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Silicon dioxide-protection boosting the peroxidase-like activity of Fe single-atom catalyst for combining chemo-photothermal therapy

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Nano Research 2024年第6期17卷 4924-4933页

作者： Yu Fan Yu Yi hongpan rong Jiatao Zhang Beijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green Applications School of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 100081China CAS Center for Excellence in Nanoscience CAS KeyLaboratory for Biomedical Effects of Nanomaterials and NanosafetyNational Center for Nanoscience and Technology(NCNST)Beijing 100190China Key Laboratory of Medical Molecule Science and Pharmaceutics Engineering Ministry of Industry and Information TechnologySchool of Chemistry&Chemical EngineeringBeijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green ApplicationsSchool of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China

Carbon-based single-atom catalysts(SACs)have been widely studied in the field of biomedicine due to their excellent catalytic performance.However,carbon-based SACs usually aggregate during pyrolysis,which leads to the reduction of catalytic activity.Here,we describe a method to improve the monodispersion of SACs using silicon dioxide as a protective layer.The decoration of silicon dioxide serves as a buffer layer for individual nanoparticles,which is not destroyed during the pyrolysis process,ensuring the single-particle dispersion of the nanoparticles after etching.This approach increased the hydroxyl groups on the surface of Fe-SAC(Fe-SAC-SE)and improved its water solubility,resulting in a four times enhancement of the peroxidase(POD)-like activity of Fe-SAC-SE(58.4 U/mg)than that of non-protected SACs(13.9 U/mg).The SiO_(2)-protection approach could also improve the catalytic activities of SACs with other metals such as Mn,Co,Ni,and Cu,indicating its generality for SACs preparation.Taking advantage of the high POD-like activity,photothermal properties,and large specific surface area of Fe-SAC-SE,we constructed a synergistic therapeutic system(Fe-SAC-SE@DOX@PEG)for combining the photothermal therapy,catalytic therapy,and chemotherapy.It was verified that the photothermal properties of Fe-SAC-SE@DOX@PEG could effectively improve its POD-like activity,exhibiting excellent tumor-killing performance at the cellular level.This work may provide a general approach to improve the performances of SACs for disease therapy and diagnosis.

关键词： single-atom catalysts peroxidase-like activity SiO2-protection photothermal therapy catalytic therapy chemotherapy

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Size-controlled synthesis of Fe3O4 and Fe3O4@SiO2 nanoparticles and their superparamagnetic properties tailoring

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Progress in Natural Science:Materials International 2023年第1期33卷 116-119页

作者： Muhammad Sajid Sidra Shuja hongpan rong Jiatao Zhang Beijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green Applications School of Materials Science & Engineering Beijing Institute of Technology Beijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green Applications Key Laboratory of Medical Molecule Science and Pharmaceutics Engineering School of Chemistry and Chemical Engineering Institute of Engineering Medicine Beijing Institute of Technology

Superparamagnetic properties and fine-tuning of colloidal Fe3O4nanoparticles are important for their widespread biomedical applications. Herein, colloidal Fe3O4nanoparticles(NPs) of different sizes(8–20 nm) were prepared,and their hydrophilization with SiO2shell coating to be Fe3O4@SiO2core-shell had been realized successively.The size of Fe3O4NPs was controlled by different heating rates. Transmission electron microscope(TEM), powder X-ray diffractometry(XRD), and vibrating sample magnetometer(VSM) were performed to examine the morphology, crystallinity, and magnetic properties of the prepared Fe3O4and Fe3O4@SiO2core-shell NPs,respectively. In addition, high resolution transmission electron microscope(HRTEM) results suggested that Fe3O4NPs had well crystallization. Enabled by such, their superparamagnetic properties can be fine-tuned accordingly and cater to their potential applications.

关键词： Fe 3 O 4 nanoparticles Fe 3 O 4 @SiO 2 hydrophilization Superparamagnetic Core-shell Aqueous inverse microemulsion

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Single-atom cobalt nanozymes promote spinal cord injury recovery by anti-oxidation and neuroprotection

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Nano Research 2023年第7期16卷 9752-9759页

作者： Yuxing Jiang Hongtao rong Yifan Wang Shange Liu Peng Xu Zhen Luo Lamei Guo Tao Zhu(✉) hongpan rong Dingsheng Wang Jiatao Zhang Yu Yi Hao Wang Tianjin Medical University General Hospital Tianjin 300052China CAS Center for Excellence in Nanoscience CAS Key Laboratory for Biomedical Effects of Nanomaterials and NanosafetyNational Center for Nanoscience and TechnologyBeijing 100190China Beijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green Applications Key Laboratory of Medical Molecule Science and Pharmaceutics EngineeringMinistry of Industry and Information TechnologySchool of Materials Science&EngineeringSchool of Chemistry and Chemical EngineeringInstitute of Engineering MedicineBeijing Institute of TechnologyBeijing 100081China Department of Chemistry Tsinghua UniversityBeijing 100084China University of Chinese Academy of Sciences Beijing 100049China

Oxidative stress and inflammation are central pathophysiological processes in a traumatic spinal cord injury(SCI).Antioxidant therapies that reduce the reactive oxygen and nitrogen species(RONS)overgeneration and inflammation are proved promising for improving the outcomes.However,efficient and long-lasting antioxidant therapy to eliminate multiple RONS with effective neuroprotection remains challenging.Here,a single-atom cobalt nanozyme(Co-SAzyme)with a hollow structure was reported to reduce the RONS and inflammation in the secondary injury of SCI.Among SAzymes featuring different single metal-N sites(e.g.,Mn,Fe,Co,Ni,and Cu),this Co-SAzyme showed a versatile property to eliminate hydrogen peroxide(H_(2)O_(2)),superoxide anion(O_(2)·^(-)),hydroxyl radical(·OH),nitric oxide(·NO),and peroxynitrite(ONOO^(-))that overexpressed in the early stage of SCI.The porous hollow structure also allowed the encapsulation and sustained release of minocycline for neuroprotection in synergy.In vitro results showed that the Co-SAzyme reduced the apoptosis and pro-inflammatory cytokine levels of microglial cells under oxidative stress.In addition,the Co-SAzyme combined with minocycline achieved remarkable improved functional recovery and neural repairs in the SCI-rat model.

关键词： single-atom catalysis spinal cord injury reactive oxygen and nitrogen species anti-inflammation neuroprotection

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Modulating the local coordination environment of single-atom catalysts for enhanced catalytic performance

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Nano Research 2020年第7期13卷 1842-1855页

作者： Xinyuan Li hongpan rong Jiatao Zhang Dingsheng Wang Yadong Li Beijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green Applications Experimental Center of Advanced Materials School of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 100081China Department of Chemistry Tsinghua UniversityBeijing 100084China

The local coordination environment of catalysts has been investigated ftor an extended period to obtain enhanced catalytic performance.Especially with the advancement of single-atom catalysts(SACs),research on the coordination environment has been advanced to the atomic level.The surrounding coordination atoms of central metal atoms play important roles in their catalytic activity,selectivity and stability.In recent years,remarkable improvements of the catalytic performance of SACs have been achieved by the tailoring of coordination atoms,coordination numbers and second-or higher-coordination shells,which provided new opportunities for the further development of SACs.In this review,the characterization of coordination environment,tailoring of the local coordination environment,and their related adjustable catalytic performance will be discussed.We hope this review will provide new insights on further research of SACs.

关键词： single-atom catalysts coordination environment catalytic performance energy conversion

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Compressive surface strained atomic-layer Cu2O on Cu@Ag nanoparticles

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Nano Research 2019年第5期12卷 1187-1192页

作者： Xiyue Zhu hongpan rong Xiaobin Zhang Qiumei Di Huishan Shang Bing Bai Jiajia Liu Jia Liu Meng Xu Wenxing Chen Jiatao Zhang Beijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green Applications Experimental Center of Advanced MaterialsSchool of Materials Science & EngineeringBeijing Institute of TechnologyBeijing 100081China Center for Nano Materials and Technology Japan Advanced Institute of Science and Technology1-1 AsahidaiNomiIshikawa 923-1292Japan

Control of surface structure at the atomic level can effectively tune catalytic properties of nanomaterials.Tuning surface strain is an effective strategy for enhancing catalytic activity;however,the correlation studies between the surface strain with catalytic performance are scant because such mechanistic studies require the precise control of surface strain on catalysts.In this work,a simple strategy of precisely tuning compressive surface strain of atomic-layer Cu2O on Cu@Ag (AL-Cu2O/Cu@Ag) nanoparticles (NPs) is demonstrated.The AL-Cu2O is synthesized by structure evolution of Cu@Ag core-shell nanoparticles,and the precise thickness-control of AL-Cu2O is achieved by tuning the molar ratio of Cu/Ag of the starting material.Aberration-corrected high-resolution transmission electron microscopy (AC-HRTEM) and EELS elemental mapping characterization showed that the compressive surface strain of AL-Cu2O along the [111] and [200] directions can be precisely tuned from 6.5% to 1.6% and 6.6% to 4.7%,respectively,by changing the number of AL-Cu2O layer from 3 to 6.The as-prepared AL-Cu2O/Cu@Ag NPs exhibited excellent catalytic property in the synthesis of azobenzene from aniline,in which the strained 4-layers Cu2O (4.5% along the [111] direction,6.1% along the [200] direction) exhibits the best catalytic performance.This work may be beneficial for the design and surface engineering of catalysts toward specific applications.

关键词： compressive surface strain atomic-layer Cu2O precise thickness-control catalytic activity

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Vacuum-tuned-atmosphere induced assembly of Au@Ag core/shell nanocubes into multi-dimensional superstructures and the ultrasensitive IAPP proteins SERS detection

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Nano Research 2019年第6期12卷 1375-1379页

作者： Meng Xu Guopeng Tu Muwei Ji Xiaodong Wan Jiajia Liu Jia Liu hongpan rong Yanlian Yang Chen Wang Jiatao Zhang Beijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green Applications Experim ental Center of Advanced Materials School of Materials Science & EngineeringBeijing Institute of TechnologyBeijing 100081China Institute of Low-dimensional Materials Genome Initiative College of chemistry and environmental engineeringShenzhen UniversityGuangdong Shenzhen 518060China Graduate School at Shenzhen Tsinghua UniversityShenzhen 518055China National Center for Nanoscience and Technology (NCNST) Chinese Academy of SciencesBeijing 100190China

Utilizing vacuum-tuned-atmosphere induced dip coating method,we achieve the cross-dimensional macroscopic diverse self-assemblies by using one building block with one chemical functionality.Coordinated modulating the vacuum degree,colloid concentration and evaporation atmosphere,Au@Ag core/shell nanocubes (NCs) can controllably assemble into diverse multi-dimensional superstructures.Under 0.08 MPa,we obtained the two-dimensional (2D) stepped superstructures with continuously tunable step width.In addition,we generated a series of tailorable nanoscale-roughened 2D Au@Ag NCs superstructures at 0.04 MPa,which exhibited the label-free ultrasensitive SERS detection for the different mutants of IAPP8-37 proteins.Under 0.01 MPa,we obtained the cross-dimensional tailorable Au@Ag NCs assemblies from random to macroscale 2D and three-dimensional (3D) densest superstructures by adjusting the capping ligand-environmental molecule interactions.This is a flexible method to generate as-prepared Au@Ag core/shell NCs into well-defined macroscopic diverse superstructures and to promote the exploitation into biological applications.

关键词： superstructure Au@Ag core/shell nanocubes (NCs) self-assembly surface enhanced Raman scattering (SERS) detection islet arnyloid-like polypeptide

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大麦HhH-DGS全基因组鉴定及表达分析

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分子植物育种 2022年第23期20卷 7657-7670页

作者：王容蔡海亚焦春海安兵壮王红盼李博杨彩仙徐延浩长江大学农学院荆州434100 湖北省农业科学院粮食作物研究所粮食作物种质创新与遗传改良湖北省重点实验室武汉430064

螺旋-发夹-螺旋DNA糖基化酶超基因家族(helix-hairpin-helix DNA glycosylases superfamily,HhH-DGS)是DNA碱基切除修复(base excision repair, BER)的关键酶之一,在保持基因组的稳定中发挥着重要作用。本研究分析了大麦(Hordeum vulgare L.) HhH-DGS基因家族的分子特征、系统发育、组织表达模式并探究了该基因家族对辐射的响应规律。在大麦基因组的6条染色体上共鉴定到15个HhH-DGS基因,系统发育将其分为9个亚群。不同亚族间HhH-DGS基因外显子数量变异很大,为2~12个。种间与种内共线性分析表明,该基因家族存在于单子叶与双子叶分化前,在大麦基因组内没有发生大规模扩增。HhH-DGS基因启动子含有大量的光调节因子。大麦萌发期的茎基部及花前期的顶端组织中HhH-DGS基因表达量显著高于其他组织器官;HhH-DGS基因HORVU.MOREX.r3.7HG0667530、HORVU.MOREX.r3.3HG0221280、HORVU.MOREX.r3.3HG0223220和HORVU.MOREX.r3.6HG0561680在大麦不同的器官中稳定表达,并在4种辐射处理后表达都上调。HORVU.MOREX.r3.5HG0469860、HORVU.MOREX.r3.7HG0634400和HORVU.MOREX.r3.1HG0074440表现出特异辐射方式响应模式。本研究在解析大麦HhH-DGS基因家族的特征、进化与功能的基础上,为大麦辐射育种提供了参考。

关键词：大麦 HhH-DGS家族碱基切除修复表达模式辐射应答

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铂基金属间化合物纳米晶的最新进展:可控合成与电催化应用

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物理化学学报 2020年第9期36卷 95-116页

作者：杨天怡崔铖戎宏盼张加涛王定胜北京理工大学材料学院结构可控先进功能材料与绿色应用北京市重点实验室北京100081 清华大学化学系北京100084

铂基金属间化合物纳米晶因其高度有序的结构特点,优异的抗氧化及耐腐蚀性能,作为电极材料被广泛应用于各类电催化反应,目前已有的PtCo金属间化合物纳米晶在燃料电池阴极反应(氧还原反应)中的活性和稳定性均达到了美国能源部(DOE)2020年... 详细信息

铂基金属间化合物纳米晶因其高度有序的结构特点,优异的抗氧化及耐腐蚀性能,作为电极材料被广泛应用于各类电催化反应,目前已有的PtCo金属间化合物纳米晶在燃料电池阴极反应(氧还原反应)中的活性和稳定性均达到了美国能源部(DOE)2020年的目标。为了进一步提高金属间化合物纳米晶的电催化性能,需要对影响纳米晶电催化性能的因素进行深入研究。本文综述了铂基金属间化合物纳米晶的研究现状,着重介绍了铂基金属间化合物的可控合成策略及其在电催化领域的最新研究进展,分析总结了该领域存在的问题,并展望了其未来发展方向。

关键词：铂基金属间化合物纳米晶可控合成结构有序电催化反应

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零维纳米晶体自组装形成微米级二维准纳米片:从单组分到多组分组装单元

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Science China Materials 2020年第7期63卷 1265-1271页

作者：常瑜徐萌黄柳潘容容刘佳佳刘佳戎宏盼陈文星张加涛 Beijing Key Laboratory of Construction-Tailorable Advanced Functional Materials and Green Applications Experimental Center of Advanced MaterialsSchool of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 100081China

胶体纳米晶(NCs)具有优良的性能和广阔的应用前景,将其自下而上自组装形成结构复杂且可控的大面积超晶格是一个重要的研究方向.等离子体纳米晶之间可控的间隙有益于电场增强,因此常常被用作组装单元来构建长程有序的大面积超结构,尤其... 详细信息

胶体纳米晶(NCs)具有优良的性能和广阔的应用前景,将其自下而上自组装形成结构复杂且可控的大面积超晶格是一个重要的研究方向.等离子体纳米晶之间可控的间隙有益于电场增强,因此常常被用作组装单元来构建长程有序的大面积超结构,尤其是单层纳米晶的大规模组装.本文采用溶剂挥发诱导气-液界面自组装工艺,成功得到了由单组分Au纳米晶和多组分Au@ZnS核壳异质纳米晶(HNCs)自组装形成的大面积二维准纳米片(QNS).整个自组装过程在气-液界面上进行,通过改变环境温度和胶体纳米晶溶液的浓度来对自组装过程进行调控,即通过精确控制溶剂的挥发速率和胶体纳米晶浓度,可以获得不同层数、不同堆积模式的大面积二维准纳米片.

关键词：纳米片自组装纳米晶体长程有序溶剂挥发组装工艺环境温度挥发速率

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表面等离子共振热电子注入机理及在光催化与光电催化应用中的研究进展

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应用化学 2018年第8期35卷 890-901页

作者：刘佳潘容容张二欢李岳美刘佳佳徐萌戎宏盼陈文星张加涛北京理工大学材料学院结构可控先进功能材料与绿色应用北京市重点实验室北京100081

由于金属纳米晶表面等离子共振产生的热电子效应,金属/半导体异质纳米晶的可控合成对于增强半导体光催化与光电催化性能具有显著的促进作用。本综述阐述了热电子产生与驰豫的微观机制,探讨了影响热电子在金属-半导体异质纳米晶中界面传... 详细信息

由于金属纳米晶表面等离子共振产生的热电子效应,金属/半导体异质纳米晶的可控合成对于增强半导体光催化与光电催化性能具有显著的促进作用。本综述阐述了热电子产生与驰豫的微观机制,探讨了影响热电子在金属-半导体异质纳米晶中界面传递效率的关键因素及异质界面调控合成的重要性,简要介绍了热电子注入效应在光催化与光电催化制备太阳能燃料研究中的应用进展,分析了目前存在的主要问题并对该领域未来的发展趋势进行了展望。

关键词：金属/半导体异质纳米晶表面等离子共振光催化光电催化热电子注入

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