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Lanthanide-DNA supramolecular hydrogels with tunable and responsive luminescence

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Science China(Technological Sciences) 2022年第5期65卷 1043-1051页

作者： YANG Sen PAN XiaoRui TANG JianPu YAO Chi YANG DaYong Frontiers Science Center for Synthetic Biology Key Laboratory of Systems Bioengineering(MOE)Institute of Biomolecular and Biomedical EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin300350China

Supramolecular DNA hydrogels have been synthesized based on the assembly of DNA building-blocks such as branched DNA and long DNA chains.The structures and functions of sole-module DNA hydrogels remain limitations.New methodologies by integrating hybrid components are desired to expand the synthesis of DNA hydrogel.Herein,we synthesized a Ln^(3+)-containing luminescent supramolecular hydrogel by employing the coordination and electrostatic interactions between lanthanide ions(Tb^(3+)and Eu^(3+))and linear single-stranded DNA(ssDNA).Through the coordination between ssDNA and Ln^(3+),a series of luminescent supramolecular hydrogels were synthesized,among which the Tb-G_(n)/T_(n)and Eu-T_(n)hydrogels emitted the characteristic luminescence of Tb and Eu,respectively.The luminescent intensities of the hydrogels were adjusted by designing DNA sequences with programmable bases and chain lengths.Notably,the Tb/Eu co-doped luminescent supramolecular hydrogel displayed tunable luminescence from green to yellow by regulating the stoichiometric ratio of Tb/Eu.Moreover,the hydrogel had reversible luminescent stimulation responsiveness toward Ag^(+)/L-Cys.We expected that the synthesis of Ln^(3+)-containing luminescent supramolecular hydrogels enriched the strategies of the construction of DNA hydrogels,and promoted the development of stimuli-responsive supramolecular materials.

关键词： DNA hydrogel supramolecular self-assembly luminescent hydrogel lanthanide complex stimuli-responsiveness

Construction of Polymeric DNA Network and Application for Cell Manipulation

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Chinese Journal of Chemistry 2023年第15期41卷 1875-1887页

作者： Lele Chang Rui Zhang Jing Wang Chi Yao Dayong Yang Frontiers Science Center for Synthetic Biology Key Laboratory of Systems Bioengineering(MOE)Institute of Biomolecular and Biomedical EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin300350China

Comprehensive Summary Deoxyribonucleic acid(DNA)is a biomacromolecule,as well as a polymeric material,whose sequences with different manipulative structures enable them to implement a series of functions,such as reorganization,target,and catalysis.Compared to existing traditional materials incapable of multifunctional integration,the polymeric DNA network is a form of material that can achieve functional integration while maintaining specific DNA properties.Furthermore,precise target enabled by DNA network is one of the most essential components of cellular manipulation.Hence,the DNA network is indispensable and irreplaceable to cell manipulation that it is a versatile tool for the understanding of basic laws of living life and treatments of diseases,such as cell isolation,cell delivery,and cell interference.Herein,the construction of polymeric DNA network is briefly introduced from the aspects of assembly modules,construction methods,and properties.

关键词： DNA network DNA nanotechnology Cell manipulation Cell isolation and interference

Selective hydrodeoxygenation of guaiacol to cyclohexanol using activated hydrochar-supported Ru catalysts

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Frontiers of Chemical Science and engineering 2024年第5期18卷 13-22页

作者： Kaile Li Shijie Yu Qinghai Li Yanguo Zhang Hui Zhou Key laboratory for Thermal Science and Power engineering of Ministry of Education Beijing Key Laboratory of CO2 Utilization and Reduction TechnologyDepartment of Energy and Power EngineeringTsinghua UniversityBeijing 100084China Department of Chemical and biomolecular engineering National University of SingaporeSingapore117585Singapore

Lignin,an abundant aromatic polymer in nature,has received significant attention for its potential in the production of bio-oils and chemicals owing to increased resource availability and environmental issues.The hydrodeoxygenation of guaiacol,a lignin-derived monomer,can produce cyclohexanol,a nylon precursor,in a carbon-negative and environmentally friendly manner.This study explored the porous properties and the effects of activation methods on the Ru-based catalyst supported by environmentally friendly and cost-effective hydrochar.Highly selective cleavage of C_(ary)-O bonds was achieved under mild conditions(160°C,0.2 MPa H2,and 4 h),and alkali activation further improved the catalytic activity.Various characterization methods revealedthat hydrothermal treatment and alkali activation relatively contributed to the excellent performance of the catalysts and influenced their porous structure and Ru dispersion.X-ray photoelectron spectroscopy results revealed an increased formation of metallic ruthenium,indicating the effective regulation of interaction between active sites and supports.This synergistic approach used in this study,involving the valorization of cellulose-derived hydrochar and the selective production of nylon precursors from lignin-derived guaiacol,indicated the comprehensive and sustainable utilization of biomass resources.

关键词： hydrochar guaiacol cyclohexanol activation full-component utilization

A step through the looking glass

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Science China(Life Sciences) 2016年第9期59卷 979-980页

作者： Youyun Liang Ee Lui Ang Huimin Zhao Metabolic engineering Research laboratory Science and Engineering InstitutesAgency for Science Technology and Research Department of Chemical and biomolecular engineering University of Illinois at Urbana-Champaign

Despite our many advances in deconstructing and understanding cellular and biomolecular machineries,the homochirality of life remains an enigma.Since our earliest ancestors,the central dogma has operated solely on

关键词：镜子分子机器中心法则

具有协同双导电层的超疏水导电橡皮筋用于宽范围敏感应变传感器

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Science Bulletin 2022年第16期67卷 1669-1678,M0004页

作者：孙红玲卜一冰刘虎王靖雯杨文科栗乾明郭占虎刘春太申长雨 Key laboratory of Materials Processing and Mold(Zhengzhou University) Ministry of EducationNational Engineering Research Center for Advanced Polymer Processing TechnologyZhengzhou UniversityZhengzhou 450002China National laboratory of Solid State Microstructures College of Engineering and Applied SciencesNanjing UniversityNanjing 210023China Integrated Composites laboratory(ICL) Department of Chemical&Biomolecular EngineeringUniversity of TennesseeKnoxville TN 37996USA

随着可穿戴智能设备的快速发展,迫切需要低成本、高灵敏度、低检测限、环境耐候性佳的可穿戴柔性应变传感器.本文采用“溶胀-涂敷”工艺在橡皮筋表面依次构筑了稳定的碳纳米管(CNTs)层和具有超灵敏微裂纹结构的石墨烯(rGO)层,由其制备... 详细信息

随着可穿戴智能设备的快速发展,迫切需要低成本、高灵敏度、低检测限、环境耐候性佳的可穿戴柔性应变传感器.本文采用“溶胀-涂敷”工艺在橡皮筋表面依次构筑了稳定的碳纳米管(CNTs)层和具有超灵敏微裂纹结构的石墨烯(rGO)层,由其制备的应变传感器在双导电层的协同作用下具有极低的检测限(0.1%应变)、高灵敏度(482%应变下的灵敏度为685.3)、宽工作应变范围(0~482%)、快速响应/恢复(200 ms/200 ms),以及良好的可靠性和可重复性(>1000循环).进一步,通过疏水性气相二氧化硅(Hf-SiO_(2))的处理,赋予其优异的超疏水性、自清洁性和耐腐蚀性,使该传感器即使在水环境中也可实现对人体运动和生理信号的全方位监测.此外,所制备的超疏水导电橡皮筋还可以编织成触觉感知电子纺织品,用于空间压力分布测量.该研究所制备的高性能柔性应变传感器在新一代智能可穿戴电子领域具有巨大的应用潜力.

关键词：超疏水应变传感器气相二氧化硅橡皮筋导电层生理信号耐腐蚀性可穿戴

Quantification/mechanism of interfacial interaction modulated by electric potential in aqueous salt solution

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Friction 2021年第3期9卷 513-523页

作者： Shaowei LI Pengpeng BAI Yuanzhe LI Noshir SPESIKA Yonggang MENG Liran MA Yu TIAN State Key laboratory of Tribology Department of Mechanical EngineeringTsinghua UniversityBeijing 100084China Department of Chemical and biomolecular engineering Tulane UniversityNew OrleansLA 70118USA

With the development of surface and interface science and technology,methods for the online modulation of interfacial performance by external stimuli are in high demand.Switching between ultra-low and high friction states is a particular goal owing to its applicability to the development of precision machines and nano/micro-electromechanical systems.In this study,reversible switching between superlubricity and high friction is realized by controlling the electric potential of a gold surface in aqueous salt solution sliding against a SiO_(2) microsphere.Applying positive potential results creates an ice-like water layer with high hydrogen bonding and adhesion at the interface,leading to nonlinear high friction.However,applying negative potential results in free water on the gold surface and negligible adhesion at the interface,causing linear ultra-low friction(friction coefficient of about 0.004,superlubricity state).A quantitative description of how the external load and interfacial adhesion affected friction force was developed,which agrees well with the experimental results.Thus,this work quantitatively reveals the mechanism of potential-controlled switching between superlubricity and high-friction states.Controlling the interfacial behavior via the electric potential could inspire novel design strategies for nano/micro-electromechanical and nano/micro-fluidic systems.

关键词： electrochemical potential reversible switching superlubricity nonlinear friction adhesion

光催化CO_(2)还原多原子催化剂的设计与制备进展

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Science China Materials 2024年第2期67卷 397-423页

作者：汪忠浩邹国军 Jong Hyeok Park 张侃 School of Materials Science and engineering and School of Chemistry and Chemical engineering Nanjing University of Science and TechnologyNanjing 210094China Department of Chemical and biomolecular engineering Yonsei University50 Yonsei-roSeodaemun-guSeoul120-749Republic of Korea Chemistry and Chemical engineering Guangdong laboratory Shantou 515031China

光催化CO_(2)还原合成太阳能燃料对缓解CO_(2)排放引起的全球变暖和降低化石燃料消耗具有重要意义.然而,目前的光催化剂仍然存在反应动力学缓慢和选择性不理想的问题,特别是对于C_(2+)产物的生成,极大地限制了光催化的工业化进程.过去... 详细信息

光催化CO_(2)还原合成太阳能燃料对缓解CO_(2)排放引起的全球变暖和降低化石燃料消耗具有重要意义.然而,目前的光催化剂仍然存在反应动力学缓慢和选择性不理想的问题,特别是对于C_(2+)产物的生成,极大地限制了光催化的工业化进程.过去几十年中,关于太阳能驱动的CO_(2)还原的研究展示出鼓舞人心的结果,包括活性位点的构建.本综述重点介绍了通过构建活性位点制备原子级分散催化剂在光催化CO_(2)还原中的最新进展,包括两个独立的活性位点、成对双活性位点和基于活性位点构型的纳米团簇.此外,详细讨论了CO_(2)在活性位点上的活化机制和表征方法.特别是考虑到实验研究与实际应用之间的差距,整合实验和理论的结果,以实现潜在的结构-活性关系和高目标产物选择性发展.最后,概述了该领域存在的挑战,并展望了活性位点的合理设计和机理研究.

关键词： photocatalytic CO_(2)reduction precise engineering multiple active sites structure-activity relationships mechanistic investigation

Hybridization chain reaction-based DNA nanomaterials for biosensing,bioimaging and therapeutics

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Chinese Chemical Letters 2024年第2期35卷 223-231页

作者： Zhaoyue Lv Mengxue Huang Peiran Li Mengdi Xu Chi Yao Dayong Yang Frontiers Science Center for Synthetic Biology Key Laboratory of Systems Bioengineering (MOE)Institute of Biomolecular and Biomedical EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China Zhejiang Institute of Tianjin University Ningbo 315201China

DNA nanomaterials hold great promise in biomedical fields due to its excellent sequence programmability,molecular recognition ability and biocompatibility.Hybridization chain reaction(HCR)is a simple and efficient isothermal enzyme-free amplification strategy of DNA,generating nicked double helices with repeated units.Through the design of HCR hairpins,multiple nanomaterials with desired functions are assembled by DNA,exhibiting great potential in biomedical applications.Herein,the recent progress of HCR-based DNA nanomaterials for biosensing,bioimaging and therapeutics are summarized.Representative works are exemplified to demonstrate how HCR-based DNA nanomaterials are designed and constructed.The challenges and prospects of the development of HCR-based DNA nanomaterials are discussed.We envision that rationally designing HCR-based DNA nanomaterials will facilitate the development of biomedical applications.

关键词： DNA nanotechnology Hybridization chain reaction DNA nanomaterials Biosensing Bioimaging Therapeutics

Interface catalytic reduction of alumina by nickle for the aluminum nanowire growth: Dynamics observed by in situ TEM

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Nano Research 2024年第3期17卷 1225-1231页

作者： Zichun Wang Dan Wang Ang Li Lizhuo Wang Xiaodong Han Yijiao Jiang Jianfeng Chen Jun Huang Beijing Advanced Innovation Center for Soft Matter Science and engineering State Key Laboratory of Organic–Inorganic CompositesBeijing University of Chemical TechnologyBeijing 100029China laboratory for Catalysis engineering School of Chemical and Biomolecular EngineeringThe University of SydneyNew South Wales 2006Australia Beijing Key laboratory of Microstructure and Property of Advanced Materials Beijing University of TechnologyBeijing 100024China Department of engineering Macquarie UniversitySydneyNew South Wales 2109Australia

Metal nanowires show promise in a broad range of applications and can be fabricated via a number of methods,such as vapor–liquid–solid process and template-based electrodeposition.However,the synthesis of Al nanowires(NWs)is still challenging from the stable alumina substrate.In this work,the Ni-catalyzed fabrication of Al NWs has been realized using various Al_(2)O_(3) substrates.The growth dynamics of Al NWs on Ni/Al_(2)O_(3) was studied using in situ transmission electron microscopy(TEM).The effect of alumina structures,compositions,and growth temperature were investigated.The growth of Al NWs correlates with the Na addition to the alumina support.Since no eutectic mixture of nickel aluminide was formed,a mechanism of Ni-catalyzed reduction of Al_(2)O_(3) for Al NWs growth has been proposed instead of the vapor–liquid–solid mechanism.The key insights reported here are not restricted to Ni-catalyzed Al NWs growth but can be extended to understanding the dynamic change and catalytic performance of Ni/Al_(2)O_(3) under working conditions.

关键词： in situ transmission electron microscopy(TEM) Al nanowires alumina reduction nanowire growth