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Modulator-directed assembly of hybrid composites based on metalorganic frameworks and upconversion nanoparticles

Nano Research 2023年第1期16卷 1482-1490页

作者： Yanhui Feng Xingjun Li Shan Lu Renfu Li Zhongliang Gong xiaoying shang Yifan Pei Wei Zheng Datao Tu Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterialsand State Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of chemistry Fuzhou universityFuzhou 350108China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350117China

Hybrid composites made of metal-organic frameworks(MOFs)and lanthanide-doped upconversion nanoparticles(UCNPs)have attracted considerable interest for their synergistically enhanced functions in various applications such as chemical sensing,photocatalysis,anticounterfeiting and nanomedicine.However,precise assembly of MOF/UCNP hybrid composites with tunable morphologies remains a challenge due to the lack of effective synthetic methods and fundamental understanding of the growth mechanisms.Herein,we propose a modulator-directed assembly strategy to synthesize a series of ZIF-8@UCNP composites(ZIF-8=zeolitic imidazolate framework-8).The UCNPs densely paved on the surface of ZIF-8 microcrystals and endowed the composites with intense upconversion blue emission,which were verified by steady-state/transient photoluminescence(PL)spectroscopy and single-particle imaging.Ethylenediamine(EDA)was firstly used as a modulator to fine-tune the predominant MOF facets and realized distinct morphologies of the composites.By adjusting the concentration of EDA from 0 to 25 mmol/L,the morphology of the ZIF-8@UCNP composites was tuned from rhombic dodecahedron(RD)to truncated rhombic dodecahedron(TRD),cube with truncated edges(CTE),cube,and finally a unique form of interpenetration twins(IT).The nucleation and growth process of the ZIF-8@UCNP composites was monitored by time-dependent scanning electron microscopy(SEM)images and the formation mechanism was thoroughly revealed.Furthermore,we demonstrated that the strategy for assembly of morphology-controllable ZIF-8@UCNP composites was generally applicable to various UCNPs with different sizes and shapes.The proposed strategy is expected to open up new avenues for the controllable synthesis of MOF/UCNP composites toward diverse applications.

关键词： metal-organic frameworks upconversion nanoparticles hybrid composites ethylenediamine modulator

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Boosting the Energy Migration Upconversion through Inter-Shell Energy Transfer in Tb^(3+)-Doped Sandwich Structured Nanocrystals

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CCS Chemistry 2022年第6期4卷 2031-2042页

作者： Dan Xu Jin Xu xiaoying shang Shaohua Yu Wei Zheng Datao Tu Renfu Li Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterialsand State Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhouFujian 350002 University of Chinese Academy of Sciences Beijing 100049 Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China FuzhouFujian 350108

It remained challenging to fabricate Tb^(3+)-doped lanthanide nanocrystals(NCs)to simultaneously acquire strong energy migration upconversion(EMU)emissions of Tb^(3+)while suppressing the Tm3+UV upconversion emissions that cause background biofluorescence issues in bioapplications based on Tb^(3+)-doped EMU NCs.Herein,we report a novel sandwich structured core@shell@shell scheme for the design of EMU NCs,for example,NaLuF4∶Yb/Gd@NaGdF4∶Tm@NaLuF4∶Tb NCs,wherein Yb^(3+),Tm^(3+),and Tb^(3+)are incorporated separately into the inner core,middle shell,and outer shell,respectively.We found that in the sandwich structured NCs,the effective inter-shell energy transfer from Gd^(3+)in the middle shell to Tb^(3+)in the outer shell accelerated the Yb^(3+)-Tm^(3+)five-photon upconversion and the subsequent Tm^(3+)to Gd^(3+)energy transfer processes,which could eventually lead to almost complete inhibition of Tm^(3+)UV upconversion emissions,concurrent with the strong EMU emissions of Tb^(3+).Our findings might stimulate new concepts for manipulating upconversion emissions of lanthanide NCs.

关键词： lanthanide nanocrystals energy migration upconversion sandwich structured inter-shell energy transfer energy management

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Sub-10 nm lanthanide-doped SrFCl nanoprobes:Controlled synthesis,optical properties and bioimaging

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Journal of Rare Earths 2019年第7期37卷 691-698页

作者： Jiaojiao Wei Wei Lian Wei Zheng xiaoying shang Meiran Zhang Tao Dai Xueyuan Chen College of Chemistry Fuzhou UniversityFuzhou 350116China CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China

Alkaline-earth dihalide nanocrystals(NCs) such as SrFCl, owing to their high chemical stability and low phonon energy, are excellent host materials for lanthanide(Ln3+) doping to achieve desirable optical properties for various bioapplications, Herein, we report a novel strategy for the synthesis of sub-10 nm Ln3+-doped SrFCl NCs with efficient upconverting and downshifting luminescence through a facile onestep hot-injection method. Utilizing the temperature-dependent upconverting luminescence(UCL) from the thermally coupled 2H11/2 and 4S3/2 levels of Er3+, we showed the potential of SrFCl:Yb,Er NCs as sensitive UCL nanoprobes for non-contact thermal sensing with a maximum detection sensitivity of 0.0066 K-1, which is among the highest values for thermal sensing based on Er3+-activated UCL nanoprobes. Furthermore, by employing the intense downshifting luminescence from Tb3+ and Eu3+, we demonstrated the successful use of biotinylated SrFCl:Ce,Tb and SrFCl:Eu3+ nanoprobes for biotin receptor-targeted cancer cell imaging, thus revealing the great promise of SrFCl:Ln3+ nanoprobes for versatile bioapplications.

关键词： Lanthanide SrFCl nanocrystals Upconverting luminescence Thermal sensing Bioimaging Rare earths

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降雪、温差作用下大尺寸砂岩风化模拟试验研究

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岩石力学与工程学报 2024年第6期43卷 1519-1534页

作者：刘晓颖郭青林张博尚东娟余静裴强强敦煌研究院甘肃敦煌736200 国家古代壁画与土遗址保护工程技术研究中心甘肃敦煌736200 甘肃莫高窟文化遗产保护设计咨询有限公司甘肃敦煌736200 甘肃省敦煌文物保护研究中心甘肃敦煌736200

砂岩质石窟寺在冻融循环作用下,会引起不同程度的风化病害。以甘肃北石窟寺为研究对象,以所处赋存环境的多因素变量耦合关系为依据,在多场耦合实验室开展降雪-温差条件下的大尺寸砂岩风化模拟试验。结果表明,反复的降雪-温差作用下,在... 详细信息

砂岩质石窟寺在冻融循环作用下,会引起不同程度的风化病害。以甘肃北石窟寺为研究对象,以所处赋存环境的多因素变量耦合关系为依据,在多场耦合实验室开展降雪-温差条件下的大尺寸砂岩风化模拟试验。结果表明,反复的降雪-温差作用下,在微观上,冻胀消融使得砂岩表现出表层砂岩胶结物几乎全部消失,内部砂岩胶结方式以接触式为主以及孔隙增多增大的劣化特征;宏观上,呈现出水分入渗深度增大、损伤区域及损伤程度逐步扩展,并伴随着起翘脱落、变色加深、裂隙发育的表观现象,力学上,表现为强度逐渐降低的趋势,并根据不同岩性砂岩划分出5类响应敏感区域,揭示了降雪-温差作用下砂岩的渐进累计风化机制。

关键词：岩石力学砂岩石窟寺冻融循环降雪-温差多因素变量耦合风化机制

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Multiplexed intracellular detection based on dual-excitation/dualemission upconversion nanoprobes

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Nano Research 2020年第7期13卷 1955-1961页

作者： Jianxi Ke Shan Lu Zhuo Li xiaoying shang Xingjun Li Renfu Li Datao Tu Zhuo Chen Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China School of Physical Science and Technology ShanghaiTech UniversityShanghai 201210China University of Chinese Academy of Sciences Beijing 100049China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China

Multiplexed intracellular detection is desirable in biomedical sciences for its higher eficiency and accuracy compared to the single-analyte detection.However,it is very challenging to construct nanoprobes that possess multiple fluorescent signals to recognize the different intracellular species synchronously.Herein,we proposed a novel dual-excitation/dual-emission upconversion strategy for multiplexed detection through the design of upconversion nanoparticles(UCNP)loaded with two dyes for sensitization and quenching of the upconversion luminescence(UCL),respectively.Based on the two independent energy transfer processes of near-infrared(NIR)dye IR845 to UCNP and UCNP to visible dye PAPS-Zn,CIO-and Zn2+were simultaneously detected with a limit of detection(LOD)of41.4 and 10.5 nM,respectively.By tilizing a purpose built 830/980 nm dual-laser confocal microscope,both intrinsic and exogenous CIO and Zn2+in live MCF-7 cells have been accurately quantified.Such dual-excitation/dual-emission ratiometric UCL detection mode enables not only monitoring multiple intracellular analytes but also eliminating the detection deviation caused by inhomogeneous probe distribution in cells.Through modulation of NIR dye and visible dye with other reactive groups,the nanoprobes can be extended to analyze various intraellular species,which provides a promising tool to study the biological activities in live cells and diagnose diseases.

关键词： upconversion nanoparticles energy transfer dual-excitation dye sensitization ratiometric probe multiplexed detection

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Highly efficient luminescent Ⅰ-Ⅲ-Ⅵ semiconductor nanoprobes based on template-synthesized CuInS2 nanocrystals

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Nano Research 2019年第8期12卷 1804-1809页

作者： Xian Li Datao Tu Shaohua Yu Xiaorong Song Wei Lian Jiaojiao Wei xiaoying shang Renfu Li Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350007China

CuInS2 semiconductor nanocrystals (NCs) exhibit large absorption coefficient, size-dependent photoluminescence and low toxicity, making them excellent candidates in a variety of bioapplications. However, precise control of both their composition and morphology to improve the luminescent efficiency remains a great challenge via conventional direct synthesis. Herein, we present a novel low-temperature template synthesis of highly efficient luminescent CuInS2 nanoprobes from In2S3 NCs via a facile cation exchange strategy. The proposed strategy enables synthesis of a series of CuInS2 NCs with broad size tunability from 2.2 to 29.6 nm. Through rationally manipulating the stoichiometry of Cu/In, highly efficient luminescence of CuInS2 with the maximum quantum yield of 28.6% has been achieved, which is about one order of magnitude improvement relative to that of directly synthesized NCs. By virtue of the intense emission of CuInS2 nanoprobes, we exemplify their application in sensitive homogeneous biodetection for an important biomolecule of adenosine triphosphate (ATP) with the limit of detection down to 49.3 nM. Moreover, the CuInS2 nanoprobes are explored for ATP-targeted cancer cell imaging, thus revealing their great potentials in the field of cancer diagnosis and prognosis.

关键词： CuInS2 semiconductor nanocrystals cation exchange luminescent nanoprobes biosensing

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自体散光透镜重塑转位术矫正超高度散光1例

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中国眼耳鼻喉科杂志 2024年第S1期24卷 47-52页

作者：尚建慜黄佳王晓瑛周行涛复旦大学附属眼耳鼻喉科医院眼科上海200031

18岁男性,因“双眼散光”,要求行手术矫正就诊。患者诉自幼高度散光,无戴镜史。裸眼视力:右眼0.05,左眼0.15。主觉验光:右眼-4.00/-6.75×175°→1.0-,左眼+1.00/-11.00×175°→0.8。外观双眼睑裂狭长。裂隙灯检查未见明显异常。诊断... 详细信息

18岁男性,因“双眼散光”,要求行手术矫正就诊。患者诉自幼高度散光,无戴镜史。裸眼视力:右眼0.05,左眼0.15。主觉验光:右眼-4.00/-6.75×175°→1.0-,左眼+1.00/-11.00×175°→0.8。外观双眼睑裂狭长。裂隙灯检查未见明显异常。诊断为双眼超高度散光,双眼屈光参差,圆锥角膜待排;予配框架镜,定期随访。1年后,双眼角膜曲率较前略增加,予双眼跨上皮角膜交联手术。2年后,患者再次随访,要求手术矫正。检查发现角膜情况稳定,决定采用首创的自体散光透镜重塑转位术进行矫正:首先应用飞秒激光进行散光透镜制作,之后采用准分子激光重塑透镜,再对透镜进行90°转位,最后将角膜瓣复位完成矫正。术后裸眼视力在术后1个月起稳定在0.8,最佳矫正视力与术前保持稳定。主觉验光:右眼0/-1.25×100°→1.0,左眼+1.50/-1.50×150°→0.8。对于高度散光寻求手术矫正的患者,首先需要通过全面的检查和必要的随访判断是否有圆锥角膜的可能,是否有术后发生角膜扩张性疾病的风险,对于存疑的,可尝试跨上皮角膜交联手术稳定角膜情况,对于常规手术方式难以矫正的超高度散光,在角膜条件稳定的情况下,可尝试自体散光透镜重塑转位术,可获得较为满意的视觉效果,且能最大限度保留角膜组织,安全性高。

关键词：高度散光圆锥角膜透镜重塑透镜转位

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Effect of potential difference between nano-Al_(2)O_(3)whisker and Mg matrix on the dispersion of Mg composites

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International Journal of Minerals,Metallurgy and Materials 2023年第1期30卷 104-111页

作者： xiaoying Qian Hong Yang Chunfeng Hu Ying Zeng Yuanding Huang Xin shang Yangjie Wan Bin Jiang Qingguo Feng National Engineering Research Center for Magnesium Alloys Chongqing UniversityChongqing 400044China College of Materials Science and Engineering Chongqing UniversityChongqing 400044China Key Laboratory of Advanced Technologies of Materials Ministry of EducationSchool of Material Science and EngineeringSouthwest Jiaotong UniversityChengdu 610031China Institute of Metallic Biomaterials Helmholtz-Zentrum HereonMax-Planck-Str.1D-21502 GeesthachtGermany School of Mechanical Engineering Dongguan University of TechnologyDongguan 523808China

The potential difference between positive and negative ions was utilized to improve the homogenized dispersion of nanoscale Al_(2)O_(3) whiskers in Mg matrix composites.The Mg powders were decorated with sodium dodecylbenzene sulfonate(C_(18)H_(29)NaO_(3)S,SDBS)and were introduced to the cathode group on their surface.The Al_(2)O_(3) whiskers were modified by the cetyl trimethyl ammonium bromide(C_(19)H_(42)BrN,CTAB)and were featured in the anode group.The suitable contents of CTAB and SDBS,the application atmosphere,and the type of solvents were investigated.Dispersion results showed that adding 2wt%SDBS into Mg powders and adding 2wt%CTAB into Al_(2)O_(3) whiskers pro-moted the formation of more uniformly mixed composite powders,compared to those of conventional ball milling via scanning electron micro-scopy(SEM)analysis.Meanwhile,the calculated results derived from first-principle calculations also demonstrated the stronger cohesion between Al_(2)O_(3) whisker reinforcements and Mg matrix than undecorated composite powders.After preparation by powder metallurgy,the mor-phology,grain size,hardness,and standard deviation coefficient of composites were analyzed to evaluate the dispersed efficiency.The results indicated that the modification of homogenized dispersed Al_(2)O_(3) whiskers in composites contributed to the refinement of 26%in grain size and the improvement of 20%in hardness compared with pure Mg,and the reduction of 32.5%in the standard deviation coefficient of hardness compared with the ball-milling sample.

关键词： magnesium-based composites Al_(2)O_(3)whiskers potential difference dispersion

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超支化聚硅氧烷在改性BMI/CE树脂方面的研究进展

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山东化工 2024年第9期53卷 117-119页

作者：黄晓瑛尚宇王威王列平毛明珍西北工业大学化学与化工学院陕西西安710129 西安近代化学研究所氟氮化工资源高效开发与利用国家重点实验室陕西西安710065 陕西省环境监测中心站陕西西安710054

综述了近年来超支化聚硅氧烷改性双马来酰亚胺和氰酸酯树脂的研究进展,重点总结了超支化聚硅氧烷在改性树脂力学性能、热性能及阻燃性能方面的应用,并对超支化有机硅功能高分子未来的发展作出了展望。

关键词：超支化聚硅氧烷改性树脂

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联苯吡菌胺关键中间体3′,4′-二氯-5-氟-1,1′-联苯-2-胺的合成

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世界农药 2024年第1期46卷 38-41,49页

作者：黄晓瑛尚宇王威王列平毛明珍西安近代化学研究所氟氮化工资源高效开发与利用国家重点实验室西安710065 陕西省环境监测中心站西安710054

为获得联苯吡菌胺关键中间体3′,4′-二氯-5-氟-1,1′-联苯-2-胺的适合工业化生产工艺路线,对其合成工艺进行了优化。以3,4-二氯溴苯和2-溴-4-氟苯胺为原料,经格氏和Suzuki偶联2步反应合成了3′,4′-二氯-5-氟-1,1′-联苯-2-胺,其结构经... 详细信息

为获得联苯吡菌胺关键中间体3′,4′-二氯-5-氟-1,1′-联苯-2-胺的适合工业化生产工艺路线,对其合成工艺进行了优化。以3,4-二氯溴苯和2-溴-4-氟苯胺为原料,经格氏和Suzuki偶联2步反应合成了3′,4′-二氯-5-氟-1,1′-联苯-2-胺,其结构经1H NMR、MS表征确证,并对合成条件进行了优化。优化条件下,3′,4′-二氯-5-氟-1,1′-联苯2-胺合成总收率61.9%,纯度98%。该工艺成本低,收率高,具有工业化生产前景。

关键词： 3′,4′-二氯-5-氟-1,1′-联苯-2-胺合成联苯吡菌胺

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