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Regularly Tuning Quantum Interference in Single-Molecule Junctions through Systematic Substitution of Side Groups with Varied Electron Effects

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Chinese Journal of Chemistry 2024年第11期42卷 1217-1222页

作者： Xianjing Xie Yirong Zhang Junrui Zhang Xingyuan Cui Wei Liu Xunshan Liu Key Laboratory of Surface&Interface science of Polymer Materials of zhejiang Province School of Chemistry and Chemical EngineeringZhejiang Sci-Tech University928 Second StreetHangzhouZhejiang310018 China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchunJilin130022 China School of Materials science and Engineering Nanjing University of Science and TechnologyNanjingJiangsu210094 China

Investigating the quantum interference effect in single molecules is essential to comprehensively understand the underlying mechanism of single-molecule charge *** this study,we employed the mother molecule m-OPE and introduced a series of side groups with various electronic effects at the 2-position of the central phenyl ring,creating four daughter m-OPE *** single molecular conductivities of these molecule wires were measured using the scanning tunneling microscope breaking junction *** findings demonstrate that the substitutions regularly modulate the destructive quantum interference occurring within the m-OPE *** combining optical and electrochemical investigations,along with density functional theory computations,we discover that the conductivity of the molecules corresponds to the electron-donating/withdrawing ability of the ***,by adjusting the electron structures of the molecular backbone,we can systematically tailor the destructive quantum interference in the m-OPE molecules.

关键词： Quantum interference Single-molecule junctions Electron effect substituents Charge transport Molecular devices

Accelerating solar driven CO_(2) reduction via sulfur-doping boosted water dissociation and proton transfer

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Nano research 2024年第3期17卷 1056-1065页

作者： Ke Yan Liang Chen Yangguang Hu Ting Wang Cong Chen Chao Gao Youju Huang Benxia Li School of Chemistry and Chemical Engineering Key Laboratory of Surface&Interface Science of Polymer Materials of Zhejiang ProvinceZhejiang Sci-Tech UniversityHangzhou 310018China College of Material Chemistry and Chemical EngineeringKey Laboratory of Organosilicon Chemistry and Material TechnologyMinistry of EducationHangzhou Normal UniversityHangzhou 311121China School of Chemistry and Materials science University of Science and Technology of ChinaHefei 230026China

Exploring efficient photocatalysts for solar driven CO_(2) reduction with water(H_(2)O)as a proton donor is highly imperative but remains a great challenge because the synchronous enhancement of CO_(2) activation,H_(2)O dissociation and proton transfer is hardly achieved on a ***,the sluggish H_(2)O dissociation impedes the photocatalytic CO_(2) reduction reaction involving multiple proton–electron coupling transfer ***,a sulfur-doped BiOCl(S-BiOCl)photocatalyst with abundant oxygen vacancies(OV)is developed,which exhibits broadband-light harvesting across solar spectrum and distinct photothermal effect due to *** photocatalytic CO_(2) reduction with H_(2)O in a gas–solid system,the high CO yield of 49.76μmol·g_(cat)^(-1)·h^(-1) with 100%selectivity is achieved over the S-BiOCl catalyst under a simulated *** H_(2)O-assisted CO_(2) reduction reaction on S-BiOCl catalyst is triggered by photocatalysis and the photothermal heating further enhances the reaction *** kinetic isotope experiments indicate that the sluggish H_(2)O dissociation affects the whole photocatalytic CO_(2) reduction *** presence of oxygen vacancies promotes the adsorption and activation of H_(2)O and CO_(2),and the doped S sites play a crucial role in boosting H_(2)O dissociation and accelerating the dynamic migration of hydrogen *** a result,the ingenious integration of OV defects,S sites and photothermal effect in S-BiOCl catalyst conjointly contributes to the significant improvement in photocatalytic CO_(2) reduction performance.

关键词： BiOCl sulfur doping photocatalytic CO_(2)reduction H_(2)O activation proton feeding

Equivariant Tautological Integrals on Flag Varieties

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Chinese Annals of Mathematics,Series B 2024年第3期45卷 463-486页

作者： Xiaobo ZHUANG Department of Mathematical sciences Zhejiang Sci-Tech UniversityHangzhou 310018China

The author apples the Atiyah-Bott-Berline-Vergne formula to the equivariant tautological integrals over flag varieties of types A,B,C,D,and recovers the formulas expressing the integrals as iterated residues at infini... 详细信息

关键词： Localization Flag variety Residue

Multifunctional Peptide-Melanin Hybrid Nanodots with Robust Anti-Cutaneous Photoaging Activity

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Journal of Analysis and Testing 2024年第3期8卷 395-401页

作者： Peizhe Li Qiming Zhu Baozhu Wang Shanshan He Qi Xu Kaiyan Li Yongmiao Shen Miao Su Zhijun Zhang Key Laboratory of Surface & Interface science of Polymer Materials of zhejiang Province School of Chemistry and Chemical Engineering Zhejiang Sci-Tech University College of Textile science and Engineering (International Silk Institute) Zhejiang Sci-Tech University Shanghai Beautyart Biotechnology Co. Ltd. Shengzhou Innovation research Institute of zhejiang scitech university

Skin aging is a systematic and complex process, mainly including intrinsic aging caused by time change and extrinsic aging caused by environmental factors. Photoaging caused by ultraviolet (UV) irradiation is the principle extrinsic factor of skin aging, which can directly or indirectly cause damage to DNA and other biomolecules, generate reactive oxygen species(ROS), and induce a decrease in collagen synthesis and other adverse eff ect. Herein, to address the causative factors and multiple side eff ects of skin photoaging, we constructed multifunctional peptide-melanin hybrid nanodots (PMHDs) to achieve multifaceted synergistic anti-skin aging by using melanin-like nanodots (MDs) and functional peptides as active *** them, the peptide has the activity of promoting collagen synthesis, while the MDs have the function of absorbing UV light and scavenging free radicals. Additionally, the MDs also act as a carrier to increase the cellular uptake of the *** anti-photoaging eff ects of the PMHDs were systematically verifi ed in a multidimensional manner at the biochemical,cellular and small animal levels, respectively.

关键词： Nanodots

Defect Engineering and Carbon Supporting to Achieve Ni‑Doped CoP_(3) with High Catalytic Activities for Overall Water Splitting

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Nano-Micro Letters 2024年第11期16卷 569-584页

作者： Daowei Zha Ruoxing Wang Shijun Tian Zhong‑Jie Jiang Zejun Xu Chu Qin Xiaoning Tian Zhongqing Jiang Department of Physics Zhejiang Sci-Tech UniversityHangzhou 310018People’s Republic of China Department of Materials and Chemical Engineering Ningbo University of TechnologyNingbo 315211People’s Republic of China Guangzhou Key Laboratory for Surface Chemistry of Energy Materials Guangdong Engineering and Technology Research Center for Surface Chemistry of Energy MaterialsCollege of Environment and EnergySouth China University of TechnologyGuangzhou 510006People’s Republic of China

This work reports the use of defect engineering and carbon supporting to achieve metal-doped phosphides with high activities and stabilities for the hydrogen evolution reaction(HER)and the oxygen evolution reaction(OER)in alkaline ***,the nitrogen-doped carbon nanofiber-supported Ni-doped CoP_(3) with rich P defects(Pv·)on the carbon cloth(p-NiCoP/NCFs@CC)is synthesized through a plasma-assisted phosphorization *** p-NiCoP/NCFs@CC is an efficient and stable catalyst for the HER and the *** only needs overpotentials of 107 and 306 mV to drive 100 mA cm^(-2) for the HER and the OER,*** catalytic activities are higher than those of other catalysts reported *** high activities of the p-NiCoP/NCFs@CC mainly arise from its peculiar structural *** density functional theory calculation indicates that the Pv·richness,the Ni doping,and the carbon supporting can optimize the adsorption of the H atoms at the catalyst surface and promote the strong electronic couplings between the carbon nanofiber-supported p-NiCoP with the surface oxide layer formed during the OER *** gives the p-NiCoP/NCFs@CC with the high activities for the HER and the *** used in alkaline water electrolyzers,the p-NiCoP/NCFs@CC shows the superior activity and excellent stability for overall water splitting.

关键词： Plasma Electrocatalysis Hydrogen evolution reaction Oxygen evolution reaction Water splitting

Peroxidase-like nanozyme based microenvironment-responsive injectable hydrogel for bacteria-infected wound healing

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science China technological sciences 2024年第10期67卷 3247-3260页

作者： ZHOU Wei LI XiaNan TANG MengCheng PAN LingFeng WANG BeiBei ZHANG Hao ZHANG Han WANG ShiBo KONG XiangDong Institute of Smart Biomaterial Materials School of Materials Science and EngineeringZhejiang University of Science & Technology zhejiang-Mauritius Joint research Center for Biomaterials and Tissue Engineering Zhejiang University of Science & Technology

Hydrogel stands out as one of the most attractive wound dressings due to its excellent moisturizing properties and capacity to absorb wound exudates. However, conventional hydrogel dressings often lack responsiveness to the microenvironment, merely acting as protective barriers for the wound. Consequently, they exhibit limited effectiveness in preventing infection and facilitating wound repair. To address these problems, we have developed a multifunctional injectable hydrogel, CF/MS@HG, based on peroxidase-like nanozymes, aiming at rapidly healing bacterial-infected wounds. The hydrogel is mainly composed of oxidized sodium alginate, aminated gelatin, and polylysine, encapsulating MIL-101(CuFe) NPs(CF) and manganese selenide nanoparticles(MnSe2NPs, or MS NPs). After injection, the complex rapidly gelatinizes at the infected wound site through a Schiff base reaction. In vitro experiments have demonstrated the hydrogel's strong adhesion and self-healing ***, CF exhibiting peroxidase(POD)-like activity, catalyzes in situ hydrogen peroxide(H2O2) to generate highly toxic hydroxyl radicals(·OH) within the wound microenvironment, inducing oxidative damage to bacteria. Meanwhile, MS decomposes into H2Se in the slightly acidic wound microenvironment, disrupting bacterial metabolism and inhibiting *** addition of polylysine further enhances the hydrogel's antibacterial properties. In vivo experiments have shown that the hydrogel exhibits excellent biological safety and significantly promotes wound healing. This multifunctional smart hydrogel holds great promise for the treatment of bacterial-infected wounds.

关键词： peroxidase-like nanozyme manganese selenide injectable hydrogel bacterial infection wound healing

ELABELA-derived peptide ELA13 attenuates kidney fibrosis by inhibiting the Smad and ERK signaling pathways

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Journal of zhejiang university-science B(Biomedicine & Biotechnology) 2024年第4期25卷 341-353页

作者： Zhibin YAN Ying SHI Runling YANG Jijun XUE Caiyun FU zhejiang Provincial Key Laboratory of Silkworm Bioreactor and Biomedicine College of Life Sciences and MedicineZhejiang Sci-Tech UniversityHangzhou310018China State Key Laboratory of Applied Organic Chemistry College of Chemistry and Chemical EngineeringLanzhou University Lanzhou 730000China Key Laboratory of Preclinical Study for New Drugs of Gansu Province School of Basic Medical Sciences&Research Unit of Peptide ScienceChinese Academy of Medical Sciences2019RU066Lanzhou UniversityLanzhou 730000China

Kidney fibrosis is an inevitable result of various chronic kidney diseases(CKDs)and significantly contributes to end-stage renal ***,there is no specific treatment available for renal ***13(amino acid sequence:RRCMPLHSRVPFP)is a conserved region of ELABELA in all vertebrates;however,its biological activity has been very little *** the present study,we evaluated the therapeutic effect of ELA13 on transforming growth factor-β1(TGF-β1)-treated NRK-52E cells and unilateral ureteral occlusion(UUO)*** results demonstrated that ELA13 could improve renal function by reducing creatinine and urea nitrogen content in serum,and reduce the expression of fibrosis biomarkers confirmed by Masson staining,immunohistochemistry,real-time polymerase chain reaction(RT-PCR),and western *** biomarkers were increased after UUO and decreased by administration of ***,we found that the levels of essential molecules in the mothers against decapentaplegic(Smad)and extracellular signal-regulated kinase(ERK)pathways were reduced by ELA13 treatment in vivo and in *** conclusion,ELA13 protected against kidney fibrosis through inhibiting the Smad and ERK signaling pathways and could thus be a promising candidate for anti-renal fibrosis treatment.

关键词： ELA13 Kidney fibrosis Inflammation Smad Extracllular signal-regulated kinase(ERK)

纵向数据下精度矩阵的替代的修正Cholesky分解

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中国科学技术大学学报 2024年第3期54卷 46-61,I0008页

作者：芦飞曾宇婷浙江理工大学理学院浙江杭州310018

纵向数据下相关系数矩阵可能具有科学意义。然而,在精度矩阵具有典型结构时,很少有文献同时关注对模型误识别稳健的相关系数矩阵估计和对于数据中离群值的稳健性。本文中我们为纵向数据的精度矩阵提出了一种替代的修正Cholesky分解(alte... 详细信息

纵向数据下相关系数矩阵可能具有科学意义。然而,在精度矩阵具有典型结构时,很少有文献同时关注对模型误识别稳健的相关系数矩阵估计和对于数据中离群值的稳健性。本文中我们为纵向数据的精度矩阵提出了一种替代的修正Cholesky分解(alternative modified Cholesky decomposition, AMCD),从而得到了关于新息方差模型误识别稳健的相关系数矩阵估计。我们建立了基于多元正态分布和AMCD的联合均值-协方差模型,发展了拟Fisher得分算法,证明了其极大似然估计的相合性和渐近正态性。进一步,我们建立了基于多元Laplace分布和AMCD的双稳健联合建模方法,为其极大似然估计发展了拟Newton算法。模拟研究和实际数据分析验证了所提AMCD方法的有效性。

关键词： Cholesky分解精度矩阵相关系数矩阵多元Laplace分布稳健性

通过烷基官能化的框架材料调控SP@Tb-MOFs的动态荧光材料性能并探究其在时间分辨信息加密中的应用

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science China Materials 2024年第8期67卷 2590-2599页

作者：朱姜昆卫尤豪高阳旸倪骅程蔡海涛武聪浩杨玉慧 School of Materials science and Engineering Zhejiang Sci-Tech UniversityHangzhou 310018China Department of Polymer Materials Zhejiang Sci-Tech UniversityHangzhou 310018China Institute of Smart Biomedical Materials Zhejiang Sci-Tech UniversityHangzhou 310018China

动态荧光材料在数据存储和防伪技术领域受到广泛关注.在此,我们提出了一种得到动态荧光材料的新方法,即在烷基链修饰的镧系金属有机框架(Ln-MOFs)中引入螺吡喃(SP)分子.烷基化配体既可用作桥接配体,也可用作结构导向剂,以调节镧系金属... 详细信息

动态荧光材料在数据存储和防伪技术领域受到广泛关注.在此,我们提出了一种得到动态荧光材料的新方法,即在烷基链修饰的镧系金属有机框架(Ln-MOFs)中引入螺吡喃(SP)分子.烷基化配体既可用作桥接配体,也可用作结构导向剂,以调节镧系金属有机框架的形态.通过控制烷基链的长度,可以调整Tb-MOFs的形态,从而进一步调节复合体系的光致变色行为.当烷基链较短时,复合体系只能发出黄色或者绿色的光.只有SP@Tb-MOF-10C能在545 nm波长处发出Tb^(3+)的绿色发射,在650 nm波长处发出SP的红色发射.在365 nm紫外光的持续照射下,SP分子发生了光异构化过程,变成了开环形式,从而导致Tb-MOF与其光异构体(MC)之间发生了显著的荧光共振能量转移(FRET).在白光照射下,这些复合材料的动态荧光行为可完全恢复到初始状态.此外,本文通过将该复合体系掺杂聚二甲基硅氧烷(PDMS),制备了复合薄膜,并探究了其在防伪标签和时间分辨动态加密方面的应用.

关键词：信息加密防伪标签金属有机框架荧光材料动态加密光异构化防伪技术时间分辨