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Highly selective and eco-friendly dihydroisoquinoline synthesis via Cu/Co synergistic catalysis in Cu NPs@MOFs catalyst under mild conditions

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Science China Chemistry 2024年第5期67卷 1561-1568页

作者： Peng-Fei Guo Ze-Long Liang Yue-E Jiao Hang Xu Bin Zhao Key Laboratory of Advanced energy Material Chemistry Renewable Energy Conversion and Storage CenterDepartment of ChemistryNankai UniversityTianjin 300071China

3,4-Dihydroisoquinoline(DHIQ)is an important precursor used in the production of drugs for treating cancer,HIV,Alzheimer's disease,*** studies on DHIQ synthesis show low catalytic selectivity due to the susceptible over-oxidation feedstock of1,2,3,4-tetrahydroisoquinoline(THIQ),which often requires alkali ***,it is desirable yet challenging to explore a highly selective and efficient oxydehydrogenation capacity for DHIQ synthesis under eco-friendly reaction ***,a novel framework 1 was synthesized,exhibiting 1D channels with the size of 4.6 A×9.6 A and high solvent/p H/thermal stability.A stable framework allows it to encapsulate Cu nanoparticles(NPs)to form Cu NPs@1-x(x=1,2,3,and 4)with varying loading amounts of Cu NPs at 2.0 wt%,3.0 wt%,4.0 wt%,and 6.0 wt%,*** NPs@1-3 could selectively catalyze the reaction from THIQ to DHIQ with a high selectivity of 98%and a recorded turnover frequency(TOF)of 22.1 h-1under eco-friendly mild *** corresponding catalytic activity can maintain at least five recyclings and can be further applied to gram-scale ***,the efficient preparation of DHIQ catalyzed by Cu NPs@1-3 could be realized even under air ***,the anticancer molecule precursor synthesis of 6,7-dimethoxy-3,4-dihydroisoquinoline was also selectively catalyzed by Cu NPs@*** investigations revealed that high catalytic performance can be attributed to the stable framework and the synergistic catalytic effect of the loaded Cu NPs and Co metal *** importantly,this work represents the first example of MOF catalysts for selectively thermo-catalytic DHIQ synthesis and demonstrates a simple approach to obtain efficient catalysts for selective oxydehydrogenation in the production of unsaturated compounds.

关键词： metal-organic frameworks Cu NPs@MOFs 3 4-dihydroisoquinoline selective oxydehydrogenation synergistic catalysis

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Multifunctional photon conversion materials for enhancing silicon solar cells

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Light(Science & Applications) 2024年第4期13卷 598-601页

作者： Yiyan Zhang Guanying Chen MIIT Key Laboratory of Critical Materials Technology for New energy conversion and storage School of Chemistry and Chemical EngineeringHarbin Institute of Technology150001 HarbinChina

A type of multifunctional erbium(Er^(3+))and ytterbium(Yb^(3+))codoped NaY(WO4)2 phosphors,with simultaneous photon upconversion,photon quantum cutting,and luminescence ratiometric temperature sensing abilities,have b... 详细信息

关键词： photon luminescence quantum

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A-site assisted perovskite crystallization via ion-exchange MOFs for high efficient and stable perovskite solar cells

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Journal of energy Chemistry 2024年第6期93卷 436-442,I0011页

作者： Xingrui Zhang Jian Zhang Wei Wang Boyuan Hu Yayu Dong Debin Xia Kaifeng Lin Yulin Yang MIIT Key Laboratory of Critical Materials Technology for New energy conversion and storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HeilongjiangChina

Here,a novel strategy is proposed targeting the volatility of A-site cations and the disordered arrangement of perovskite grains through employing Cs~+contained metal-organic frameworks In-aip(Cs)obtained by ion-exchange and crystalline *** forces between Cs-O atoms split the pore channels of the pristine In-aip,endowing In-aip(Cs)with multidimensional charge transport channels,In addition,the partially freed Cs~+in the interlayer compensates for the vacancy of A-site cations during the perovskite preparation *** In-aip(Cs)modified perovskite films have a flat morphology,large grains and excellent optoelectronic *** from the high-quality perovskite films and faster charge extraction,the In-aip(Cs)-modified PSCs achieved a champion PCE of 23.03%,superior to the In-aip-modified(22.29%)and control device(21.13%),More importantly,the unencapsulated PSCs modified with In-aip(Cs)exhibited outstanding humidity and thermal *** a period of almost 1000 h,the unencapsulated In-aip(Cs)-modified device retained 85%of its initial PCE after storing in a glove box at 85℃,and retained 87%of the primary PCE upon storage in ambient condition at 25℃under a humidity of 40%.

关键词： Metal-organic frameworks PSCs Stability Defect passivation

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Cation-Dipole Interaction-Induced Coacervate Underwater Adhesives in Natural Seawater

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Chinese Journal of Polymer Science 2024年第7期42卷 984-991,I0009页

作者： Xu-Fei Liu Chong-Rui Zhang Hua-Wen Peng Qiang Zhao Key Laboratory of Material Chemistry for energy conversion and storage Ministry of EducationSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan430074China

Significant progress has been made in wet adhesives for low salinity water,but exploration of general ionic adhesives for natural seawater is less developed because the high salinity could weaken interfacial bonding and shields electrostatic interactions,resulting in adhesion ***,the design of adhesives for natural seawater represents challenges less ***,a cationic polyelectrolyte(PECHIA)containing imidazolacetonitrile unit was explored to prepare adhesives enabled by natural *** combining the ion shielding effect with the“cation-dipole”interactions between PECHIA chains,aqueous solution of the PECHIA underwent coacervation and self-crosslinking in natural seawater,allowing for underwater adhesion to various substrates in *** instantaneous lap-shear and tensile adhesion strengths are 47 and 119 kPa,respectively,while the cured adhesive shows~739 k Pa tensile adhesion in natural *** design of PECHIA enables wet adhesives viable for applications in the diversified scenarios of natural seawater.

关键词： Coacervate Underwater adhesives Seawater Cation-dipole interaction

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Dual-functional POM@IL complex modulate hole transport layer properties and interfacial charge dynamics for highly efficient and stable perovskite solar cells

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Chinese Chemical Letters 2024年第7期35卷 461-464页

作者： Boyuan Hu Jian Zhang Yulin Yang Yayu Dong Jiaqi Wang Wei Wang Kaifeng Lin Debin Xia MIIT Key Laboratory of Critical Materials Technology for New energy conversion and storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001China

The severe interfacial charge recombination as well as the stability issues brought by the Li-TFSI still hinder the commercialization of high-performance perovskite solar cells(PSCs).Here,a polyoxometalates(POMs)-based complex,POM@ionic liquid(IL),is synthesized and applied as an effective additive that simultaneously enhances the performance and stability of *** interactions between POM@IL complex and Li-TFSI inhibit the aggregation of *** synergistic oxidation of POM@IL complex and Li-TFSI towards 2,2,7,7-tetrakis[N,N-di(4-methoxyphenyl)amino]-9,9'-spirobifluorene(Spiro-OMeTAD)effectively enhances the electrical properties of hole transport layer film and the photovoltaic performances of *** champion device modified with the POM@IL complex yields an excellent power conversion efficiency(PCE)of 22.73%.Moreover,the incorporation of POM@IL improves the humidity stability of *** storing under high humidity conditions(25℃,60%RH)for 1200 h,the POM@IL modified device retained a remarkable 81.2%of its initial *** work provides new insight into constructing POMs-based materials for high-performance photovoltaic devices.

关键词： Polyoxometalates Ionic liquid Perovskite solar cells energy alignment Humidity stability

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Solid-state synthesis and ion transport characteristics of the β-KSbF_(4) for all-solid-state fluoride-ion batteries

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Journal of energy Chemistry 2024年第7期94卷 758-767页

作者： Jiali Liu Huahui Zhao Jingcheng Xia Lingguang Yi Xiaoyi Chen Dongdu Li Shuhan Ni Xinyi Su Yixuan Chen Min Liu Xianyou Wang National Base for International Science&Technology Cooperation National Local Joint Engineering Laboratory for Key Materials of New Energy Storage BatteryHunan Province Key Laboratory of Electrochemical Energy Storage&ConversionSchool of ChemistryXiangtan UniversityXiangtan 411105HunanChina College of New energy Ningbo University of TechnologyNingbo 315336ZhejiangChina

All-solid-state fluoride ion batteries(FIBs)have been recently considered as a post-lithium-ion battery system due to their high safety and high energy *** like all solid-state lithium batteries,the key to the development of FIBs lies in room-temperature electrolytes with high ionic conductivity.β-KSbF_(4) is a kind of promising solid-state electrolyte for FIBs owing to its rational ionic conductivity and relatively wide electrochemical stability window at room ***,the previous synthesis routes ofβ-KSbF_(4) required the use of highly toxic hydrofluoric acid and the ionic conductivity of as-prepared product needs to be further ***,the β-KSbF_(4) sample with an ionic conductivity of 1.04×10^(-4)s cm^(-1)(30°C)is synthesized through the simple solid-state *** order to account for the high ionic conductivity of the as-synthesizedβ-KSbF_(4),X-ray diffraction(XRD),scanning electron microscopy(SEM),and energy dispersive X-ray spectroscopy(EDS)are used to characterize the physic-ochemical *** results show that the as-synthesizedβ-KSbF_(4) exhibits higher carrier concentra-tion of 1.0×10^(-6)S cm-Hz^(-1)K and hopping frequency of 1.31×10^(6)Hz at 30°C due to the formation of the fluorine ***,the hopping frequency shows the same trend as the changes of ionic conductivity with the changes of temperature,while the carrier concentration is found to be almost *** two different trends indicate the hopping frequency is mainly responsible for the ionic conduc-tion behavior withinβ-KSbF_(4).Furthermore,the all-solid-state FIBs,in which Ag and Pb+PbF_(2) are adopted as cathode and anode,andβ-KSbF_(4) as fluoride ion conductor,are capable of reversible charge and *** assembled FIBs show a discharge capacity of 108.4 mA h g^(-1) at 1st cycle and 74.2 mA h g^(-1) at 50th *** on an examination of the capacity decay mechanism,it has been found that deterioration of the electrolyte/electrode int

关键词： Solid-state electrolyte Carrier concentration Hopping frequency β-KSbF_(4) All-solid-state fluoride ion batteries

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Elaborate Design of Two Novel Fluorescent Zinc-based Metal-Organic Frameworks for Highly Efficient Tetracycline Antibiotics Detection

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Chemical Research in Chinese Universities 2024年第3期40卷 499-507页

作者： TAO He JI Chengshan ZHANG Jian YIN Yuanyuan JIA Wenwen JIANG Xin XU Jie YANG Yulin MIT Key Laboratory of Critical Materials Technology for New energy conversion and storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001P.R.China

The abuse of tetracycline antibiotics has caused great harm to human health and *** inexpensive,convenient and sensitive methods for the detection of tetracycline antibiotics is highly ***,based on the H_(4)ddp ligand[H_(4)ddp=3-(3,5-dicarboxyphenyl)pyridine-2,6-dicarboxylic acid],two novel zinc-based metal-organic frameworks(MOFs){[Zn_(3)(ddp)_(2)(H_(2)O)_(4)]·3H_(2)O}n(Zn1-ddp)and{[Zn_(3)(ddp)_(2)(H_(2)O)_(4)]·3H_(2)O}n(Zn2-ddp)were successfully designed by delicate structural *** Zn1-ddp and Zn2-ddp exhibited excellent water and chemical stability and showed excellent fluorescence quenching performance for tetracycline ***,the more advanced framework structure and better fluorescent performance make Zn1-ddp more sensitive than Zn2-ddp in fluorescent detection with a detection limit of 0.29µmol/L for tetracycline(TC),0.09µmol/L for doxycycline(DOX),0.10µmol/L for minocycline(MIN)and metacycline(MEL),0.19µmol/L for chlortetracycline(CTC),and 0.67µmol/L for oxytetracycline(OTC)among tetracycline *** fluorescence quenching mechanism of Zn1-ddp and Zn2-ddp for tetracycline antibiotics detection was deeply *** reasons for the superior detection performance of Zn1-ddp over Zn2-ddp were also analyzed in depth through Fourier transform infrared spectrophotometry(FTIR),X-ray photoelectron spectroscopy(XPS)analysis and framework structure *** developed method opens up a new perspective for antibiotics detection based on zinc-based MOFs.

关键词： Water system Metal-organic framework Fluorescent detection Tetracycline antibiotic

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Manipulating fast Li_(2)S redox via carbon confinement and oxygen defect engineering of In_(2)O_(3)for lithium-sulfur batteries

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Nano Research 2024年第6期17卷 5179-5187页

作者： Jinlei Qin Rui Wang Zilong Yuan Pei Xiao Deli Wang Key Laboratory of Material Chemistry for energy conversion and storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

Lithium-sulfur(Li-S)batteries have been considered as promising energy storage systems due to the merits of high energy density and low ***,the lithium polysulfides(LiPSs)diffusion and sluggish redox kinetics hamper the battery *** this work,low-bandgap indium oxide(In_(2)O_(3))with dense oxygen vacancies(In_(2)O_(3−x),0engineering demonstrates great promise in the development of practical Li-S batteries.

关键词： Li-S batteries nitrogen-doped carbon confinement oxygen vacancies bidirectional Li_(2)S redox

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Advances of Synergistic Electrocatalysis Between Single Atoms and Nanoparticles/Clusters

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Nano-Micro Letters 2024年第11期16卷 377-412页

作者： Guanyu Luo Min Song Qian Zhang Lulu An Tao Shen Shuang Wang Hanyu Hu Xiao Huang Deli Wang Key Laboratory of Material Chemistry for energy conversion and storage(Huazhong University of Science and Technology)Ministry of Education School of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074People’s Republic of China

Combining single atoms with clusters or nanoparticles is an emerging tactic to design efficient *** synergy effect and high atomic utilization of active sites in the composite catalysts result in enhanced electrocatalytic performance,simultaneously provide a radical analysis of the interrelationship between structure and *** this review,the recent advances of single-atomic site catalysts coupled with clusters or nanoparticles are ***,the synthetic strategies,characterization,dynamics and types of single atoms coupled with clusters/nanoparticles are introduced,and then the key factors controlling the structure of the composite catalysts are ***,several clean energy catalytic reactions performed over the synergistic composite catalysts are ***,the encountering challenges and recommendations for the future advancement of synergistic structure in energy-transformation electrocatalysis are outlined.

关键词： Single atoms Nanoparticles Clusters Synergistic composite catalysts Synergistic effect

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Performance of iron-air battery with iron nanoparticle-encapsulated C-N composite electrode

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Frontiers in energy 2024年第1期18卷 42-53页

作者： Can FANG Xiangmei TANG Jiaoyan WANG Qingfeng YI School of Chemistry and Chemical engineering Hunan University of Science and TechnologyXiangtan 411201China Hunan Provincial Key Laboratory of Advanced Materials for New energy storage and conversion Xiangtan 411201China

Highly efficient and stable iron electrodes are of great significant to the development of iron-air battery(IAB).In this paper,iron nanoparticle-encapsulated C–N composite(NanoFe@CN)was synthesized by pyrolysis using polyaniline as the C–N *** performance of the NanoFe@CN in different electrolytes(alkaline,neutral,and quasi-neutral)was investigated via cyclic voltammetry(CV).The IAB was assembled with NanoFe@CN as the anode and IrO_(2)+Pt/C as the *** effects of different discharging/charging current densities and electrolytes on the battery performance were also *** K_(2)SO_(4)electrolyte can effectively suppress the passivation of iron electrode,and the battery showed a good cycling stability during 180 charging/discharging *** to the pure nano-iron(NanoFe)battery,the NanoFe@CN battery has a more stable cycling stability either in KOH or NH_(4)Cl+KCl electrolyte.

关键词： energy storage and conversion metallic composites nanocomposites iron-air battery iron anode

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