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Carbon Energy 2024年第8期6卷 205-213页

作者： Yida Zhang Qingyu Wang Lihui Wu Haibin Pan Chengyuan Liu yue lin Gongming Wang Xusheng Zheng National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefeiAnhuiChina College of Chemistry and Materials Science University of Science and Technology of ChinaHefeiAnhuiChina Department of Chemistry Hefei National Research Center for Physical Sciences at the MicroscaleUniversity of Science and Technology of ChinaHefeiAnhuiChina

The key to designing photocatalysts is to orient the migration of photogenerated electrons to the target active sites rather than dissipate at inert ***,we demonstrate that the doping of phosphorus(P)significantly enriches photogenerated electrons at Ni active sites and enhances the performance for CO_(2)reduction into *** photocatalytic CO_(2)reduction,Ni single‐atom‐anchored P‐modulated carbon nitride showed an impressive syngas yield rate of 85μmol gcat^(−1)h^(−1)and continuously adjustable CO/H_(2)ratios ranging from 5:1 to 1:2,which exceeded those of most of the reported carbon nitride‐based single‐atom *** studies reveal that P doping improves the conductivity of catalysts,which promotes photogenerated electron transfer to the Ni active sites rather than dissipate randomly at low‐activity nonmetallic sites,facilitating the CO_(2)‐to‐syngas photoreduction process.

关键词： carbon nitride CO_(2)photoreduction electron flow Ni single atoms syngas

Enhancing the Electrocatalytic Oxidation of 5-Hydroxymethylfurfural Through Cascade Structure Tuning for Highly Stable Biomass Upgrading

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Nano-Micro Letters 2024年第12期16卷 449-467页

作者： Xiaoli Jiang Xianhui Ma Yuanteng Yang Yang Liu Yanxia Liu lin Zhao Penglei Wang Yagang Zhang yue lin Yen Wei School of Materials and Energy University of Electronic Science and Technology of ChinaChengdu 611731People’s Republic of China Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026People’s Republic of China The Key Laboratory of Bioorganic Phosphorus Chemistry and Chemical Biology(Ministry of Education) Department of ChemistryTsinghua UniversityBeijing 100084People’s Republic of China School of Materials Science and Engineering North Minzu UniversityYinchuan 750021People’s Republic of China

Electrocatalytic 5-hydroxymethylfurfural oxidation reaction(HMFOR)provides a promising strategy to convert biomass derivative to highvalue-added ***,a cascade strategy is proposed to construct Pd-NiCo_(2)O_(4)electrocatalyst by Pd loading on Ni-doped Co3O4 and for highly active and stable synergistic HMF *** elevated current density of 800 mA cm^(-2)can be achieved at 1.5 V,and both Faradaic efficiency and yield of 2,5-furandicarboxylic acid remained close to 100%over 10 consecutive *** and theoretical results unveil that the introduction of Pd atoms can modulate the local electronic structure of Ni/Co,which not only balances the competitive adsorption of HMF and OH-species,but also promote the active Ni^(3+)species formation,inducing high indirect oxidation *** have also discovered that Ni incorporation facilitates the Co2+pre-oxidation and electrophilic OH*generation to contribute direct oxidation *** work provides a new approach to design advanced electrocatalyst for biomass upgrading.

关键词： 5-Hydroxymethylfurfural oxidation reaction Competitive adsorption Cascade strategy Elevated current density

Microstructure and Mechanical Behavior of Mg-Based Bimetal Plates with High Formability Sleeve by Co-extrusion

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Acta Metallurgica Sinica(English Letters) 2024年第3期37卷 499-512页

作者： yue-Hui Dang Sheng-lin Liu Xiao-Lei Ai Xiao-Wei Feng Bo Feng Zhuo Tian Ying-Fei lin Huan-Tao Chen Kai-Hong Zheng School of Materials Science and Engineering Chang’an UniversityShaanxi 710064China Guangdong Key Laboratory of Metal Toughening Technology and Application Institute of New MaterialsGuangdong Academy of SciencesGuangzhou 510650China

In this study,microstructure and mechanical behavior of two types of Mg-based bimetal plates with a high formability sleeve were systematically studied,with a great emphasis on the effect of the interface characteristic and the sleeve fraction on the plasticity of composite *** rule of mixtures(ROM)for elongation was also *** results show that when there is no or thin diffusion layer with thickness of about 3μm,Mg-based bimetal plates have a good plasticity with elongation of about 19-24%,and the ROM predicted elongations are very close to the experimental *** contrast,with a diffusion layer about 95-155μm thick,Mg-based bimetal plates exhibit a poor plasticity with elongation of about 11-17%,and the experimental elongations largely deviate from the ROM *** plasticity of Mg-based bimetal plates increases with increasing sleeve *** study provides new insights on the plastic deformation of Mg-based bimetal composites with a high formability sleeve.

关键词： Mg-based composites Co-extrusion Microstructure Mechanical behavior Plastic deformation

Iridium-Catalyzed Asymmetric Hydrogenation of Dialkyl Imines

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CCS Chemistry 2024年第4期6卷 905-911页

作者： Zheng Wang Xin-Yi Yang yue Xu Qi-lin Zhou State Key Laboratory and Institute of Elemento-Organic Chemistry College of ChemistryFrontiers Science Center for New Organic MatterNankai UniversityTianjin 300071

Asymmetric hydrogenation of dialkyl imines to chiral amines is difficult because the two alkyls of imines are so similar in spatial and electronic structure that chiral catalysts are difficult to distinguish between *** this study,we described an asymmetric hydrogenation of dialkyl imines by a chiral iridium catalyst containing spiro phosphine-amine-phosphine *** precisely adjusting the chiral pocket of catalyst,a highly efficient catalyst was *** this catalyst,a variety of dialkyl imines were hydrogenated to chiral amines with high yield and enantioselectivity.

关键词： spiro PNP ligand iridium catalyst enantioselective hydrogenation dialkyl imines chiral amines

Achieving Negatively Charged Pt Single Atoms on Amorphous Ni(OH)_(2)Nanosheets with Promoted Hydrogen Absorption in Hydrogen Evolution

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Nano-Micro Letters 2024年第10期16卷 213-224页

作者： yue Liu Gui Liu Xiangyu Chen Chuang Xue Mingke Sun Yifei Liu Jianxin Kang Xiujuan Sun lin Guo School of Chemistry Beijing Advanced Innovation Center for Biomedical EngineeringKey Laboratory of Bio-inspired Smart Interfacial Science and TechnologyBeihang UniversityBeijing 100191People's Republic of China School of Chemistry Key Laboratory of Environmentally Friendly Chemistry and Applications of Ministry of EducationXiangtan UniversityXiangtan 411105HunanPeople'Republic of China

Single-atom(SA)catalysts with nearly 100%atom utilization have been widely employed in electrolysis for decades,due to the outperforming catalytic activity and ***,most of the reported SA catalysts are fixed through the strong bonding between the dispersed single metallic atoms with nonmetallic atoms of the substrates,which greatly limits the controllable regulation of electrocatalytic activity of SA *** this work,Pt-Ni bonded Pt SA catalyst with adjustable electronic states was successfully constructed through a controllable electrochemical reduction on the coordination unsaturated amorphous Ni(OH)_(2)nanosheet *** on the X-ray absorption fine structure analysis and first-principles calculations,Pt SA was bonded with Ni sites of amorphous Ni(OH)_(2),rather than conventional O sites,resulting in negatively charged Pt^(δ-).In situ Raman spectroscopy revealed that the changed configuration and electronic states greatly enhanced absorbability for activated hydrogen atoms,which were the essential intermediate for alkaline hydrogen evolution *** hydrogen spillover process was revealed from amorphous Ni(OH)_(2)that effectively cleave the H-O-H bond of H_(2)O and produce H atom to the Pt SA sites,leading to a low overpotential of 48 mV in alkaline electrolyte at-1000 mA cm^(-2)mg^(-1)_(Pt),evidently better than commercial Pt/C *** work provided new strategy for the control-lable modulation of the local structure of SA catalysts and the systematic regulation of the electronic states.

关键词： Hydrogen evolution reaction Amorphous Pt single atoms Hydrogen spillover

Azocalixarenes: a scaffold of universal excipients with high efficiency

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Science China Chemistry 2024年第5期67卷 1697-1706页

作者： Yu-Xin yue Yi-lin lin Meng-Meng Chen Han-Wen Tian Rong Ma Ze-Han Wang Fang-Yuan Chen Yu-Chen Pan Dong-Sheng Guo College of Chemistry State Key Laboratory of Elemento-Organic ChemistryKey Laboratory of Functional Polymer Materials(Ministry of Education)Frontiers Science Center for New Organic MatterCollaborative Innovation Center of Chemical Science and Engineering(Tianjin)Nankai UniversityTianjin 300071China

Excipients are important components of pharmaceutical preparations that affect their quality, safety, and efficacy. Macrocyclic receptors are a family of supramolecular excipients with several advantages, including molecular-level protection, small sizes,fast kinetics of host-guest recognition, and modular construction. With the continuous advances in the medical field, personalized and precision medicine requires the development of excipients with low dosages, integrated modifying effects, universality,and controlled release. To meet these requirements, we have developed a new family of macrocyclic excipients based on calixarenes by integrating their covalent(broad chemical design space) and noncovalent(wide range of substrates) ***, azocalixarenes(Azo CAs) were designed, showing high binding affinities to a broad spectrum of active pharmaceutical ingredients(APIs), selectivity to interferents, and responsiveness to hypoxic microenvironments. Due to their highly efficient and controllable recognition, Azo CAs serve as low-dose excipients for 30 APIs. Molecular encapsulation by Azo CAs results in the integrated modification of the physicochemical properties of APIs, including solubility, stability, bioavailability,and biocompatibility. Moreover, Azo CAs can be reduced by azoreductases overexpressed in hypoxic microenvironments,leading to the controlled release of APIs. Collectively, Azo CA excipients have broad application prospects for a series of diseases such as enteritis, arthritis, stroke, cancer, bacterial infection and kidney injury, with diverse therapeutic modalities,including chemotherapy, photodynamic therapy, photothermal therapy, immunotherapy, boron neutron capture therapy, radiotherapy, fluorescence imaging, and their combinations.

关键词： supramolecular chemistry host-guest systems excipient calixarene molecular recognition

Present situation and prospect of immunotherapy for unresectable locally advanced esophageal cancer during peri-radiotherapy

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World Journal of Gastrointestinal Oncology 2024年第1期16卷 1-7页

作者： Feng-Mei Wang Peng Mo Xue Yan Xin-yue lin Zhi-Chao Fu Department of Obstetrics and Gynecology Fuzong Clinical Medical College(900th Hospital)Fujian Medical UniversityFuzhou 350025Fujian ProvinceChina Department of Obstetrics and Gynecology Dongfang HospitalXiamen UniversityFuzhou 350025Fujian ProvinceChina Department of Radiotherapy Fuzong Clinical Medical College(900th Hospital)Fujian Medical UniversityFuzhou 350025Fujian ProvinceChina Department of Radiotherapy Dongfang HospitalXiamen UniversityFuzhou 350025Fujian ProvinceChina

Four major studies(Checkmate577,Keynote-590,Checkmate649 and Attraction-4)of locally advanced esophageal cancer published in 2020 have established the importance of immunotherapy,represented by anti-programmed death protein(PD)-1 in postoperative adjuvant treatment and advanced first-line treatment of locally advanced or advanced esophageal cancer and esophagogastric junction cancer,from the aspects of proof of concept,long-term survival,overall survival rate and progression-free *** unresectable or inoperable nonmetastatic esophageal cancer,concurrent radiotherapy and chemotherapy is the standard treatment recommended by various *** its curative effect is still not ideal,it is necessary to explore radical radiotherapy and chemotherapy in the future,and it is considered to be promising to combine them with immunotherapeutic drugs such as *** paper mainly discusses how to combine radical concurrent radiotherapy and chemotherapy with immunotherapy for unresectable local advanced esophageal cancer.

关键词： Esophageal carcinoma Locally advanced Radiotherapy Immunotherapy

Hydrogel bioadhesives harnessing nanoscale phase separation for Achilles tendon repairing

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Nano Research 2024年第2期17卷 778-787页

作者： Jun Zhang Xingmei Chen Jingseng lin Pei Zhang Iek Man Lei yue Tao Jiajun Zhang Tian Luo Ji Liu Department of Mechanical and Energy Engineering Southern University of Science and TechnologyShenzhen 518055China Research and Innovation Center SKG Health TechnologyShenzhen 518000China SAFE(Shenzhen)Medical Technology Company Limited Shenzhen 518000China Shenzhen Key Laboratory of Biomimetic Robotics and Intelligent Systems Department of Mechanical and Energy EngineeringSouthern University of Science and TechnologyShenzhen 518055China Guangdong Provincial Key Laboratory of Human-Augmentation and Rehabilitation Robotics in Universities Southern University of Science and TechnologyShenzhen 518055China

Repairing Achilles tendon has emerged as a long-standing challenge in the orthopaedic *** suture is the gold standard for re-attaching and repairing the fractured Achilles tendons in clinical surgeries,it is still subjected to numerous adverse side-effects,including chronic inflammatory,tendon tissue re-rupture,scar formation,and post-surgical peritendinous *** this work,we develop a class of hydrogel bioadhesives with tailored nanoscale phase separation for Achilles tendon *** address the existing limitations of sutures,our hydrogel bioadhesives encompass three core functionalities:(i)instant and tough adhesion to Achilles tendon tissues,(ii)extraordinary long-term adhesion robustness under wet and dynamic in vivo conditions,and(iii)anti-postsurgical peritendinous *** our hydrogel bioadhesives with sutures,such kind of integrated approach enables a conformable yet robust biointerface with the tendon tissues,and prevents the fibroblast migration and formation of connective tissues,thus facilitating the tendon *** hydrogel bioadhesives reported here open up new opportunities for the repairing of fractured Achilles tendons in diverse and complicated clinical scenarios.

关键词： hydrogels phase separation bioadhesion robustness tendon repairing

Visual test paper based on Au/δ-MnO_(2) hollow nanosphere oxidase-like activity regulation using hexavalent chromium as a smart switch

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Rare Metals 2024年第2期43卷 711-722页

作者： Wen-Chang Zhuang Hai-yue Zhang Zhen-Yang Chen Wen-Jing Cheng Wei-Dan Na Zhao Li lin Tian School of Materials and Chemical Engineering Xuzhou University of TechnologyXuzhou221018China School of Chemistry and Environmental Science Yili Normal UniversityYining835000China

Paper-based sensing platform is a point of need analytical toolkit for safety ***,the sensitivity,specificity,and simplicity are still ***,we report a novel strategy(Au/δ-MnO_(2) hollow nanosphere and 3,3′,5,5′-tetramethylbenzidine(TMB)induced test strips for signal-on detection)that can be utilized for hexavalent chromium(Cr^(6+))***,Cr^(6+)(CrO_(4)^(2−)) as a smart switch can remarkably enhance the oxidase-like activity of Au/δ-MnO_(2) hollow *** presence of Cr^(6+) can regulate the surface electronic redistribution of Au/δ-MnO_(2) and adjust the geometric configuration,which leads to the improvement in oxidase-like activity of Au/δ-MnO_(2).As a proof-of-concept application,a visual paper-based sensing platform of Cr^(6+) along with quantitative analysis by the test strips was successfully *** paper-based sensing platform exhibits a linear range with excellent selectivity for other interfering substances and lower limit of detection of 0.09μmol·L^(−1),providing a promising toolkit at-home Cr^(6+) measurement and environmental monitoring.

关键词： Point of need Colorimetric biosensing platform Au/δ-MnO_(2) hollow nanosphere Test strip Cr^(6+)

N:ZnO/MoS_(2)-heterostructured flexible synaptic devices enabling optoelectronic co-modulation for robust artificial visual systems

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Nano Research 2024年第3期17卷 1902-1912页

作者： Lei Xu Wenxiao Wang Yang Li Yonghui lin Wenjing yue Kai Qian Qinglei Guo Jeonghyun Kim Guozhen Shen School of Information Science and Engineering University of JinanJinan 250022China School of Microelectronics Shandong UniversityJinan 250101China Department of Electronic Convergence Engineering Kwangwoon UniversitySeoul 01897Republic of Korea School of Integrated Circuits and Electronics Beijing Institute of TechnologyBeijing 100081China

With the merits of non-contact,highly efficient,and parallel computing,optoelectronic synaptic devices combining sensing and memory in a single unit are promising for constructing neuromorphic computing and artificial visual *** on this,a N:ZnO/MoS_(2)-heterostructured flexible optoelectronic synaptic device is developed in this work,and its capability in mimicking the synaptic behaviors is systemically investigated under the electrical and light *** synaptic functions,including synaptic plasticity,long-term/short-term memory,and learning-forgetting-relearning property,have been achieved in this synaptic ***,an artificial visual memory system integrating sense and memory is emulated with the device array,and the visual memory behavior can be regulated by varying the light ***,the optoelectronic co-modulation behavior is verified by applying mixed electric and light signals to the *** detail,a transient recovery property is discovered when the electric signals are applied in synergy during the decay of the light response,of which property facilitates the development of robust artificial visual ***,by superimposing electrical signals during the light response process,a differentiated response of the array is achieved,which can be used as a proof of concept for the color perception of the artificial visual system.

关键词： flexible synaptic device synaptic plasticity optoelectronic synapse robust visual memory optoelectronic co-modulation artificial visual system