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Introducing urea into tirapazamine derivatives to enhance anticancer therapy

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National Science Review 2024年第4期11卷 245-253页

作者： Yajun Xu Jianlin Lv Chaoying Kong Ya Liu Kun Wang Zhaohui Tang Xuesi Chen Key laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of Sciences School of applied Chemistry and Engineering University of Science and Technology of China

Tirapazamine（TPZ） has been approved for multiple clinical trials relying on its excellent anticancer ***,as a typical hypoxia-activated prodrug（HAP）,TPZ did not exhibit survival advantages in Phase Ⅲ clinical trials when used in combination therapy due to the insufficient hypoxia levels in patients' *** this study,to improve the therapeutic effects of TPZ,we first introduced urea to synthesize a series of urea-containing derivatives of *** urea-containing TPZ derivatives showed increased hypoxic cytotoxicity（9.51-30.85-fold） compared with TPZ,while maintaining hypoxic ***,one of these derivatives,showed 20-fold higher cytotoxicity than TPZ while maintaining a similar hypoxic cytotoxicity *** highly efficiently deliver TPZP to the tumors and reduce its side effects on healthy tissues,we further prepared TPZP into a nanodrug with fibrin-targeting ability:***4-NPs,a vascular disrupting agent,was used to increase the fibrin level within tumors and exacerbate tumor *** being combined with CA4-NPs,FT11-TPZP-NPs can accumulate in the hypoxia-aggravated tumors and activate sufficiently to kill tumor *** a single-dose treatment,FT11-TPZP-NPs+CA4-NPs showed a high inhibition rate of 98.1% against CT26 tumor models with an initial volume of ～480 mm3and four out of six tumors were completely eliminated;it thereby exerted a significant antitumor *** study provides a new strategy for improving the therapeutic effect of TPZ and other HAPs in anticancer therapy.

关键词： tirapazamine vascular disrupting agent hypoxia-activated prodrug combretastatin A4 urea

Polyoxometalates: metallodrug agents for combating amyloid aggregation

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National Science Review 2024年第7期11卷 279-291页

作者： Mengmeng Ma Zhenqi Liu Huisi Zhao Haochen Zhang Jinsong Ren Xiaogang Qu laboratory of Chemical Biology and State Key laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of Sciences School of applied Chemistry and Engineering University of Science and Technology of China

Alzheimer's disease(AD) is a devastating neurodegenerative disease that affects ～50 million people globally. The accumulation of amyloid-β(Aβ) plaques, a predominant pathological feature of AD, plays a crucial role in AD pathogenesis. In this respect, Aβ has been regarded as a highly promising therapeutic target for AD treatment. Polyoxometalates(POMs) are a novel class of metallodrugs being developed as modulators of Aβ aggregation, owing to their negative charge, polarity, and three-dimensional *** traditional discrete inorganic complexes, POMs contain tens to hundreds of metal atoms,showcasing remarkable tunability and diversity in nuclearities, sizes, and shapes. The easily adjustable and structurally variable nature of POMs allows for their favorable interactions with Aβ. This mini-review presents a balanced overview of recent progress in using POMs to mitigate amyloidosis. Clear correlations between anti-amyloid activities and structural features of POMs are also elaborated in detail. Finally, we discuss the current challenges and future prospects of POMs in combating AD.

关键词： amyloid inhibition metallodrug polyoxometalate amyloid-β Alzheimer's disease

Amphipathic Janus Nanofibers Aerogel for Efficient Solar Steam Generation

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Energy & Environmental Materials 2024年第4期7卷 422-432页

作者： Rui Wang Jinshuo Deng Ping Wu Qianli Ma Xiangting Dong Wensheng Yu Guixia Liu Jinxian Wang Lei Liu Chongqing Research Institute Changchun University of Science and Technology Key laboratory of applied Chemistry and Nanotechnology at Universities of Jilin Province Changchun University of Science and Technology

Solar steam generation is a promising water purification technology due to its low-cost and environmentally friendly applications in water purification and ***,hydrophilic or hydrophobic materials alone are insufficient in achieving necessary characteristics for constructing highquality solar steam generators with good comprehensive properties.

关键词： aerogels electrospinning photothermal materials solar desalination solar steam generation

Degradation mechanisms and stabilization strategies of ruthenium-based catalysts for OER in the proton exchange membrane water electrolyzer

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Progress in Natural Science:Materials International 2024年第1期34卷 207-222页

作者： Ming Yang Hongxiang Wu Zhaoping Shi Yibo Wang Jiahao Yang Jing Ni Pengbo Wang Yuqing Cheng Ziang Wang Meiling Xiao Changpeng Liu Wei Xing laboratory of Advanced Power Sources Changchun Institute of Applied Chemistry Chinese Academy of Sciences School of applied Chemistry and Engineering University of Science and Technology of China Jilin Province Key laboratory of Low Carbon Chemical Power Sources State Key laboratory of Electroanalytical Chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences

Designing economical oxygen evolution reaction(OER) electrocatalysts with high activity and long-term stability is essential to promote the scale-up applications of proton exchange membrane water electrolyzer(PEMWE) for hydrogen production. Ruthenium(Ru)-based materials with high intrinsic activity are hailed as the most promising catalysts, but still infeasible for practical application considering their long unresolved poor stability(only dozens of lifespan). Thus, tremendous efforts have been devoted to uncovering the degradation mechanisms and developing stabilization strategies for the Ru-based catalysts. In this review, starting from summarizing the fundamental understanding of deactivation mechanisms, a picture of the stability issue of Ru-based catalysts is proposed, which is followed by a detailed discussion on the recently developed strategies and progress made on enhancing durability. Finally, insights on the prospects for the future development of stable and practical Rubased OER catalysts are provided.

关键词： OER Ru-based catalysts PEMWE Degradation mechanisms Stabilization strategies

Alignment of inertialess spheroidal particles in flow-structure-dominated regions of turbulent channel flow:shape effect

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Acta Mechanica Sinica 2024年第8期40卷 45-66页

作者： Zhiwen Cui Lihao Zhao applied Mechanics laboratory Department of Engineering MechanicsTsinghua UniversityBeijing100084China laboratory of Flexible Electronics technology Tsinghua UniversityBeijing100084China

The alignment of elongated fibers and thin disks is known to be significantly influenced by the presence of fluid coherent structures in near-wall turbulence(Cui et al.2021).However,this earlier study is confined to the spheroids with infinitely large or small aspect ratio,and the shape effect of finite aspect ratio on the alignment is not *** current study investigates the shape-dependent alignment of inertialess spheroids in structure-dominated regions of channel *** utilizing an ensemble-averaged approach for identifying the structure-dominated regions,we analyze the eigensystem of the linear term matrix in the Jeffery equation,which is governed by both particle shape and local fluid velocity *** contrast to earlier conventional analysis based on local vorticity and strain rate,our findings demonstrate that the eigensystem of the Jeffery equation offers a convenient,effective,and universal framework for predicting the alignment behavior of inertialess spheroids in turbulent *** leveraging the eigensystem of the Jeffery equation,we uncover a diverse effect of fluid coherent structures on spheroid alignment with different particle ***,we provide explanations for both shape-independent alignments observed in vortical-core regions and shape-dependent alignments around near-wall streamwise vortices.

关键词： Non-spherical particle Direct numerical simulation Wall turbulence Particle-laden flow

A universal strategy of multi-objective active learning to accelerate the discovery of organic electrode molecules

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Science China Chemistry 2024年第11期67卷 3681-3687页

作者： Jiayi Du Jun Guo Wei Liu Ziwei Li Gang Huang Xinbo Zhang State Key laboratory of Rare Earth Resource Utilization Changchun Institute of Applied Chemistry Chinese Academy of Sciences School of applied Chemistry and Engineering University of Science and Technology of China School of Materials Science and Engineering Changchun University of Science and Technology

Organic electrode molecules hold significant potential as the next generation of cathode materials for Li-ion batteries. In this study, we have introduced a multi-objective active learning framework that leverages Bayesian optimization and non-dominated sorting genetic algorithms-Ⅱ. This framework enables the selection of organic molecules characterized by high theoretical energy density and low gap(LUMO-HOMO)(LUMO, lowest unoccupied molecular orbital; HOMO, highest occupied molecular orbital). Remarkably, after only two cycles of active learning, the determination of coefficient can reach 0.962 for theoretical energy density and 0.920 for the gap with a modest dataset of 300 molecules, showcasing superior predictive capabilities. The 2,3,5,6-tetrafluorocyclohexa-2,5-diene-1,4-dione, selected by non-dominated sorting genetic algorithms-Ⅱ, has been successfully applied to Li-ion batteries as cathode materials, demonstrating a high capacity of 288 m Ah g-1and a long cycle life of 1,000 cycles. This outcome underscores the high reliability of our framework. Furthermore, we have also validated the universality and transferability of our framework by applying it to two additional databases, the QM9 and OMEAD. When the training dataset of the model includes at least 500 molecules, the determination of coefficient essentially reaches approximately0.900 for four targets: gap, reduction potential, LUMO, and HOMO. Therefore, the universal framework in our work provides innovative insights applicable to other domains to expedite the screening process for target materials.

关键词： organic electrode molecules Li-ion batteries active learning multi-objective Bayesian optimization

Modularized viromimetic polymer nanoparticle vaccines(VPNVaxs) to elicit durable and effective humoral immune responses

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National Science Review 2024年第3期11卷 200-214页

作者： Zichao Huang Xinyu Zhuang Liping Liu Jiayu Zhao Sheng Ma Xinghui Si Zhenyi Zhu Fan Wu Ningyi Jin Mingyao Tian Wantong Song Xuesi Chen Key laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of Sciences School of applied Chemistry and Engineering University of Science and Technology of China Changchun Veterinary Research Institute Chinese Academy of Agricultural Sciences Jilin Biomedical Polymers Engineering laboratory State Key laboratory of Polymer Physics and Chemistry Changchun Institute of Applied Chemistry Chinese Academy of Sciences

Virus-like particle(VLP) vaccines had shown great potential during the COVID-19 pandemic, and was thought to be the next generation of antiviral vaccine technology due to viromimetic structures. However,the time-consuming and complicated processes in establishing a current recombinant-protein–based VLP vaccine has limited its quick launch to the out-bursting pandemic. To simplify and optimize VLP vaccine design, we herein report a kind of viromimetic polymer nanoparticle vaccine(VPNVax), with subunit receptor-binding domain(RBD) proteins conjugated to the surface of polyethylene glycol-b-polylactic acid(PEG-b-PLA) nanoparticles for vaccination against SARS-CoV-2. The preparation of VPNVax based on synthetic polymer particle and chemical post-conjugation makes it possible to rapidly replace the antigens and construct matched vaccines at the emergence of different viruses. Using this modular preparation system, we identified that VPNVax with surface protein coverage of 20%–25% had the best immunostimulatory activity, which could keep high levels of specific antibody titers over 5 months and induce virus neutralizing activity when combined with an aluminum adjuvant. Moreover, the polymer nano-vectors could be armed with more immune-adjuvant functions by loading immunostimulant agents or chemical chirality design. This VPNVax platform provides a novel kind of rapidly producing and efficient vaccine against different variants of SARS-CoV-2 as well as other viral pandemics.

关键词： vaccine polymer nanomaterials SARS-CoV-2

Effect of Y,Al Co‑Doping on Hydrogen Storage Properties of La–Mg–Ni‑Based Alloys

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Acta Metallurgica Sinica(English Letters) 2024年第8期37卷 1399-1410页

作者： Guanjiu Wu Yichao Xie Yuan Li Qing Wang Chenfeng Fan Wenfeng Wang Lu Zhang Shumin Han Hebei Key laboratory of applied Chemistry Yanshan UniversityQinhuangdao 066004China State Key laboratory of Metastable Materials Science and technology Yanshan UniversityQinhuangdao 066004China

La–Mg–Ni-based hydrogen storage alloys have excellent hydrogen storage *** work reports the hydrogen storage performance of a series of A_(2)B_(7)-type La_(0.96)Mg_(0.04)N_(i3.34)Al_(0.13)alloy and La_(0.96-x)Y_(x)Mg_(0.04)Ni_(3.47–0.6x)Al_(0.6x)(x=0,0.22,0.33,0.44)alloys,and explores the effect of Y and Al element combined substitution on the microstructure and hydrogen storage performance of A_(2)B_(7)-type La–Mg–Ni-based *** alloys are composed of Ce_(2)Ni_(7)phase and LaNi_(5)*** the increase of x,the cell volume of Ce_(2)Ni_(7)phase decreases,while that of LaNi_(5)phase increases,indicating that Y atom mainly enters Ce_(2)Ni_(7)phase and Al atom mainly enters LaNi_(5)*** appropriate amount of co-substitution increases the hydrogen storage capacity and reduces the hydrogen absorption/desorption plateau pressure hysteresis of the *** x=0.44,the hydrogen storage capacity of the alloy is 1.449 wt%,and the hysteresis coefficient is *** cell volume of Ce_(2)Ni_(7)phase and LaNi_(5)phase expands to different degrees after 20 absorption/desorption *** the increase of x,the volume expansion rate decreases,and the cycle capacity retention rate also gradually *** is related to the amorphization of Ce_(2)Ni_(7)*** x=0.22,the capacity retention rate of the alloy is 91.4%.

关键词： La-Mg-Ni-based alloys Gas-phase hydrogen storage performance Ce_(2)Ni_(7)phase LaNi_(5)phase Capacity retention rate

Local tetragonal distortion of Pt alloy catalysts for enhanced oxygen reduction reaction efficiency

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Carbon Energy 2024年第7期6卷 41-52页

作者： Xiaoke Li Xiao Duan Kang Hua Yongkang Wu Zhiyan Rui Rui Ding Aidong Li Chen Ouyang Jia Li Ting Li Jianguo Liu National laboratory of Solid-State Microstructures College of Engineering and Applied Sciencesand Collaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjingChina Long-Life Fuel cell Key laboratory in Sichuan Province Dongfang Electric(Chengdu)Hydrogen Fuel Cell Technology Co.Ltd.ChengduChina Institute of Energy Power Innovation North China Electric Power UniversityBeijingChina

Platinum-based alloy nanoparticles are the most attractive catalysts for the oxygen reduction reaction at present,but an in-depth understanding of the relationship between their short-range structural information and catalytic performance is still ***,we present a synthetic strategy that uses transition-metal oxide-assisted thermal ***/C catalysts with localized tetragonal distortion were obtained by controlling the thermal diffusion process of transition-metal *** localized structural distortion induced a significant strain effect on the nanoparticle surface,which further shortened the length of the Pt-Pt bond,improved the electronic state of the Pt surface,and enhanced the performance of the ***/C catalysts with special short-range structures achieved excellent mass activity(2.27 Amg_(Pt)^(-1))and specific activity(3.34 A cm^(-2)).In addition,the localized tetragonal distortion-induced surface compression of the Pt skin improved the stability of the *** mass activity decreased by only 13%after 30,000 *** catalyst activity and excellent durability have also been demonstrated in the proton exchange membrane fuel cell *** study provides valuable insights into the development of advanced Pt-based nanocatalysts and paves the way for reducing noble-metal loading and increasing the catalytic activity and catalyst stability.

关键词： electrocatalysts fuel cells local tetragonal distortion oxygen reduction