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Transforming liquid flow fuel cells to controllable reactors for highlyefficient oxidation of 5-hydroxymethylfurfural to 2, 5-furandicarboxylic acid at low temperature

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Journal of Energy Chemistry 2024年第3期90卷 621-631,I0014页

作者： Ye Qiang Xi Liu Denghao Ouyang Zhao Jiang Xuebing Zhao Key Laboratory of Industrial Biocatalysis Ministry of EducationTsinghua UniversityBeijing 100084China Institute of applied Chemistry Department of Chemical EngineeringTsinghua UniversityBeijing 100084China School of chemical Engineering and technology Xi'an Jiaotong UniversityXi'an 710049ShaanxiChina

Highly-efficient oxidation of 5-hydroxymethylfurtural(HMF) to 2,5-furandicarboxylic acid(FDCA) at low temperature with air as the oxidant is still ***,inspired by the respirato ry electron transport chain(ETC) of living cells mediated by electron carriers,we constructed artificial ETCs and transformed liquid flow fuel cells(LFFCs) to flexible reactors for efficient oxidation of HMF to produce FDCA under mild *** LFFC reactor employed an electrodeposition modified nickel foam as an anode to promote HMF oxidation and(VO_(2))_(2)SO_(4) as a cathode electron carrier to facilitate the electron transfer to *** reaction rate could be easily controlled by selecting the anode catalyst,adjusting the external loading and changing the cathodic electron carrier or oxidants.A maximal power density of 44.9 mW cm^(-2) at room temperature was achieved,while for FDCA production,short-circuit condition was preferred to achieve quick transfer of *** a single batch operation with 0.1 M initial HMF,FDCA yield reached 97.1%.By fed-batch operation,FDCA concentration reached 144.5 g L^(-1) with a total yield of 96%.Ni^(2+)/Ni^(3+) redox couple was the active species mediating the electron transfer,while both experimental and DFT calculation results indicated that HMFCA pathway was the preferred reaction mechanism.

关键词： 5-Hydroxymethylfurfural 2 5-Furandicarboxylic acid Electrodeposition Electron transport chain Liquid flow fuel cell

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Stable operation of highly loaded pure Si-Fe anode under ambient pressure via carboxy silane-directed robust solid electrolyte interphase

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Journal of Energy Chemistry 2024年第7期94卷 568-576页

作者： Guntae Lim Dong Guk Kang Hyeon Gyu Lee Yen Hai Thi Tran Kihun An Junghyun Choi Kwang Chul Roh Do Youb Kim Seung-Wan Song department of chemical Engineering&applied Chemistry Chungnam National University Daejeon 34134Republic of Korea Energy Storage Materials Center Korea Institute of Ceramic Engineering&TechnologyJinju 52851Republic of Korea Advanced Energy Materials Research Center Korea Research Institute of Chemical TechnologyDaejeon 34114Republic of Korea

Incorporation of higher content Si anode material beyond 5 wt% to Li-ion batteries(LIBs)is challenging,owing to large volume change,swelling,and solid electrolyte interphase(SEI)instability ***,a strategy of diacetoxydimethylsilane(DAMS)additive-directed SEI stabilization is proposed for a stable operation of Si-0.33FeSi_(2)(named as Si-Fe)anode without graphite,which provides siloxane inorganics and organics enrichment that compensate insufficient passivation of fluoroethylene carbonate(FEC)additive and reduce a dependence on *** stable cycling performance of highly loaded(3.5 mA h cm^(-2))pure Si-Fe anode is achieved with 2 wt%DAMS combined with 9 wt%FEC additives under ambient pressure,yielding high capacity 1270 mA h g^(-1)at 0.5 C and significantly improved capacity retention of 81% after 100 cycles,whereas short circuit and rapid capacity fade occur with FEC only ***-directed robust SEI layer dramatically suppresses swelling and particles crossover through separator,and therefore prevents short circuit,demonstrating a possible operation of pure Si or Sidominant anodes in the next-generation high-energy-density and safe LIBs.

关键词： High-energy Li-ion battery Pure Si-Fe anode without graphite Silane additive SEI layer Suppressed swelling

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Recent progress in MOFs-based nanozymes for biosensing

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Nano Research 2024年第1期17卷 39-64页

作者： Imamdin Chandio Yongjian Ai Lei Wu Qionglin Liang MOE Key Laboratory of Bioorganic Phosphorus Chemistry&chemical biology Department of ChemistryLaboratory of Flexible Electronics TechnologyCenter for Synthetic and Systems BiologyTsinghua University-Peking University Joint Centre for Life SciencesTsinghua UniversityBeijing 100084China

Nanozymes are nanomaterials with enzyme-mimicking catalytic *** to natural enzymes,nanozymes show various properties such as easy to manufacture,stable,adjustable,and *** play key roles in biosensing,biocatalysis,and disease *** an important kind of nanozymes,metal-organic framework(MOF)-based nanozymes are receiving a lot of attention due to their structural properties and *** developing MOF with enzymes-like catalytic properties has opened new perspectives in *** review summarizes the up-to-date developments in synthesizing two-dimensional and three-dimensional MOF-based nanozymes and their applications in ***,classification of nanozymes obtained by MOFs is categorized,and different properties of MOF-based nanozymes are ***,the distinctive applications of MOF-based nanozymes in identifying various analytes are thoroughly ***,the recent challenges and progressive directions in this area are highlighted.

关键词： metal-organic frameworks nanozymes metal-organic framework (MOF)-based nanozymes biosensing analytes

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Enhanced Redox Electrocatalysis in High‑Entropy Perovskite Fluorides by Tailoring d–p Hybridization

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Nano-Micro Letters 2024年第3期16卷 333-350页

作者： Xudong Li Zhuomin Qiang Guokang Han Shuyun Guan Yang Zhao Shuaifeng Lou Yongming Zhu department of applied Chemistry Harbin Institute of Technology at WeihaiWeihai 264209People’s Republic of China MIIT Key Laboratory of Critical Materials technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001People’s Republic of China

High-entropy catalysts featuring exceptional properties are,in no doubt,playing an increasingly significant role in aprotic lithium-oxygen *** extensive effort devoted to tracing the origin of their unparalleled performance,the relationships between multiple active sites and reaction intermediates are still ***,enlightened by theoretical screening,we tailor a high-entropy perovskite fluoride(KCoMnNiMgZnF_(3)-HEC)with various active sites to overcome the limitations of conventional catalysts in redox *** entropy effect modulates the d-band center and d orbital occupancy of active centers,which optimizes the d–p hybridization between catalytic sites and key intermediates,enabling a moderate adsorption of LiO_(2)and thus reinforcing the reaction *** a result,the Li–O2 battery with KCoMnNiMgZnF_(3)-HEC catalyst delivers a minimal discharge/charge polarization and long-term cycle stability,preceding majority of traditional catalysts *** encouraging results provide inspiring insights into the electron manipulation and d orbital structure optimization for advanced electrocatalyst.

关键词： Lithium-oxygen batteries KCoMnNiMgZnF_(3)-HEC perovskite fluoride Entropy effect Catalytic kinetics d-p orbital hybridization

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Electric-field-controlled highly regioselective thiocyanation of N-containing heterocycles

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Science China Chemistry 2024年第4期67卷 1263-1269页

作者： Ming Gong Qian Wu Jung Keun Kim Mengmeng Huang Yabo Li Yangjie Wu Jong Seung Kim Henan Key Laboratory of chemical biology and Organic Chemistry Key Laboratory of Applied Chemistry of Henan UniversitiesCollege of ChemistryZhengzhou UniversityZhengzhou 450052China department of Chemistry Korea UniversitySeoul 02841Korea

Achieving highly regioselective synthesis in organic chemistry is challenging due to the uncontrollable orientation between reacting *** electric fields(EEFs)can influence the reactivity and selectivity of the substrate by causing directional ***,scalable and efficient techniques for using EEFs as“smart catalysts”have been lacking,hindering their *** this study,we present a novel method for modifying the regioselectivity of quinoxaline-2(1H)-ones by functionalizing their C7-position using the electric double layer(EDL)*** approach led to moderate to good yields of the corresponding C7-thiocyanation *** calculations and control experiments demonstrated that EEFs could reverse the regioselectivity of quinoxaline-2(1H)-ones,allowing the C7-thiocyanation to proceed via a radical reaction ***,the resulting 7-thiocyano-1-methylquinoxaline-2(1H)-ones exhibited promising AIE *** work showcases a promising strategy for achieving highly regioselective functionalization by aligning the electric field with the desired reaction/bond axis.

关键词： electric fields reaction-axis rule electric double layer C7-thiocyanation C-S bond formation

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A2B7-type La-Mg-Ni alloys prepared by Mg thermal diffusion for improved hydrogen storage performance

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Rare Metals 2024年第7期43卷 3260-3272页

作者： Yong-Xi Zhang Guan-Jiu Wu Jing Gu Hong-Xing Kang Yuan Li Di Zhou Wen-Feng Wang Lu Zhang Shu-Min Han Hebei Key Laboratory of applied Chemistry School of Environmental and Chemical EngineeringYanshan University department of Chemistry and Biochemistry San Diego State University State Key Laboratory of Metastable Materials Science and technology Yanshan University

A novel approach based on thermal diffusion was used to achieve controllable Mg content in A2B7-type La-Mg-Ni-based *** formation mechanism of the A2B7-type phase as a result of the thermal diffusion process and the effect of Mg content on hydrogen storage performance were investigated.X-ray diffraction（XRD） patterns and Rietveld refinement results showed that increased Mg transformed the LaNi5phase in the La0.74Sm0.03Y0.23Ni4.32Al0.04precursor alloy into a superlattice *** electron microscopy（SEM） images showed that Mg was evenly distributed in the alloy *** in the superlattice significantly inhibited the phase decomposition of the superlattice structure during the hydrogen absorption/desorption *** A2B7-type La0.57Sm0.02Y0.18Mg0.23Ni3.38Al0.03alloy composed of Gd2Co7and Ce2Ni7phases was successfully *** pressure-composition isotherm profiles showed that the alloy had a hydrogen storage capacity as high as 1.73 wt%,with good cycling *** 50 cycles of hydrogen absorption/desorption,the alloy retained a hydrogen storage capacity of 1.45 wt%,with a capacity retention rate of up to 84.28%.The Mg thermal diffusion process thus provides a new approach for the controlled preparation of La-Mg-Ni-based alloys.

关键词： La–Mg–Ni-based hydrogen storage alloy A 2 B 7 -type superlattice alloy Mg thermal diffusion process Phase transformation Hydrogen storage property

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Inhibition of Defect-Induced Ice Nucleation, Propagation, and Adhesion by Bioinspired Self-Healing Anti-Icing Coatings

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Research 2024年第1期2023卷 237-246页

作者： Shu Tian Ruiqi Li Xinmeng Liu Jiancheng Wang Junyu Yu Sijia Xu Yunqing Tian Jing Yang Lei Zhang department of Biochemical Engineering Frontier Science Center for Synthetic Biology and Key Laboratory of Systems Bioengineering(MOE)School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China Binzhou Institute of technology Weiqiao-UCAS Science and Technology ParkBinzhou CityShandong Province 256606China

Anti-icing coatings on outdoor infrastructures inevitably suffer from mechanical injuries in numerous icing scenarios such as hailstorms,sandstorms,impacts of foreign objects,and icing–deicing ***,the mechanisms of surface-defect-induced icing are *** the defects,water molecules exhibit stronger adsorption and the heat transfer rate increases,accelerating the condensation of water vapor as well as ice nucleation and ***,the ice–defect interlocking structure increases the ice adhesion ***,a self-healing(at−20℃)antifreeze-protein(AFP)-inspired anti-icing coating is *** coating is based on a design that mimics the ice-binding and non-ice-binding sites in *** enables the coating to markedly inhibit ice nucleation(nucleation temperature<−29.4℃),prevent ice propagation(propagation rate<0.00048 cm^(2)/s),and reduce ice adhesion on the surface(adhesion strength<38.9 kPa).More importantly,the coating can also autonomously self-heal at−20℃,as a result of multiple dynamic bonds in its structure,to inhibit defect-induced icing *** healed coating sustains high anti-icing and deicing performance even under various extreme *** work reveals the in-depth mechanism of defect-induced ice formation as well as adhesion,and proposes a self-healing anti-icing coating for outdoor infrastructures.

关键词： coating defect clarified

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Microglia in drug addiction:A perspective from neuroimmunopharmacology

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Zoological Research 2024年第3期45卷 704-706页

作者： Cong Lin Xiaohui Wang Laboratory of chemical biology Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchunJilin 130022China Beijing National Laboratory for Molecular Sciences Beijing 100190China School of applied Chemistry and Engineering University of Science and Technology of ChinaHefeiAnhui 230026China

Drug addiction refers to a state of dependence that arises from habitual drug intake and can result in specific withdrawal symptoms upon *** most commonly abused substances include psychostimulants,cannabinoids,and *** drugs are consumed,they stimulate the release of dopamine,a neurotransmitter crucial for the pleasure and reward centers of the *** repeated drug use,the brain undergoes various changes,leading to tolerance,dependence,and addiction(Lüscher et al.,2020).The mechanisms involved in drug addiction are highly complex and involve diverse cell types within the brain.

关键词： addiction drugs intake

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Strain-promoted S-arylation and alkenylation of sulfinamides using arynes and cyclic alkynes

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Science China Chemistry 2024年第3期67卷 928-935页

作者： Xi Zou Boming Shen Gao-lin Li Qian Liang Yanhua Ouyang Binghe Yang Peiyuan Yu Bing Gao State Key Laboratory of Chemo/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringInstitute of Chemical Biology and NanomedicineHunan UniversityChangsha 410082China department of Chemistry and Shenzhen Grubbs Institute Guangdong Provincial Key Laboratory of CatalysisSouthern University of Science and TechnologyShenzhen 518055China

The conversion of commercially available chiral sulfinamides into pharmaceutically useful chiral sulfoximines via direct SIVfunctionalization is synthetically attractive but challenging due to the competitive reaction of N-functionalization. Herein, we disclose a novel strain-release strategy to access stereospecific and chemoselective SIV-arylation and alkenylation of sulfinamides using arynes and strained cyclic alkynes. This method tolerates an unprecedented chemical diversity of functional groups attached to the nitrogen center(N-R). The origin of the high SIV-selectivity is elucidated by density functional theory calculations, suggesting a stepwise mechanism for the aryne substrates and a concerted mechanism for the cyclic alkynes.

关键词： arylation alkenylation sulfoximines sulfinamides arynes

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Nano-alumina@cellulose-coated separators with the reinforcedconcrete-like structure for high-safety lithium-ion batteries

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Chinese Journal of chemical Engineering 2024年第4期68卷 83-93页

作者： Zhihao Yang Li Chen Jian Xue Miaomiao Su Fangdan Zhang Liangxin Ding Suqing Wang Haihui Wang Guangdong Provincial Key Lab of Green chemical Product technology School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China Beijing Key Laboratory of Membrane Materials and Engineering Department of Chemical EngineeringTsinghua UniversityBeijing 100084China

Separators play a critical role in the safety and performance of lithium-ion ***,commercial polyolefin separators are limited by their poor affinity with electrolytes and low melting *** this work,we constructed a reinforced-concrete-like structure by homogeneously dispersing nano-Al_(2)O_(3) and cellulose on the separators to improve their stability and *** this reinforcedconcrete-like structure,the cellulose is a reinforcing mesh,and the nano-Al_(2)O_(3) acts as concrete to support the *** constructing the reinforced-concrete-like structure,the separators exhibit good stability even at 200℃(thermal shrinkage of 0.3%),enhanced tensile strain(tensile stress of 133.4 MPa and tensile strains of 62%),and better electrolyte wettability(a contact angle of 6.5°).Combining these advantages,the cells with nano-Al_(2)O_(3)@cellulose-coated separators exhibit stable cycling performance and good rate ***,the construction of the reinforced-concretelike structure is a promising technology to promote the application of lithium-ion batteries in extreme environments.

关键词： Alumina Nanomaterials Lithium-ion batteries Membranes Cellulose Reinforced-concrete-like structure

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