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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

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

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

key role of electron accessibility at the noble metal-free catalytic interface in hydrogen evolution reaction

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Nano Research 2024年第4期17卷 2538-2545页

作者： Dongchen Han Nanxing Gao Yuyi Chu Zhaoping Shi Ying Wang Junjie Ge Meiling Xiao Changpeng Liu Wei Xing State key laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China School of applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026China laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China Jilin Province key laboratory of Low Carbon Chemical Power Sources Changchun 130022China State key laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

The reactant concentration at the catalytic interface holds the key to the activity of electrocatalytic hydrogen evolution reaction(HER),mainly referring to the capacity of adsorbing hydrogen and electron accessibility.With hydrogen adsorption free energy(ΔGH)as a reactivity descriptor,the volcano curve based on Sabatier principle is established to evaluate the hydrogen evolution activity of catalysts.However,the role of electron as reactant received insufficient attention,especially for noble metal-free compound catalysts with poor conductivity,leading to cognitive gap between electronic conductivity and apparent catalytic activity.Herein we successfully construct a series of catalyst models with gradient conductivities by regulating molybdenum disulfide(MoS_(2))electronic bandgap via a simple solvothermal method.We demonstrate that the conductivity of catalysts greatly affects the overall catalytic activity.We further elucidate the key role of intrinsic conductivity of catalyst towards water electrolysis,mainly concentrating on the electron transport from electrode to catalyst,the electron accumulation process at the catalyst layer,and the charge transfer progress from catalyst to reactant.Theoretical and experimental evidence demonstrates that,with the enhancement in electron accessibility at the catalytic interface,the dominant parameter governing overall HER activity gradually converts from electron accessibility to combination of electron accessibility and hydrogen adsorbing energy.Our results provide the insight from various perspective for developing noble metal-free catalysts in electrocatalysis beyond HER.

关键词： conductivity molybdenum disulfide catalytic interface electron accessibility hydrogen evolution charge transfer.

Precisely Control Relationship between Sulfur Vacancy and H Absorption for Boosting Hydrogen Evolution Reaction

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Nano-Micro Letters 2024年第4期16卷 14-24页

作者： Jing Jin Xinyao Wang Yang Hu Zhuang Zhang Hongbo Liu Jie Yin Pinxian Xi College of chemistry and Chemical Engineering Frontiers Science Center for Rare IsotopesState Key Laboratory of Applied Organic ChemistryLanzhou UniversityLanzhou 730000People’s Republic of China

Ef fective and robust catalyst is the core of water splitting to produce hydrogen.Here, we report an anionic etching method to tailor the sulfur vacancy(VS) of NiS_(2) to further enhance the electrocatalytic performance for hydrogen evolution reaction(HER). With the VS concentration change from 2.4% to 8.5%, the H* adsorption strength on S sites changed and NiS_(2)-VS 5.9% shows the most optimized H* adsorption for HER with an ultralow onset potential(68 m V) and has long-term stability for 100 h in 1 M KOH media. In situ attenuated-total-reflection Fourier transform infrared spectroscopy(ATR-FTIRS) measurements are usually used to monitor the adsorption of intermediates. The S-H* peak of the Ni S_(2)-VS 5.9% appears at a very low voltage, which is favorable for the HER in alkaline media. Density functional theory calculations also demonstrate the Ni S_(2)-VS 5.9% has the optimal |ΔG^(H*)| of 0.17 e V. This work offers a simple and promising pathway to enhance catalytic activity via precise vacancies strategy.

关键词： Hydrogen evolution reaction S vacancies Nanosheet H Adsorption

Electric-field-controlled highly regioselective thiocyanation of N-containing heterocycles

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Science China chemistry 2024年第4期67卷 1263-1269页

作者： Ming Gong Qian Wu Jung Keun Kim Mengmeng Huang Yabo Li Yangjie Wu Jong Seung Kim Henan key laboratory of Chemical Biology and Organic chemistry Key Laboratory of Applied Chemistry of Henan UniversitiesCollege of ChemistryZhengzhou UniversityZhengzhou 450052China Department of chemistry Korea UniversitySeoul 02841Korea

Achieving highly regioselective synthesis in organic chemistry is challenging due to the uncontrollable orientation between reacting partners.External electric fields(EEFs)can influence the reactivity and selectivity of the substrate by causing directional adsorption.However,scalable and efficient techniques for using EEFs as“smart catalysts”have been lacking,hindering their application.In this study,we present a novel method for modifying the regioselectivity of quinoxaline-2(1H)-ones by functionalizing their C7-position using the electric double layer(EDL)theory.This approach led to moderate to good yields of the corresponding C7-thiocyanation products.DFT calculations and control experiments demonstrated that EEFs could reverse the regioselectivity of quinoxaline-2(1H)-ones,allowing the C7-thiocyanation to proceed via a radical reaction mechanism.Additionally,the resulting 7-thiocyano-1-methylquinoxaline-2(1H)-ones exhibited promising AIE properties.Our work showcases a promising strategy for achieving highly regioselective functionalization by aligning the electric field with the desired reaction/bond axis.

关键词： electric fields reaction-axis rule electric double layer C7-thiocyanation C-S bond formation