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A Stable Open-Shell Conjugated Diradical Polymer with Ultra-High Photothermal Conversion Efficiency for NIR-Ⅱ Photo-Immunotherapy of Metastatic Tumor

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Nano-Micro Letters 2024年第2期16卷 1-14页

作者： Yijian Gao Ying Liu Xiliang Li Hui Wang Yuliang yang Yu Luo Yingpeng Wan chun‑sing Lee Shengliang Li Xiao‑Hong Zhang College of Pharmaceutical Sciences Soochow UniversitySuzhou 215123People’s Republic of China Institute of Functional Nano&Soft Materials(FUNSOM) Soochow UniversitySuzhou 215123People’s Republic of China Center of Super‑Diamond and Advanced Films(COSDAF)&Department of Chemistry City University of Hong Kong83 Tat Chee AvenueKowloonHong Kong SARPeople’s Republic of China

Massive efforts have been concentrated on the advance of eminent near-infrared(NIR) photothermal materials(PTMs) in the NIR-Ⅱ window(1000–1700 nm), especially organic PTMs because of their intrinsic biological safety compared with inorganic PTMs. However, so far, only a few NIR-Ⅱresponsive organic PTMs was explored, and their photothermal conversion efficiencies(PCEs) still remain relatively low. Herein, donor–acceptor conjugated diradical polymers with open-shell characteristics are explored for synergistically photothermal immunotherapy of metastatic tumors in the NIR-Ⅱ window. By employing side-chain regulation, the conjugated diradical polymer TTB-2 with obvious NIR-Ⅱ absorption was developed, and its nanoparticles realize a record-breaking PCE of 87.7% upon NIR-Ⅱ light illustration. In vitro and in vivo experiments demonstrate that TTB-2 nanoparticles show good tumor photoablation with navigation of photoacoustic imaging in the NIR-Ⅱ window, without any side-effect. Moreover, by combining with PD-1 antibody,the pulmonary metastasis of breast cancer is high-effectively prevented by the efficient photo-immunity effect. Thus, this study explores superior PTMs for cancer metastasis theranostics in the NIR-Ⅱ window, offering a new horizon in developing radical-characteristic NIR-Ⅱ photothermal materials.

关键词： NIR-Ⅱconjugated polymer Photothermal Radical Nanoparticles Cancer therapy

Remote sensing of air pollution incorporating integrated-path differential-absorption and coherent-Doppler lidar

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Defence Technology（防务技术） 2024年第1期31卷 594-601页

作者： Ze-hou yang Yong Chen chun-li Chen Yong-ke Zhang Ji-hui Dong Tao Peng Xiao-feng Li Ding-fu Zhou School of Physics Beijing Institute of TechnologyBeijing 100081China Southwest Institute of Technical Physics Chengdu 610041SichuanChina School of Optics and Photonics Beijing Institute of TechnologyBeijing 100081China

An innovative complex lidar system deployed on an airborne rotorcraft platform for remote sensing of atmospheric pollution is proposed and *** system incorporates integrated-path differential absorption lidar(DIAL) and coherent-doppler lidar(CDL) techniques using a dual tunable TEA CO_(2)laser in the 9—11 μm band and a 1.55 μm fiber *** combining the principles of differential absorption detection and pulsed coherent detection,the system enables agile and remote sensing of atmospheric *** static tests validate the system’s real-time detection capabilities,including the measurement of concentration-path-length product(CL),front distance,and path wind speed of air pollution plumes over long distances exceeding 4 *** experiments is conducted with the *** of the pollutant concentration and the wind field is carried out in an approximately 1 km slant range over scanning angle ranges from 45°to 65°,with a radial resolution of 30 m and10 *** test results demonstrate the system’s ability to spatially map atmospheric pollution plumes and predict their motion and dispersion patterns,thereby ensuring the protection of public safety.

关键词： Differential absorption LIDAR Coherent Doppler lidar Remoting sensing Atmospheric pollution

Electronic structure regulation and built-in electric field synergistically strengthen photocatalytic nitrogen fixation performance on Ti-BiOBr/TiO_(2)heterostructure

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Rare Metals 2024年第3期43卷 1125-1138页

作者： Ru-Qi Li Yu-Jie Bian chun-Ming yang Li Guo Tao-Xia Ma Chuan-Tao Wang Feng Fu Dan-Jun Wang College of Chemistry and Chemical Engineering Yan’an UniversityYan’an Key Laboratory of Green Catalysis and Quality Improvement and Utilization of Low Rank CoalYan’an716000China

At present,industrial synthetic ammonia was still obtained through the Hubble-Bosch process,with large energy *** is a research hotspot to realize green synthetic ammonia by using solar *** difficulty of photocatalytic ammonia synthesis was that the photo-excited electrons have not enough energy to active N≡*** this study,Ti was doped into BiOBr by one-step hydrothermal method,which was oxidized into TiO_(2)when the doping amount reaches the maximum,in situ forming Ti_(0.31)B_(0.69)OB/TiO_(2)*** from the synergistic effect of Ti doping and S-scheme heterojunction,the synthetic ammonia efficiency of Ti_(0.31)B_(0.69)OB/TiO_(2)-11.96 reached 1.643 mmol·g_(cat)^(-1)at mild conditions and without hole scavenger for up to 7 h,the efficiency of synthetic ammonia is 115 times,10.5 times and 3.3 times of that of BiOBr,Ti_(0.31)B_(0.69)OB and TiO_(2),***,DFT calculation confirms that Ti doping accurately refine the electronic structure of BiOBr,facilitate nitrogen adsorption activation and reduce hydrogenation reaction energy barrier,thus accelerating the reaction kinetics of photocatalytic nitrogen reduction(NRR),Meanwhile,constructing S-scheme heterojunction boosts the separation and transfer of photogenerated electron-hole pairs,improving the reduction ability of electrons in the conduction band of TiO_(2)and the oxidation ability of holes in the valence band of Ti_(0.31)B_(0.69)OB.

关键词： S-scheme heterostructure Electronic structure regulation Built-in electric field Synergistical stren4gthening Photocatalytic nitrogen fixation

Computational Screening of Pt1@Ti_(3)C_(2)T_(2)(T=O,S)MXene Catalysts for Water-Gas Shift Reaction

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Precision Chemistry 2024年第2期2卷 70-80页

作者： yang Meng Haiyan Wang Jin-Xia Liang chun Zhu Jun Li School of Chemistry and Chemical Engineering Guizhou UniversityGuiyang 550025China Department of Chemistry and Guangdong Provincial Key Laboratory of Catalytic Chemistry Southern University of Science and TechnologyShenzhen 518055China Department of Chemistry and Engineering Research Center of Advanced Rare-Earth Materials of Ministry of Education Tsinghua UniversityBeijing 100084China

Single-atom catalysts(SACs)provide an oppor-tunity to elucidate the catalytic mechanism of complex reactions in heterogeneous *** low-temperature water-gas shift(WGS)reaction is an important industrial technology to obtain high purity ***,we study the catalytic activity of Pt1@Ti_(3)C_(2)T_(2)(T=O,S)SACs,where one subsurface Ti atom with three T vacancies in the functionalized Ti_(3)C_(2)T_(2)(T=O,S)MXene is substituted by one Pt atom,for the low-temperature show that Pt1@Ti_(3)C_(2)T_(2)provides an excellent platform for the WGS reaction by its bowl-shaped vacancy derived from the Pt1 single atom and three T defects surrounding ***,Pt1@Ti_(3)C_(2)S_(2)SAC has higher catalytic performance for the WGS reaction,due to the weaker electronegativity of the S atom than the O atom,which significantly reduces the energy barrier of H*migration in the WGS reaction,which is often the rate-determining *** the most favorable redox mechanism of the WGS reaction on Pt1@Ti_(3)C_(2)S_(2),the rate-determining step is the dissociation of OH*into O*and H*with the energy barrier as low as 1.12 *** results demonstrate that Pt1@Ti_(3)C_(2)S_(2)is promising in the application of MXenes for low-temperature WGS reactions.

关键词： single-atom catalyst(SAC) density functional theory(DFT) water gas shift(WGS)reaction defective MXene thermocatalysis

Single transition-metal atoms anchored on a novel Diracdispersiveπ-πconjugated holey graphitic carbon nitride substrate:computational screening toward efficient bifunctional OER/ORR electrocatalysts

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Rare Metals 2024年第8期43卷 3819-3832页

作者： chun-Yao Fang Xi-Hang Zhang Qiang Zhang Di Liu Xiao-Meng Cui Jing-Cheng Xu Cheng-Long Shi Meng-Yu yang College of Science University of Shanghai for Science and TechnologyShanghai 200093China School of Materials and Chemistry University of Shanghai for Science and TechnologyShanghai 200093China

Nonprecious-metal-group single-metal-atom catalysts with bifunctional catalytic capabilities toward the oxygen evolution reaction(OER)and oxygen reduction reaction(ORR)are highly sought after in energy-conversion and storage ***,producing renewable and sustainable energy sources remains ***,single-transition metal atoms anchored onπ-πconjugated two-dimensional(2D)graphitic carbon nitride substrates formπ-d conjugated conductive channels that enhance the overall electrocatalytic ***,firstprinciples calculations were carried out to design and demonstrate a novel macropore graphitic carbon nitride(gC_(10)N_(3))as a promising 2D electrocatalyst substrate to support single-transition metal(TM,from Sc to Au).The"donation-acceptance"charge interaction in the TM-N_(2)moiety effectively balances the adsorption strength of oxygenated intermediates in Ni@g-C_(10)N_(3)and Rh@gC_(10)N_3,making them effective bifunctional OER/ORR electrocatalysts with IrO_(2)/Pt-beyond overpotentials being as low as 0.39/0.38 V and 0.54/0.44 V,***,they possess high stability and conductivity and are less susceptible to oxidation and corrosion under working *** guarantees high activity under ambient ***,the origin of the OER/ORR activity of TM@g-C_(10)N_(3) is explained using multilevel descriptors:intrinsic(p,Bader charge,integral crystal orbital Hamilton population(ICOHP),bond length,and d-band center(εd).In particular,for optimal Ni@g-C_(10)N_(3),the clear hybridization between the Ni-d orbital and surface O-p orbital causes the paired electrons to occupy the bonding *** enables OH~*to be adsorbed on the Ni@g-C_(10)N_(3),thereby achieving the highest catalytic performance.

关键词： First-principles calculation Oxygen evolution reaction Oxygen reduction reaction Bifunctional electrocatalysts Single-metal-atom electrocatalysts

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面向蓄意攻击的网络异常检测方法

东北大学学报（自然科学版） 2020年第10期41卷 1376-1381页

作者：赵海郑春阳王进法司帅宗东北大学计算机科学与工程学院辽宁沈阳110169 中国科学院信息工程研究所/物联网安全北京市重点实验室北京100093

针对复杂网络受蓄意攻击频繁,而现有的检测方法大多忽略全局拓扑突变特征的问题.从网络全局拓扑的异常演化特征出发,提出网络路径相对变化系数(network path change coefficient,NPCC)r,量化节点间传输路径的变化.由斐波那契数列衍生出... 详细信息

针对复杂网络受蓄意攻击频繁,而现有的检测方法大多忽略全局拓扑突变特征的问题.从网络全局拓扑的异常演化特征出发,提出网络路径相对变化系数(network path change coefficient,NPCC)r,量化节点间传输路径的变化.由斐波那契数列衍生出斐波那契演化域,用于区分正常和异常演化.将r作为核心度量参量,构建斐波那契演化域,形成网络异常检测方法,实现对异常的判定.结果表明,该检测方法的平均准确率为90%以上,高于最大公共子图(maximum common subgraph,MCS)及图编辑距离(graph edit distance,GED)的准确率,证明了所提检测方法的有效性.

关键词：网络异常检测斐波那契演化域路径变化系数蓄意攻击网络科学

Hollow Multishelled Structure: Synthesis Chemistry and Application

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Chemical Research in Chinese Universities 2024年第3期40卷 346-393页

作者： MAO Dan WANG Chao LI Wei ZHOU Liang LIU Jian zheng Zjian ZHAO Yong CAO An-min WANG Shutao HUANG Jiaxing HUO Fengwei CHEN Hongyu MAI Liqiang YU Ranbo WANG Lianzhou LU Yunfeng YU Chengzhong yang Qihua yang Zhenzhong ZENG Hua chun ZHAO Hujun TANG Zhiyong ZHAO Dongyuan WANG Dan State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChineseAcademy of SciencesBeijing 100190P.R.China Key Laboratory of Biopharmaceutical Preparation and Delivery Chinese Academy of SciencesBejing 100190P.R.China School of Fashion and Textiles The Hong Kong Polytechnic UniversityHong Kong SARP.R.China Department of Chemistry Fudan UniversityShanghai 200433P.R.China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070P.R.China State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023P.R.China School of Chemistry Beihang UniversityBejing 100191P.R.China CAS Key Laboratory of Molecular Nanostructure and Nanotechnology and Beijing National Laboratory for Molecular Sciences Institute of ChemistryChinese Academy of SciencesBeijing 100190P.R.China CAS Key Laboratory of Bio-inspired Materials and Interfacial Science Technical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190P.R.China School of Engineering Westlake UniversityHangzhou 310024P.R.China School of Flexible Electronics(Future Technologies) Nanjing Tech UniversityNanjing 211816P.R.China School of Science Westlake UniversityHangzhou 310024P.R.China School of Materials Science and Engineering Wuhan University of TechnologyWuhan 430070P.R.China School of Metallurgical and Ecological Engineering University of Science and Technology BeijingBeijing 100083P.R.China School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnology The University of QueenslandBrisbaneQueensland 4072Australia College of Life Science and Technology Bejing University of Chemical TechnologyBejing 100029P.R.China School of Chemistry and Molecular Engineering East China Normal UniversityShanghai 200241P.R.China College of Life Sciences Zhejiang Normal UniversityJinhua 321004P.R.China Department of Chemical Engineering Tsinghua UniversityBeijing 100

Hollow multishelled structure(HoMS),a promising and complex multifunctional structural system,features at least two shells that are separated by internal *** unique structure endows it with numerous advantages including low density,high loading capacity,large specific surface area,facilitated mass transport,and multiple spatial confinement *** the past twenty years,benefiting from the booming development of synthesis methods,various HoMS materials have been prepared and show promising applications in diverse areas.

关键词： Hollow multishelled structure Synthesis chemistry Energy storage Catalysis Electromagnetic wave absorption Drug delivery Sensor

Research on the solid particle erosion wear of pipe steel for hydraulic fracturing based on experiments and numerical simulations

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Petroleum Science 2024年第4期21卷 2779-2792页

作者： Si-Qi yang Jian-chun Fan Ming-Tao Liu De-Ning Li Jun-Liang Li Li-Hong Han Jian-Jun Wang Shang-Yu yang Si-Wei Dai Lai-Bin Zhang State Key Laboratory of Oil and Gas Equipment CNPC Tubular Goods Research Institute Key Laboratory of Oil and Gas Safety and Emergency Technology China University of Petroleum Oil Production Technology Research Institute of Liaohe Oilfield Company Tianjin Gas Storage Branch PetroChina Dagang Oilfield Company Petroleum Production Engineering Research Institute Daqing Oilfield Company

Erosion wear is a common failure mode in the oil and gas industry. In the hydraulic fracturing, the fracturing pipes are not only in high-pressure working environment, but also suffer from the impact of the high-speed solid particles in the fracturing fluid. Beneath such complex conditions, the vulnerable components of the pipe system are prone to perforation or even burst accidents, which has become one of the most serious risks at the fracturing site. Unfortunately, it is not yet fully understood the erosion mechanism of pipe steel for hydraulic fracturing. Therefore, this article provides a detailed analysis of the erosion behavior of fracturing pipes under complex working conditions based on experiments and numerical simulations. Firstly, we conducted erosion experiments on AISI 4135 steel for fracturing pipes to investigate the erosion characteristics of the material. The effects of impact angle, flow velocity and applied stress on erosion wear were comprehensively considered. Then a particle impact dynamic model of erosion wear was developed based on the experimental parameters, and the evolution process of particle erosion under different impact angles, impact velocities and applied stress was analyzed. By combining the erosion characteristics, the micro-structure of the eroded area, and the micro-mechanics of erosion damage, the erosion mechanism of pipe steel under fracturing conditions was studied in detail for the first time. Under high-pressure operating conditions, it was demonstrated through experiments and numerical simulations that the size of the micro-defects in the eroded area increased as the applied stress increased, resulting in more severe erosion wear of fracturing pipes.

关键词： Erosion wear Applied stress Particle impact dynamics Erosion mechanism

Establishment of a cholangiocarcinoma risk evaluation model based on mucin expression levels

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World Journal of Gastrointestinal Oncology 2024年第4期16卷 1344-1360页

作者： chun-Yuan yang Li-Mei Guo yang Li Guang-Xi Wang Xiao-Wei Tang Qiu-Lu Zhang Ling-Fu Zhang Jian-Yuan Luo Department of Pathology Institute of Systems BiomedicineSchool of Basic Medical Sciences Peking UniversityPeking University Third HospitalPeking University Health Science CenterBeijing 100191China Department of General Surgery Peking University Third HospitalBeijing 100191China Department of Medical Genetics Department of Biochemistry and BiophysicsSchool of Basic Medical Sciences Peking UniversityPeking University Health Science CenterBeijing 100191China

BACKGROUND Cholangiocarcinoma(CCA)is a highly malignant cancer,characterized by frequent mucin ***1 has been identified as a critical oncogene in the progression of ***,the comprehensive understanding of how the mucin family influences CCA progression and prognosis is still *** To investigate the functions of mucins on the progression of CCA and to establish a risk evaluation formula for stratifying CCA *** Single-cell RNA sequencing data from 14 CCA samples were employed for elucidating the roles of mucins,complemented by bioinformatic ***-quent validations were conducted through spatial transcriptomics and *** construction of a risk evaluation model utilized the least absolute shrinkage and selection operator regression algorithm,which was further confirmed by independent cohorts and diverse data *** CCA tumor cells with elevated levels of MUC1 and MUC4 showed activated nucleotide metabolic pathways and increased ***5AC-high cells were found to promote CCA progression through WNT ***5B-high cells exhibited robust cellular oxidation activities,leading to resistance against antitumoral ***13-high cells were observed to secret chemokines,recruiting and transforming macrophages into the M2-polarized state,thereby suppressing antitumor ***16-high cells were found to promote tumor progression through interleukin-1/nuclear factor kappa-light-chain-enhancer of activated B cells signaling upon interaction with *** the expression levels of these mucins,a risk factor evaluation formula for CCA was developed and validated across multiple *** samples with higher risk factors exhibited stronger metastatic potential,chemotherapy resistance,and poorer *** Our study elucidates the functional mechanisms through which mucins contribute to CCA development,and provides tools for risk stratification in CCA.

关键词： Mucin Cholangiocarcinoma Single-cell RNA sequencing Spatial transcriptomics Prognosis