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JOURNAL OF POLYMER SCIENCE · 2022 ·Vol. 60 ·期 23 ·3176-3185 · IF 3.046

NIR-triggered hydrogel with dynamic stiffness via ion chelation to modulate macrophage phenotypes

Peiqi Yuan,Yilun Luo,Lie Ma

The immune system plays a central role in tissue repair and regeneration. Macrophages have emerged as a primary target because of their critical roles in regulating multiple phases of tissue repair through their unique plasticity and ability to rapidly shift phenotypes. Smart biomaterials, which able to harness macrophage phenotypes on demand during the healing process, have become a promising strategy. Here, a novel integrated hydrogel with near-infrared (NIR) responsive dynamic stiffness was conducted, and found sequentially polarizing bone marrow-derived macrophages from pro-inflammatory to anti-inflammatory phenotype in situ. Under NIR irradiation, ethylene diamine tetraacetic acid released from the IR780-mixed phase change material into the hydrogel, resulting in the decrease of hydrogel stiffness in situ by chelating the calcium ion (Ca 2+ ) in the calcium alginate hydrogel. The up-regulation of arginase-1 and interleukin-10 were quantified by immunostaining and enzyme-linked immune sorbent assay, respectively. The result indicated the transformation of macrophage from the pro-inflammatory to anti-inflammatory phenotype by dynamic stiffness drop. The modulation of macrophage phenotypes by stiffness-degradation without the stimuli of cytokines offers an effective and noninvasive strategy to manipulate inflammatory or tissue-regenerative immune responses to achieve optimized healing or therapeutical outcomes. Graphical

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ACS Sensors · 2022 · IF 9.618

Lanthanide/Cu2–xSe Nanoparticles for Bacteria-Activated NIR-II Fluorescence Imaging of Infection

Leilei Sun,Sisi Shi,Zeming Wu,Yao Huang,Chenhui Ji,Craig A. Grimes,Xinxin Feng,Qingyun Cai

A material system enabling specific NIR-II fluorescence imaging of Gram-positive bacteria is described. The material system is based on the electrostatic binding of Cu2–xSe and vancomycin-modified NaGdF4:Nd,Yb@NaGdF4 downconversion nanoparticles (DCNPs), the fluorescence of which is weak owing to the spectral overlap of Cu2–xSe absorption with the DCNP NIR emission. The presence of Gram-positive bacteria precisely disconnects the bond between vancomycin-modified DCNPs and Cu2–xSe, thus enabling a strong fluorescent signal. In vivo studies show that the material system can be specifically activated at the site of Gram-positive bacterial infection but is essentially nonfluorescent in the area of Gram-negative bacterial infection.

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JOURNAL OF NANOBIOTECHNOLOGY · 2022 ·Vol. 20 ·期 1 ·1-17 · IF 9.429

Extracellular matrix-degrading STING nanoagonists for mild NIR-II photothermal-augmented chemodynamic-immunotherapy

Zhan Meixiao,Yu Xiangrong,Zhao Wei,Peng Yongjun,Peng Shaojun,Li Jingchao,Lu Ligong

Regulation of stimulator of interferon genes (STING) pathway using agonists can boost antitumor immunity for cancer treatment, while the rapid plasma clearance, limited membrane permeability, and inefficient cytosolic transport of STING agonists greatly compromise their therapeutic efficacy. In this study, we describe an extracellular matrix (ECM)-degrading nanoagonist (dNAc) with second near-infrared (NIR-II) light controlled activation of intracellular STING pathway for mild photothermal-augmented chemodynamic-immunotherapy of breast cancer. The dNAc consists of a thermal-responsive liposome inside loading with ferrous sulfide (FeS2) nanoparticles as both NIR-II photothermal converters and Fenton catalysts, 2′3′-cyclic guanosine monophosphate-adenosine monophosphate (cGAMP) as the STING agonist, and an ECM-degrading enzyme (bromelain) on the liposome surface. Mild heat generated by dNAc upon NIR-II photoirradiation improves Fenton reaction efficacy to kill tumor cells and cause immunogenic cell death (ICD). Meanwhile, the generated heat triggers a controlled release of cGAMP from thermal-responsive liposomes to active STING pathway. The mild photothermal activation of STING pathway combined with ICD promotes anti-tumor immune responses, which leads to improved infiltration of effector T cells into tumor tissues after bromelain-mediated ECM degradation. As a result, after treatment with dNAc upon NIR-II photoactivation, both primary and distant tumors in a murine mouse model are inhibited and the liver and lung metastasis are effectively suppressed. This work presents a photoactivatable system for STING pathway and combinational immunotherapy with improved therapeutic outcome.Graphical Abstract

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ACS Biomaterials Science & Engineering · 2022 · IF 5.395

Fabrication of Laponite-Reinforced Dextran-Based Hydrogels for NIR-Responsive Controlled Drug Release

Jinwei Luo,Zewei Ma,Fengjuan Yang,Tianhua Wu,Shengwu Wen,Jingxian Zhang,Langhuan Huang,Suiping Deng,Shaozao Tan

Natural polymer gels with sensitivity to near-infrared (NIR) light have attracted the attention of scientists working on intelligent drug delivery systems. Compared to ultraviolet or visible light, NIR light has the advantages of strong trigger levels, deep penetration through affected tissues, and fewer side effects. Herein, we present a topical photothermal hydrogel for NIR-controlled drug delivery. The proposed DexIEM-GM-Laponite hydrogel was prepared through free radical polymerization of vinyl-functionalized dextran (DexIEM), vinyl-modified graphene oxide (GM), and Laponite; thereafter, the hydrogel was loaded with ciprofloxacin (CIP, an antibacterial drug) as a model drug. With the Laponite content increased, the density of crosslinking in the hydrogel increased, and its mechanical properties improved noticeably. Under NIR irradiation, the DexIEM-GM-Laponite hydrogel exhibited a photothermal property, where the surface temperature increased from 26.8 to 55.5 °C. The simulation of subcutaneous drug delivery experiments ex vivo showed that under the specified pork tissue thickness (2, 4, and 6 mm), the CIP release remained NIR-controllable. Additionally, the results of the antibacterial performance tests indicated the excellent antibacterial effect of the hydrogel, and the blood hemolysis ratio of the hydrogel was less than 5%, signifying good blood compatibility. This work will provide an avenue for the application of NIR light-responsive materials in antimicrobial therapy.

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Journal of Materials Chemistry B · 2022 ·Vol. 10 ·期 8 ·1250-1264 · IF 7.571

Orange-red to NIR emissive carbon dots for antimicrobial, bioimaging and bacteria diagnosis

Rixiang Su,Hongjun Yan,Xiantao Jiang,Ying Zhang,Peiyuan Li,Wei Su

Antimicrobial photodynamic therapy (aPDT) has become a popular technology for the treatment of bacterial infections. The development of antimicrobial agents combining diagnosis and treatment remains a major challenge. Herein, curcumin carbon quantum dots (Cur-NRCQDs) with antibacterial and imaging effects were synthesized using a hydrothermal method. The fluorescence absorption range of the Cur-NRCQDs in aqueous solution was 555 to 850 nm, showing orange-red to near infrared (NIR) fluorescence, and its maximum emission wavelength was 635 nm. At the same time, Cur-NRCQDs improved the efficiency of Cur as the photosensitizer (PS), showed good storage and light stability, and enhanced the efficiency of reactive oxygen (ROS) generation and antibacterial activity. Under the irradiation of a xenon lamp, Cur-NRCQDs inactivated 100% Staphylococcus aureus (S. aureus) and Escherichia coli (E. coli) at concentrations of 10 and 15 μM, respectively. The possible reason for this was that under PDT, the ROS produced by the Cur-NRCQDs destroyed the integrity of the cell membrane, resulting in leakage of the contents. In addition, the Cur-NRCQDs showed good cell compatibility, as they can also enter bacteria and cells for imaging, so they can be employed for the detection of bacteria and cell tissues. Therefore, Cur-NRCQDs are an ideal candidate material for aPDT treatment and fluorescent bioimaging.

CAS / MDL: 458-37-7
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Environmental Science-Nano · 2022 ·Vol. 9 ·期 4 ·1330-1340 · IF 9.473

Thermo-responsive polymer–black phosphorus nanocomposites for NIR-triggered bacterial capture and elimination

Shuo Deng,Dongsheng Wang,Zhiqiang Xiong,Siyu Zhang,Dengyu Li,Jin Zeng,Xuejiao Zhang,Qing Zhao

Water contamination by pathogenic bacteria is a major challenge to human health. The conventional disinfection methods produce disinfection by-products that may be carcinogenic, while the recently-developed nanotechnologies face the difficulties of low efficiency and rate, secondary pollution, and tedious processes. To solve these problems, we designed a thermo-responsive poly(N-isopropylacrylamide)-functionalized black phosphorus (named BP–PNIPAM) to capture and eliminate bacterial cells under the stimuli of near-infrared (NIR) irradiation. PNIPAM is covalently linked to the surface of BP nanosheets by aryl diazonium reaction and in situ atom transfer radical polymerization (ATRP). Under short-time NIR irradiation, bacterial cells are captured and co-precipitated with BP–PNIPAM due to the thermally induced hydrophilic-to-hydrophobic phase transition of PNIPAM. If the irradiation time is prolonged, the wrapped bacteria are disinfected due to hyperthermia. More than 80% of E. coli and S. aureus are captured by 100 μg mL−1 BP–PNIPAM within 5 min-NIR irradiation, while the elimination efficiency towards E. coli, S. aureus, and anti-ampicillin E. coli reaches 100% in the presence of 50 μg mL−1 BP–PNIPAM within 20 min-NIR irradiation. Moreover, BP–PNIPAM exhibits no obvious toxicity to Caco-2 cells up to 100 μg mL−1 within 24 h. Therefore, BP–PNIPAM offers an efficient, biocompatible, and convenient approach for the capture and sterilization of pathogenic bacteria in water.

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Small · 2023 · IF 13.3

Biomimetic Nano-Immunoactivator via Ionic Metabolic Modulation for Strengthened NIR-II Photothermal Immunotherapy

Xiaodan Wei,Honglin Huang,Junhan Guo,Ningxi Li,Qingzhi Li,Tian Zhao,Geng Yang,Lulu Cai,Hong Yang,Chunhui Wu,Yiyao Liu

Reprogramming the immunologically “cold” environment of solid tumors is currently becoming the mainstream strategy to elicit powerful and systemic anticancer immunity. Here, a facile and biomimetic nano-immunnoactivator ( CuS/Z@M 4T1 ) is detailed by engineering a Zn 2+ -bonded zeolitic imidazolate framework-8 (ZIF-8) with CuS nanodots (NDs) and cancer cell membrane for amplified near-infrared-II (NIR-II) photothermal immunotherapy via Zn 2+ metabolic modulation. Taking advantage of the NIR-II photothermal effect of CuS NDs and the acidic responsiveness of ZIF-8, CuS/Z@M 4T1 rapidly causes intracellular Zn 2+ pool overload and disturbs the metabolic flux of 4T1 cells, which effectively hamper the production of heat shock proteins and relieve the resistance of photothermal therapy (PTT). Thus, amplified immunogenic cell death is evoked and initiates the immune cascade both in vivo and in vitro as demonstrated by dendritic cells maturation and T-cell infiltration. Further combination with antiprogrammed death 1 (aPD-1) achieves escalated antitumor efficacy which eliminates the primary, distant tumor and avidly inhibits lung metastasis due to cooperation of enhanced photothermal stimulation and empowerment of cytotoxic T lymphocytes by aPD-1. Collectively, this work provides the first report of using the intrinsic modulation property of meta-organometallic ZIF-8 for enhanced cancer photoimmunotherapy together with aPD-1, thereby inspiring a novel combined paradigm of ion-rich nanomaterials for cancer treatment.

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Nanoscale · 2023 · IF 6.7

A NIR-driven green affording-oxygen microrobot for targeted photodynamic therapy of tumors

Lishan Zhang,Xiaoting Zhang,Hui Ran,Ze Chen,Yicheng Ye,Jiamiao Jiang,Ziwei Hu,Miral Azechi,Fei Peng,Hao Tian,Zhili Xu,Yingfeng Tu

Photodynamic therapy (PDT) is a light-activated local treatment modality that has promising potential in cancer therapy. However, ineffective delivery of photosensitizers and hypoxia in the tumor microenvironment severely restrict the therapeutic efficacy of PDT. Herein, phototactic Chlorella (C) is utilized to carry photosensitizer-encapsulated nanoparticles to develop a near-infrared (NIR) driven green affording-oxygen microrobot system (CurNPs-C) for enhanced PDT. Photosensitizer (curcumin, Cur) loaded nanoparticles are first synthesized and then covalently attached to C through amide bonds. An in vitro study demonstrates that the developed CurNPs-C exhibits continuous oxygen generation and desirable phototaxis under NIR treatment. After intravenous injection, the initial 660 nm laser irradiation successfully induces the active migration of CurNPs-C to tumor sites for higher accumulation. Upon the second 660 nm laser treatment, CurNPs-C produces abundant oxygen, which in turn induces the natural product Cur to generate more reactive oxygen species (ROS) that significantly inhibit the growth of tumors in 4T1 tumor-bearing mice. This contribution showcases the ability of a light-driven green affording-oxygen microrobot to exhibit targeting capacity and O2 generation for enhancing photodynamic therapy.

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Nanoscale · 2023 · IF 6.7

Biomimetic submicromotor with NIR light triggered motion and cargo release inspired by cuttlefish

Jiameng Feng,Junjie Zou,Xiaoyu Li,Xin Du

Biomimetic design is very helpful and significant for the smart construction of micro/nanomotors with artificial intelligence. In this work, inspired by cuttlefish, who can rapidly eject poisonous ink and are also capable of fast movement to escape, we designed and fabricated a biomimetic submicromotor with the ability of simultaneous quick movement and a temperature threshold caused explosive cargo release triggered by near infra-red (NIR) light irradiation, which was approximately equivalent to the action of cuttlefish when encountering a predator. The yolk@shell structured polydopamine@mesoporous silica (PDA@MS60) with immovable and asymmetric yolk distribution was employed as a platform, and this was followed by the simultaneous encapsulation of phase change materials (PCM) and cargo molecules. The NIR light irradiation could not only propel the direct motion of the submicromotor, but also caused the explosive release of the cargo loaded in the submicromotor when the temperature exceeded the melting point of the PCM.

CAS / MDL: 143-07-7 57-11-4
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Advanced Healthcare Materials · 2023 · IF 10

NIR-Actuated Targeted Janus Nanomotors Remodel Immunosuppressive Tumor Microenvironment for Augmented Cancer Immunotherapy

Xiaoyu Zhou,Enhui Ma,Yingying Zhang,Yujuan Xing,Wenbei Xu,Liang Chen,Hong Zhou,Xinran Zhang,Canran Jiang,Kai Xu,Hong Wang,Shaohui Zheng

Tumor-associated macrophages (TAMs) always display immunosuppressive M2 phenotype in the tumor microenvironment to facilitate tumor growth, invasion and metastasis. Ibrutinib (IBR), a novel irreversible Bruton's tyrosine kinase (BTK) inhibitor, has been employed to repolarize the BTK-overexpressed TAMs from M2 to M1 phenotype to remodel the immunosuppressive tumor microenvironment. However, the poor solubility of IBR extremely hinders its bioavailability, which results in low tumor accumulation and TAMs uptake in vivo. Herein, we proposed NIR laser-actuated Janus nanomotors for the effective and deep delivery of IBR to TAMs in solid tumor for targeted immunotherapy. Under NIR irradiation, the Janus nanomotors exhibited efficient photothermal conversion to produce powerful propulsion via self-thermophoresis with a speed of 12.15 μm −1 s. Combined with the salic acid targeting and IBR loading, the nanomotors significantly boosted their binding and uptake efficacy by M2-like macrophages during the active motion, which highly facilitated the reprogramming of M2 to M1 macrophages in vitro. Furtherly, the autonomous motion also validly improved in-vivo accumulation and penetration depth in tumors to alter the M1/M2 polarization balance and activate T cells. Overall, the synthesized IC@MSA JNMs would provide a promising strategy for the efficient delivery of immunological agents toward targeted cancer immunotherapy. This article is protected by copyright. All rights reserved

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LANGMUIR · 2023 · IF 3.9

Degradable PDA@PNIPAM-TA Nanocomposites for Temperature- and NIR light-Controlled Pesticide Release

Manting Wang,Rongrong Fan,Qingjian Yu,Jie-Xin Wang,Yuan Le,Jian-Feng Chen

Controlled pesticide delivery systems offer many distinctive advantages over conventional pesticide formulations. In this work, degradable poly(N-isopropylacrylamide) (PNIPAM)–tannic acid (TA) microgels and multifunctional PDA@PNIPAM-TA nanocomposites were prepared in a high-gravity rotating packed bed reactor (RPB) for smart pesticide delivery and release. The as-prepared microgels and nanocomposites showed reversible temperature-dependent swelling/deswelling behavior and irreversible pH-induced degradation. A dynamic contact angle test suggested that the introduction of TA and PDA into the PNIPAM matrix could enhance foliar adhesion and deposition efficiency. The nanocomposites were further used for the encapsulation and delivery of imidacloprid (IMI) to protect it from rapid photolysis and improve its pest-control efficiency. Their thermoresponsive behavior as well as pesticide loading capacity could be tuned by tailoring the PNIPAM-TA shell thickness, which could be varied by the NIPAM amount. The release rate of IMI from the core/shell nanocomposites was positively correlated with environmental temperature and near-infrared (NIR) light, which was adaptive to the positive temperature-dependent toxicity correlation of IMI and the increasing trend of pests under high temperature. The cumulative release of IMI was 23.5% at 25 °C, while it was 81.2% at 40 °C after 24 h of incubation, and the release rate was greatly enhanced under NIR irradiation. The results indicated that the facile control of pesticide release could be realized by regulating environmental conditions. This work also provides an idea for using high-gravity technology to conveniently construct a smart, effective, and environmentally friendly pesticide delivery system for sustainable crop protection.

CAS / MDL: 110-26-9
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NEW JOURNAL OF CHEMISTRY · 2021 ·Vol. 45 ·期 17 ·7893-7899 · IF 3.591

NIR responsive AuNR/pNIPAM/PEGDA inverse opal hydrogel microcarriers for controllable drug delivery

L. Z. Liu,X. Y. Sun,Z. Y. Yan,B. F. Ye

Particle-based delivery systems have emerged as a powerful platform in controlled drug release. In the present study, we developed a new inverse opal hydrogel microcarrier system composed of gold nanorods (AuNRs) for near-infrared light (NIR) activated drug delivery. AuNRs with a desired aspect ratio were prepared by a seed-mediated growth method. The inverse opal hydrogel microcarriers composited with AuNRs were synthesized by negatively replicating silica colloidal crystal beads (SCCBs). The NIR-thermo response of the microcarriers was due to the NIR photothermal heating effect of AuNRs and the thermo responsive volume transition of poly(N-isopropylacrylamide) (pNIPAM) hydrogel. It was found that the NIR-controlled reversible shrinking response of the microcarriers was ideal for the controllable drug release with real-time self-reporting color indication.

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