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Research Article Dynamically crosslinked nanocapsules for the efficient and serumresistant cytosolic protein delivery

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Nano Research 2024年第3期17卷 1760-1771页

作者： Qiang Yang Ningyu Liu Ziyin Zhao Xun Liu lichen yin Institute of Functional Nano and Soft Materials(FUNSOM) Jiangsu Key Laboratory of Carbon-Based Functional Materials and DevicesSoochow UniversitySuzhou 215123China Department of Thoracic Surgery The Second Affiliated Hospital of Soochow UniversitySuzhou 215004China

Intracellular protein delivery is critical to the development of protein-based biopharmaceuticals and ***,current delivery vectors often suffer from complicated syntheses,low generality among various proteins,and insufficient serum ***,we developed an enlightened cytosolic protein delivery strategy by dynamically crosslinking epigallocatechin gallate(EGCG),low-molecular-weight polyethylenimine(PEI 1.8k),and 2-acetylphenylboric acid(2-APBA)on the protein surface,hence forming the EPP-protein nanocapsules(NCs).EGCG enhanced protein encapsulation via hydrogen bonding,and reduced the positive charge density of PEI to endow the NCs with high serum tolerance,thereby enabling effective cellular internalization in *** formation of reversible imine and boronate ester among 2-APBA,EGCG,and PEI 1.8k allowed acid-triggered dissociation of EPP-protein NCs in the endolysosomes,which triggered efficient intracellular release of the native *** strategy therefore showed high efficiency and universality for diversities of proteins with different molecular weights and isoelectric points,including enzyme,toxin,antibody,and CRISPR(clustered regularly interspaced short palindromic repeats)-Cas9 ribonucleoprotein(RNP),outperforming the commercial protein transduction reagent PULSin and RNP transfection reagent lipofectamine ***,intravenously(i.v.)injected EPP-saporin NCs efficiently delivered saporin into 4T1 tumor cells to provoke robust antitumor *** simple,versatile,and robust cytosolic protein delivery system holds translational potentials for the development of protein-based therapeutics.

关键词： nanocapsules dynamic crosslinking cytosolic protein delivery serum resistance antitumor therapy genome editing

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Gene delivery into isolated Arabidopsis thaliana protoplasts and intact leaves using cationic, a-helical polypeptide

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Frontiers of Chemical Science and Engineering 2017年第4期11卷 521-528页

作者： Zheng, Nan Song, Ziyuan Liu, Yang Cheng, Jianjun yin, lichen Univ Illinois Dept Mat Sci & Engn Urbana IL 61801 USA Dalian Univ Technol Sch Chem Engn Dept Polymer Sci & Engn State Key Lab Fine Chem Dalian 116024 Peoples R China Soochow Univ Inst Funct Nano & Soft Mat FUNSOM Jiangsu Key Lab Carbon Based Funct Mat & Devices Collaborat Innovat Ctr Suzhou Nano Sci & Technol Suzhou 215123 Peoples R China

The application of gene delivery materials has been mainly focused on mammalian cells while rarely extended to plant engineering. Cationic polymers and lipids have been widely utilized to efficiently deliver DNA and siRNA into mammalian cells. However, their applica- tion in plant cells is limited due to the different membrane structures and the presence of plant cell walls. In this study, we developed the cationic, a-helical polypeptide that can effectively deliver DNA into both isolated Arabidopsis thaliana protoplasts and intact leaves. The PPABLG was able to condense DNA to form nanocomplexes, and they exhibited significantly improved transfection efficiencies compared with commercial transfection reagent Lipofec- tamine 2000 and classical cell penetrating peptides such as poly（L-lysine）, HIV-TAT, arginine9, and poly（L-arginine）. This study therefore widens the utilities of helical polypeptide as a unique category of gene delivery materials, and may find their promising applications toward plant gene delivery.

关键词： a-helical polypeptide plant gene delivery,protoplast intact leaves transfection

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青藏高原现代冰川冰缘区形变研究综述

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地理科学 2024年第7期44卷 1133-1141页

作者：贺璐方王欣王琼张法刚雷东钰尹力辰张勇魏俊锋湖南科技大学地球科学与空间信息工程学院湖南湘潭411201 湖南科技大学资源环境与安全工程学院湖南湘潭411201

冰缘区系冻融作用强烈的冻土区,易发生地表隆沉、失稳滑移等形变,是冰川灾害的物源区。系统解析冰缘区活动层水-热-力效应引起形变的作用机制,对研究冰缘区地表形变类型和冰川灾害防治具有重要意义。当前青藏高原发育现代冰川冰缘区面积... 详细信息

冰缘区系冻融作用强烈的冻土区,易发生地表隆沉、失稳滑移等形变,是冰川灾害的物源区。系统解析冰缘区活动层水-热-力效应引起形变的作用机制,对研究冰缘区地表形变类型和冰川灾害防治具有重要意义。当前青藏高原发育现代冰川冰缘区面积1.05×10^(6) km^(2),其中在过去几十年由于冰川退缩新增冰缘区面积约0.15×10^(5) km^(2)。冰缘区在气候、地形和现代冰川作用的综合影响下,产生以冻胀融沉为机理的垂直形变和以重力运移为主导的水平形变。未来研究应利用多源数据,结合冰缘区历史地表形变环境及致灾过程,借助人工智能实现现代冰川冰缘区地质灾害高效识别和预测预报,完善现代冰川冰缘区形变的监测-模拟-预测体系,为区域防灾减灾提供基础数据与理论支撑。

关键词：青藏高原现代冰川冰缘区多年冻土形变监测

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Accelerated Ring-Opening Polymerization of α-Amino Acid N-Carboxyanhydride via Inorganic Nano-initiators

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Chinese Journal of Chemistry 2023年第19期41卷 2476-2482页

作者： Junliang Zhu Yunjie He Chenglong Ge Wenting Si Ziyuan Song lichen yin Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhouJiangsu215123 China

While the accelerated polymerization of N-carboxyanhydrides (NCAs) has been utilized to synthesize versatile polypeptide materials in an efficient manner with minimized side reactions, the preparation of polypeptide-based inorganic/organic hybrid materials with the acceleration strategy remained largely unexplored. Herein, we report the accelerated ring-opening polymerization (ROP) of NCAs mediated by amine-modified inorganic nano-initiators, such as mesoporous silica nanoparticles (MSN-NH2), which is driven by the cooperative effect of the neighboring α-helical polypeptide chains in a dichloromethane (DCM)/water biphasic system. Well-defined nano-hybrids were prepared within 15 min from non-purified NCA monomers, through in situ purification and subsequent ultrafast polymerization process. NCAs can be rapidly initiated by amino groups of MSN uniformly dispersed at the interface of DCM and water, and subsequently formed the well-defined polypeptides within 15 min. The prepared inorganic/organic nano-hybrid with MSN as the core and polypeptide as the shell adopted spherical morphology and uniform size distribution due to the excellent controllability of ROP. Besides, this system is also suitable for a variety of NCAs and inorganic nano-initiators. This research allows efficient and rapid preparation of inorganic/organic nano-hybrids, and further promotes the extensive application of this material in the biomedical fields.

关键词： Polypeptide N-Carboxyanhydride Inorganic organic nano-hybrids Cooperative covalent polymerization Ring-opening polymerization Kinetics Synthetic methods

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Cardiomyocyte-targeted anti-inflammatory nanotherapeutics against myocardial ischemia reperfusion (IR) injury

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Nano Research 2022年第10期15卷 9125-9134页

作者： Min Lan Mengying Hou Jing Yan Qiurong Deng Ziyin Zhao Shixian Lv Juanjuan Dang Mengyuan yin Yong Ji lichen yin Institute of Functional Nano and Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials and DevicesSoochow UniversitySuzhou 215123China Department of Cardiothoracic Surgery Wuxi People’s Hospital Affiliated to Nanjing Medical UniversityWuxi 214023China

Myocardial ischemia reperfusion(IR)injury is closely related to the overwhelming inflammation in the ***,cardiomyocyte-targeted nanotherapeutics were developed for the reactive oxygen species(ROS)-ultrasensitive co-delivery of dexamethasone(Dex)and RAGE small interfering RNA(siRAGE)to attenuate myocardial ***,a ROSdegradable polycation based on PGE2-modified,PEGylated,ditellurium-crosslinked polyethylenimine(PEI)was developed to surface-decorate the Dex-encapsulated mesoporous silica nanoparticles(MSNs),which simultaneously condensed siRAGE and gated the MSNs to prevent the Dex *** intravenous injection to IR-injured rats,the nanotherapeutics could be efficiently transported into the inflamed cardiomyocytes via PGE2-assisted recognition of over-expressed E-series of prostaglandin(EP)receptors on the cell ***,the over-produced ROS degraded PPTP into small segments,promoting the release of siRAGE and Dex to mediate effective RAGE silencing(72%)and cooperative antiinflammatory *** a consequence,the nanotherapeutics notably suppressed the myocardial fibrosis and apoptosis,ultimately recovering the systolic ***,the current nanotherapeutics represent an effective example for the codelivery and on-demand release of nucleic acid and chemodrug payloads,and might find promising utilities toward the synergistic management of myocardial inflammation.

关键词： small interfering RNA(siRNA)delivery reactive oxygen species(ROS)responsiveness ditellurium-crosslinked polyethylenimine(PEI) myocardial ischemia reperfusion injury anti-inflammation

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iRGD-reinforced, photo-transformable nanoclusters toward cooperative enhancement of intratumoral penetration and antitumor efficacy

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Nano Research 2020年第10期13卷 2706-2715页

作者： Jing Yan Rongying Zhu Fan Wu Ziyin Zhao Huan Ye Mengying Hou Yong Liu lichen yin Institute of Functional Nano and Soft Materials(FUNSOM) Jiangsu Key Laboratory of Carbon-Based Functional Materials and DevicesCollaborative Innovation Center of Suzhou Nano Science&TechnologySoochow UniversitySuzhou 215123China Department of Thoracic Surgery The Second Afliated Hospital of Soochow UniversitSuzhou 215004China

Insufficient intratumoral penetration greatly hurdles the anticancer performance of nanomedicine. To realize highly efficient tumor penetration in a precisely and spatiotemporally controlled manner, far-red light-responsive nanoclusters (NCs) capable of size shrinkage and charge conversion were developed and co-administered with iRGD to synergistically improve the intratumoral penetration and the anticancer efficacy. The NCs were constructed using the singlet oxygen-sensitive (SOS) polyethylene glycolpolyurethane-polyethylene glycol (PEG-(1O2)PU-PEG) triblock copolymer to encapsulate the doxorubicin (DOX)-loaded, chlorin e6 (Ce6)-conjugated polyamindoamine (PAMAM) dendrimer (DCD) via the double-emulsion method. Co-administration of iRGD notably increased the permeability of NCs within tumor vasculature and tumor tissues. In addition, upon far-red light irradiation (660 nm) of tumors at low optical density (10 mW/cm2), the generated 1O2 could disintegrate the NCs and release the DCD with positive surface charge and ultra-small size (~ 5 nm), which synergized with iRGD to enable deep intratumoral penetration. Consequently, the local 1O2 at lethal concentrations along with the released DOX efficiently and cooperatively eradicated tumor cells. This study provides a convenient approach to spatiotemporally promote the intratumoral penetration of nanomedicine and mediate programmed anticancer therapy.

关键词： intratumoral penetration light-responsiveness singlet oxygen-degradable polymer size shrinkage charge conversion iRGD

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MicroRNA-208a silencing against myocardial ischemia/reperfusion injury mediated by reversibly camouflaged biomimetic nanocomplexes

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Nano Research 2023年第8期16卷 11176-11185页

作者： Jianhui Lu Jiaheng Zhang Wen Yan Chenglong Ge Yang Zhou Rongying Zhu Shanzhou Duan lichen yin Yongbing Chen Department of Thoracic Surgery Suzhou Key Laboratory of Thoracic OncologyThe Second Affiliated Hospital of Soochow UniversitySuzhou 215004China Center of Stomatology The Second Affiliated Hospital of Soochow UniversitySuzhou 215004China Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices Institute of Functional Nano&Soft Materials(FUNSOM)Collaborative Innovation Center of Suzhou Nano Science&TechnologySoochow UniversitySuzhou 215123China

MicroRNA-208a(miR-208a)plays critical roles in the severe fibrosis and heart failure post myocardial ischemia/reperfusion(IR)***-208a inhibitor(mI)with complementary RNA sequence can silence the expression of miR-208a,while it is challenging to achieve efficient and myocardium-targeted ***,biomimetic nanocomplexes(NCs)reversibly coated with red blood cell membrane(RM)were developed for the myocardial delivery of *** construct the NCs,membrane-penetrating helical polypeptide(PG)was first adopted to condense mI and form the cationic inner core,which subsequently adsorbed catalase(CAT)via electrostatic interaction followed by surface coating with *** membrane-coated NCs enabled prolonged blood circulation after systemic administration,and could accumulate in the injured myocardium via passive *** the oxidative microenvironment of injured myocardium,CAT decomposed H_(2)O_(2)to produce O_(2)bubbles,which drove the shedding of the outer RM to expose the positively charged inner core,thus facilitated effective internalization by cardiac *** on the combined contribution of mI-mediated miR-208a silencing and CAT-mediated alleviation of oxidative stress,NCs effectively ameliorated the myocardial microenvironment,hence reducing the infarct size as well as fibrosis and promoting recovery of cardiac *** study provides an effective strategy for the cytosolic delivery of nucleic acid cargoes in the myocardium,and it renders an enlightened approach to resolve the blood circulation/cell internalization dilemma of cell membrane-coated delivery systems.

关键词： myocardial ischemia/reperfusion(IR)injury microRNA-208a silencing red blood cell membrane reversible membrane coating H_(2)O_(2)responsiveness membrane-penetratingα-helical polypeptide

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Efficient and targeted drug/siRNA co-delivery mediated by reversibly crosslinked polymersomes toward anti-inflammatory treatment of ulcerative colitis (UC)

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Nano Research 2019年第3期12卷 659-667页

作者： Xin Xu Weijing Yang Qiujun Liang Yanan Shi Wenxin Zhang Xiao Wang Fenghua Meng Zhiyuan Zhong lichen yin Jiangsu Key Laboratory for Carbon-Based Functional Materials and Devices Institute of Functional Nano and Soft Materials (FUNSOM) the Collaborative Innovation Center of Suzhou Nano Science and Technology Soochow University Suzhou 215123 China Biomedical Polymers Laboratory and Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China

Co-delivery of anti-inflammatory siRNA and hydrophilic drug provides a promising approach for the treatment of ulcerative colitis (UC). However, lack of a suitable and efficient co-delivery carrier poses critical challenge against their utilization. We herein developed macrophage-targeting, reversibly crossli nked polymersomes (TKPR-RCP) based on the TKPR-modified, poly(ethyle ne glycol)-b-poly(trimethylene carbonate-codithiolane trimethylene carbonate)-b-polyethylenimine (PEG-P(TMC-DTC)-PEI) triblock copolymer, which could efficiently encapsulate TNF-α siRNA and dexamethasone sodium phosphate (DSP) in their hydrophilic core. The cationic PEI segments provided additional electrostatic interactions with cargo molecules to promote the encapsulatiion, and disulfide crosslinking of the polymersome membrane endowed the TKPR-RCP with high colloidal stability. Because the cationic PEI was embedded in the hydrophilic core, the polymersomes displayed neutral surface charge and thus possessed high serum stability. The TKPR-RCP co-encapsulating TNF-α siRNA and DSP could be efficiently internalized by macrophages (~98%) and undergo redox-responsive membrane de-crosslinking to accelerate cargo release in the cytoplasm, thus inducing efficient gene silencing and anti-inflammatory effect .Intravenous injectio n of the co-delivery TKPR-RCP mediated pote nt and cooperative anti-inflammatory effect in inflamed colons of UC mice, and significantly prevented animals from colonic injury. This study therefore provides a promising approach for the co-delivery of hydrophilic drug/siRNA toward the treatment of inflammatory bowel diseases.

关键词： ulcerative colitis (UC) anti-inflammatory therapy polymersomes reversible crosslinking siRNA/drug co-delivery macrophage targeting

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Macrophage-targeting gene silencing orchestrates myocardial microenvironment remodeling toward the anti-inflammatory treatment of ischemia-reperfusion (IR) injury

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Bioactive Materials 2022年第11期7卷 320-333页

作者： Yao Wang Mengying Hou Shanzhou Duan Ziyin Zhao Xuejie Wu Yongbing Chen lichen yin Department of Cardiothoracic Surgery the Second Affiliated Hospital of Soochow UniversitySuzhou215002China Institute of Functional Nano and Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials and DevicesSoochow UniversitySuzhou215123China Yancheng First Hospital Affiliated Hospital of Nanjing University Medical SchoolYancheng224005China

Ischemia-reperfusion (IR) injury represents a major cause of myocardial dysfunction after infarction and thrombolytic therapy, and it is closely related to the free radical explosion and overwhelming inflammatory responses. Herein, macrophage-targeting nanocomplexes (NCs) are developed to mediate efficient co-delivery of siRNA against MOF (siMOF) and microRNA-21 (miR21) into myocardial macrophages, cooperatively orches-trating the myocardial microenvironment against IR injury. Bioreducible, branched poly(β-amino ester) (BPAE-SS) is designed to co-condense siMOF and miR21 into NCs in a multivalency-reinforced approach, and they are surface-decorated with carboxylated mannan (Man-COOH) to shield the positive surface charges and enhance the serum stability. The final MBSsm NCs are efficiently internalized by myocardial macrophages after systemic administration, wherein BPAE-SS is degraded into small segments by intracellular glutathione to promote the siMOF/miR21 release, finally provoking efficient gene silencing. Thus, cardiomyocyte protection and macro-phage modulation are realized via the combined effects of ROS scavenging, inflammation inhibition, and autophagy attenuation, which ameliorates the myocardial microenvironment and restores the cardiac function via positive cellular crosstalk. This study renders promising solutions to address the multiple systemic barriers against in vivo nucleic acid delivery, and it also offers new options for IR injury by manipulating multiple reciprocal bio-reactions.

关键词： Myocardial ischemia-reperfusion(IR)injury Reduction-responsive branched poly(β-amino ester) siRNA/miRNA delivery Anti-inflammation Microenvironment remodeling

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Photodynamic therapy-triggered on-demand drug release from ROS-responsive core-cross-linked micelles toward synergistic anti-cancer treatment

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Nano Research 2019年第5期12卷 999-1008页

作者： Yongjuan Li Jian Hu Xun Liu Yong Liu Shixian Lv Juanjuan Dang Yong Ji Jinlin He lichen yin Institute of Functional Nano and Soft Materials (FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials and DevicesSoochow UniversitySuzhou 215123China College of Chemistry Chemical Engineering and Materials ScienceSuzhou Key Laboratory of Macromolecular Design and Precision SynthesisJiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationSoochow UniversitySuzhou 215123China Department of Biomedical Engineering University of Groningen and University Medical Center GroningenAntonius Deusinglaan 19713 AV Groningen The Netherlands Department of Cardiothoracic Surgery Wuxi Peoples Hospital Affiliated to Nanjing Medical UniversityWuxi 214023China

Polymeric micelles have demonstrated wide utility for chemodrug delivery,which however,still suffer from shortcomings such as undesired drug loading,disassembly upon dilution,pre-leakage of drug cargoes during systemic circulation,and lack of cancer-selective drug ***,a poly(ethylene glycol)(PEG)-polyphosphoester-based,reactive oxygen species (ROS)-responsive,core-cross-linked (CCL) micellar system was developed to encapsulate both chemodrug (doxorubicin,Dox) and photosensitizer (chlorin e6,Ce6).The hydrophobic core of the micelles was cross-linked via a thioketal (TK)-containing linker,which notably enhanced the drug loading and micelle *** tumor cells,far-red light irradiation of Ce6 generated ROS to cleave the TK linkers and disrupt the micelle *** such,micelles were destabilized and Dox release was promoted,which thereafter imparted synergistic anti-cancer effect with ROS-mediated photodynamic *** study provides an effective approach to realize the precise control over drug loading,formulation stability,and cancer-selective drug release using polymeric micelles,and would render promising utilities for the programmed anti-cancer combination therapy.

关键词： core-cross-linked micelles on-demand drug release photodynamic therapy reactive oxygen species (ROS) responsiveness synergistic an ti-cancer therapy

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