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Difluoromethyl phenoxathiinium salt: A new general and versatile difluoromethylating reagent with divergent ·CF_(2)H, CF_(2)H^(+), and :CF_(2) reactivities

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Science China Chemistry 2024年第3期67卷 953-962页

作者： Yuan-Qing gu Hong-Xin long Dan-Dan Zhang Mei-Feng Ruan guo-Kai Liu School of Pharmacy Shenzhen University Medical SchoolShenzhen UniversityShenzhen 518055China

Development of practical and versatile electrophilic difluoromethylating reagent is still a grand challenge so far due to its inherent instability or low reactivity.Herein,we report the design and synthesis of difluoromethyl phenoxathiinium tetrafluoroborate(PT-CF_(2)H^(+)BF_(4)^(-)) as a novel difluoromethylating reagent,which proves to be a bench-stable,general,powerful and versatile reagent with divergent·CF_(2)H,CF_(2)H^(+),and:CF_(2) reactivities.Making use of this reagent,we demonstrated a vast array of difluoromethyl radical transfer reactions via diverse pathways involving photocatalyst-free visible-light induction,visible-light photoredox catalysis and visible-light mediation single electron transfer of EDA complex.Moreover,the green and highly effective CF_(2)H^(+) and:CF_(2) transfer reactions were also readily accomplished.

关键词： difluoromethyl phenoxathiinium salt versatile difluoromethylating reagent difluoromethyl radical difluoromthyl cation difluorocarbene

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Differential bonding behaviors of sodium/potassium-ion storage in sawdust waste carbon derivatives

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Chinese Chemical Letters 2024年第4期35卷 496-501页

作者： Jun-Ming Cao Kai-Yang Zhang Jia-Lin Yang Zhen-Yi gu Xing-long Wu MOE Key Laboratory for UV Light-Emitting Materials and Technology Northeast Normal UniversityChangchun 130024China Department of Chemistry Northeast Normal UniversityChangchun 130024China

Sodium-ion batteries(SIBs) and potassium-ion batteries(PIBs) are the most promising alternatives to lithium-ion batteries, and thus have drawn intensive research attention. Porous carbon materials from different precursors have been widely used as anode materials owing to their compatible storage effectiveness of both larger radii sodium and potassium ions. However, the differential bonding behaviors of Na and K ions with porous carbon-based anode are the significant one worth investigating, which could provide a clean picture of alkali ions storage mechanism. Therefore, in this work, we prepare a porous carbon network derived from sawdust(SDC) wastes, to further analyze the differences on sodium and potassium ions storage behaviors in terms of bond-forming process. It is found that, as-prepared SDC anodes could deliver stable sodium and potassium storage capacities, however, there are notable distinctions in terms of electrochemical behaviors and diffusion processes. By virtue of ex-situ XRD and Raman spectroscopy, the phase transition reaction of potassium ions could be well-observed, and the results shows that the multiple intercalated compounds was formed in SDC network during ions insertion, further resulting in slower diffusion kinetics and larger resistance compared to non-bonded process of sodium ions storage. This study provides more insights into the differences between sodium and potassium ions storage, as well as the energy storage mechanism of porous carbon as anodes for secondary batteries.

关键词： Porous carbon Sodium-ion storage Potassium-ion storage Bonding behaviors Batteries

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Potential therapeutic role of spermine via Rac1 in osteoporosis:Insights from zebrafish and mice

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Zoological Research 2024年第2期45卷 367-380页

作者： Rui-Xue Jiang Nan Hu Yu-Wei Deng long-Wei Hu Hao gu Nan Luo Jin Wen Xin-Quan Jiang Department of Prosthodontics Shanghai Ninth People’s HospitalShanghai Jiao Tong University School of MedicineShanghai 200011China College of Stomatology Shanghai Jiao Tong UniversityNational Center for StomatologyNational Clinical Research Center for Oral DiseasesShanghai Key Laboratory of StomatologyShanghai Research Institute of StomatologyShanghai Engineering Research Center of Advanced Dental Technology and MaterialsShanghai 200125China Department of Endodontics Shanghai Ninth People’s HospitalShanghai Jiao Tong University School of MedicineShanghai Jiao Tong UniversityShanghai 200011China Department of Oral and Maxillofacial-Head and Neck Oncology Shanghai Ninth People’s HospitalSchool of MedicineShanghai Jiao Tong UniversityShanghai 200011China Department of Preventive Dentistry Shanghai Ninth People’s HospitalShanghai Jiao Tong University School of MedicineShanghai Jiao Tong UniversityShanghai 200011China

Osteoporosis(OP)is a prevalent metabolic bone disease.While drug therapy is essential to prevent bone loss in osteoporotic patients,current treatments are limited by side effects and high costs,necessitating the development of more effective and safer targeted therapies.Utilizing a zebrafish(Danio rerio)larval model of osteoporosis,we explored the influence of the metabolite spermine on bone homeostasis.Results showed that spermine exhibited dual activity in osteoporotic zebrafish larvae by increasing bone formation and decreasing bone resorption.Spermine not only demonstrated excellent biosafety but also mitigated prednisolone-induced embryonic neurotoxicity and cardiotoxicity.Notably,spermine showcased protective attributes in the nervous systems of both zebrafish embryos and larvae.At the molecular level,Rac1 was identified as playing a pivotal role in mediating the antiosteoporotic effects of spermine,with P53 potentially acting downstream of Rac1.These findings were confirmed using mouse(Mus musculus)models,in which spermine not only ameliorated osteoporosis but also promoted bone formation and mineralization under healthy conditions,suggesting strong potential as a bonestrengthening agent.This study underscores the beneficial role of spermine in osteoporotic bone homeostasis and skeletal system development,highlighting pivotal molecular mediators.Given their efficacy and safety,human endogenous metabolites like spermine are promising candidates for new anti-osteoporotic drug development and daily bone-fortifying agents.

关键词： Osteoporosis Spermine Rac1 Zebrafish Mice

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Accurate and efficient floor localization with scalable spiking graph neural networks

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Satellite Navigation 2024年第1期5卷 191-206页

作者： Fuqiang gu Fangming guo Fangwen Yu Xianlei long Chao Chen Kai Liu Xuke Hu Jianga Shang Songtao guo College of Computer Science Chongqing UniversityChongqingChina Department of Precision Instrument Tsinghua UniversityBeijingChina Institute of Data Science German Aerospace Center(DLR)JenaGermany School of Computer Science China University of GeosciencesWuhanChina

Floor localization is crucial for various applications such as emergency response and rescue,indoor positioning,and recommender systems.The existing floor localization systems have many drawbacks,like low accuracy,poor scalability,and high computational costs.In this paper,we first frame the problem of floor localization as one of learning node embeddings to predict the floor label of a subgraph.Then,we introduce FloorLocator,a deep learning-based method for floor localization that integrates efficient spiking neural networks with powerful graph neural networks.This approach offers high accuracy,easy scalability to new buildings,and computational efficiency.Experimental results on using several public datasets demonstrate that FloorLocator outperforms state-of-the-art methods.Notably,in building B0,FloorLocator achieved recognition accuracy of 95.9%,exceeding state-of-the-art methods by at least 10%.In building B1,it reached an accuracy of 82.1%,surpassing the latest methods by at least 4%.These results indicate FloorLocator’s superiority in multi-floor building environment localization.

关键词： Indoor positioning Deep learning Floor localization Spiking neural networks Graph neural networks

Zincophilic Ti_(3)C_(2)Cl_(2)MXene and anti-corrosive Cu NPs for synergistically regulated deposition of dendrite-free Zn metal anode

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Journal of Materials Science & Technology 2024年第2期169卷 137-147页

作者： Yunfei Shen Yi Liu Kaisheng Sun Tiantian gu Gang Wang Yue Yang Jianxiang Pang Yang Zheng Xiaodong Yang long Chen Key Laboratory for Green Process of Chemical Engineering of Xinjiang Bingtuan School of Chemistry and Chemical EngineeringShihezi UniversityShihezi 832003China Institute for Chemistry Chemnitz University of TechnologyChemnitz 09107Germany CAS Key Laboratory of Functional Materials and Devices for Special Environments Xinjiang Key Laboratory of Electronic Information Materials and DevicesCenter of Materials Science and Optoelectronics EngineeringXinjiang Technical Institute of Physics and Chemistry of CASUrumqi 830011China Key Laboratory of Ecophysics and Department of Physics College of ScienceShihezi UniversityShihezi 832003China

Dendrites growth,chemical corrosion,and hydrogen evolution reaction(HER)on zinc anodes are the main barriers for the development of aqueous zinc-ion batteries(AZIBs).Constructing interfacial protec-tive layer is an effective way to alleviate the side reactions on the anodes.Herein,Cu/Ti_(3)C_(2)Cl_(2)MXene(CMX)with high zincophilic and hydrophobic property is prepared by the lewis molten salts etching method,and the CMX interface protection layer is constructed by a simple spin coating.The CMX coat-ing layer can provide abundant nucleation sites and uniformize the charge distribution through the zin-cophilic Ti_(3)C_(2)Cl_(2)MXene matrix,leading to homogenous Zn deposition.In addition,the hydrophobic coat-ing contained anti-corrosive Cu nanoparticles can prevent the Zn anode from the electrolyte,beneficial for suppressing the chemical corrosion and HER.Therefore,the stable and reversible Zn plating/stripping is achieved for the Zn anode coated by the CMX,which exhibits the lifespan of over 1400 h at 0.5 mA cm^(−2),and even can steadily run for 700 h with 65 mV at 10 mA cm^(−2).Furthermore,CMX@Zn shows a high coulombic efficiency of over 100%for 3800 cycles,which indicates that the CMX@Zn electrode has excellent stability and reversibility of Zn stripping/plating.The full batteries assembled with ZnCoMnO/C(ZCM)cathodes also exhibits higher capacity(450.6 mAh g^(−1)at 0.1 A g^(−1))and cycle stability(capacity retention of 70%after 1500 cycles).This work enhanced the lifespan of AZIBs and broaden the research of multifunctional coating layer to other secondary batteries based on metal anodes.

关键词： Zinc anode Spin coating Zincophilic MXene Anti-corrosive Cu NPs Multifunctional coating

Branched glycopolymer prodrug-derived nanoassembly combined with a STING agonist activates an immuno-supportive status to boost anti-PD-L1 antibody therapy

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Acta Pharmaceutica Sinica B 2024年第5期14卷 2194-2209页

作者： Zhilin Li Qianfeng Zhang Zhiqian Li long Ren Dayi Pan Qiyong Gong Zhongwei gu Hao Cai Kui Luo Department of Radiology Huaxi MR Research Center(HMRRC)Clinical Research Center for BreastDepartment of Breast SurgeryDepartment of Thoracic Surgery and Institute of Thoracic OncologyFrontiers Science Center for Disease-Related Molecular NetworkState Key Laboratory of BiotherapyWest China Hospital Sichuan UniversityChengdu 610041China Functional and Molecular Imaging Key Laboratory of Sichuan Province and Research Unit of PsychoradiologyChinese Academy of Medical SciencesChengdu 610041China Department of Radiology West China Xiamen Hospital of Sichuan UniversityXiamen 361021China Key Laboratory of Medicinal Chemistry for Natural Resource Ministry of EducationYunnan Key Laboratory of Research and Development for Natural ProductsSchool of PharmacyYunnan UniversityKunming 650500China

Despite the great potential of anti-PD-L1 antibodies for immunotherapy,their low response rate due to an immunosuppressive tumor microenvironment has hampered their application.To address this issue,we constructed a cell membrane-coated nanosystem(mB4S)to reverse an immunosuppressive microenvironment to an immuno-supportive one for strengthening the anti-tumor effect.In this system,Epirubicin(EPI)as an immunogenic cell death(ICD)inducer was coupled to a branched glycopolymer via hydrazone bonds and diABZI as a stimulator of interferon genes(STING)agonist was encapsulated into mB4S.After internalization of mB4S,EPI was acidic-responsively released to induce ICD,which was characterized by an increased level of calreticulin(CRT)exposure and enhanced ATP secretion.Meanwhile,diABZI effectively activated the STING pathway.Treatment with mB4S in combination with an anti-PD-L1 antibody elicited potent immune responses by increasing the ratio of matured dendritic cells(DCs)and CD8+T cells,promoting cytokines secretion,up-regulating M1-like tumor-associated macrophages(TAMs)and down-regulating immunosuppressive myeloid-derived suppressor cells(MDSCs).Therefore,this nanosystem for co-delivery of an ICD inducer and a STING agonist achieved promotion of DCs maturation and CD8+T cells infiltration,creating an immuno-supportive microenvironment,thus potentiating the therapy effect of the anti-PD-L1 antibody in both 4T1 breast and CT26 colon tumor mice.

关键词： Glycopolymer Polymer prodrug Immunogenic cell death Nanoassembly Epirubicin STING pathway Immuno-supportive microenvironment Immunotherapy

A cell transcriptomic profile p ovides insights into adipocytes of porcine mammary gland across development

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Journal of Animal Science and Biotechnology 2024年第1期15卷 182-200页

作者： Yongliang Fan long Jin Zhiping He Tiantian Wei Tingting Luo Jiaman Zhang Can Liu Changjiu Dai Chao A Yan Liang Xuan Tao Xuebin Lv Yiren gu Mingzhou Li State Key Laboratory of Swine and Poultry Breeding Industry College of Animal Science and TechnologySichuan Agricultural UniversityChengdu 611130China Key Laboratory of Qinghai‑Tibetan Plateau Animal Genetic Resource Reservation and Utilization Southwest Minzu UniversityChengdu 610041China Animal Breeding and Genetics Key Laboratory of Sichuan Province Sichuan Animal Science AcademyChengdu 610000China

Background Studying the composition and developmental mechanisms in mammary gland is crucial for healthy growth of newborns. The mammary gland is inherently heterogeneous, and its physiological function dependents on the gene expression of multiple cell types. Most studies focused on epithelial cells, disregarding the role of neighboring adipocytes.Results Here, we constructed the largest transcriptomic dataset of porcine mammary gland cells thus far. The dataset captured 126,829 high-quality nuclei from physiological mammary glands across five developmental stages(d 90 of gestation, G90;d 0 after lactation, L0;d 20 after lactation, L20;2 d post natural involution, PI2;7 d post natural involution, PI7). Seven cell types were identified, including epithelial cells, adipocytes, endothelial cells, fibroblasts cells, immune cells, myoepithelial cells and precursor cells. Our data indicate that mammary glands at different developmental stages have distinct phenotypic and transcriptional signatures. During late gestation(G90), the differentiation and proliferation of adipocytes were inhibited. Meanwhile, partly epithelial cells were completely differentiated. Pseudo-time analysis showed that epithelial cells undergo three stages to achieve lactation, including cellular differentiation, hormone sensing, and metabolic activation. During lactation(L0 and L20), adipocytes area accounts for less than 0.5% of mammary glands. To maintain their own survival, the adipocyte exhibited a poorly differentiated state and a proliferative capacity. Epithelial cells initiate lactation upon hormonal stimulation. After fulfilling lactation mission, their undergo physiological death under high intensity lactation. Interestingly, the physiological dead cells seem to be actively cleared by immune cells via CCL21-ACKR4 pathway. This biological process may be an important mechanism for maintaining homeostasis of the mammary gland. During natural involution(PI2 and PI7), epithelial cell populations dedifferentiate into mesenchymal stem cells t

关键词： Adipocytes Cell–cell interaction Development Mammary gland snRNA-seq

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Unraveling magnetic properties and martensitic transformation in Mn-rich Ni-Mn-Sn alloys:first-principles calculations and experiments

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Rare Metals 2024年第4期43卷 1769-1785页

作者： Yu Zhang Jing Bai Ke-Liang guo Jia-Xin Xu Jiang-long gu Nicola Morley Qui-Zhi Gao Yu-Dong Zhang Claude Esling Xiang Zhao Liang Zuo Key Laboratory for Anisotropy and Texture of Materials (Ministry of Education) School of Material Science and EngineeringNortheastern University Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province School of Resources and Materials Northeastern University at Qinhuangdao Department of Material Science and Engineering University of Sheffield State Key Laboratory of Metastable Materials Science and Technology Yanshan University Laboratoire d'Etude des Microstructures Et de Mecanique des Materiaux University of Lorraine

We have investigated the phase stability,magnetic properties,and martensitic transformation thermodynamics/kinetics of the Ni24-xMn18+x+ySn6-y(x,y=0,1,2) system by combining the first-principles calculations and experiments.The calculation results show that the optimized lattice parameters are consistent with the experimental data.Respectively,we obtain the relation equation for the austenite formation energy(Eform-A) and Mn content(XMn):Eform-A=507.358XMn-274.126,as well as for the six-layer modulated(6M) martensite formation energy(Eform-6M) and Ni content(XNi):Eform-6M=-728.484XNi+264.374.The ternary phase diagram of the total magnetic moment was established.The excess Mn will reduce the total magnetic moment of 6M(Mag6M) and non-modulated(NM)(MagNM) martensites,with the following equations relating the total magnetic moment and Mn content:Mag6M=-15.905XMn+7.902and MagNM=-14.781XMn+7.411,while the effect on austenite is complex.The variation of total magnetic moment is mainly dominated by the Mn atomic magnetic moment.The 3d electrons of MnSn(Mn at Sn sublattice)play an important role in magnetic properties from the perspective of the electronic density of states.Based on the thermodynamics of martensitic transformation,the alloys will likely undergo austenite?6M?NM transformation sequence.Combining the thermodynamic and kinetic results,the martensitic transformation temperature decreases with x increasing and increases with y increasing.These results are expected to provide reference for predicting the phase stability and magnetic properties of NiMn-Sn alloys.

关键词： Ni–Mn–Sn First-principles calculations Martensitic transformation Magnetic property Kinetics

Cold-Induced Reprogramming of Subcutaneous White Adipose Tissue Assessed by Single-Cell and Single-Nucleus RNA Sequencing

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Research 2024年第1期2023卷 763-778页

作者： Qing Liu Qiaoyun long Jiayu Zhao Wenjie Wu Zexin Lin Wei Sun Ping gu Tuo Deng Kerry Martin Loomes Donghai Wu Alice P.S.Kong Jingying Zhou Alfred S.Cheng Hannah Xiaoyan Hui School of Biomedical Sciences The Chinese University of Hong KongHong KongChina Department of Pharmacology and Pharmacy The University of Hong KongHong KongChina guangzhou Institute of Biomedicine and Health Chinese Academy of SciencesGuangzhouChina China-New Zealand Joint Laboratory on Biomedicine and Health Chinese Academy of SciencesGuangzhouChina Department of Endocrinology Jinling HospitalNanjing UniversitySchool of MedicineNanjingChina National Clinical Research Center for Metabolic Diseases and Department of Metabolism and EndocrinologyThe Second Xiangya Hospital of Central South UniversityChangshaChina Key Laboratory of Diabetes Immunology Ministry of Educationand Metabolic Syndrome Research CenterThe Second Xiangya Hospital of Central South UniversityChangshaChina Clinical Immunology Center The Second Xiangya Hospital of Central South UniversityChangshaChina School of Biological Sciences and Maurice Wilkins Centre University of AucklandAucklandNew Zealand Department of Medicine and Therapeutics The Chinese University of Hong KongHong KongChina Hong Kong Institute of Diabetes and Obesity The Chinese University of Hong KongPrince of Wales HospitalShatinHong KongChina Li Ka Shing Institute of Health Sciences The Chinese University of Hong KongPrince of Wales HospitalShatinHong KongChina

Adipose browning has demonstrated therapeutic potentials in several diseases.Here,by conducting transcriptomic profiling at the single-cell and single-nucleus resolution,we reconstituted the cellular atlas in mouse inguinal subcutaneous white adipose tissue(iWAT)at thermoneutrality or chronic cold condition.All major nonimmune cells within the iWAT,including adipose stem and progenitor cells(ASPCs),mature adipocytes,endothelial cells,Schwann cells,and smooth muscle cells,were recovered,allowing us to uncover an overall and detailed blueprint for transcriptomes and intercellular cross-talks and the dynamics during white adipose tissue brown remodeling.Our findings also unravel the existence of subpopulations in mature adipocytes,ASPCs,and endothelial cells,as well as new insights on their interconversion and reprogramming in response to cold.The adipocyte subpopulation competent of major histocompatibility complex class Ⅱ(MHCⅡ)antigen presentation is potentiated.Furthermore,a subcluster of ASPC with CD74 expression was identified as the precursor of this MHCⅡ^(+)adipocyte.Beige adipocytes are transdifferented from preexisting lipid generating adipocytes,which exhibit developmental trajectory from de novo differentiation of amphiregulin cells(Aregs).Two distinct immune-like endothelial subpopulations are present in iWAT and are responsive to cold.Our data reveal fundamental changes during cold-evoked adipose browning.

关键词： evoked programming generating