, both in vitro and in vivo treatments guided by MR imaging on liver cancer cells reveal the complete cell/tumor eradication under a single wavelength of 660 nm laser irradiation, implying the simultaneous synergistic PDT/PTT effects triggered by PB-MnO2@PDA-Ce6 nanoplatform, which are much higher than individual treatment. Taken together, our phototherapeutic nanoagents exhibit an excellent therapeutic performance, which may act as a nanoplatform to find safe and clinically translatable routes to accelerate cancer therapeutics.
D2O plays important roles in a variety of fields (such as the nuclear industry and bioorganic analysis), and thus its isotopic purity (H2O contents) is highly concerned. Due to its highly similar physical properties to H2O and large excess amounts of H2O over D2O, it is challenging to distinguish D2O from H2O. On the basis of the characteristic NIR-II phosphorescence of singlet oxygen (1O2), and the fact that H2O is a more efficient quencher for 1O2 than D2O, here, we proposed to simply use the 1275 nm emission of 1O2 for the analysis of the isotopic purity of D2O. In normal cases (a xenon lamp for excitation), such steady-state emission is extremely weak for valid analytical applications, we thus employed laser excitation for intensification. To this goal, a series of photosensitizers were screened, and eventually polythiophene PT10 was selected with high singlet oxygen quantum yield (ΦΔ = 0.51), high H2O/D2O contrast, and excellent photostability. Upon excitation with a 445 nm laser, a limit of detection (LOD, 3σ) of 0.1% for H2O in D2O was achieved. The accuracy of the proposed method was verified by the analysis of the isotopic purity of several D2O samples (with randomly added H2O). More interestingly, the hygroscopicity of D2O was sensitively monitored with the proposed probe in a real-time manner; the results of which are important for strengthening the care of D2O storage and the importance of humidity control during related investigations. Besides D2O isotopic purity evaluation, this work also indicated the potential usefulness of the NIR-II emission of singlet oxygen in future analytical detection.
The development of ultraviolet to near-infrared (UV-Vis-NIR) responsive photocatalysts offers a unique opportunity for the full use of solar energy to solve the energy and the environmental problems. Here, successful preparation of a three-dimensional (3D) porous photocatalyst of graphitic carbon nitride quantum dot (CNQDs) modified g-C 3 N 4 /graphene oxide composite aerogel (CNGO/CNQDs) via hydrothermal and vacuum injection method was reported. In this unique ternary 3D photocatalyst, graphene oxide could improve the separation of photogenerated electrons and holes and promote the charge separation, while the aerogel's 3D network structure provided a rich active site. Simultaneously, due to the appropriate up-conversion performance of the nitrogen carbide quantum dots, CNGO/CNQDs achieved a light response from ultraviolet (UV) to near-infrared (NIR). These properties endow it with a good photocatalytic performance. The hydrogen production efficiency of CNGO/CNQDs reached 1231 μmol h −1 , which was 16 times more than that of matrix material . In addition, the apparent quantum yields (AQY) of CNGO/CNQDs at wavelengths of 420 nm and 700 nm were 13% and 0.116%, respectively.
Recently, the fluorescence detection of H 2 S in biological systems has attracted the attention of many analytical chemists. However, most of H 2 S probes showed shorter fluorescence emission (<600 nm) with fluorescence intensity change induced by H 2 S, which has some disadvantages of shallower tissue penetration and bigger autofluorescence interference. Herein, we have rationally designed a near-infrared and ratiometric fluorescent probe ( YC−1 ) for the detection of H 2 S based on isophorone. The detection process can be monitored by naked-eye. Addition of H 2 S, YC−1 showed that the emission ratios of fluorescence intensity at 540 and 660 nm (I540/I660) with an obvious enhancement from 0.05 to 13.3. Besides, the color of YC−1 changes from pink to yellow. As a probe for H 2 S, YC−1 exhibited better selectivity, better sensitivity and lower detection limits (0.17 μM). Moreover, YC−1 showed lower toxicity to HepG−2 cells and can be used for cell imaging .
Near-infrared (NIR) light responsive devices have attracted extensive scientific attention due to their wide range of applications in biomedical devices, soft robotics and wearable electronics. However, the easy fabrication of these devices and the corresponding shape memory materials is still a challenge. Herein, we synthesized a series of novel NIR-induced shape memory ionomers with multistage responsiveness using commercialized polymers as the framework and various metal ions as cross-linked junctions, which exhibit a high shape recovery ratio of over 93%. The light-induced shape memory properties of the ionomer can be freely tailored by merely adjusting the species and content of metal ions due to the specific photothermal effect of each ion. Moreover, the dynamic ionic cross-linked interaction also causes light-induced plasticity, leading to repeatable programming of these ionomers to new permanent shapes without sacrificing their shape memory properties. The combination of these ionomers containing different bridge ions is able to achieve light-induced multistage shape modulation, which was further used to fabricate several devices, such as light-operated actuators and switches, demonstrating their versatile application potential in various fields.
The design and preparation of novel liquid crystalline elastomers (LCEs) are highly desirable for the development of smart soft materials with quick stimuli-responsive characteristics. In this work, we present a facile preparation strategy of near infrared (NIR)-responsive gold nanorod/liquid crystalline elastomer (GNR/LCE) composite films exhibiting fascinating re-shapeable and reusable properties. A random side-chain liquid crystalline copolymer containing biphenyl mesogens and cinnamate side groups has been prepared via ring-opening metathesis polymerization (ROMP), with the [2+2] (retro)cycloaddition of cinnamate groups triggered by various wavelength UV light serving as the reversible dynamic crosslinks for the construction of re-shapeable LCEs. The GNR/LCE composite films with uniformly doped monodisperse GNRs demonstrate remarkable photothermal effects and multi-mode NIR-driven macroscopic deformation capabilities. Furthermore, a single-layer dual-phase composite film composed of periodic micro-patterned monodomain (M) and polydomain (P) structures has been fabricated, which is promising for precise localized NIR-responsive actuation and fully photo-controlled LCE composite devices.
Herein, an NIR-responsive polymeric microneedle (MN) system incorporated with metformin-loaded and polydopamine/lauric-acid-coated (PDA/LA-coated) hollow mesoporous SiO2 has been developed for transdermal delivery of antidiabetic drug (metformin). First, an antidiabetic drug was loaded within hollow mesoporous SiO2 nanoparticles (HMSNs) by a diffusion method. Then, PDA as photothermal conversion agent and lauric acid (LA) as phase change material (PCM) were coated onto the HMSN to form NIR-responsive drug nanocarriers. Finally, these metformin-loaded and PDA/LA-coated HMSNs were encapsulated into poly(vinylpyrrolidone) (PVP) MNs. After insertion into skin tissue, LA could melt with the photothermal conversion of PDA under NIR light, thus enabling release of encapsulated metformin from MNs. The in vivo release behavior of metformin from MNs into skin was further studied to investigate its hypoglycemic effect on diabetic rats. Compared with the subcutaneous injection of metformin, the bioavailability of MN–NIR groups was 95.8 ± 2.7%. The antidiabetic drug can be precisely released by adjustment of exposure time and power densities of NIR light.
The combination therapy has exhibited important potential for the treatment of cancers, especially for drug-resistant cancers. In this report, bi-functional nanoprobes based on doxorubicin (DOX)-loaded NaYF 4 :Yb/Tm–TiO 2 inorganic photosensitizers (FA-NPs-DOX) were synthesized for in vivo near infrared (NIR)-triggered inorganic photodynamic therapy (PDT) and enhanced chemotherapy to overcome the multidrug resistance (MDR) in breast cancers. Using the up-conversion luminescence (UCL) performance of NaYF 4 :Yb/Tm converting near-infrared (NIR) into ultraviolent (UV) lights, reactive oxygen species (ROS) were triggered from TiO 2 inorganic photosensitizers for PDT under the irradiation of a 980 nm laser, by which the deep-penetration and low photo-damage could be reached. Moreover, nanocarrier delivery and folic acid (FA) targeting promoted the cellular uptake, and accelerated the release of DOX in drug-sensitive MCF-7 and resistant MCF-7/ADR cells. The toxicity assessment in vitro and in vivo revealed the good biocompatibility of the as-prepared FA-NPs-DOX nanocomposites . By the combination of enhanced chemotherapy and NIR-triggered inorganic PDT, the viability of MCF-7/ADR cells could decrease by 53.5%, and the inhibition rate of MCF-7/ADR tumors could increase up to 90.33%, compared with free DOX. Therefore, the MDR of breast cancers could be obviously overcome by enhanced chemotherapy and NIR-triggered inorganic PDT of FA-NPs-DOX nanocomposites under the excitation of a 980 nm laser.
Metal oxides are receiving an incremental attention in recent years for their potential applications in ablation of cancer cells due to their efficient photothermal conversion and good biocompatibility, but the large sizes and poor photo-stability will seriously limit their practical application. Herein, hydrous RuO2 nanoparticles were synthesized by a facile hydrothermal treatment and surface-modified with polyvinylpyrrolidone (PVP) coating. PVP-coated RuO2 nanoparticles exhibit a well dispertion in saline solution, strong characteristic plasmonic absorption in NIR region, enhanced photothermal conversion efficiency of 54.8% and remarkable photo-stability under the irridation of an 808 nm laser. The nanoparticles were further employed as a new photothermal ablation agent for cancer cells which led rapidly to cellular deaths both in vitro and in vivo.
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