ACS Nano
·
2024
·
IF 15.8
Yufeng Sun,Fei Qu,Rui Geng,Wanyue Xiao,Duohang Bi,Bijin Xiong,Yijing Liu,Jintao Zhu,Xiaoyuan Chen
The precise control of the assembly structure and size of gold nanoclusters (AuNCs) can potentially amplify their near-infrared II (NIR-II) fluorescence imaging and targeting properties. However, the conventional electrostatic assembly of AuNCs and charged molecules faces challenges in balancing the inherent electrostatic repulsions among charged units and regulating the diffusion of assembly units. These difficulties limit precise control over assembly size and structure, along with limited options for coassembled molecules, thereby restricting imaging properties and targeting capability. To circumvent this challenge, we developed a reverse emulsion-confined electrostatic assembly method. This technique efficiently constructs AuNC nanoassemblies with diverse coassembled molecules, allowing for the fine-tuning of assembly size and structure, including both core–satellite and homogeneous AuNC nanoassemblies. The development of two distinct nanoassemblies can be partially attributed to the varying diffusive rates of AuNCs or the AuNCs/polymer complex within the fused emulsion droplets. This variance arises from steric hindrances encountered during the emulsion fusion process. Interestingly, core–satellite nanoassemblies exhibit the strongest NIR-II fluorescence enhancement. Finally, the introduction of a hyaluronic acid coating on the surfaces of nanoassemblies with varying sizes enables the nanoprobes to achieve enhanced lymph node imaging through size modulation and macrophage targeting, which are used for surgical navigation to remove lymph node metastases. We envision that this self-assembly strategy can be extended to a wide range of electrostatic assembly systems for the development of multicomponent functional materials.
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Advanced Healthcare Materials
·
2024
·
IF 10
Jianshuai Bao,Zengyin Li,Deliang Wang,Jiefei Wang,Guan Huang,Jianlei Qian,Xiaoyan Yang,Peng-Cheng Duan,Sheng Zhang,Feng Bai,Yong Zhong
Near-infrared second region (NIR-II) fluorescence imaging provides enhanced tissue penetration, achieving efficient NIR-II fluorescence and photoacoustic imaging (PA)-guided photothermal therapy (PTT) all in one material remains a challenging yet promising approach in cancer treatment. Herein, open-shell V═O metalloradical complex (VONc) is self-assembled into VONc nanospheres (VONc NPs). VONc NPs exhibit light absorption from 300 to 1400 nm, fluorescence spectra ranging from 900 to 1400 nm, and a distinct fluorescence signal even at 1550 nm. Moreover, VONc NPs exhibit outstanding photostability and a higher photothermal conversion efficiency of 46.6% than that of closed-shell zinc naphthalocyanine nanorods (ZnNc NRs). V═O centered metalloradical serves as transient electron-withdrawing groups to facilitate charge transfer (CT), introducing additional nonradiative energy dissipation pathways and enhancing efficient heat generation. In vitro experiments of VONc NPs indicate that a highly effective photothermal action causes harm to both mitochondria and lysosomes, resulting in the death of tumor cells, closed-shell ZnNc NPs exhibit almost no cell killing as contrast. In vivo anti-tumor therapy results of VONc NPs demonstrate excellent NIR-II fluorescence imaging-guided PTT against tumors with a favorable biosafety profile. “Centered metalloradical boosting CT” toward open-shell metal complexes provides significant insight for developing single-material integrated nanosystems for diagnostic and therapeutic applications.
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ACS Applied Nano Materials
·
2024
·
IF 5.3
Xiang Meng,Xiaolong Jing,Jiang Cheng,Hua Tang,Xihao Chen,Xianju Zhou,Lu Li
Phase control of nanomaterials, determined by thermodynamic or kinetic conditions, is essential to sulfides’ characteristics, offering opportunities for exploring advanced applications in the field of optoelectronics. However, the one-step, high-yield, and defect-free synthesis of phase-pure nanoscale sulfides remains challenging. In this work, the low-cost solvothermal process enabled precise regulation of the phase evolution process to synthesize the expected sulfide (three phases in the Cu–Fe–S system) nanocrystals in a phase-pure form at low temperatures. These nanocrystals exhibited broadband photoabsorption ranging from the visible to the near-infrared (NIR) region. Subsequently, a solution-processed uniform CuFeS2 nanocrystal film was deposited on CdS by the same one-step route to create the first CuFeS2-based self-powered NIR photodetector. These devices demonstrated a superior stable and reproducible detection performance without bias voltage under NIR illumination, even up to 1050 nm, resulting from their suitable size. The rapid rise and decay times of ∼38 and ∼49 ms indicated that the devices are capable of high-frequency switching detection. Moreover, detailed chemical processes through accurately tuning the oxidation states, the influence of CuFeS2 nanoparticle size, phase control, and film thickness on performance were proposed in detail.
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JOURNAL OF NANOBIOTECHNOLOGY
·
2024
·Vol. 22
·期 1
·1-14
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IF 10.6
Liu Xueyan,Hu Tingting,Jia Yijiang,Yang Shuqing,Yang Yu,Cui Zhuolin,Wang Tao,Liang Ruizheng,Tan Chaoliang,Wang Yuji
The rapid proliferation of tumors is highly dependent on the nutrition supply of blood vessels. Cutting off the nutrient supply to tumors is an effective strategy for cancer treatment, known as starvation therapy. Although various hydrogel-based biomaterials have been developed for starvation therapy through glucose consumption or intravascular embolization, the limitations of single-mode starvation therapy hinder their therapeutic effects. Herein, we propose a dual-function nutrition deprivation strategy that can block the nutrients delivery through extravascular gelation shrinkage and inhibit neovascularization through angiogenesis inhibitors based on a novel NIR-responsive nanocomposite hydrogel. CuS nanodots-modified MgAl-LDH nanosheets loaded with angiogenesis inhibitor (sorafenib, SOR) are incorporated into the poly(n-isopropylacrylamide) (PNIPAAm) hydrogel by radical polymerization to obtain the composite hydrogel (SOR@LDH-CuS/P). The SOR@LDH-CuS/P hydrogel can deliver hydrophobic SOR with a NIR-responsive release behavior, which could decrease the tumor vascular density and accelerate cancer cells apoptosis. Moreover, the SOR@LDH-CuS/P hydrogel exhibits higher (3.5 times) compressive strength than that of the PNIPAAm, which could squeeze blood vessels through extravascular gelation shrinkage. In vitro and in vivo assays demonstrate that the interruption of nutrient supply by gelation shrinkage and the prevention of angiogenesis by SOR is a promising strategy to inhibit tumor growth for multimode starvation therapy.
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Small
·
2025
·
IF 12.1
Xinyuan Cui,Cheng Cao,Wanting Hao,Xinni Pan,Yu Cao,Yanfei Fu,Huifang Hao,Yingao Jiao,Shujing Lin,Shengsheng Cui,Ruokun Li,Yanlei Liu,Fuhua Yan
Advanced hepatocellular carcinoma (HCC) presents a strongly immunosuppressive tumor microenvironment, which enables tumor cells to evade immune cell attacks and hinder effective drug killing, thereby hindering the achievement of the desired therapeutic effect. In response, a novel nanoplatform- AuHNR@γ-Fe 2 O 3 @Lenvatinib@β-Glucan (AFLG) with surface modified β-1,3-glucan is developed, which exhibits potent immunostimulatory effect and the capability of repolarizing macrophages, to counteract the immunosuppressive conditions present in the tumor microenvironment. Leveraging the hollow structure of gold nanorods, Lenvatinib is efficiently loaded, a first-line targeted drug for HCC, which effectively inhibits tumor angiogenesis. Additionally, through atomic layer deposition, γ-Fe 2 O 3 is generated on the hollow gold nanorod surface, endowing it with chemodynamic therapy and magnetic resonance T 2 -weighted imaging capabilities while excellently maintaining the gold nanorod's superior photothermal therapy and photoacoustic imaging properties under 1064 nm excitation. These AFLG NPs feature dual-modal imaging and quadruple-modal synergistic therapy capabilities, along with their powerful potential in remodeling the immunosuppressive tumor microenvironment, offering an encouraging novel approach for the treatment of hepatocellular carcinoma.
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Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Meng Fu,Chang Luo,Qi Yuan,Zequn Ma,Quansheng Long,Baihui Liu,Dang Wu,Jingshui Xu,Xiangming Li
The development of bacterial resistance to antibiotics and its global spread highlights the urgent need for new alternative antimicrobial agents. Here, we have developed a biosafe antibacterial material based on reduced graphene oxide/polyelectrolytes nanolayers and gold nanoparticles functionalized molybdenum disulfide (rGP 1.5 /MoS 2 -AuNPs) via in situ synthesis and electrostatic assembly. The rGP 1.5 /MoS 2 -AuNPs has high visible and near-infrared absorption, which can efficiently provide remarkable photothermal conversion efficiency and generate reactive oxygen species (·O 2 - , ·OH, 1 O 2 ) via photocatalytic oxygen reduction and water oxidation. The rGP 1.5 /MoS 2 -AuNPs combines the photocatalysis with photothermal effect, exhibiting a biosafe and effective killing for Gram-negative and Gram-positive bacterial. The rGP 1.5 /MoS 2 -AuNPs simultaneously optimizes three key parts for antibacterial: i) polyelectrolytes component promotes bacterial adhesion, ii) reduced graphene oxide and AuNPs components provide photothermal conversion capacity and increase light absorption, iii) MoS 2 component generates photogenerated electron-hole pairs, and the electrons are rapidly conducted from the AuNPs to the reactants, which promotes the rapid separation of the electron-hole pairs, resulting in the generation of reactive oxygen species. This work provides a simple but powerful way to prepare photocatalytic and photothermal material for antibacterial applications.
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Nano Today
·
2020
·
IF 16.907
Feng Ren,Hanghang Liu,Hao Zhang,Zhilin Jiang,Bing Xia,Cécile Genevois,Tao He,Mathieu Allix,Qiao Sun,Zhen Li,Mingyuan Gao
Highly sensitive and specific discrimination of brain tumor margins from the surrounding parenchyma remains a formidable challenge. Limited by the short of photostable probes with deep tissue penetration and high efficiency of crossing the blood-brain-barrier (BBB), the development of fluorescence-guided surgery (FGS) of brain tumors was markedly constrained. Herein, we report the capability of the strong second near-infrared-IIb (NIR IIb, 1500−1700 nm) fluorescence from Er-based lanthanide nanoparticles in imaging-guided surgery of orthotopic glioma. We designed an energy-cascaded Er 3+ -Ce 3+ -A 3+ (A = Yb, Ho, Tm) system and prepared a series of NaErF 4 : [email protected] 4 @NaLuF 4 down-conversion nanoparticles (DCNPs) for optimizing the influence of NaAF 4 interlayer and Ce 3+ dopants. We modified the optimal NaErF 4 :2.5 % [email protected] 4 (0.9 nm)@NaLuF 4 DCNPs with Dye-brush polymer (Dye-BP) to facilitate 4 I 13/2 → 4 I 15/2 transition, which leads to an impressive 675-fold enhancement of 1525 nm fluorescence in aqueous solution under 808 nm excitation due to the excellent energy-cascaded downconversion (ECD), in comparison with that of NaErF 4 nanoparticles. We further modified these highly bright nanoparticles with tumor-targeting angiopep-2 peptide, and efficiently delivered them to the glioma by using the focused ultrasound sonication (FUS) to temporarily open the BBB. We obtained the highest tumor-to-background ratio (TBR = 12.5) ever reported in the targeted NIR IIb fluorescence imaging of small orthotopic glioma (size < 3 mm, depth> 3 mm) through intact skull and scalp, which was drastically improved to ∼150 after cardiac perfusion and craniotomy to ensure the precise resection of tumor. More importantly, the size of glioma measured from the width of fluorescence profile is very close to that from T 2 -weighted MRI images. Our work provides the insights into engineering NIR IIb fluorescence of lanthanide nanoparticles, and demonstrates the great potential of NIR IIb fluorescence imaging-guided surgery of tumor.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jiahui He,Zhenlong Li,Jueying Chen,Jiaxin Wang,Lipeng Qiao,Baolin Guo,Juan Hu
It is still challenging to design stimuli-responsive smart hydrogel dressing to promote bacteria-infected diabetic wound healing from the whole healing stage by intelligently responding to external stimuli or wound microenvironment. In addition, nitric oxide (NO) and oxygen (O 2 ) have been shown to accelerate diabetic wound healing by promoting angiogenesis and alleviating hypoxia. A series of NIR/glucose stimuli-responsive multifunctional smart hydrogels with NO/O 2 dual gas-releasing properties was designed based on N-carboxyethyl chitosan-grafted-phenylboronic acid (CECP), oxidized dextran (OD), ε-polylysine (EPL)-coated manganese dioxide (EMn), and β-cyclodextrin-reduced graphene oxide/N, N’-di-sec-butyl-N, N’-dinitroso-1,4-phenylenediamine (rGB) via dual dynamic crosslinking to promote bacteria-infected diabetic wound healing. The added rGB and EMn as photothermal agents rapidly kill bacteria through photothermal therapy. Meanwhile, rGB endows CECP/OD/EMn/rGB hydrogels to release NO under NIR stimulation to promote angiogenesis. Nanozyme EMn with catalase (CAT)/superoxide dismutase (SOD)-like activity can scavenge ROS and release O 2 to alleviate hypoxia and oxidative stress. The phenylboronic acid in CECP forming phenylboronate ester structure endows hydrogel with glucose-controlled release of doxycycline. NIR/glucose stimuli-responsive CECP/OD/EMn/rGB hydrogels with NO/O 2 dual gas-releasing property in a full-thickness skin wound-infected diabetic model reduced the inflammation, promoted wound contraction, collagen deposition, angiogenesis, and alleviated wound hypoxia, providing new ideas for treating bacteria-infected diabetic wounds.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Xiao-Meng Liu,Zhen-Zhen Zhu,Xin-Rui He,Yun-Hong Zou,Qian Chen,Xiao-Ya Wang,Hui-Mei Liu,Xin Qiao,Xu Wang,Jing-Yuan Xu
Platinum(II) drugs as a first-line anticancer reagent are limited by side effects and drug resistance. Stimuli-responsive nanosystems hold promise for precise spatiotemporal manipulation of drug delivery, with the aim to promote bioavailability and minimize side effects. Herein, a multitargeting octahedral platinum(IV) prodrug with octadecyl aliphatic chain and histone deacetylase inhibitor (phenylbutyric acid, PHB) at axial positions to improve the therapeutic effect of cisplatin was loaded on the upconversion nanoparticles (UCNPs) through hydrophobic interaction. Followed attachment of DSPE-PEG2000 and arginine-glycine-aspartic (RGD) peptide endowed the nanovehicles with high biocompatibility and tumor specificity. The fabricated nanoparticles (UCNP/Pt(IV)-RGD) can be triggered by upconversion luminescence (UCL) irradiation and glutathione (GSH) reduction to controllably release Pt(II) species and PHB, inducing profound cytotoxicity. Both in vitro and in vivo experiments demonstrated that UCNP/Pt(IV)-RGD exhibited remarkable antitumor efficiency, high tumor-targeting specificity, and real-time UCL imaging capacity, presenting an intelligent platinum(IV) prodrug-loaded nanovehicle for UCL-guided dual-stimuli-responsive combination therapy.
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Biomaterials Research
·
2024
·
IF 8.1
Xulu Ma,Zhao Luan,Qingxin Zhao,Anli Yang,Jinming Li
Stem cell therapy is an attractive approach to bone tissue regeneration in osteoporosis (OP); however, poor cell engraftment and survival within injured tissues limits its success in clinical settings. Nitric oxide (NO) is an important signaling molecule involved in various physiological processes, with emerging evidence supporting its diverse roles in modulating stem cell behavior, including survival, migration, and osteogenic differentiation. To control and enhance osteogenic differentiation of mesenchymal stem cells (MSCs) for OP therapy, we designed a near-infrared (NIR) light-triggered NO-releasing nanoplatform based on upconversion nanoparticles (UCNPs) that converts 808-nm NIR light into visible light, stimulating NO release by light control. We demonstrate that the UCNP nanoplatforms can encapsulate a light-sensitive NO precursor, Roussin’s black salt (RBS), through the implementation of a surface mesoporous silica coating. Upon exposure to 808-nm irradiation, NO is triggered by the controlled upconversion of UCNP visible light at the desired time and location. This controlled release mechanism facilitates photoregulated differentiation of MSCs toward osteogenic lineage and avoids thermal effects and phototoxicity on cells, thus offering potential therapeutic applications for treating OP in vivo. Following the induction of osteogenic differentiation, the UCNP nanoplatforms exhibit the capability to serve as nanoprobes for the real-time detection of differentiation through enzymatic digestion and fluorescence recovery of UCNPs, enabling assessment of the therapeutic efficacy of OP treatment. Consequently, these UCNP-based nanoplatforms present a novel approach to control and enhance osteogenic differentiation of MSCs for OP therapy, simultaneously detecting osteogenic differentiation for evaluating treatment effectiveness.
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ACS Photonics
·
2024
·
IF 6.5
Wenxia Wu,Yazhao Wang,Limin Wu,Huiting Zhang,Zhonghua Zhu,Shengdi Ta,Peng Zhang,Shoulei Xu,Bernard A. Goodman,Wen Deng
Under excitation at 980 nm, Tm3+ may emit ultraviolet, blue, and red light, and Ho3+ may emit green light through multiphoton upconversion processes in Yb/Tm/Ho codoped materials. However, because the probability of the electron population of the higher excited state energy levels is much lower than that of the lower ones in multiphoton upconversion processes, it is difficult to observe the ultraviolet emission of Tm3+-doped single crystals under excitation at 980 nm. Here, we report that high-quality single crystals of cubic ZrO2 codoped with Tm2O3, Ho2O3, and Yb2O3 are successfully grown by the optical floating zone method, and ultraviolet emission at 308 nm was observed for the first time from multiphoton upconversion transitions in these highly transparent, low phonon energy single crystals under excitation at 980 nm. This result demonstrates the prospect of making ultraviolet solid-state lasers pumped by near-infrared light. Moreover, bright white light was emitted from the single crystal prepared with 5.00 mol % Yb2O3, 0.75 mol % Tm2O3, 0.0075 mol % Ho2O3, 2.2425 mol % Y2O3, and 92.00 mol % ZrO2 under excitation at 980 nm, and a bright solid white light source excited by a near-infrared light-emitting diode for practical use is presented.
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Advanced Optical Materials
·
2025
·
IF 7.2
Xiaolong Dong,Xin Zhao,Lifan Shen,Maosen Hu,Edwin Yue Bun Pun,Hai Lin
The construction of perovskite-based luminescent systems for multifunctional integrated platforms via reciprocal energy transfer (ET) cascades emerges as a central focus, but the material design and photophysical control remain a significant challenge. Herein, a strong power-dependent quantum yield behavior is observed in Cs 2 NaInCl 6 : Ho 3+ -Yb 3+ (CNIC: Ho-Yb) phosphors with ultra-low phonon energy, and quantified multiphoton upconversion (UC) efficiencies exhibit ultra-linear enhancement with the increasing excitation power, ensuring practical applicability for UC-based temperature sensing. Moreover, an efficient quantum cutting process is unveiled in the CNIC: Ho-Yb, where a single high-energy photon of Ho 3+ is converted into multiple NIR emissions of Yb 3+ via energy redistribution under 453 nm laser excitation, offering significant potential for enhancing near-infrared (NIR) imaging capability in biological tissues. To address the inherent structural and functional limitations of powder-based materials, the CNIC: Ho-Yb/polyacrylonitrile (CNIC: Ho-Yb/PAN) nanofibers are synthesized by electrospinning, and the functional integration platform based on the efficient bidirectional ET is built by coupling 453 and 980 nm lasers to enable selective applications in flexible thermal monitoring and NIR bioimaging. These findings enable next-generation flexible thermometry platforms with higher sensitivity, signal fidelity, and device-level applicability, while also paving the way for non-invasive and high-contrast deep-tissue imaging in biomedical diagnostics.
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