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Liquid metal biomaterials: translational medicines,challenges and perspectives

National Science Review 2024年第2期11卷 264-284页

作者： Hanchi Xu Jincheng Lu Yikuang Xi Xuelin Wang Jing Liu Department of Biomedical Engineering School of Medicine Tsinghua University Beijing Tsinghua Changgung Hospital School of Clinical Medicine Tsinghua University Shanghai World Foreign Language Academy Beijing Advanced Innovation Center for Biomedical Engineering School of Engineering MedicineBeihang University Beijing Key lab.of Cryo-Biomedical Engineering and Key lab.of Cryogenics Technical Institute of Physics and Chemistry Chinese Academy of Sciences

Until now, significant healthcare challenges and growing urgent clinical requirements remain incompletely addressed by presently availab.e biomedical materials. This is due to their inadequate mechanical compatibility, suboptimal physical and chemical properties, susceptibility to immune rejection, and concerns about long-term biological safety. As an alternative, liquid metal(LM) opens up a promising class of biomaterials with unique advantages like biocompatibility, flexibility, excellent electrical conductivity,and ease of functionalization. However, despite the unique advantages and successful explorations of LM in biomedical fields, widespread clinical translations and applications of LM-based medical products remain limited. This article summarizes the current status and future prospects of LM biomaterials, interprets their applications in healthcare, medical imaging, bone repair, nerve interface, and tumor therapy, etc.Opportunities to translate LM materials into medicine and obstacles encountered in practices are discussed.Following that, we outline a blueprint for LM clinics, emphasizing their potential in making new-generation artificial organs. Last, the core challenges of LM biomaterials in clinical translation, including bio-safety,material stability, and ethical concerns are also discussed. Overall, the current progress, translational medicine bottlenecks, and perspectives of LM biomaterials signify their immense potential to drive future medical breakthroughs and thus open up novel avenues for upcoming clinical practices.

关键词： liquid metal biomaterials translational medicine clinical device healthcare therapeutics

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Editorial

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Magnetic Resonance Letters 2024年第2期4卷 1-1页

作者： Yong Yang Riqiang Fu Hua Huo State Key lab.of Physical chemistry of Solid Surfaces Xiamen UniversityChina National High Magnetic Field lab.(NHMFL) Florida State UniversityUSA School of chemistry and Chemical Engineering Harbin Institute of TechnologyChina

In pursuit of higher energy density,lower cost,longer lifespan and safety,remarkable research efforts have been taken to innovate various types of energy storage materials/devices,especially metal-ion batteries such as Li-ion batteries(LIBs).One of the major challenges is to elucidate the working mechanisms and/or the controlling factors of any new material in a full battery,which requires adequate characterization/diagnosis techniques.Among the numerous electrochemical ex-situ and insitu characterization techniques,magnetic resonance techniques,including nuclear magnetic resonance(NMR),magnetic resonance imaging(MRI)and electron paramagnetic resonance(EPR),are unique in terms of providing structural information at the atomic level and real-time phase and morphology evolution and characterizing ionic motion at various timescales.This special issue is dedicated to an editorial and a selection of papers on the theme of investigating energy storage materials/devices using magnetic resonance techniques.As the guest editors of this special issue,we are honored to introduce the following high-quality research articles and review articles.

关键词： NMR pursuit characterizing

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Supramolecular systems for bioapplications:recent research progress in China

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Science China chemistry 2024年第5期67卷 1397-1441页

作者： Yue-Yang Liu Xiao-Yong Yu Yu-Chen Pan Hang Yin Shuang Chao Yujie Li He Ma Minzan Zuo Kun-Xu Teng Jun-Li Hou Yong Chen Dong-Sheng Guo Ruibing Wang Yuxin Pei Zhichao Pei Jiang-Fei Xu Xiao-Yu Hu Chunju Li Qing-Zheng Yang Leyong Wang Yu Liu Zhan-Ting Li State Key lab.ratory of Organometallic chemistry Key Laboratory of Synthetic and Self-Assembly Chemistry for Organic Functional MoleculesShanghai Institute of Organic ChemistryChinese Academy of SciencesUniversity of Chinese Academy of SciencesShanghai 200032China Department of chemistry Fudan UniversityShanghai 200438China College of chemistry State Key Laboratory of Elemento-Organic ChemistryCollaborative Innovation Center of Chemical Science and EngineeringNankai UniversityTianjin 300071China State Key lab.ratory of Quality Research in Chinese Medicine Institute of Chinese Medical SciencesUniversity of MacaoMacao 999078China College of chemistry&Pharmacy Northwest A&F UniversityYangling 712100China Key lab.of Organic Optoelectronics&Molecular Engineering Department of ChemistryTsinghua UniversityBeijing 100084China College of Materials Science and Technology Nanjing University of Aeronautics and AstronauticsNanjing 211106China Key lab.ratory of Radiopharmaceuticals Ministry of EducationCollege of ChemistryBeijing Normal UniversityBeijing 100875China Tianjin Key lab.ratory of Structure and Performance for Functional Molecules College of ChemistryTianjin Normal UniversityTianjin 300387China State Key lab.ratory of Analytical chemistry for Life Science Jiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Supramolecular systems feature dynamic,reversible and stimuli-responsive characteristics,which are not easily achieved by molecular entities.The last decade has witnessed tremendous advances in the investigations of supramolecular systems for various bioapplications,which include drug delivery,anticancer therapy,antibacterial therapy,photodynamic therapy,photothermal therapy,combination therapy,antidotes for residual drugs or toxins,and bioimaging and biosensing.Host-guest chemistry has played a key role in the development of such bioactive supramolecular systems,and natural macrocycles(such as cyclodextrins),synthetic macrocycles(such as calixarenes,cucurbit[n]urils,and pillararenes),and porous framework polymers(such as supramolecular organic frameworks and flexible organic frameworks)have been most successfully used as hosts to build different kinds of host-guest systems for attaining designed biofunctions.The self-assembly of rationally designed amphiphilic molecules,macromolecules and polymers represent another important approach for the construction of supramolecular architectures with advanced biofunctions.In this review,we summarize the important contributions made by Chinese researchers in this field,with emphasis on those reported in the past five years.

关键词： host-guest chemistry drug delivery anticancer and antibacterial photodynamic therapy photothermal therapy antidote transmembrane channel bioimaging and biosensing

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Lattice-distorted Pt wrinkled nanoparticles for highly effective hydrogen electrocatalysis

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Nano Research 2024年第5期17卷 3819-3826页

作者： Xue Li Xiang Han Zhenrui Yang Shun Wang Yun Yang Juan Wang Jiadong Chen Zhongwei Chen Huile Jin Wenzhou Key lab.of Advanced Energy Storage and Conversion Zhejiang Province Key Lab of Leather EngineeringCollege of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China Institute of New Materials and Industry Technology College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China Department of Chemical Engineering Waterloo Institute for NanotechnologyUniversity of WaterlooWaterlooOntario N2L 3G1Canada

Modulating Pt surfaces through the introduction of lattice distortion emerges as immensely effective strategy that enhances the kinetics of alkaline hydrogen evolution and oxidation processes.In this study,we fabricated lattice-distorted Pt wrinkled nanoparticles(LD-Pt WNPs)for efficient hydrogen electrocatalysis.The LD-Pt WNPs not only outperform the Pt/C benchmark in hydrogen oxidation reaction,achieving an excellent mass-specific current of 968.5 mA·mg_(Pt)^(-1)(9 times that of Pt/C),but also demonstrate outstanding hydrogen evolution reaction activity with a small overpotential of 58.0 mV.Comprehensive experiments and density functional theory calculations reveal that lattice defects introduce an abundance of unsaturated coordination atoms while modifying the d-band center of Pt.This dual effect optimizes the binding strength of crucial H and OH intermediates,leading to a significant reduction in the energy barrier of the reaction bottleneck,commonly known as the Volmer step.This work unveils a fresh viewpoint on projecting and developing high efficiency electrocatalysts through defect engineering.

关键词： distortion nanoparticle hydrogen evolution reaction defect engineering hydrogen oxidation reaction

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Intrinsic pentagon defect engineering in multiple spatial-scale carbon frameworks for efficient triiodide reduction

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Journal of Energy chemistry 2024年第8期95卷 20-28页

作者： Siyi Hou Xuedan Song Chang Yu Jiangwei Chang Yiwang Ding Yingbin Liu Xiubo Zhang Weizhe Liu Jieshan Qiu State Key lab.of Fine Chemicals Liaoning Key Lab for Energy Materials and Chemical Engineering Frontier Science Center for Smart Materials School of Chemical EngineeringDalian University of Technology Liaoning Key lab.for Energy Materials and Chemical Engineering Frontier Science Center for Smart Materials School of Chemistry Dalian University of Technology State Key lab.ratory of Chemical Resource Engineering College of Chemical Engineering Beijing University of Chemical Technology

Intrinsic topological defect engineering has been proven as a promising strategy to elevate the electrocatalytic activity of carbon materials. However, the controllab.e construction of high-density and specific topological defects in carbon frameworks to reveal the relationship between reactivity and defect structure remains a challenging task. Herein, the intrinsic pentagon carbon sites that can favor electron overflow and enhance their binding affinity towards the intermediates of catalytic reaction are firstly presented by the work function and the p-band center calculations. To experimentally verify this, the cage-opening reaction of fullerene is proposed and utilized for synthesizing carbon quantum dots with specific pentagon configuration(CQDs-P), subsequently utilizing CQDs-P to modulate the micro-scale defect density of three-dimensional reduced graphene oxide(rGO) via π-π interactions. The multiple spatial-scale rGO-conjugated CQDs-P structure simultaneously possesses abundant pentagon and edge defects as catalytic active sites and long-range-ordered π electron delocalization system as conductive network. The defects-rich CQDs-P/rGO-4 all-carbon-based catalyst exhibits superb catalytic activity for triiodide reduction reaction with a high photoelectric conversion efficiency of 8.40%, superior to the Pt reference(7.97%). Theoretical calculations suggest that pentagon defects in the carbon frameworks can promote charge transfer and modulate the adsorption/dissociation behavior of the reaction intermediates, thus enhancing the electrocatalytic activity of the catalyst. This work confirms the role of intrinsic pentagon defects in catalytic reactions and provides a new insight into the synthesis of defects-rich carbon catalysts.

关键词： Carbon quantum dots Defect engineering Electrocatalytic activity Pentagon carbon Triiodide reduction

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Bimolecular reduction of carbon dioxide: double synthons for alkynes trifunctionalization

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Science China chemistry 2024年第3期67卷 841-847页

作者： Wenfang Xiong Xiaobin Tan Hongjian Liu Baiyao Zhu Jinwu Zhao Jianxiao Li Chaorong Qi Huanfeng Jiang School of Pharmacy Guangdong Medical UniversityDongguan 523808China Key lab.of Functional Molecular Engineering of Guangdong Province School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China

Carbon dioxide reduction, as a sustainable and versatile strategy for the access of chemical fuels, has attracted increasing attention and enormous efforts have been devoted to it in recent years. However, employing carbon dioxide as double synthons via bimolecular reduction remains challenging. Here, by leveraging the bimolecular reduction of carbon dioxide to carbonyl and methyl respectively, we describe a Pd-catalyzed trifunctionalization of alkynes with aryl iodide for the first time and showcase its advantages on the formation of various β-diketones and their application in the constructing of heterocyclic compounds with important biological activity, including pyrimidine, oxazole, pyrazole.

关键词： carbon dioxide bimolecular reduction trifunctionalization double synthons

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Nearly lattice-defect-free MOF membranes

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Science China chemistry 2024年第3期67卷 741-743页

作者： Yuzhang Zhu Yang Liu Jian Jin i-lab Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123China College of chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China

Membrane technology has widely accepted as the most energy efficient technology for the separation of ions or molecules. As the core of the membrane technology, the chemical and structure nature of membrane materials determines the application and energy-efficiency of the technology. An advanced membrane that has a remarkable ability to selectively differentiate ions and molecules can significantly enhance the separation technology and revolutionize industrial separation processes.

关键词： processes. separation defect

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Exploring the impact of Nafion modifier on electrocatalytic CO_(2) reduction over Cu catalyst

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Journal of Energy chemistry 2024年第1期88卷 543-551,I0012页

作者： Yingshi Su Yonghui Cheng Zhen Li Yanjia Cui Caili Yang Ziyi Zhong Yibing Song Gongwei Wang Lin Zhuang College of chemistry&Chemical Engineering and Key lab.ratory for Preparation and Application of Ordered Structural Materials of Guangdong Province Shantou UniversityShantou 515063GuangdongChina College of chemistry and Molecular Sciences Hubei Key Lab of Electrochemical Power SourcesWuhan UniversityWuhan 430072HubeiChina The Institute for Advanced Studies Wuhan UniversityWuhan 430072HubeiChina Department of chemistry Engineering Guangdong Technion-Israel Institute of Technology(GTIIT)Shantou 515063GuangdongChina Technion-Israel Institute of Technology(IIT) Haifa 32000Israel

Nafion as a universal polymer ionomer was widely applied for nanocatalysts electrode preparation.However,the effect of Nafion on electrocatalytic performance was often overlooked,especially for CO_(2)electrolysis.Herein,the key roles of Nafion for CO_(2)RR were systematically studied on Cu nanoparticles(NPs)electrocatalyst.We found that Nafion modifier not only inhibit hydrogen evolution reaction(HER)by decreasing the accessibility of H_(2)O from electrolyte to Cu NPs,and increase the CO_(2)concentration at electrocatalyst interface for enhancing the CO_(2)mass transfer process,but also activate CO_(2)molecule by Lewis acid-base interaction between Nafion and CO_(2)to accelerate the formation of^(*)CO,which favor of C–C coupling for boosting C_(2)product generation.Owing to these features,the HER selectivity was suppressed from 40.6%to 16.8%on optimal Cu@Nafion electrode at-1.2 V versus reversible hydrogen electrode(RHE),and as high as 73.5%faradaic efficiencies(FEs)of C_(2)products were achieved at the same applied potential,which was 2.6 times higher than that on bare Cu electrode(~28.3%).In addition,Nafion also contributed to the long-term stability by hinder Cu NPs morphology reconstruction.Thus,this work provides insights into the impact of Nafion on electrocatalytic CO_(2)RR performance.

关键词： Nafion modifier CO_(2)reduction Cu nanoparticles In situ ATR-SEIRAS C_(2)product

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Ultrasound-responsive spherical nucleic acid against c-Myc/PD-L1 to enhance anti-tumoral macrophages in triple-negative breast cancer progression

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Science China(Life Sciences) 2024年第4期67卷 698-710页

作者： Runtian Wang Gaigai Li Fangyan Gao Feng Xu Xintong Li Jian Zhang Jinbo Li Xiaoxiang Guan Department of Oncology The First Affiliated Hospital of Nanjing Medical UniversityNanjing 210029China State Key lab.ratory of Analytical chemistry for Life Sciences Jiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringChemistry and Biomedicine Innovation Center(ChemBIC)Nanjing UniversityNanjing 210023China Department of Medical Oncology Fudan University Shanghai Cancer CenterDepartment of OncologyShanghai Medical CollegeFudan UniversityShanghai 200032China Jiangsu Key lab.of Cancer Biomarkers Prevention and TreatmentCollaborative Innovation Center for Cancer Personalized MedicineNanjing Medical UniversityNanjing 211166China

Triple-negative breast cancer(TNBC)is the most challenging breast cancer subtype because of its aggressive behavior and limited therapeutic targets.c-Myc is hyperactivated in the majority of TNBC tissues,however,it has been considered an“undruggable”target due to its disordered structure.Herein,we developed an ultrasound-responsive spherical nucleic acid(SNA)against c-Myc and PD-L1 in TNBC.It is a self-assembled and carrier-free system composed of a hydrophilic small-interfering RNA(si RNA)shell and a hydrophobic core made of a peptide nucleic acid(PNA)-based antisense oligonucleotide(ASO)and a sonosensitizer.We accomplished significant enrichment in the tumor by enhanced permeability and retention(EPR)effect,the controllab.e release of effective elements by ultrasound activation,and the combination of targeted therapy,immunotherapy and physiotherapy.Our study demonstrated significant anti-tumoral effects in vitro and in vivo.Mass cytometry showed an invigorated tumor microenvironment(TME)characterized by a significant alteration in the composition of tumor-associated macrophages(TAM)and decreased proportion of PD-1-positive(PD-1+)T effector cells after appropriate treatment of the ultrasound-responsive SNA(USNA).Further experiments verified that tumor-conditioned macrophages residing in the TME were transformed into the anti-tumoral population.Our finding offers a novel therapeutic strategy against the“undruggable”c-Myc,develops a new targeted therapy for c-Myc/PD-L1 and provides a treatment option for the TNBC.

关键词： triple-negative breast cancer c-Myc spherical nucleic acid self-assembly

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Two-color emissive AIEgens with anti-Kasha property for dual-organelle imaging and phototherapy

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Science China chemistry 2024年第5期67卷 1740-1752页

作者： Pu Chen Guogang Shan Qingli Nie Yuting Yan Pengfei Zhang Zujin Zhao Hai-Tao Feng Ben Zhong Tang AIE Research Center Shaanxi Key Laboratory of PhytochemistryCollege of Chemistry and Chemical EngineeringBaoji University of Arts and SciencesBaoji 721013China Institute of Functional Material chemistry and National&Local United Engineering lab.for Power Battery Faculty of ChemistryNortheast Normal UniversityChangchun 130024China College of chemistry&Materials Science Northwest UniversityXi’an 710127China Guangdong Key lab.ratory of Nanomedicine CAS-HK Joint Lab of BiomaterialsCAS Key Laboratory of Biomedical Imaging Science and SystemShenzhen Engineering Laboratory of Nanomedicine and NanoformulationsCAS Key Lab for Health InformaticsShenzhen Institutes of Advanced TechnologyChinese Academy of SciencesShenzhen 518055China State Key lab.ratory of Luminescent Materials and Devices Key Laboratory of Luminescence from Molecular Aggregates of Guangdong ProvinceSouth China University of TechnologyGuangzhou 510640China School of Science and Engineering Shenzhen Institute of Aggregate Science and TechnologyThe Chinese University of Hong KongShenzhen(CUHK-Shenzhen)Shenzhen 518172China

Despite the rapid development of probes for targeting single organelle, the construction of robust dual-organelle targeting probes with multicolor emission was rarely reported. Herein, two dual-emissive aggregation-induced emission luminogens(AIEgens)with donor-π-acceptor structures were designed and synthesized, namely QT-1 and QF-2. Both two AIEgens exhibited excitation wavelength-dependence defying the Kasha's rule, and could stain lipid droplets(LDs) and mitochondria in blue and red fluorescence, respectively. Moreover, thanks to the near-infrared emission and abundant reactive oxygen species(ROS) generation efficiency of QT-1, it was chosen as a photodynamic therapy agent to selectively kill cancer cells from normal cells. Upon light irradiation, an obvious decrease of mitochondrial membrane potential(MMP) and serious change of mitochondrial shape in cells were observed, which corresponded to the efficient inhibition of tumor growth in vivo. This work afforded a promising strategy for the construction of multicolor emission by tuning anti-Kasha behaviors and expanding their application in dualorganelle targeting-based phototheranostics.

关键词： aggregation-induced emission anti-Kasha luminescence fluorescent probe bioimaging photodynamic therapy

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