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Rare Metals 2024年第4期43卷 1658-1671页

作者： Jin-Kang Liu Tian-Shuo Yang Zhi-Bin Ren Adekunle-Adedapo Obisanya Xin-Yi Tan Yan-Di Rao Jun-Shuang Zhou Fa-Ming Gao Jian-Ren Wang hebei key laboratory of applied chemistry Yanshan University

Although pseudocapacitive manganese dioxide（MnO2） integrates the high-power merit of carbonaceous materials with the high-energy merit of battery-type materials,it still has a long way to go in achieving a more satisfactory balance of higher energy and power density,and in decoupling the relationship of structural characteristics with energy storage performance.To realize such goals,a bottom-up [WO6]-perturbed [MnO6] assembly strategy has been developed here due to their similar structure,yet mismatched lattice parameters.This facile protocol is capable of finely controlling the morphology and crystal structure of MnO2by adjusting its internal[WO6] concentration.Therefore,the as-prepared WxMnO2is treated as an ideal platform to scrutinize the correlations of the structure with the energy storage performance.The operando Raman spectra and finite element analysis have fully demonstrated the superiority of the locally ordered defects-enriched structure of W0.02-MnO2,which could reach a favorable balance between the ion diffusion equilibrium time and the number of active sites.As a result,the W0.02-MnO2is able to deliver a high capacitance of 292 F·g-1at a current density of 1 A·g-1and a remarkable rate performance with a 60% capacity retention at a current density of 50 A·g-1.The further unveiled structure-performance relationship provides a guideline for the design of better pseudocapacitive energy storage devices.

关键词： Supercapacitors Pseudocapacitive materials MnO 2 Tungsten doping Crystal structure regulation

Lanthanum promoting bone formation by regulating osteogenesis,osteoclastogenesis and angiogenesis

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Journal of Rare Earths 2024年第3期42卷 621-628,I0007页

作者： Dandan Zou Runlian Lin Yu Han Juan Jia Guoqiang Zhou Haisong Zhang Kun Ge hebei key laboratory of Chronic Kidney Diseases and Bone Metabolism Affiliated Hospital of Hebei UniversityBaoding071000China key laboratory of Medicinal chemistry and Molecular Diagnosis of the Ministry of Education Key Laboratory of Chemical Biology of Hebei ProvinceCollege of Chemistry and Environmental ScienceHebei UniversityBaoding071002China

With lanthanum(La) in agriculture, medicine, and the chemical industry, La shows accumulation in the body, especially in the bone, because of its similar structure to calcium. Moreover, La has a direct role in bone formation regulating osteoblasts and osteoclasts. Nevertheless, bone formation is complex under the regulation of osteogenesis, osteoclastogenesis, and angiogenesis in the bone microenvironment. It is difficult to comprehensively understand the regulation of bone homeostasis from a single kind of cell.Herein, some bone microenvironment-related cells and mouse calvaria culture models were used to study the regulatory effect of La-based compound-lanthanum nitrate(La(NO_(3))_(3)) on bone formation.La(NO_(3))_(3) has good biological safety, and the osteogenic differentiation is significantly increased under La(NO_(3))_(3) treatment for bone marrow mesenchymal stem cells(BMMSC). In contrast, the differentiation,maturation, and bone erosion ability of osteoclasts are significantly decreased. Meanwhile, the angiogenesis ability of human umbilical vein endothelial cells(HUVEC) is significantly promoted when treated with La(NO_(3))_(3). Furthermore, bone metabolism and angiogenesis are improved under La(NO_(3))_(3) treatment in the calvaria ex vivo culture model and BMMSC-HUVEC co-culture system. These results suggest that La has the beneficial effect of promoting bone metabolism and improving bone formation in the bone microenvironment.

关键词： Lanthanum Bone microenvironment Osteogenic differentiation Angiogenesis Rare earths

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 potential.However,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' tumors.In this study,to improve the therapeutic effects of TPZ,we first introduced urea to synthesize a series of urea-containing derivatives of TPZ.All urea-containing TPZ derivatives showed increased hypoxic cytotoxicity（9.51-30.85-fold） compared with TPZ,while maintaining hypoxic selectivity.TPZP,one of these derivatives,showed 20-fold higher cytotoxicity than TPZ while maintaining a similar hypoxic cytotoxicity ratio.To 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:FT11-TPZP-NPs.CA4-NPs,a vascular disrupting agent,was used to increase the fibrin level within tumors and exacerbate tumor hypoxia.By being combined with CA4-NPs,FT11-TPZP-NPs can accumulate in the hypoxia-aggravated tumors and activate sufficiently to kill tumor cells.After 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 effect.This 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

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

High-efficiency crystalline white organic lightemitting diodes

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Light(Science & Applications) 2024年第4期13卷 747-759页

作者： Yijun Liu Feng Zhu Yue Wang Donghang Yan State key laboratory of Polymer Physics and chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China. School of applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China. State key laboratory of Supramolecular Structure and Materials Jilin UniversityChangchun 130012China

Crystalline white organic light-emitting diodes(C-WOLEDs)are promising candidates for lighting and display applications.It is urgently necessary,however,to develop energy-saving and high-efficiency C-WOLEDs that have stable and powerful emission to meet commercial demands.Here,we report a crystalline host matrix(CHM)with embedded nanoaggregates(NA)structure for developing high-performance C-WOLEDs by employing a thermally activated delayed fluorescence(TADF)material and orange phosphorescent dopants(Phos.-D).The CHM-TADFNA-D WOLED exhibit a remarkable EQE of 12.8%,which is the highest performance WOLEDs based on crystalline materials.The device has a quick formation of excitons and a well-designed energy transfer process,and possesses a fast ramping of luminance and current density.Compared to recently reported high-performance WOLEDs based on amorphous material route,the C-WOLED achieves a low series-resistance Joule-heat loss ratio and an enhanced photon output,demonstrating its significant potential in developing the next-generation WOLEDs.

关键词： diodes dopant crystalline

Suppressing the lattice oxygen diffusion via high-entropy oxide construction towards stabilized acidic water oxidation

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Nano Research 2024年第3期17卷 1107-1113页

作者： Jing Ni Zhaoping Shi Yibo Wang Jiahao Yang Hongxiang Wu Pengbo Wang Kai Li Meiling Xiao Changpeng Liu Wei Xing State key laboratory of Electroanalytic chemistry Jilin Province Key Laboratory of Low Carbon Chemistry PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China State key laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

The scale-up deployment of ruthenium(Ru)-based oxygen evolution reaction(OER)electrocatalysts in proton exchange membrane water electrolysis(PEMWE)is greatly restricted by the poor stability.As the lattice-oxygen-mediated mechanism(LOM)has been identified as the major contributor to the fast performance degradation,impeding lattice oxygen diffusion to inhibit lattice oxygen participation is imperative,yet remains challenging due to the lack of efficient approaches.Herein,we strategically regulate the bonding nature of Ru–O towards suppressed LOM via Ru-based high-entropy oxide(HEO)construction.The lattice disorder in HEOs is believed to increase migration energy barrier of lattice oxygen.As a result,the screened Ti_(23)Nb_(9)Hf_(13)W_(12)Ru_(43)O_(x) exhibits 11.7 times slower lattice oxygen diffusion rate,84%reduction in LOM ratio,and 29 times lifespan extension compared with the state-of-the-art RuO_(2) catalyst.Our work opens up a feasible avenue to constructing stabilized Ru-based OER catalysts towards scalable application.

关键词： ruthenium-based high-entropy oxide suppressing the lattice oxygen diffusion acidic oxygen evolution reaction

Engineering oxygen vacancies on Tb-doped ceria supported Pt catalyst for hydrogen production through steam reforming of long-chain hydrocarbon fuels

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Chinese Journal of Chemical Engineering 2024年第4期68卷 181-192页

作者： Zhourong Xiao Changxuan Zhang Peng Li Desong Wang Xiangwen Zhang Li Wang Jijun Zou Guozhu Li State key laboratory of Metastable Materials Science and Technology(MMST) Hebei Key Laboratory of Applied ChemistryCollege of Environmental and Chemical EngineeringYanshan UniversityQinhuangdao 066004China key laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Steam reforming of long-chain hydrocarbon fuels for hydrogen production has received great attention for thermal management of the hypersonic vehicle and fuel-cell application.In this work,Pt catalysts supported on CeO_(2)and Tb-doped CeO_(2)were prepared by a precipitation method.The physical structure and chemical properties of the as-prepared catalysts were characterized by powder X-ray diffraction,scanning electron microscopy,transmission electron microscopy,Raman spectroscopy,H_(2)temperature programmed reduction,and X-ray photoelectron spectroscopy.The results show that Tb-doped CeO_(2)supported Pt possesses abundant surface oxygen vacancies,good inhibition of ceria sintering,and strong metal-support interaction compared with CeO_(2)supported Pt.The catalytic performance of hydrogen production via steam reforming of long-chain hydrocarbon fuels(n-dodecane)was tested.Compared with 2Pt/CeO_(2),2Pt/Ce_(0.9)Tb_(0.1)O_(2),and 2Pt/Ce_(0.5)Tb_(0.5)O_(2),the 2Pt/Ce_(0.7)Tb_(0.3)O_(2)has higher activity and stability for hydrogen production,on which the conversion of n-dodecane was maintained at about 53.2%after 600 min reaction under 700℃at liquid space velocity of 9 ml·g^(-1)·h^(-1).2Pt/CeO_(2)rapidly deactivated,the conversion of n-dodecane was reduced to only 41.6%after 600 min.

关键词： Steam reforming n-Dodecane Hydrogen production Pt-based catalyst Oxygen vacancy CeO_(2)

Ligand-controlled NiH-catalyzed regiodivergent hydroalkylation of 2-alkenylazaarenes

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Science China chemistry 2024年第6期67卷 1935-1940页

作者： Ya-Ping Shao Zhuo-Min Chi Yong-Min Liang State key laboratory of applied Organic chemistry School of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou730000China

A nickel-hydride(Ni H)-catalyzed migratory and nonmigratory hydroalkylation reaction of 2-alkenyl azaarenes with alkyl iodines has been established through strategic modulation of N-or P-donor ligands.This method enables the synthesis of diverseβ-orγ-branched aromatic N-heterocycles.The mild regiodivergent protocols exhibit wide substrate scope,excellent functional tolerance,and great reaction yield with remarkable regioselectivity.Importantly,deuterium labeling studies reveal Ni H-catalyzed interrupted chain-walking mode as the mechanism behind remotedβ-selective hydroalkylation reaction—an interesting phenomenon mediated through aromatic imine directing groups.

关键词： NiH regiodivergent hydroalkylation azaarenes interrupted chain-walking

Application of "Three-in-One" Strategy Based on MOF-199 in Determination of Phenylenediamine Isomers and Cr(Ⅵ)

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Journal of Analysis and Testing 2024年第1期8卷 28-39页

作者： Yueci Xiang Jiantao Wei Huipeng Sun Ruiyi Zhao Zehua Han Shuangtong Wu Xiaoyan Liu Haixia Zhang State key laboratory of applied Organic chemistry and College of chemistry and Chemical Engineering Lanzhou UniversityLanzhou 730000China

Industry progressing caused the pollutants into the surface and groundwater,including organic pollutants such as phenylenediamine(PD)and heavy metals such as Cr(Ⅵ).Herein,a simple"three-in-one"strategy based on MOF-199 was demonstrated.The MOF-199 catalytic system could be used for the rapid detection of Cr(Ⅵ)and o-phenylenediamine(OPD)in linear ranges of 0.5-50.0μmol/L and 7.0-250.0μmol/L,with the limits of detection of 0.1 and 0.5μmol/L,respectively.This method can also efficiently discriminate PD isomers in just 15 min.Meanwhile,Cr(Ⅵ)was reduced to Cr(Ⅲ)and the elimination of OPD was carried out.Given simple synthesis,high sensitivity,easy operation,and low cost,this method presented a potential platform for on-site detection of pollutants in water samples.

关键词： On-site detection “Three-in-one”strategy Phenylenediamine isomers

Dynamically switchable porphyrin-based molecular tweezer for on-off fullerene recognition

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Chinese Chemical Letters 2024年第6期35卷 283-287页

作者： Zhimin Sun Xin-Hui Guo Yue Zhao Qing-Yu Meng Li-Juan Xing He-Lue Sun College of chemistry and Materials Science Hebei Key Laboratory of Organic Functional MoleculesHebei Normal UniversityShijiazhuang 050024China

Herein,a novel molecular tweezer based on 2,2'-bipyridine-bridged porphyrin subunits was constructed for efficient fullerenes recognition.The syn conformation of the molecule,which was obtained by Zn(Ⅱ)coordination,gives rise to a proper cavity to interact with fullerene guests to form a stable 1:1 complex in toluene solution.It exhibits distinct binding selectivity towards C_(60)over C_(70).Moreover,the fullerene recognition capacity can be adequately suppressed by importing H_(2)PO_(4)^(-)to competitively capture Zn(Ⅱ)along with syn-anti conformational conversion.Subsequently,the molecular tweezer regenerated to bind the fullerene by introducing the Ca^(2+)into the system.Significantly,the association-disassociation process can be switched reversibly and repeatedly.

关键词： Molecular tweezer Fullerene recognition Supramolecular chemistry Conformation conversion Coordination