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Co-electrolysis of ethylene glycol and carbon dioxide for formate synthesis

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Science China Chemistry 2024年第5期67卷 1539-1544页

作者： Dongfeng Du Fusong Kang Shiru Yang Bin shao Jingshan Luo Institute of Photoelectronic Thin Film Devices and Technology State Key Laboratory of Photovoltaic Materials and CellsKey Laboratory of Photoelectronic Thin Film Devices and Technology of TianjinMinistry of Education Engineering Research Center of Thin Film Photoelectronic TechnologyNankai UniversityTianjin 300350China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China Frontiers Science Center for New Organic Matter Nankai UniversityTianjin 300071China College of Electronic Information and Optical Engineering Tianjin Key Laboratory of Optoelectronic Sensor and Sensing Network TechnologyNankai UniversityTianjin 300350China

Co-electrolysis of waste plastics and carbon dioxide(CO_(2)) into value-added chemicals or fuels is a promising pathway for a sustainable society, but efficient and selective conversion remains a challenge. Herein, a gold-mediated nickel hydroxide(Au/Ni(OH)_(2)) is developed to oxidize waste plastic-derived ethylene glycol(EG) into formate. In-situ electrochemical experiments and theoretical results reveal that the introduction of Au favors the redox properties and EG adsorption behavior of Ni(OH)_(2). The Au/Ni(OH)_(2) catalyst shows an excellent formate selectivity of >90% at high current densities of above 100 m A cm^(-2). When coupled with sputtered bismuth(Bi) cathode for CO_(2) reduction, a high formate Faradic efficiency(FE) of 188.2% at 200 m A cm^(-2)and a good formate productivity of 7.33 mmol m^(-2)s^(-1)at 10 A are obtained in a flow cell and a zero-gap membrane electrode assembly(MEA) cell, respectively. This work demonstrates a promising strategy to convert waste plastics and CO_(2) into valuable products.

关键词： waste plastic upcycling ethylene glycol oxidation carbon dioxide reduction electrocatalysis formate synthesis

Synergistic asymmetric diarylation of tethered alkenes via C–H functionalization of simple(hetero)arenes

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Science China Chemistry 2024年第8期67卷 2710-2718页

作者： Jian Yao Can Zhao Lili shao Xiaohong Huo Xiaoming Wang Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs Frontiers Science Center for Transformative MoleculesSchool of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory of Organometallic Chemistry and Shanghai Hongkong Joint Laboratory in Chemical Synthesis Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China School of Chemistry and Materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China

By virtue of the atom-and step-economy, utilization of simple arenes as a supplant of pre-prepared aryl metal species or aryl halides for the synthesis of arylated chiral molecules has attracted great attention from the synthetic community. While transition-metal-catalyzed enantioselective diarylation of tethered alkenes has been employed to prepare important chiral cyclic compounds, the direct use of simple arenes as aryl precursors is still underdeveloped, probably due to the difficulties in the effective control of the reactivity, site-selectivity and/or enantioselectivity. Herein we report an asymmetric Pd/Ag dual metal catalytic system for the non-directed, site-and enantioselective domino Heck/intermolecular C–H functionalization of *** studies showed that Pd and Ag act in cooperation in the catalysis and the chiral bisphosphine ligand plays a bifunctional role, i.e., assisting the silver species in the cleavage of the aryl C–H bond, while inducing the enantioselectivity on direct complexation with palladium. This method provides an efficient approach to the corresponding chiral oxindoles with good enantiomeric excesses from a broad scope of arenes, including fluoroarenes, heteroarenes and several complex products derived from medicines or natural products.

关键词： asymmetric Pd/Ag dual metal catalytic system simple arenes C–H functionalization bifunctional role chiral oxindoles

To be or not to be direct:The role of neuromedin U in neuro-eosinophil crosstalk

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Science Bulletin 2024年第2期69卷 148-150页

作者： Ruichao Liu Wenhao shao Jun Xu Coco Chu SXMU-Tsinghua Collaborative Innovation Center for Frontier Medicine Taiyuan 030001China Insttute for Immunogy Department of Basic Medical SciencesSchool of Medicinesinghua UnierstyBejing 100084China Tsinghua-Peking Center for Life Sciences Tsinghua UniversityBeijing 100084China Shanxi Medical University Taiyuan 030012China Department of Surgery First Hospital of Shanxi Medical UniversityShanxi Provincial Key Laboratory for Digestive Diseases and Organ TransplantationTaiyuan 030001China Beijing Key Laboratory for Immunological Research on Chronic Diseases Tsinghua UniversityBejing 100084China

With the development of new experimental techniques(e.g.,single-cell RNA sequencing(scRNA-seq),light sheet microscopy,and clustered regularly interspaced palindromic repeats(CRISPR)/CRISPR-associated protein 9(Cas9),emerging studies have begun to uncover the interactions between the nervous system and the immune system,both in health and *** example,in mucosal tissues such as the lung and the intestine,neurotransmitters including acetylcholine[1]and adrenaline[2]can directly regulate the immune cell functions thus affect the results of allergy,asthma,and anti-pathogen host defense[3].

关键词： intestine lung asthma

Differential Operator Approach to■quantum Groups and Their Oscillator Representations

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Acta Mathematica Sinica,English Series 2024年第5期40卷 1360-1374页

作者： Zhao Bing FAN Ji Cheng GENG shao Long HAN College of Mathematical Science Harbin Engineering UniversityHarbin 150001P.R.China

For a quasi-split Satake diagram,we define a modified q-Weyl algebra,and show that there is an algebra homomorphism between it and the corresponding■quantum *** other words,we provide a differential operator approach to■quantum ***,the oscillator representations of■quantum groups are *** crystal basis of the irreducible subrepresentations of these oscillator representations are constructed.

关键词： ■quantum group differential operator oscillator representation crystal basis

Crystalline-amorphous M@MN_x(M=Co,Fe,Ni)encapsulated in nitrogen-doped carbon for enhanced efficient and durable hydrogen evolution reaction

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Rare Metals 2024年第4期43卷 1547-1556页

作者： Yang Yang Xiao-Chuan Duan shao-Hui Guo Xian-Ming Zhang College of Materials Science and Engineering College of ChemistryKey Laboratory of Interface Science and Engineering in Advanced MaterialsTaiyuan University of TechnologyYuci030600China

Developing earth-abundant electrocatalysts for hydrogen evolution reaction(HER)is important for the sustainable energy ***,efficient and stable heterocatalysts consisting of crystalline-amorphous M@MN_(x)(M=Co,Fe,Ni)encapsulated in N-doped carbon layers supported with N-doped graphene sheets(denoted as M@MN_(x)@NC-NG)are synthesized by facile hydrothermal reaction and nitridation *** the nitriding process,metal ions in M(tzbc)_2(H_(2)O)_4(tzbc=4-(1H-1,2,4-triazol-1-yl)benzoic acid)complexes are reduced to crystalline M cores,accompanied by the formation of amorphous MN_(x)shells;the tzbc ligands are insitu carbonized to form outermost N-doped carbon(NC)layers that connect with inner MN_(x)via M-N-C motifs inherited from the complex precursors and inhibit the transition of MN_(x)from amorphous to crystalline *** Co@CoN_(x)@NC-NG catalyst exhibits excellent HER activity with small overpotentials of 45 and 64 mV at a cathode current density of 10 mA·cm^(-2)and low Tafel slopes of 40 and 85 mV·dec^(-1)in 0.5 mol·L^(-1)H_(2)SO_4 and1.0 mol·L^(-1)KOH electrolytes,*** Co@CoN_(x)@NC-NG retains 97%of the initial overpotential after 100,000 s in both acidic and alkaline *** outstanding HER performance originates from the crystalline-amorphous Co@CoN_(x)that redistributes electrons around the heterointerfaces,facilitating the conversion process of H^(+)/H_(2)O to hydrogen and thereby promoting HER *** outermost NC layers serve as the armor of Co@CoN_(x),and graphene nanosheets act as carriers of egg-like Co@CoN_(x)@NC and conduction paths for electron shuttles,ensuring stable and continuous electrocatalytic hydrogen production.

关键词： Hydrogen evolution reaction Electrocatalysts Iron group metals Heterojunction Crystalline-amorphous structure

Highly active and durable core-shell electrocatalysts for proton exchange membrane fuel cells

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Nano Research 2024年第10期17卷 8772-8784页

作者： Hsiwen Wu Fei Xiao Jing Wang Meng Gu Minhua shao Department of Chemical and Biological Engineering The Hong Kong University of Science and TechnologyClear Water BayHong KongChina Department of Materials Science and Engineering Southern University of Science and TechnologyShenzhen 518055China Fok Ying Tung Research Institute The Hong Kong University of Science and TechnologyGuangzhou 511458China Energy Institute and Chinese National Engineering Research Center for Control&Treatment of Heavy Metal Pollution The Hong Kong University of Science and TechnologyClear Water BayHong KongChina

This work presents simple post-treatment methods to selectively and partially remove the Pd core of Pd-Pt core–shell(Pt@Pd/C)*** proton exchange membrane fuel cell with the post-treated Pt@Pd/C cathode(Pt loading:0.10 mg·cm^(-2))delivers an impressive peak power density of 1.2 W·cm^(-2).The partial removal of Pd core endows an ultrahigh oxygen reduction reaction(ORR)mass activity of 0.32 A·g_(PGM)-1 when normalized to the platinum group metal(PGM)mass,or equivalently 0.55 A·mg_(Pt)^(-1) at 0.9 V measured in a fuel *** post-treatment thickens the Pt shells and mitigates the Pd dissolution during potential *** a result,the post-treated core-shell catalyst demonstrates superior durability in ORR mass activity and polarization power density retention than untreated core-shell catalyst and benchmark Pt/***-situ inductively coupled plasmamass spectrometry(ICP-MS)results highlight that the amount of dissolved Pd in post-treated core–shell catalyst is 17-times lower than that of the untreated *** findings highlight the importance of structural tuning of catalysts in enhancing their mass activity and durability.

关键词： core-shell catalyst platinum monolayer proton exchange membrane fuel cell oxygen reduction reaction durability

Unraveling the role of NiSnPH@OOH/CC perovskite hydroxide for efficient electrocatalytic oxidation of methanol to formate

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Nano Research 2024年第4期17卷 2388-2399页

作者： Jing shao Yusheng Fang Xiaobing Wu Muhammad Imran Abdullah Youkun Tao College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060China School of Science Harbin Institute of TechnologyShenzhen 518055China

The sluggish kinetics of oxygen evolution reaction(OER)is the key tailback for hydrogen production from the water *** OER with thermodynamically auspicious methanol oxidation reaction(MOR)can significantly boost the H_(2) and value-added products ***,it is currently challenging to achieve a synergistic manipulation of product selectivity and performance for MOR ***,we report NiSnPH@OOH/CC(CC=carbon cloth)perovskite hydroxide nanosphere as an efficient MOR electrocatalyst with high activity,stability,and selectivity towards methanol oxidation to formate.A surface amorphous layer of defect rich NiOOH was generated in operando by selective Sn leaching with stable perovskite hydroxide bulk structure,which mitigates the oxidative power and optimizes the local coordination environment of the active NiOOH *** situ Raman combined with electrochemical studies further confirm the key active species,NiOOH,generated in operando enhance the MOR and blocking the over oxidation of methanol to CO_(2).As a result,NiSnPH@OOH/CC effectively masks the OER and attains>99%selectivity with 100%Faradic efficiency for *** results of this study show the advances of NiSnPH@OOH/CC as an efficient electrocatalyst for MOR and also suggest its potential applications for various small organic molecules oxidation.

关键词： perovskite hydroxide small organic molecules nickel oxy(hydroxide) value-added products methanol oxidation reaction

In situ visualization of the cellular uptake and sub-cellular distribution of mussel oligosaccharides

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Journal of Pharmaceutical Analysis 2024年第6期14卷 840-850页

作者： Zhenjie Yu Huarong shao Xintian shao Linyan Yu Yanan Gao Youxiao Ren Fei Liu Caicai Meng Peixue Ling Qixin Chen Key Laboratory for Biotechnology Drugs of National Health Commission School of Pharmaceutical Sciences&Institute of Materia MedicaMedical Science and Technology Innovation CenterShandong First Medical University&Shandong Academy of Medical SciencesJinan250117China Key Laboratory of Biopharmaceuticals Engineering Laboratory of Polysaccharide DrugsNational-Local Joint Engineering Laboratory of Polysaccharide DrugsShandong Academy of Pharmaceutical ScienceJinan250101China Shenzhen Research Institute of Xiamen University ShenzhenGuangdong518057China School of Life Sciences Medical Science and Technology Innovation CenterShandong First Medical University&Shandong Academy of Medical SciencesJinan250117China Departments of Diagnostic Radiology SurgeryChemical and Biomolecular Engineeringand Biomedical EngineeringYong Loo Lin School of Medicine and Faculty of EngineeringNational University of SingaporeSingapore119074Singapore School of Pharmaceutical Sciences Shandong UniversityJinan250101China

Unlike chemosynthetic drugs designed for specific molecular and disease targets,active small-molecule natural products typically have a wide range of bioactivities and multiple targets,necessitating extensive screening and *** address this issue,we propose a strategy for the direct in situ microdynamic examination of potential drug candidates to rapidly identify their effects and mechanisms of *** a proof-of-concept,we investigated the behavior of mussel oligosaccharide(MOS-1)by tracking the subcellular dynamics of fluorescently labeled MOS-1 in cultured *** recorded the entire dynamic process of the localization of fluorescein isothiocyanate(FITC)-MOS-1 to the lysosomes and visualized the distribution of the drug within the ***,lysosomes containing FITC-MOS-1 actively recruited lipid droplets,leading to fusion events and increased cellular lipid *** drug behaviors confirmed MOS-1 is a candidate for the treatment of lipid-related ***,in a high-fat HepG2 cell model and in high-fat diet-fed apolipoprotein E(ApoE)^(-/-)mice,MOS-1 significantly promoted triglyceride degradation,reduced lipid droplet accumulation,lowered serum triglyceride levels,and mitigated liver damage and ***,our work supports the prioritization of in situ visual monitoring of drug location and distribution in subcellular compartments during the drug development phase,as this methodology contributes to the rapid identification of drug ***,this methodology is significant for the screening and development of selective small-molecule drugs,and is expected to expedite the identification of candidate molecules with medicinal effects.

关键词： Cellular imaging Fluorescence labeling Mussel oligosaccharide Lipid metabolism

第107届北美放射学会年会亮点:儿科影像学

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磁共振成像 2022年第3期13卷 107-110页

作者：张思琪邵剑波曾洪武深圳市儿童医院放射科深圳518038 汕头大学医学院汕头515041 华中科技大学同济医学院附属武汉儿童医院影像中心武汉430019

第107届北美放射学会(Radiological Society of North America,RSNA)年会儿科影像学的研究亮点聚焦于:(1)安全高效:在保证图像质量的前提下,降低辐射剂量、缩短检查时间;(2) MRI新技术:基于fMRI的儿童神经网络应用,儿童肺部MRI,儿童心... 详细信息

第107届北美放射学会(Radiological Society of North America,RSNA)年会儿科影像学的研究亮点聚焦于:(1)安全高效:在保证图像质量的前提下,降低辐射剂量、缩短检查时间;(2) MRI新技术:基于fMRI的儿童神经网络应用,儿童肺部MRI,儿童心血管系统4D Flow MRI和磁共振弹性成像技术的临床实现,以及超高场MRI在儿童疾病诊疗中的应用;(3)儿童的影像诊断标准建立,基于多中心成果融合和大数据信息互通;(4)儿童先天性、罕见性疾病的影像征象识别和鉴别诊断经验分享。本文将按照解剖系列对年会儿科方面的主要科学报告及其相关研究进展进行综述。

关键词：儿科影像学电子计算机断层扫描超声磁共振成像人工智能深度学习