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Two-dimensional ultrathin vanadium oxide nanosheets as catalytic bactericide

Science China Materials 2024年第9期67卷 2965-2976页

作者： Zhimin Zhang Zhao Guo Zesong Ruan Min Ge shibo Cao Jiayi Yuan Zhen Xu Lieying Fan Ming Zong Han Lin jianlin shi State Key Laboratory of High Performance Ceramics and Superfine Microstructures Shanghai Institute of Ceramics Chinese Academy of SciencesResearch Unit of Nanocatalytic Medicine in Specific Therapy for Serious DiseaseChinese Academy of Medical SciencesShanghai200050China Department of Orthopedic Surgery Shanghai Institute of Microsurgery on ExtremitiesShanghai Sixth People’s Hospital Affiliated to Shanghai Jiao Tong University School of MedicineShanghai200233China Department of Clinical Laboratory Shanghai East HospitalTongji University School of MedicineShanghai200120China Department of Electrical and Electronic Engineering The University of Hong KongHong KongChina Shanghai Tenth People’s Hospital Shanghai Frontiers Science Center of Nanocatalytic MedicineSchool of MedicineTongji UniversityShanghai200331China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing100049China

Infectious diseases caused by pathogenic bacteria are a serious threat to global public ***,antibiotics and other clinical drugs suffer from some fundamental disadvantages such as narrow-spectrum antibacterial effect and the risk to induce drug resistance,while inorganic functional nanomaterials with biological catalytic activities have been developed as novel antibacterial *** this study,we prepared two-dimensional ultrathin vanadium oxide nanosheets(VO_(x)NSs)with mixed valence states from the oxidised layer of vanadium powder(bulk V)by ultrasonically assisted liquid *** conveniently switching between V^(IV)and V^(V),VO_(x)NSs can efficiently catalyse H_(2)O_(2)enriched in bacterially infected areas to generate hydroxyl radicals(·OH),which induce bacterial oxidative stress and *** process can occur in both weakly alkaline and acidic environments,thus being independent of the pH value in infection *** addition,contributed by the intrinsic characteristics of vanadium,two-dimensional morphology and reasonable valence state ratios,VO_(x)NSs exhibit the advantages of broad antibacterial spectrum,high catalytic activity and non-toxic *** novel nanosheet offers a new strategy to heal infected wounds and extends the application of nanocatalytic medicine towards anti-infection.

关键词： ultrathin nanosheet vanadium oxide Fenton-like reaction antibacterial

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基于乙二胺四乙酸插层锌铝双金属氢氧化物的晚期肿瘤抗转移免疫治疗研究

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无机材料学报 2024年第9期39卷 1044-1052,I0001页

作者：李世奇鲍群群胡萍施剑林中国科学院上海硅酸盐研究所高性能陶瓷和超微结构国家重点实验室上海200050 中国科学院大学材料科学与光电工程中心北京100049 同济大学附属第十人民医院上海200435

癌细胞的全身性转移是目前癌症晚期患者的主要死亡原因。由于肿瘤细胞的快速增殖和细胞外基质的异常沉积,晚期癌症大体积瘤体组织致密且刚度较高,这为晚期实体肿瘤的治疗带来了极大的困难。一方面,由于大体积肿瘤的结构特性,使得常规药... 详细信息

癌细胞的全身性转移是目前癌症晚期患者的主要死亡原因。由于肿瘤细胞的快速增殖和细胞外基质的异常沉积,晚期癌症大体积瘤体组织致密且刚度较高,这为晚期实体肿瘤的治疗带来了极大的困难。一方面,由于大体积肿瘤的结构特性,使得常规药物难以渗透至其内部,免疫细胞难以浸润;另一方面,硬基质上的肿瘤细胞具有更强的侵袭能力,这容易引起肿瘤的全身性转移。为了解决这一问题,本研究制备了乙二胺四乙酸(EDTA)插层锌铝双金属氢氧化物纳米材料(EDTA/LDH),基于两个平行的Ca^(2+)剥夺机制,开展了EDTA/LDH材料体系对晚期大体积实体瘤的抗转移免疫治疗研究。该材料在肿瘤微酸环境中,通过静电力作用贴附在肿瘤细胞膜上,并释放EDTA以螯合细胞连接蛋白中的Ca^(2+),切断部分细胞连接,从而降低大体积瘤体的致密程度,促进免疫细胞向瘤体内浸润。此外,该材料在机体内被巨噬细胞作为“异物”吞噬,引起钙库操纵性钙内流,激活巨噬细胞抗肿瘤免疫效应,抑制多形核髓系抑制性细胞(PMN-MDSCs)和调节性T细胞(Tregs)的促肿瘤侵袭作用。本研究将为晚期恶性实体瘤的抗转移治疗提供借鉴性思路和方法。

关键词：晚期癌症免疫治疗无机纳米材料离子调控

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Sonocatalytic hydrogen generation breaks the heart of super bacteria—a hydrogen solution to super bacteria?

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National Science Review 2023年第6期10卷 47-48页

作者： jianlin shi State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of Ceramics Chinese Academy of Sciences Research Unit of Nanocatalytic Medicine in Specific Therapy for Serious Disease Chinese Academy of Medical Sciences

It is quite difficult to kill super bacteria using routine anti-bacterial drugs and ***,super bacteria exhibit an extraordinarily strong drug resistance,mainly due to the blockage of dense extracellular matrix (ECM) of bacterial biofilm against drug penetration,which is quite similar to the case of solid tumors [1,2].How,then,does one effectively overcome this ECM barrier?Currently available clinical approaches are not very *** recent years,hydrogen molecules (H2) have been recognized as being able to cross various biological barriers,in cluding the blood-brain barrier and plant barriers [3],owing to its small molecular size,which also presents a bio energy-modulating effect capable of inducing apoptosis in various tumor cells and bacteria [4].Therefore,H2medication for anti-biofilm and anti-tumor is a promising therapeutic strategy by virtue of their super penetrability.

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Controllable Synthesis of Mesoporous Multipods for Enhanced Nano-bio Interactions

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Chemical Research in Chinese Universities 2019年第6期35卷 953-954页

作者： shi jianlin State Key Laboratory of High Petfonriance Ceramics and Superfine Microstructure Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050P.R.China

Precise manipulation of surface topology has been being a great challenge for the fabrication of functional *** recently Zhao and coworkers developed a surface-kinetic mediated multi-site nucleation strategy to precisely control the nucleation number of periodic mesoporous organosilicas(PMOs)on the surface of magnetic *** as-prepared mesoporous multipods(especially the Tribulus-like tetra-pods mesoporous nanoparticles)present high bacteria adhesion efficiency through multivalent interactions,which are expected to be the promising candidates for future antibacterial *** work has been published online in the Nature Communications in September 26,2019.

关键词： materials. spheres topology

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Chemical Design of Nuclear-Targeting Mesoporous Silica Nanoparticles for Intra-nuclear Drug Delivery

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Chinese Journal of Chemistry 2018年第6期36卷 481-486页

作者： Limin Pan jianlin shi Shanghai Institute of Ceramics Chines Academy of Sciences Shanghai 200050 China

Targeted drug delivery has been widely explored for efficient tumor therapy with desired efficacy but minimized side effects. It is widely known that large numbers of DNA-toxins, such as doxorubicin, genes, reactive oxygen species, serving as therapeutic agents, can result in maximized therapeutic effects via the interaction directly with DNA helix. So after cellular uptake, these agents should be further delivered into cell nuclei to play their essential roles in damaging the DNA helix in cancer ceils. Here, we demonstrate the first paradigm estabJished in our laboratory in developing nucle- ar-targeted drug delivery systems （DDSs） based on MSNs for enhanced therapeutic efficiency in the hope of speeding their translation into the ctinics. Firstly, nuclear-targeting DDSs based on MSNs, capable of intranuclear accumulation and drug release therein, were designed and constructed for the first time, resulting in much enhanced anticancer effects both in vitro and in vivo. Such an MSNs-based and nuclear-targeted drug/agent delivery strategy was further applied to overcome multidrug resistance （MDR） of malignant tumors, intra-nuclearly deliver therapeutic genes, photosensitizers, radio-enhancement agents and photothermal agents to realize efficient gene therapy, photodynamic therapy, radiation therapy and photothermal therapy, respectively.

关键词： nuclear targeting mesoporous silica nanoparticles drug delivery cancer therapy nanomedicine

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Synthesis and phase evolution of LiNb_(0.6)Ti_(0.5)O_3 powder via a sol-gel method

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Particuology 2010年第5期8卷 463-467页

作者： Xia Wang Wei Li jianlin shi School of Materials Science and Engineering East China University of Sdence and Technology 130 Meilong Road Shanghai 200237 China Shanghai Institute of Ceramics Chinese Academy of Sciences 1295 Dingxi Road Shanghai 200050 China

A simple sol-gel route was demonstrated for the synthesis of LiNb0.6Ti0.5O3 （M-phase） powder, using cheap and manageable starting materials at a relatively low temperature. The phase transitions in both chemical and solid-state processes were studied by X-ray diffraction （XRD） in detail. The results showed that in the sol-gel process the anatase TiO2 phase first appeared at 400 ℃ and then LiNbO3 solid solution （LiNbO3 55） emerged at 500 ℃. When calcined to 600 ℃, the M-phase started to appear along with the decrease of TiO2 and LiNbO3 ss. Single M-phase could be formed at 700℃, which is 300 ℃ lower than that by the traditional solid-state method. A plausible evolution mechanism of the as-synthesized powder in calcination was proposed. The produced powder has potential applications in microelectronics systems.

关键词： M-phaseSol-gel processPhase transitionX-ray diffraction

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Co-electrolysis toward value-added chemicals

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Science China Materials 2022年第1期65卷 1-9页

作者： Lisong Chen jianlin shi Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062China State Key Laboratory of High Performance Ceramics and Superfine Microstructures Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China

Current major electrocatalytic reactions,such as hydrogen evolution reaction,carbon dioxide reduction reaction,and nitrogen reduction reaction,focus on single-target chemical production,which suffers from strong competitive reactions at the same electrodes and/or high energy barrier reactions at the counterpart *** co-electrolysis of more than one kind,typically two kinds,of chemical precursors in one electrolytic system is therefore a highly attractive strategy for both energy input reduction and concurrent production of double value-added *** progress has been achieved in this area recently,and a timely review on this specific topic will be highly *** this review,the reported co-electrolysis systems are classified into four categories:(1)agent sacrificing at one electrode promoting electrochemical precursor conversion at the other;(2)parallel electrochemical precursor conversions,i.e.,electrosyntheses,simultaneously at both sides;(3)electrochemical conversions of two precursors at both sides into one/the same product;(4)double/multiple electrochemical conversions at one *** current challenges and future opportunities of co-electrolysis toward high value-added products are discussed at the end.

关键词： co-electrolysis value-added chemicals electrocatalysts

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Efficient benzaldehyde photosynthesis coupling photocatalytic hydrogen evolution

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Journal of Energy Chemistry 2022年第3期31卷 52-60,I0003页

作者： Juanjuan Luo Min Wang Lisong Chen jianlin shi Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062China State Key Laboratory of High Performance Ceramics and Superfine Microstructures Shanghai Institute of CeramicsChinese Academy of SciencesShanghai 200050China

Photosynthesis of organic compounds in coupling with promoted hydrogen evolution under mild conditions of light irradiation is considered as one of the most efficient and promising approach to obtain high purity hydrogen and value-added chemicals concurrently by utilizing green solar ***,we report the synthesis of Ni S nanoparticle-modified Cd S nanorod composites(Ni S/Cd S)as an efficient bifunctional catalyst for the highly selective photocatalytic synthesis of high-value-added product benzaldehyde(BAD)from aqueous solution of benzyl alcohol(BA)under oxygen-free conditions,in accompanying with the efficient hydrogen *** synergetic catalytic effect between Ni S and Cd S is proposed to play an important role in elevating the photo-redox *** composition-optimized 30%Ni S/Cd S catalyst affords an extraordinarily high H;generation rate of 207.8μmol h^(-1)and a simultaneous BAD generation rate of 163.8μmol h^(-1)under visible light irradiation,which are respectively 139 and 950 times higher than those of Cd S without Ni S *** our knowledge,these are the highest photocatalytic production rates of both H_(2)and aldehyde ever reported on the concurrent photocatalytic of aldehyde synthesis and hydrogen evolution in green aqueous *** work provides a highly efficient photosynthesis strategy for the concurrent productions of high-value-added fine chemicals and hydrogen.

关键词： Photosynthesis Aromatic aldehyde Hydrogen evolution Bifunctional catalyst

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Construction of smart inorganic nanoparticle-based ultrasound contrast agents and their biomedical applications

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Science Bulletin 2015年第13期60卷 1170-1183页

作者： Ming Ma Hangrong Chen jianlin shi State Key Laboratory of High Performance Ceramics and Superfine Microstructures Shanghai Institute of CeramicsChinese Academy of Sciences

Ultrasound(US) imaging in combination with US contrast agents(UCAs) is a powerful tool in the modern biomedical field because of its high spatial resolution, easy access to patients and minimum *** microbubble-based UCAs have been widely used in clinical diagnosis; however, they are only limited to the blood pool imaging and not applicable to the tissue-penetrated imaging due to their large particle size and structural instability. Inorganic nanoparticles(NPs), such as silica,gold and Fe x O y, featured with both satisfactory echogenic properties and structural stability have the potential to be used as a new generation of UCAs. In this review, we present the most recent progresses in the tailored construction of inorganic UCAs and their biomedical applications in the US imaging-involved fields. Firstly, the typical inorganic NPs with different structures including solid, hollow and multiple-layer forms will be comprehensively introduced in terms of their structure design,physicochemical property, US imaging mechanism and diverse applications; secondly, the recent progress in exploring the gas-generating inorganic NP system for US imaging purpose will be reviewed, and these intelligent UCAs are multifunctional for simultaneous US imaging and disease therapy; thirdly, several nanocomposite platforms newly constructed by combining inorganic UCAs with other functional components will be presented anddiscussed. These multifunctional NPs are capable of further enhancing the imaging resolution by providing more comprehensive anatomical information *** but not the least, the design criteria for developing promising UCAs to satisfy both clinical demands and optimized US imaging capability will be discussed and summarized in this review.

关键词： Inorganic nanoparticle .Ultrasoundimaging . Theranostic . Contrast agent

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Nanocatalytic bacteria disintegration reverses immunosuppression of colorectal cancer

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National Science Review 2022年第11期9卷 208-222页

作者： Han Jiang Yuedong Guo Zhiguo Yu Ping Hu jianlin shi State Key Laboratory of High Performance Ceramics and Superfine Microstructures Shanghai Institute of Ceramics Chinese Academy of SciencesResearch Unit of Nanocatalytic Medicine in Specific Therapy for Serious Disease Chinese Academy of Medical Sciences Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Shanghai Tenth People's Hospital Shanghai Frontiers Science Center of Nanocatalytic Medicine School of Medicine Tongji University

Tumor-associated bacteria(TAB) play a critically important role in regulating the microenvironment of a tumor, which consequently greatly deteriorates the therapeutic effects by chemo-and radiotherapy deactivation and, more considerably, leads to substantial immunosuppression. On the contrary, herein we propose a nanocatalytic tumor-immunotherapeutic modality based on the bacteria disintegration by bacteria-specific oxidative damage under magnetic hyperthermia for highly effective immune response activation-promoted tumor regression. A monodispersed and superparamagnetic nanocatalytic medicine modified by arginyl-glycyl-aspartic acid(RGD) and(3-carboxypropyl)triphenylphosphonium bromide(TPP), named as MNP-RGD-TPP herein, has been synthesized, which features selective accumulation at the TAB by the electrostatic affinity, enabling effective TAB disintegration by the nanocatalytic Fenton reaction producing abundant cytotoxic hydroxyl radicals in situ under alternating magnetic field-induced hyperthermia. More importantly, the lipopolysaccharide has been metabolically secreted from the destructed TAB as pathogen-associated molecular patterns(PAMPs) to M1-polarize tumor-associated macrophages(TAMs) and promote the maturation of dendritic cells(DCs) for innate immuno-response activation of TAMs, followed by cytotoxic T lymphocytes awakening under the PAMPs presentation by the mature DCs against tumor cells. The integrated innate and adaptive immunity activations based on this TAB-promoted nanocatalytic immunomedicine, instead of magnetic heating-induced hyperthermia or the released Fe2+/Fe3+Fenton agent, has been found to achieve excellent therapeutic efficacy in an orthotopic colorectal cancer model, demonstrating the great potential of such an integrated immunity strategy in clinical tumor immunotherapy.

关键词： tumor-associated bacteria nanocatalytic bacteria disintegration immunosuppressive reversal colorectal cancer immunotherapy

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