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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

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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

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Optimal timing of invasive intervention for high-risk non-ST-segment-elevation myocardial infarction patients

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Journal of Geriatric Cardiology 2024年第8期21卷 807-815页

作者： Juan-Juan ZHENG yue-Qiao SI Tian-Yang XIA Bing-Jun LU chun-yu ZENG Wei-Eric WANG Department of Geriatrics Southwest HospitalThird Military Medical UniversityChongqingChina Department of Cardiology Daping HospitalThird Military Medical UniversityChongqingChina

OBJECTIVE To compare the immediate,early,and delayed percutaneous coronary intervention(PCI)strategies in non-ST-segment-elevation myocardial infarction(NSTEMI)patients with *** Medical records of patients treated at the Daping Hospital,Third Military Medical University,Chongqing,China between 2011 and 2021 were retrospectively *** patients with complete available information were *** patients assigned into three groups based on the timing of PCI including immediate(<2 h),early(2–24 h)and delayed(≥24 h)*** Cox hazards regression and simpler nonlinear models were *** A total of 657 patients were included in the *** median follow-up length was 3.29(interquartile range:1.45–4.85)*** PCI strategy improved the major adverse cardiac event(MACE)outcome compared to the immediate or delayed PCI *** PCI,diabetes mellitus,and left main or/and left anterior descending or/and left circumflex stenosis or/and right coronary artery≥99%were predictors for MACE *** optimal timing range for PCI to reduce MACE risk is 3–14 h *** high-risk NSTEMI patients,early PCI reduced primary clinical outcomes compared to immediate or delayed PCI,and the optimal timing range was 3–14 h *** PCI was superior for NSTEMI with chronic kidney *** Delayed invasive strategy was helpful to reduce the incidence of MACE for high-risk NSTEMI with chronic kidney *** immediate PCI strategy might increase the rate of MACE.

关键词： patients infarction Chongqing

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Z-scheme Bi_(4)O_(5)Br_(2)/NH_(2)-MIL-125(Ti)heterojunctions enable exceptional visible photocatalytic degradation of organic pollutant

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Rare Metals 2024年第7期43卷 3161-3172页

作者： Feng Huang Muhammad Humayun Gang Li Ting-Ting Fan Wen-Lin Wang yu-Lin Cao Anton Nikiforov chun-Dong Wang Jing Wang Key Laboratory of Analytical Science and Technology of Hebei Province Key Laboratory of Medicinal Chemistry and Molecular Diagnosis of the Ministry of EducationState Key Laboratory of New Pharmaceutical Preparations and ExcipientsCollege of Chemistry and Materials ScienceHebei UniversityBaoding071002China Energy Water and Environment LabCollege of Humanities and SciencesPrince Sultan University11586 RiyadhSaudi Arabia Baoding Green Yijia Environmental Protection Technology Ltd Baoding 071051China Physics Laboratory Industrial Training CenterShenzhen Polytechnic UniversityShenzhen 518055China Department of Applied Physics Ghent University9000 GhentBelgium School of Integrated Circuits Wuhan National Laboratory for OptoelectronicsHuazhong University of Science and TechnologyWuhan 430074China

One key strategy to enhance photocatalytic performance is to improve the transfer and separation efficiency of photogenerated carriers by building optimized ***,novel Bi_(4)O_5Br_(2)/NH_(2)-MIL-125(Ti)Z-scheme heterojunctions are fabricated and used as photocatalysts for organic pollutant *** NH_(2)-MIL-125(Ti)nanosheets are exfoliated via a self-developed alkali solution stripping approach and then uniformly decorated on Bi_(4)O_(5)Br_(2).The as-prepared Bi_(4)O_(5)Br_(2)/NH_(2)-MIL-125(Ti)presents more than 90%degradation of various pollutants,outperforming the counterpart individual *** various characterization results suggest that the enhanced degradation rate is due to the more intimate face-to-face interfacial contact of the lamellar Z-scheme heterojunction materials,in which the migration path of carriers from the material's interior to the surface can be reduced,in turn enhancing migration efficiency and separation capability significantly.A possible photocatalytic reaction mechanism is proposed based on the photoelectric behaviors,radical trapping experiments and liquid chromatography mass spectrometry *** work promotes the development of new photocatalytic materials for heterojunctions with face-to-face interfacial contacts,as well as the effective purification of wastewater in environmental remediation.

关键词： Z-scheme heterojunctions Photocatalysis Alkaline solution stripping Bi_(4)O_(5)Br_(2) NH_(2)-MIL-125(Ti)

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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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Helicobacter pylori infection alters gastric microbiota structure and biological functions in patients with gastric ulcer or duodenal ulcer

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World Journal of Gastroenterology 2024年第24期30卷 3076-3085页

作者： Ling-Xiao Jin yu-Peng Fang Chen-Mei Xia Teng-Wei Cai Qian-Qian Li yu-yin Wang Hai-Fan Yan Xia Chen Department of Gastroenterology Wenling Hospital of Wenzhou Medical University(The First People’s Hospital of Wenling)Wenling 317500Zhejiang ProvinceChina

BACKGROUND Helicobacter pylori(***)infection is closely associated with gastrointestinal *** preliminary studies have indicated that *** infection had a significant impact on the mucosal microbiome structure in patients with gastric ulcer(GU)or duodenal ulcer(DU).AIM To investigate the contributions of *** infection and the mucosal microbiome to the pathogenesis and progression of ulcerative *** Patients with *** infection and either GU or DU,and healthy individuals without *** infection were *** or duodenal mucosal samples was obtained and subjected to metagenomic *** compositions of the microbial communities and their metabolic functions in the mucosal tissues were *** Compared with that in the healthy individuals,the gastric mucosal microbiota in the ***-positive patients with GU was dominated by ***,with signi-ficantly reduced *** intergroup differential functions,which were enriched in the ***-positive GU patients,were all derived from ***,particularly those concerning transfer RNA queuosine-modification and the synthesis of demethylmenaquinones or menaquinones.A significant enrichment of the uibE gene was detected in the synthesis *** was no significant difference in microbial diversity between the ***-positive DU patients and healthy *** *** infection significantly alters the gastric microbiota structure,diversity,and biological functions,which may be important contributing factors for GU.

关键词： Helicobacter pylori Gastric ulcer Duodenal ulcer Metagenomic sequencing Transfer RNA queuosine-modification Menaquinones

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Two polyoxovanadoborates with over 100 nuclei assembled from a {V_(14)Co_(12)B_(72)} cluster

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Science China Chemistry 2024年第8期67卷 2578-2585页

作者： Shuang-Xue Wu yu-Jiao Dong Yang Yang Chao Qin chun-Yi Sun Wei Guan Xin-Long Wang Zhong-Min Su Key Laboratory of Polyoxometalate and Reticular Material Chemistry of Ministry of Education Northeast Normal UniversityChangchun 130024China School of Chemistry and Environmental Engineering Changchun University of Science and TechnologyChangchun 130013China Key Laboratory of Advanced Materials of Tropical Island Resources Hainan UniversityHaikou 570228China

Combining theoretical prediction and experimental exploration, the first sandwich-type polyoxovanadoborate(POVB) with an odd number of nuclei, [V_(11)B_(26)O_(73)(OH)_(10)]^(8-)(1), was discovered under hydrothermal conditions. Density-functional theory(DFT)gives a rationalization for the existence of this structure and the structural feature is consistent with the {V_NB_(2N+X)}(X = 2, 4, 6, 8)general formula. Excitingly, when Co and 1,10-phenanthroline(phen) are introduced into the synthesis of vanadoborates system,a 100-nuclei [Co_6(phen)_(10)(H_(2)O)_8][V_(14)Co_(12)B_(72)O_(144)(OH)_(20)]·28H_(2)O(2) and a 102-nuclei [Co_6(phen)_(14)(H_(2)O)_(4)][V_(14)Co_(12)B_(72)O_(144)(OH)_(20)]·23H_(2)O(3) with the same core structure of [V_(14)Co_(12)B_(72)]^(12-)are obtained. The vase-shaped [V_(14)Co_(12)B_(72)] polyanion is a multilayered sandwich-type structure containing seven distinct structural layers and is the largest known POVB. Furthermore, 2demonstrates exceptional thermal and chemical stability and serves as an efficient and stable catalyst for the photoreduction of carbon dioxide.

关键词： boronate metallic materials polyoxovanadoborates density functional theory photocatalysis CO_(2)reduction

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Sperm acrosin activity may be a useful factor in choosing between ICSI and IVF for infertile male patients

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Asian Journal of Andrology 2024年第1期26卷 85-90页

作者： Ye-Na Hu Liang Hu Xin-yu yin Huan Zhang Yang-Qin Peng Gang Liu Ge Lin Wei-Na Li The Institute of Reproductive and Stem Cell Engineering School of Basic Medical ScienceCentral South UniversityChangsha 410008China Department of Andrology Reproductive and Genetic Hospital of CITiC-XiangyaChangsha 410013China Clinical Research Center for Reproduction and Genetics in Hunan Province Changsha 410013China Hunan Guangxiu Hi-tech Life Technology Co. Ltd.Changsha 410013China

The clinical applications of acrosin activity are *** analyzed 61578 male partners in infertile couples who visited the outpatient department of the Reproductive and Genetic Hospital of CITIC-Xiangya(Changsha,China)between August 2014 and December 2019 to determine the reference ranges and thresholds for acrosin activity in infertile Chinese men;to determine whether correlations exist between acrosin activity and age,sperm concentration,sperm morphology,or sperm motility;and to evaluate whether acrosin activity could serve as an effective prognostic indicator for choosing between in vitro fertilization(IvF)and intracytoplasmic sperm injection(icsl)in the *** cut-off value for the normal reference range of acrosin activity for male partners in infertile couples was 24.78μlU per 106 *** was no significant association between acrosin activity and age,sperm concentration,semen volume,total sperm count,progressive motility,or total motile spermatozoa.A weak positive correlation was found between acrosin activity and normal sperm *** was a statistically significant difference in abnormal acrosome morphology between the group with high acrosin activity(>24.78μlU per 106 sperm)and the group with low acrosin activity(<24.78μlU per 106 sperm).The group with a low IVF fertilization rate had a high index of abnormal acrosomal morphology at 21.2%,while the group with a high IVF fertilization rate had a low index of 0.2%.At an acrosin activity of<24.78μlU per 10 sperm,in one cycle of the same patient,the fertilization rate,normal fertilization rate,and good-quality embryo rate for Icsl were significantly higher than those for ***,the most promising application of acrosin activity could be in the selection of IcsI over IVF for infertile male patients with complete fertilization failure or a low fertilization rate.

关键词： acrosin activity fertilization rate ICSI IVF semen parameters

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Three positive charge nonapoptotic-induced photosensitizer with excellent water solubility for tumor therapy

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Chinese Chemical Letters 2024年第8期35卷 205-210页

作者： Zhe Li Ping-Zhao Liang Li Xu Fei-yu Yang Tian-Bing Ren Lin yuan Xia yin Xiao-Bing Zhang State Key Laboratory of Chemo/Biosensing and Chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangsha 410082China

Photodynamic therapy(PDT)has emerged as a significant cancer therapy ***,cation-based organic small molecule aggregation-induced emission(AIE)photosensitizers(PSs)attract the wide atten-tion of many scientists,due to improved reactive oxygen species(ROS)production after ***,such PSs tend to localize only the mitochondria,limiting the death way of tumor cells(usu-ally apoptosis)during PDT process,which may affect the therapeutic effect under some ***,we designed a novel water-soluble three positive charge PS,TPAN-18F,which could be distributed uniformly in cell cytoplasm and had distribution in different sub-organelles(mitochondria,endoplasmic reticulum,lysosome).The experimental results showed that TPAN-18F-based PDT process can not only disrupt mitochondrial functions(reducing ATP production and destroying mitochondrial membrane po-tential),but also elevate the intracellular lipid peroxides(LPOs)level,which evoke the non-apoptotic death manner of tumor ***,in vivo studies showed that TPAN-18F-based PDT could effectively inhibit tumor ***,we believe that the construction of TPAN-18F is suggestive for tumor non-apoptotic therapy.

关键词： Water-soluble Three positive charge Photosensitizer Nonapoptotic Tumor therapy

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Diabetes mellitus in patients with type 1 autoimmune pancreatitis at diagnosis and after corticosteroid therapy

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Hepatobiliary & Pancreatic Diseases International 2024年第4期23卷 393-398页

作者： Mei-Zi Li Tao Guo yun-Lu Feng Sheng-yu Zhang Xiao-yin Bai Xi Wu Kai Xu Ai-Ming Yang Department of Gastroenterology State Key Laboratory of Complex Severe and Rare DiseasesPeking Union Medical College HospitalPeking Union Medical College and Chinese Academy of Medical SciencesBeijing 100730China Department of Radiology Peking Union Medical College HospitalPeking Union Medical College and Chinese Academy of Medical SciencesBeijing 100730China

Background:A high prevalence of diabetes mellitus(DM)coexisting with autoimmune pancreatitis(AIP)is ***,evidence on the circumstances under which corticosteroid therapy(CST)for AIP improves or worsens DM is *** study aimed to demonstrate and identify predictors of DM control under the influence of ***:Patients diagnosed with type 1 AIP were enrolled from a prospectively maintained cohort and were classified into three groups according to the chronology in which AIP and DM were diagnosed:pre-existing DM(pDM),concurrent DM(cDM),and non-DM(nDM).The responses of DM to CST were assessed when corticosteroid was ceased or tapered to a maintenance dose and classified as‘improvement’and‘non-improvement’(including‘no change’and‘exacerbation’).Results:Among 101 patients with type 1 AIP,52(51.5%)patients were complicated with DM at the time of AIP diagnosis,with 36 patients in the cDM group and 16 patients in the pDM *** incidences of diffuse pancreatic swelling(72.2%)and pancreatic body/tail involvement(91.7%)were significantly higher in the cDM group than in both the pDM and nDM *** the 52 patients with DM,CST was administered in 48 *** logistic analysis identified that elevated serum gamma-glutamyl transferase(GGT)level at AIP diagnosis[odds ratio(OR)=0.032,95%confidence interval(CI):0.003-0.412,P=0.008]and pancreatic atrophy after CST(OR=0.027,95%CI:0.003-0.295,P=0.003)were negatively associated with DM control ***:Patients with diffuse pancreatic swelling and pancreatic body/tail involvement in pancreatitis tended to be complicated with cDM at AIP *** exerted a beneficial effect on the clinical course of DM in nearly half of the AIP patients complicated with DM at diagnosis,particularly in those without elevated serum GGT levels at diagnosis and who did not experience pancreatic atrophy after CST.

关键词： Type 1 autoimmune pancreatitis Diabetes mellitus Corticosteroid therapy Predictive factor Pancreatic atrophy

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