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On the origin of the low immunogenicity and biosafety of a neutralα-helical polypeptide as an alternative to polyethylene glycol

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Bioactive Materials 2024年第2期32卷 333-343页

作者： Jialing Sun Junyi Chen Yiming Sun yingqin hou Zhibo Liu Hua Lu Beijing National Laboratory for Molecular Sciences Center for Soft Matter Science and EngineeringKey Laboratory of Polymer Chemistry and Physics of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China Beijing National Laboratory for Molecular Sciences Radiochemistry and Radiation Chemistry Key Laboratory of Fundamental ScienceNMPA Key Laboratory for Research and Evaluation of RadiopharmaceuticalsKey Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871China Peking University–Tsinghua University Center for Life Sciences Peking UniversityBeijing100871China

Poly(ethylene glycol)(PEG)is a prominent synthetic polymer widely used in *** its notable success,recent clinical evidence highlights concerns regarding the immunogenicity and adverse effects associated with PEG in PEGylated proteins and lipid *** studies have found a neutral helical polypeptide poly(γ-(2-(2-(2-methoxyethoxy)ethoxy)ethyl L-glutamate),namely L-P(EG3Glu),as a potential alternative to PEG,displaying lower *** comprehensively assess the immunogenicity,distribution,degradation,and biosafety of L-P(EG3Glu),herein,we employ assays including enzyme-linked immunosorbent assay,positron emission tomography-computed tomography,and fluorescent resonance energy *** investigations involve in vivo immune responses,biodistribution,and macrophage activation of interferon(IFN)conjugates tethered with helical L-P(EG3Glu)(L20k-IFN),random-coiled DL-P(EG3Glu)(DL20k-IFN),and PEG(PEG20k-IFN).Key findings encompass:minimal anti-IFN and anti-polymer antibodies elicited by L20k-IFN;length-dependent affinity of PEG to anti-PEG antibodies;accelerated clearance of DL20k-IFN and PEG20k-IFN linked to anti-IFN and anti-polymer IgG;complement activation for DL20k-IFN and PEG20k-IFN but not L20k-IFN;differential clearance with L20k-IFN kidney-based,and DL20k-IFN/PEG20k-IFN accumulation mainly in liver/spleen;enhanced macrophage activation by DL20k-IFN and PEG20k-IFN;L-P(EG3Glu)resistance to proteolysis;and safer repeated administrations of L-P(EG3Glu)in ***,this study offers comprehensive insights into the lower immunogenicity of L-P(EG3Glu)compared to DL-P(EG3Glu)and PEG,supporting its potential clinical use in protein conjugation and nanomedicines.

关键词： helical neutral activation

Co-delivery of Cisplatin and Chlorin e6 by Poly(phosphotyrosine)for Synergistic Chemotherapy and Photodynamic Therapy

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Chinese Journal of Chemistry 2022年第20期40卷 2428-2436页

作者： Haisen Zhou Yaoyi Wang yingqin hou Zhengkui Zhang Qi Wang Xiaodong Tian Hua Lu Beijing National Laboratory for Molecular Sciences Center for Soft Matter Science and EngineeringKey Laboratory of Polymer Chemistry and Physics of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing100871 China Department of General Surgery Peking University First HospitalBeijing100034 China

Nanoscale drug delivery systems(NDDSs)have emerged as promising carriers for combinational therapy by co-delivery of multiple drugs and ***,most co-delivery systems require the use of complicated materials and ***,we report the single use of a polymeric material,namely mPEG-block-poly(phosphotyrosine)(mPEG-b-PpY),as a multi-functional carrier for the facile fabrication of NDDS Pt/Ce6@mPEG-b-PpY(PtCeNP)for the co-delivery of cisplatin and photosensitizer chlorin e6(Ce6)via phosphato-platinum coordination andπ-πstacking,*** improves the solubility,cellular uptake,and bioavailability of both parental drugs,and showed strong synergistic antitumor efficacy both in vitro and in vivo through combined chemo-photodynamic *** results indicate that PpY is a biocompatible,multifunctional,and promising carrier material suitable for a variety of drugs and may simplify the design for co-delivery systems.

关键词： Drug delivery Poly(phosphotyrosine) Block copolymers Nanoparticles Combinational chemo-photodynamic therapy

Regulation of the cellular uptake of nanopartides by the orientation of helical polypeptides

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Nano Research 2019年第4期12卷 889-896页

作者： Chong Zhang Jianhua Lu Falin Tian Lindong Li yingqin hou Yaoyi Wang Lingdong Sun Xinghua Shi Hua Lu Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular Engineering Peking University Beijing 100871 China Center for Soft Matter Science and Engineering Key Laboratory of Polymer Chemistry and Physics of Ministry of Education Peking University Beijing 100871 China CAS Key Laboratory of Nanosystem and Hierarchical Fabrication CAS Center for Excellence in Nanoscience National Center for Nanoscience and Technology Beijing 100190 China State Key Laboratory of Rare Earth Materials Chemistry and Applications PKU-HKU Joint Laboratory in Rare Earth Materials and Bioinorganic Chemistry Peking University Beijing 100871 China

Controlling the cellular interactio n and internal izatio n of polymer-modified nan oparticles (NPs) is of central importa nee to the developme nt of promisi ng nano medici nes. Here, we describe the use of synthetic polypeptides for NP surface coati ng and regulati on of their cellular uptake behaviors by simply switching the conformation and anchoring orientation. Our results show that gold NPs (AuNPs) coated with a helical poly(Y-(2-(2-(2-methoxyethoxy)ethoxy)ethoxy)esteryl「glutamate)(L-P(EG3Glu)5o) from the C-terminus ((L-C)-AuNPs) exhibit greater zeta potential and more cellular uptake (2.0-5.5 fold higher) than those coated with the same polypeptide but anchored from the N-terminus ((L-N)-AuNPs), or from both the C- and N-terminus at a 1/1 molar ratio ((L-C/L-N)-AuNPs). A similar orientation-regulated cellular internalization pattern is observed in D-P(EG3Glu)50 but not the unstructured DL-P(EG3Glu)5o-rnodified AuNPs, suggesting an important and universal role of the helix-derived macrodipole in cellular uptake. Moreover, this orientation-governed internalization is successfully reproduced in P(EG3Glu)50-coated gold nano rods (AuNRs), and applied to the desig n of doxorubici reloaded polypeptide micelles. Simulation study offers time-resolved in sights regarding the NP-membrane in teracti ons and membrane remodeling. Thus, our study provides a delicate way of regulating the surface chemistry of NPs and the subsequent NP-cell interactions. Moreover, the results highlight the uniqueness of polypeptides in NP surface engineering, and urge a more careful consideration on the polymer orientation effect.

关键词： helix orientation polypeptides cellular uptake gold nanoparticles

聚氨基酸在材料科学及生物医药中的二级结构效应

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化学通报 2020年第4期83卷 343-348页

作者：张冲侯颖钦吕华北京大学化学与分子工程学院软物质科学与工程中心北京分子科学国家研究中心高分子化学与物理教育部重点实验室北京100871

聚氨基酸不仅具有优异的生物相容性和生物可降解性,其类似于蛋白质的二级结构(α-螺旋、β-折叠、无规卷曲)及二级结构的响应性转变赋予了聚氨基酸不同于常规聚合物的特殊功能,在材料及生物医药领域具有重要应用。本文简要概述了本课题... 详细信息

聚氨基酸不仅具有优异的生物相容性和生物可降解性,其类似于蛋白质的二级结构(α-螺旋、β-折叠、无规卷曲)及二级结构的响应性转变赋予了聚氨基酸不同于常规聚合物的特殊功能,在材料及生物医药领域具有重要应用。本文简要概述了本课题组近年来围绕聚氨基酸二级结构在聚合物防污涂层、纳米颗粒-细胞膜相互作用以及蛋白质改性研究中的新进展,并对聚氨基酸二级结构未来的发展方向进行了简要的展望。

关键词：聚氨基酸二级结构防污聚合物细胞摄取蛋白质-聚合物偶联物

Practical approach for detecting k-nonseparability of multipartite quantum states

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Science China(Physics,Mechanics & Astronomy) 2025年第1期Mechanics & Astronomy) .卷 32-48页

作者： Jie Guo Jinchuan hou Xiaofei Qi Kan He College of Mathematics Taiyuan University of Technology School of Mathematics and Statistics Shanxi University Key Laboratory of Complex Systems and Data Science of Ministry of Education Shanxi University

The instantaneous detection of entanglement in quantum states poses a significant challenge in the fields of quantum computation and quantum information, and there are no practical methods or tools to complete this task satisfactorily so far. We propose a sufficient and necessary criterion of k-nonseparability for any n-partite finite or infinite dimensional systems, 2 ≤ k ≤ n. This criterion serves as the foundation for a practical scheme designed to detect entanglement and k-nonseparability across multipartite finite-dimensional systems. To exemplify the application of our scheme, we have developed a software tool that facilitates swift and precise identification of entanglement, k-nonseparability, and genuine entanglement within n-qubit systems, specifically tailored for systems with 2 ≤ n ≤ 4.

关键词： multipartite systems entanglement states entanglement witnesses ${\bm~k}$-nonseparability

Low-temperature chlorination roasting technology for the simultaneous recovery of valuable metals from spent LiCoO_(2)cathode material

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International Journal of Minerals,Metallurgy and Materials 2025年第1期32卷 80-91页

作者： Junjie Shi Changle hou Jingjing Dong Dong Chen Jianzhong Li Key Laboratory for Ecological Metallurgy of Multimetallic Mineral(Ministry of Education) Northeastern UniversityShenyang 110819China School of Metallurgy Northeastern UniversityShenyang 110819China

With the continuous increase in the disposal volume of spent lithium-ion batteries(LIBs),properly recycling spent LIBs has become essential for the advancement of the circular *** study presents a systematic analysis of the chlorination roasting kinetics and proposes a new two-step chlorination roasting process that integrates thermodynamics for the recycling of LIB cathode *** activation energy for the chloride reaction was 88.41 kJ/mol according to thermogravimetric analysis–derivative thermogravimetry data obtained by using model-free,model-fitting,and Z(α)function(αis conversion rate).Results indicated that the reaction was dominated by the first-order(F1)model when the conversion rate was less than or equal to 0.5 and shifted to the second-order(F2)model when the conversion rate exceeded *** conditions were determined by thoroughly investigating the effects of roasting temperature,roasting time,and the mass ratio of NH_(4)Cl to LiCoO_(2).Under the optimal conditions,namely 400℃,20 min,and NH_(4)Cl/LiCoO_(2)mass ratio of 3:1,the leaching efficiency of Li and Co reached 99.43% and 99.05%,*** of the roasted products revealed that valuable metals in LiCoO_(2)transformed into CoCl_(2) and ***,the reaction mechanism was elucidated,providing insights for the establishment of a novel low-temperature chlorination roasting technology based on a crystal structure *** technology can guide the development of LIB recycling processes with low energy consumption,low secondary pollution,high recovery efficiency,and high added value.

关键词： spent lithium-ion battery thermodynamics chlorination roasting kinetics circular economy

Defect Engineering with Rational Dopants Modulation for High‑Temperature Energy Harvesting in Lead‑Free Piezoceramics

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Nano-Micro Letters 2025年第3期17卷 87-101页

作者： Kaibiao Xi Jianzhe Guo Mupeng Zheng Mankang Zhu Yudong hou Key Laboratory of Advanced Functional Materials Ministry of EducationCollege of Materials Science and EngineeringBeijing University of TechnologyBeijing 100124People’s Republic of China

High temperature piezoelectric energy harvester(HTPEH)is an important solution to replace chemical battery to achieve independent power supply of HT wireless ***,simultaneously excellent performances,including high figure of merit(FOM),insulation resistivity(ρ)and depolarization temperature(Td)are indispensable but hard to achieve in lead-free piezoceramics,especially operating at 250°C has not been reported ***,well-balanced performances are achieved in BiFeO3–BaTiO3 ceramics via innovative defect engineering with respect to delicate manganese *** to the synergistic effect of enhancing electrostrictive coefficient by polarization configuration optimization,regulating iron ion oxidation state by high valence manganese ion and stabilizing domain orientation by defect dipole,comprehensive excellent electrical performances(Td=340°C,ρ250°C>10^(7)Ωcm and FOM_(250°C)=4905×10^(–15)m^(2)N^(−1))are realized at the solid solubility limit of manganese *** HT-PEHs assembled using the rationally designed piezoceramic can allow for fast charging of commercial electrolytic capacitor at 250°C with high energy conversion efficiency(η=11.43%).These characteristics demonstrate that defect engineering tailored BF-BT can satisfy high-end HT-PEHs requirements,paving a new way in developing selfpowered wireless sensors working in HT environments.

关键词： Lead-free piezoceramic Defect engineering Dopants modulation High-temperature Piezoelectric energy harvester

Establishing a new testing protocol of the electrochemical stability window for electric double-layer capacitors

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Science China Chemistry 2025年第1期68卷 217-225页

作者： Ruilin hou Xiaoxi Zhao Tingting Liang Qingyun Dou Shan Xu Xingbin Yan School of Materials Science and Engineering Sun Yat-sen University Laboratory of Clean Energy Chemistry and Materials Lanzhou Institute of Chemical Physics Chinese Academy of Sciences College of Engineering and Applied Sciences Nanjing University Center of Industrial Analysis and Testing Guangdong Academy of Science

The electrochemical stability window(ESW) is crucial for determining the energy density of electric double-layer capacitors(EDLCs). However, current ESW testing protocols of EDLCs are strongly affected by artificial factors, thereby leading to unreliable result. To solve this problem, we first identify the key shortcomings of the traditional protocols by analyzing their test principles. Subsequently, taking an aqueous carbon-based EDLC as an example, we design a side reaction descriptor to represent the response difference in the charging capacitance to side reactions between the cyclic voltammetry and galvanostatic chargedischarge methods. With the aid of this descriptor, we propose a new ESW testing protocol, which is not only able to completely avoid the adverse influence of subjective factors but also fully consider the operating condition limitations. The protocol can be extended from the single electrode to the full device. This work proposes a more rigorous definition of ESW and provides a reliable protocol for evaluating the ESW of EDLCs.

关键词： electric double-layer capacitors electrochemical stability window testing protocol side reaction descriptor operating limitation

Multi-layer multi-pass friction rolling additive manufacturing of Al alloy:Toward complex large-scale high-performance components

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International Journal of Minerals,Metallurgy and Materials 2025年第2期32卷 425-438页

作者： Haibin Liu Run hou Chenghao Wu Ruishan Xie Shujun Chen College of Mechanical&Energy Engineering Beijing University of TechnologyBeijing 100124China Chongqing Research Institute of Beijing University of Technology Chongqing 401121China

At present,the emerging solid-phase friction-based additive manufacturing technology,including friction rolling additive man-ufacturing(FRAM),can only manufacture simple single-pass *** this study,multi-layer multi-pass FRAM-deposited alumin-um alloy samples were successfully prepared using a non-shoulder tool *** material flow behavior and microstructure of the over-lapped zone between adjacent layers and passes during multi-layer multi-pass FRAM deposition were studied using the hybrid 6061 and 5052 aluminum *** results showed that a mechanical interlocking structure was formed between the adjacent layers and the adja-cent passes in the overlapped center *** friction and rolling of the tool head led to different degrees of lateral flow and plastic deformation of the materials in the overlapped zone,which made the recrystallization degree in the left and right edge zones of the over-lapped zone the highest,followed by the overlapped center zone and the non-overlapped *** tensile strength of the overlapped zone exceeded 90%of that of the single-pass deposition *** is proved that although there are uneven grooves on the surface of the over-lapping area during multi-layer and multi-pass deposition,they can be filled by the flow of materials during the deposition of the next lay-er,thus ensuring the dense microstructure and excellent mechanical properties of the overlapping *** multi-layer multi-pass FRAM deposition overcomes the limitation of deposition width and lays the foundation for the future deposition of large-scale high-performance components.

关键词： aluminum alloy additive manufacturing solid-state friction stir welding multi-layer multi-pass