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Selective photosynthesis of Z-olefins through crystalline metal-organic cage-initiated expeditious cascade reactions

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Carbon Energy 2024年第3期6卷 118-131页

作者： Jia-Ni Lu Yunze Huang Yuan-Sheng Xia Long-Zhang Dong Lei Zhang Jing-Jing Liu lan-Gui Xie Jiang Liu ya-qian lan Jiangsu Key Laboratory of New Power Batteries School of Chemistry and Materials ScienceJiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNanjingChina School of Chemistry South China Normal UniversityGuangzhouChina

The semi-hydrogenation of alkyne to form Z-olefins with high conversion and high selectivity is still a huge challenge in the chemical industry.Moreover,flammable and explosive hydrogen as the common hydrogen source of this reaction increases the cost and danger of industrial production.Herein,we connect the photocatalytic hydrogen evolution reaction and the semihydrogenation reaction of alkynes in series and successfully realize the high selective production of Z-alkenes using low-cost,safe,and green water as the proton source.Before the cascade reaction,a series of isomorphic metal–organic cage catalysts(Co_(x)Zn_(8−x)L_(6),x=0,3,4,5,and 8)are designed and synthesized to improve the yield of the photocatalytic hydrogen production.Among them,Co_(5)Zn_(3)L_(6) shows the highest photocatalytic activity,with a H_(2) generation rate of 8.81 mmol g^(−1) h^(−1).Then,Co_(5)Zn_(3)L_(6) is further applied in the above tandem reaction to efficiently reduce alkynes to Z-alkenes under ambient conditions,which can reach high conversion of>98%and high selectivity of>99%,and maintain original catalytic activity after multiple cycles.This“one-pot”tandem reaction can achieve a highly selective and safe stepwise conversion from water into hydrogen into Z-olefins under mild reaction conditions.

关键词： alkyne semi-hydrogenation hydrogen evolution reaction metal-organic cages photocatalysis Z-olefins

Sulfonated poly(aryl ether ketone sulfone)modified by polyoxometalates LaW_(10) clusters for proton exchange membranes with high proton conduction performance

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Tungsten 2024年第2期6卷 454-464页

作者： Meng-Long Liu Xu Han Wen-Wen He Feng-Yu Jiang Fang Ji Wang-Wang Shen Tao Zhou Jing-Mei Xu ya-qian lan School of Chemistry and Life Science Changchun University of TechnologyChangchun 130012China Advanced Institute of Materials Science Changchun University of TechnologyChangchun 130012China School of Chemistry South China Normal UniversityGuangzhou 510006China

Polyoxometalates(POMs)are classified as solid superacids which can exhibit notable proton conductivity,making them a promising functional inorganic filler for enhancing the proton conductivity of proton exchange membranes(PEMs).In this study,a series of hybrid membranes were obtained by molecular-level hybridization of Weakley-type POM Na_(7)H_(2)LaW_(10)O_(36)(LaW_(10))clusters into sulfonated poly(aryl ether ketone sulfone)(SPAEKS).All hybrid membranes exhibited greater proton conductivity than the pristine membrane in the 30–80℃temperature range.When the doping amount of LaW 10 reached 7 wt.%,the proton conductivity of M-LaW 10^(-7)achieved 64 mS·cm^(−1)at 80℃.lanthanide ions'high coordination number property and variable coordination environment can aid to attract more water molecules from the environment.LaW 10 and these bound water can construct denser hydrogen bonds with–SO_(3)H of SPAEKS.These intensive hydrogen bonds will facilitate the constitution of more continuous proton transport channels,and improve the proton conductivity of the hybrid membrane.This work off ers a fresh approach to using POMs containing rare-earth components in PEMs.

关键词： Polyoxometalates Rare-earth elements Sulfonated poly(arylene ether ketone sulfone) Proton exchange membranes

Rational design and synthesis of advanced metal-organic frameworks for electrocatalytic water splitting

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Science China Chemistry 2023年第4期66卷 943-965页

作者： Yu-Jia Tang ya-qian lan School of Chemistry and Materials Science Institute of Advanced Materials and Flexible Electronics(IAMFE)Nanjing University of Information Science and TechnologyNanjing 210044China School of Chemistry South China Normal UniversityGuangzhou 510006China

As a promising and significant technology for hydrogen production,electrocatalytic water splitting is a research hotspot in the energy conversion field for alleviating the global energy crisis and achieving carbon neutrality goals.Metal-organic frameworks(MOFs)have been widely investigated as catalyst candidates with remarkable activity and long-term electrocatalysis durability owing to their precise and tailorable structures:tunable pore channels in the range of micropore/mesopore promote the mass/electron transfer;high specific surface areas expose abundant active species;modified metal nodes can serve as active sites;versatile organic ligands can be functionalized to further enhance the electrocatalytic activity.In this review,recent advances in the rational design and synthesis of advanced MOF electrocatalysts for water splitting are presented in the following aspects.First,we analyze the design concepts of MOF electrocatalysts from the perspective of their distinct and modifiable structures.Second,three common synthesis techniques of MOF electrocatalysts are briefly introduced.Third,we focus on the classification of different MOFs for robust electrocatalytic water splitting,including pristine MOFs,mixed-metallic MOFs,MOF nanosheets,electrically conductive MOFs,MOFs on substrates,and polyoxometalate-based MOFs.Finally,summary and outlook are proposed to uncover the next generation of advanced MOFs for electrochemical energy conversion applications.

关键词： metal-organic frameworks water splitting electrocatalysis hydrogen evolution reaction oxygen evolution reaction polyoxometalates

Fabrication of Molecularly Imprinted Electrospun Nanofibers with Mono-amidoxime Functional Ligand for Efficient Decontamination of Toxic Organophosphates

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Chinese Journal of Polymer Science 2024年第4期42卷 446-456页

作者： lan Wang Peng Jiang ya-Lin Niu Jun-Peng Cao Tian-Ying Guo Key Laboratory of Functional Polymer Materials Ministry of EducationInstitute of Polymer ChemistryCollege of Chemistry and Frontier Science Center for the Creation of New Organic SubstancesNankai UniversityTianjin300071China

There is an urgent imperative to discover practical and efficacious artificial catalysts for the expeditious decontamination of toxic organophosphates. Herein, we propose a novel molecularly imprinted approach utilizing electrospun fiber scaffolds. Specifically, an amidoxime-based functional polymer (PMAOX) has been synthesized, which contains amidoxime groups that can act as nucleophiles and ligands for the formation of catalytic active sites. This polymer was blended with polyacrylonitrile (PAN), a well-processable material, to prepare a nanofiber mat using electrospinning techniques. Then, the amidoxime side groups on fiber surface were further cross-linked after the molecular coordination of templates to complete the molecularly imprinting process. This approach can not only enhance the content of functional molecularly imprinted polymers without affecting structural stability, but also combines surface MI technology to fully expose and leverage the advantages of active sites. The as prepared molecularly imprinted electrospun nanofibers MIF-Zn-PMAOX/PAN-6/4 catalyzes the degradation of paraoxon with a half-life of 32 min, and MIF-Ag-PMAOX/PAN catalyzes the degradation of parathion with a half-life of 18 min. The maximum catalytic rate evidence rate enhancements nearly 3700-fold of the self-hydrolysis. Thus, the mono-amidoxime based molecularly imprinted fibers demonstrate the versatility and superiority as self-detoxifying for organophosphates.

关键词： Organophosphateshydrolysis Electrospinning Molecular imprinting

Sustained remission of Cronkhite-Canada syndrome after corticosteroid and mesalazine treatment: A case report

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World Journal of Clinical Cases 2024年第14期12卷 2431-2437页

作者： ya-lan Chen Rui-yao Wang Ling Mei Ran Duan Department of Gastroenterology The Affiliated Hospital of Hebei UniversityBaoding 071000Hebei ProvinceChina Department of Thoracic Surgery The Affiliated Hospital of Hebei UniversityBaoding 071000Hebei ProvinceChina Department of Medical Imageology The Affiliated Hospital of Hebei UniversityBaoding 071000Hebei ProvinceChina

BACKGROUND Cronkhite-Canada syndrome(CCS)is a rare disease of unknown etiology.The optimal treatment for CCS remains unknown.Treatment with corticosteroids is considered the mainstay treatment because of its high efficacy,but the therapeutic strategy for steroid-resistant CCS is not yet established.CASE SUMMARY This is the case of an 81-year-old woman who was diagnosed with CCS.Given her severe diarrhea,nausea,vomiting,and hypoproteinemia,hormone therapy(40 mg/d)was administered,and the symptoms improved within 1 wk.After 3 mo,the patient had no obvious symptoms.The polyps were significantly reduced on review gastroscopy and colonoscopy,thus hormone reduction gradually began.The hormone level was maintained at 10 mg/d after 6 mo.Despite the age of the patient and the side effects of hormones,the patient had no obvious discomfort.However,hormone drugs were discontinued,and mesalazine was administered orally at 3 g/d.The patient's symptoms continued to improve after a follow-up of 5 years.CONCLUSION Corticosteroids and mesalazine are potential treatment options for CCS.

关键词： Cronkhite-Canada syndrome Corticosteroids Mesalazine Gastrointestinal polyposis Case report

Endogenous Candida albicans endophthalmitis in a patient with chronic renal failure on hemodialysis

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International Journal of Ophthalmology(English edition) 2024年第5期17卷 979-981页

作者： Meng-ya Liu Zhi-Fan Chen Hao-Sheng Liu qian-Li Meng Department of Ophthalmology Guangdong Provincial People’s Hospital(Guangdong Academy of Medical Sciences)Southern Medical UniversityGuangzhou 510080Guangdong ProvinceChina The Fourth Affiliated Hospital of Guangzhou Medical University Guangzhou 511400Guangdong ProvinceChina

Dear Editor,We report a rare case of endogenous endophthalmitis caused by Candida albicans in a patient with chronic renal failure concomitant hemodialysis.A 71-year-old man with a history of hypertension and 2-year chronic renal failure on hemodialysis via a native arteriovenous fistula(AVF)was presented to the local hospital due to fever 3wk ago.No pathogens were detected through blood culture on admission,and his fever gradually subsided with intravenous ceftriaxone sodium.After a week of fever,he experienced progressive blurred vision in both eyes,accompanied by pain and headaches.Subsequent magnetic resonance imaging(MRI)of the brain revealed sinusitis.He had not undergone any previous eye surgeries or trauma.

关键词： hemodialysis albicans fever

Clinical usefulness of the baby vision test in young children and its correlation with the Snellen chart

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International Journal of Ophthalmology(English edition) 2024年第2期17卷 348-352页

作者： ya-lan Wang Jia-Jun Wang Xi-Cong Lou Han Zou Yun-E Zhao The Eye Hospital of Wenzhou Medical University Hangzhou 310000Zhejiang ProvinceChina National Clinical Research Center for Ocular Diseases Wenzhou 325027Zhejiang ProvinceChina

AIM:To investigate the efficacy of a new visual acuity(VA)screening method,the baby vision test for young children.METHODS:A total 105 eyes of 65 children aged 2-8y were included in the study.Acuity testing was conducted using a standardized recognition acuity chart(Snellen visual chart:at 3 m)and the baby vision model assessment.The baby vision device includes a screen,a near infrared camera and a computer.Children were seated at a measured distance of 33-40 cm from a display for testing.VA was estimated according to the highest resolution the children could follow.Decimal VA data were converted to logarithm of the minimum angle of resolution(logMAR)for statistical analysis.The VA results for each child were recorded and analyzed for consistency.RESULTS:The mean VA measured using the Snellen visual chart was 0.62±0.32,and that assessed using the baby vision test was 0.66±0.27.The 95%limit of agreement was-0.609 to 0.695,with 95.2%(100/105)plots within the 95%limits of agreement.VA values of the baby vision test were significantly correlated with those of the Snellen chart(R=0.274,P=0.005).CONCLUSION:The baby vision test can be used as a relatively reliable method for estimating VA in young children.This new acuity assessment might be a valid predictor of optotype-measured acuity later in preverbal children.

关键词： baby vision test acuity assessment fix-and-follow system Snellen chart

Analytical solution for the effective elastic properties of rocks with the tilted penny-shaped cracks in the transversely isotropic background

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Petroleum Science 2024年第1期21卷 221-243页

作者： Zheng-qian Ma Xing-yao Yin Zhao-Yun Zong Yuan-Yuan Tan ya-Ming yang National Key Laboratory of Deep Oil and Gas China University of Petroleum(East China)Qingdao266580ShandongChina School of Geosciences China University of Petroleum(East China)Qingdao 266580ShandongChina Pilot National Laboratory for Marine Science and Technology(Qingdao) Qingdao266200ShandongChina

Seismic prediction of cracks is of great significance in many disciplines,for which the rock physics model is indispensable.However,up to now,multitudinous analytical models focus primarily on the cracked rock with the isotropic background,while the explicit model for the cracked rock with the anisotropic background is rarely investigated in spite of such case being often encountered in the earth.Hence,we first studied dependences of the crack opening displacement tensors on the crack dip angle in the coordinate systems formed by symmetry planes of the crack and the background anisotropy,respectively,by forty groups of numerical experiments.Based on the conclusion from the experiments,the analytical solution was derived for the effective elastic properties of the rock with the inclined penny-shaped cracks in the transversely isotropic background.Further,we comprehensively analyzed,according to the developed model,effects of the crack dip angle,background anisotropy,filling fluid and crack density on the effective elastic properties of the cracked rock.The analysis results indicate that the dip angle and background anisotropy can significantly either enhance or weaken the anisotropy degrees of the P-and SH-wave velocities,whereas they have relatively small effects on the SV-wave velocity anisotropy.Moreover,the filling fluid can increase the stiffness coefficients related to the compressional modulus by reducing crack compliance parameters,while its effects on shear coefficients depend on the crack dip angle.The increasing crack density reduces velocities of the dry rock,and decreasing rates of the velocities are affected by the crack dip angle.By comparing with exact numerical results and experimental data,it was demonstrated that the proposed model can achieve high-precision estimations of stiffness coefficients.Moreover,the assumption of the weakly anisotropic background results in the consistency between the proposed model and Hudson's published theory for the orthorhombic rock.

关键词： Effective elastic property Tilted crack Transverse isotropy Analytical solution Crack opening displacement

Boosting CO_(2) electroreduction performance over fullerene-modified MOF-545-Co promoted by π –π interaction

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Chinese Chemical Letters 2023年第4期34卷 559-563页

作者： Xue Dong Zhifeng Xin Dong He Jia-Ling Zhang ya-qian lan qian-Feng Zhang Yifa Chen Institute of Molecular Engineering and Applied Chemistry Anhui University of TechnologyMa’anshan 243002China National and Local Joint Engineering Research Center of MPTES in High Energy and Safety LIBs Engineering Research Center of MTEES(Ministry of Education)Key Lab.of ETESPG(GHEI)School of ChemistrySouth China Normal UniversityGuangzhou 510006China Jiangsu Key Laboratory of New Power Batteries School of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China

Metal-organic frameworks(MOFs) have showed high promise in CO_(2)-electroreduction, yet their generally insufficient conductivity or low electron-transfer efficiency have largely restricted the wide-spread applications. Herein, fullerene molecules(i.e., C60and C70) have been successfully introduced into the pore-channels of a Co-porphyrin based MOF through a facile strategy. Thus-obtained hybrid materials present higher electron-transfer ability, enhanced CO_(2)adsorption-enthalpy and CO_(2)electroreduction activity. Notably, the charge transfer resistance(Rct) of C60@MOF-545-Co is almost 5 times lower of than that of MOF-545-Co, as well as 1.5 times increased for the CO_(2)adsorption enthalpy. As expect, the FECO of C60@MOF-545-Co(97.0%) is largely higher than MOF-545-Co(70.2%), C60@MOF-545(19.4%), C60(11.5%)and physical mixture(70.3%) and presented as one of the best CO_(2)electroreduction catalysts reported in H-cell system. The facile strategy would give rise to new insight into the exploration of powerful MOFbased hybrid materials in high-efficiency CO_(2)electroreduction.

关键词： Fullerene Metal organic framework Electrocatalytic performance π-πinteraction CO_(2)RR