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Ultrastrong room-temperature phosphorescence in cucurbituril-mediated crystalline supramolecules for ratiometric detection of phenethylamine

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Science China Chemistry 2025年第6期68卷 2671-2679页

作者： Qingyu Niu Yingxiang Ye Lingna Su Xu He Zhiqiang Li Yu Liu School of Chemical Engineering and Technology Hebei University of Technology Fujian Provincial Key Laboratory of Polymer Materials College of Chemistry and Materials Science Fujian Normal University Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Nankai University College of Chemistry State Key Laboratory of Elemento-Organic Chemistry Nankai University

It is a great challenge to modulate purely organic fluorescence-phosphorescence dual emission in aqueous solution because the excited singlet and triplet states are in competition with each other. Herein, we report a crystalline 1:2 host-guest formed by selfassembly of 4-(4-bromophenyl)-pyridinium derivatives and cucurbit[8]uril, in which a rigid environment rich in weak interactions is directly demonstrated. Due to the inhibition of non-radiative transition and stabilization of triplet exciton in the crystalline environment, the crystalline inclusion complex exhibits ultralong room-temperature phosphorescence lifetime of3.21 ms with an room-temperature phosphorescence(RTP) quantum yield up to 16.29%. Interestingly, the crystalline 1:2 hostguest complex demonstrates the ability of rapid identification and sensitive fluorescence-phosphorescence ratiometric detection behavior toward phenethylamine, a drug analogue, with a limit of detection as low as 27.5 n M. We believe that this study will undoubtedly broaden the utilizing scopes of RTP and offer a novel avenue for psychoactive substances monitoring.

关键词： room-temperature phosphorescence cucurbituril host-guest complex crystalline ratiometric detection

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Deposition of thin TiO_(2)films on fluorophlogopite particle surface by CVD in fluidized bed reactor to prepare silver pearlescent pigments

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Particuology 2024年第6期89卷 88-98页

作者： Ming Liu Guoqiang Shao Pengpeng Lv Jun Li Qingshan Zhu State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China

Two critical parameters:Glossiness and chromaticity space of pearlescent pigments were evaluated based on crystallinity and grain *** the roughness and the vertical distance evolution along the surface of deposited TiO_(2)film are affected by the *** optimal crystallinity of TiO_(2)was deposited at the temperature of 350℃.The TiCl4 concentration effectively changed the grain ***,the high flow rate of fluidizing gas and optimal gas–solid ratio(<0.11 m^(3)/(kg h))restricted the change of TiCl_(4)concentrations in fluidized bed *** this case,the grain size of the deposited TiO_(2)film was about 55 *** on the grain size,the color of pearlescent pigments was adjusted by controlling the film thickness based on TiO_(2)***,the silver pearlescent pigment with high glossiness was prepared by chemical vapor deposition method in a fluidized bed reactor.

关键词： Fluidized bed chemical vapor deposition TiO_(2)film deposition Pearlescent pigment Free powder restrain Crystal growth

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Importance of metal location in M-H zeolite for synergistically catalyzing dimethyl ether carbonylation

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Chinese Journal of chemical engineering 2022年第1期35卷 350-357页

作者： Shiyue Li Shouying Huang Kai Cai Ying Li Jing Lv Xinbin Ma Key Laboratory for Green Chemical Technology of Ministry of Education Collaborative Innovation Center of Chemical Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China

Mordenite(MOR)has shown great potential to catalyze dimethyl ether(DME)carbonylation to methyl acetate(MA)in *** synergy between metal species and Brønsted acid sites accelerates DME *** we designed and prepared two catalysts with different Ag locations by seed-directed growth method and two-step impregnation method(named as Ag@HMOR and Ag/HMOR-out,respectively),to explain the effect of Ag location on catalytic *** results of TEM,XPS,CO-IR and UV–Vis showed that Ag species mainly presented as Ag^(0) species over both Ag@HMOR and Ag/***,Ag^(0) species mainly located in the micropores of Ag@HMOR,while as for Ag/HMOR-out,Ag^(0) mainly existed on external *** comparing the performance of the catalysts with different Ag positions,we confirmed that the Ag^(0) species encapsulated in the channels of HMOR promoted the DME carbonylation,which revealed the importance of spatial adjacency on the acid-metal catalysts.

关键词： Dimethyl ether Carbonylation Silver modification Metal location

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Systematic engineering of BiVO_(4)photoanode for efficient photoelectrochemical water oxidation

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Carbon Energy 2024年第4期6卷 12-21页

作者： Zhiting Liang Meng Li Kai‐Hang Ye Tongxin Tang Zhan Lin Yuying Zheng Yongchao Huang Hongbing Ji Shanqing Zhang Guangzhou Key Laboratory of Clean Transportation Energy Chemistry School of Chemical Engineering and Light IndustryGuangdong University of TechnologyGuangzhouChina Chemical Engineering Guangdong Laboratory Jieyang Branch of ChemistryJieyangChina Key Laboratory for Water Quality and Conservation of the Pearl River Delta Institute of Environmental Research at Greater Bay AreaMinistry of EducationGuangzhou UniversityGuangzhouChina State Key Laboratory Breeding Base of Green‐Chemical Synthesis Technology Institute of Green Petroleum Processing and Light Hydrocarbon ConversionCollege of Chemical EngineeringZhejiang University of TechnologyHangzhouChina School of Environment and Science Centre for Catalysis and Clean EnergyGriffith UniversityGold Coast CampusSouthportQueenslandAustralia

BiVO_(4)is one of the most promising photoanode materials for photoelectrochemical(PEC)solar energy conversion,but it still suffers from poor photocurrent density due to insufficient light‐harvesting efficiency(LHE),weak photogenerated charge separation efficiency(Φ_(Sep)),and low water oxidation efficiency(Φ_(OX)).Herein,we tackle these challenges of the BiVO_(4)photoanodes using systematic engineering,including catalysis engineering,bandgap engineering,and morphology *** particular,we deposit a NiCoO_(x)layer onto the BiVO_(4)photoanode as the oxygen evolution catalyst to enhance theΦ_(OX)of Fe‐g‐C_(3)N_(4)/BiVO_(4)for PEC water oxidation,and incorporate Fe‐doped graphite‐phase C_(3)N_(4)(Fe‐g‐C_(3)N_(4))into the BiVO_(4)photoanode to optimize the bandgap and surface areas to subsequently expand the light absorption range of the photoanode from 530 to 690 nm,increase the LHE andΦ_(Sep),and further improve the oxygen evolution reaction activity of the NiCoO_(x)catalytic ***,the maximum photocurrent density of the as‐prepared NiCoO_(x)/Fe‐g‐C_(3)N_(4)/BiVO_(4)is remarkably boosted from 4.6 to 7.4 mA cm^(−2).This work suggests that the proposed systematic engineering strategy is exceptionally promising for improving LHE,Φ_(Sep),andΦ_(OX)of BiVO_(4)‐based photoanodes,which will substantially benefit the design,preparation,and large‐scale application of next‐generation high‐performance photoanodes.

关键词： bismuth vanadate carbon nitride charge separation heterojunction water oxidation

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Self-adaptive gas flow and phase change behaviors during hydrate exploitation by alternate injection of N_(2) and CO_(2)

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Petroleum Science 2024年第3期21卷 2120-2129页

作者： Bo-Jian Cao Yi-Fei Sun Hong-Nan Chen Jin-Rong Zhong Ming-Long Wang Ming Wang Chang-Yu Sun Guang-Jin Chen State Key Laboratory of Heavy Oil Processing China University of PetroleumBeijing102249China School of Chemistry and Chemical Engineering Changsha University of Science&TechnologyChangsha410114HunanChina

Since hydrate resources play a part of the stratigraphic framework structure in sediments,establishing a safe and economic method for hydrates exploitation remains the primary challenge to this *** the proposed methods,the spontaneous displacement of CH_(4) from hydrate cages by CO_(2) seems to be a perfect mechanism to address gas production and CO_(2) storage,especially in today's strong demand for carbon reduction and replacing clean *** extensive lab researches,in the past decade,injecting a mixture of CO_(2) and small molecule gas has become a key means to enhance displacement efficiency and has great potential for ***,there is a lack of in-depth research on gas flow in the reservoir,while the injected gas always passes through low-saturated hydrate areas with high permeability and then occurs gas channel in a short term,finally resulting in the decreases in gas production efficiency and produced gas ***,we explored a new injection-production mode of alternate injection of N2 and CO_(2) in order to fully coordinate the advantages of N_(2) in enhanced hydrate decomposition and CO_(2) in solid storage and heat *** alternate"taking"and"storing"processes perfectly repair the problem of the gas channel,achieving self-regulation effect of CH_(4) recovery and CO_(2) *** 3-D experimental results show that compared to the mixed gas injection,CH_(4) recovery is increased by>50%and CO_(2) storage is increased by>70%.Additionally,this alternate injection mode presented a better performance in CH_(4) concentration of produced gas and showed outstanding N_(2) utilization ***,we analyzed its self-adaptive gas flow mechanism and proposed an application model of"one injection and multiple production".We look forward to this study accelerating the application of CO_(2)-CH_(4) replacement technology.

关键词： Hydrate Replacement CH_(4)recovery CO_(2)storage Reservoir remediation

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Size dependence of carbon-encapsulated iron-based nanocatalysts for Fischer–Trposch synthesis

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Nano Research 2023年第5期16卷 6270-6277页

作者： Xiaoxue Han Jing Lv Shouying Huang Qiao Zhao Yue Wang Zhenhua Li Xinbin Ma Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Zhejiang Institute of Tianjin University Ningbo 315201China Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192China

The conversion from syngas derived from non-petroleum recourses to liquid fuels and chemicals via Fischer–Tropsch synthesis(FTS)is regarded as an alternative and potential *** catalyst with controllable particle size and clarifying size effect are of significance to promote the ***,we engineered carbon-encapsulation structure to restrict particle growth but avoid strong metal–support *** prepared carbon-encapsulated nanoparticles(Fe@C)showed a superior catalytic activity compared with conventional carbon-supported nanoparticles(Fe/C).By tuning particle size from 3.0 to 9.1 nm,a volcano-like trend of iron time yield(FTY)peaked at 2659μmol·gFe^(−1)·s^(−1)is obtained with an optimum particle size of 5.3 *** to temperature-programmed reduction and desorption results,a linear relationship between apparent turnover frequency and CO dissociation capacity was *** enhanced CO dissociative adsorption along with weakened H_(2)activation on larger nanoparticles resulted in higher C_(5+)*** study provides a strategy to synthesize carbon supported metal catalysts with controllable particle size and insight into size effect on Fe-based catalytic FTS.

关键词： Fischer–Tropsch synthesis iron-based catalyst carbon-encapsulation size effect

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Defective NH_(2)-UiO-66(Zr) effectively converting CO_(2) into cyclic carbonate under ambient pressure,solvent-free and co-catalyst-free conditions

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Chinese Journal of chemical engineering 2022年第3期35卷 222-229页

作者： Xueting Liu Chunhui Hu Jingjing Wu Peng Cui Fengyu Wei School of Chemistry and Chemical Engineering Hefei University of TechnologyAnhui Key Laboratory of Controllable Chemical Reaction&Material Chemical EngineeringHefei 230009China

In this study,a series of metal-organic frameworks(MOFs)NH_(2)-UiO-66-x HAc catalysts were synthesized by solvothermal method using acetic acid(HAc)as a modulator,and were applied to the cycloaddition of CO_(2)and epichlorohydrin(EPIC)under ambient *** of the modulation by HAc on morphologies and structures of the MOFs are demonstrated via PXRD,FESEM,FTIR,N_(2)adsorption-desorption,XPS and ^(1)H NMR *** results show that the MOFs containing mesoporous pores can be prepared by adjusting the concentration of *** optimizing the amount of HAc added,the specific surface area of NH_(2)-UiO-66-8 HAc is as high as 879.17 m^(2)·g^(-1),which is 28.3%higher than that of the original *** the evaluation of catalytic performance showed that HAc modulation enhanced the activity of NH_(2)-UiO-66-x HAc under mild *** exposure of Lewis acid sites,increased specific surface area and porosity via the modulation of HAc defective ligand can be supposed the key factors to determine the enhanced catalytic *** addition,considering the influence of gas concentration on the reaction,the concept of TOP(Turnover of Pressure,defined as the mass of conversions of a unit mass catalyst under unit pressure and unit time)was first proposed in this article.

关键词： CO_(2)conversion Metal-organic frameworks Acetic acid modulation Defect Mild conditions

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High-throughput structure determination of polycrystalline functional materials:a platform for automated 3DED/MicroED data collection

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Science China Chemistry 2024年第12期67卷 4158-4166页

作者： Zhenghan Zhang Zhengyin Liang Chao Ma Cong Lin Jian Li State Key Laboratory of Coordination Chemistry School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China Department of Mechanical Engineering The Hong Kong Polytechnic UniversityHong Kong 99077China

Structure determination plays the most crucial role in the discovery of novel functional materials,because only by knowing the intrinsic structures can we accurately and completely understand their properties and ***,most new materials are obtained in polycrystalline form or even as mixtures with multiple phases when first synthesized,presenting significant challenges in their structure determination and phase ***,the developed three-dimensional electron diffraction(3DED/MicroED)has provided a promising solution to overcome these *** this study,we have constructed a state-of-the-art 3DED/MicroED data acquisition equipment by integrating a hybrid-pixel detector with a script developed for Serial EM,and thus successfully developed an automated 3DED/MicroED method for the high-throughput structure *** demonstrate its effectiveness,a multiphase sample with complex porous structures is employed,showcasing that individual phases and their structures can be identified and determined,*** remarkable finding is the identification of an impurity metal-organic framework(MOF)that is completely invisible to traditional powder X-ray diffraction in a supposedly“pure”commercial MOF ***,our method also enables the atomic-resolution structure determination of flexible covalent organic framework materials,which are highly sensitive to electron ***,a new microporous aluminoborate is discovered using this rapid structure determination *** experimental results highlight the enormous potential of our 3DED/MicroED method in the field of new materials discovery,offering a powerful tool for the structure determination of polycrystalline functional materials.

关键词： 3DED/MicroED high-throughput structure determination mixed phase porous materials

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Electro-oxidation cross-coupling of primary and secondary alcohols by constructing intermediate-enriched micro-environment

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Science China Chemistry 2023年第8期66卷 2408-2415页

作者： Leitao Xu Cairong Wang Yelin Yao Wei Chen Zhonghuan Zhu Jingcheng Wu Ming Yang Yandong Wu Shuangyin Wang Yuqin Zou State Key Laboratory of Chemo/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangshaHunan410082China School of Chemistry and Chemical Engineering Jishou UniversityJishou416000China

Electrocatalytic dehydrogenative cross-coupling of various alcohols in aqueous electrolytes functionalizes alcohols to form structurally diverse long-carbon-chain ***,it remains challenging to achieve the high selectivity because of the high reactivity of involved carbonyl intermediates and different oxidation rates for the ***,the synthesis ofα,β-unsaturated ketones from alcohols was realized by the electro-oxidation cross-coupling in aqueous solutions by a“salting-out”strategy to engineer the micro-environment at electrocatalytic reaction *** calculations and electrochemical measurements demonstrated that concentrated local intermediates could inhibit the over-oxidation of alcohols and accelerate the coupling reaction kinetics between the *** strategy can couple primary and secondary alcohols to formα,β-unsaturated carbonyl compounds with a selectivity of 87% and be easily scaled up to gram *** study provides an attractive strategy for broadening the diversity of organic products in electrocatalysis.

关键词： electro-oxidation of alcohols cross-coupling cation effect microenvironment

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Green synthesis of luminescent La-MOF nanoparticle from waste poly(ethylene terephthalate) for high-performance in Fe(Ⅲ) detection

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Rare Metals 2024年第8期43卷 3833-3843页

作者： Zhi Gong Zhi-Kui Dai Zhi-Yue Dong Qiu-Xuan Liu Valentin A.Milichko Hua-Jian Liu Jie Liu Ran Niu Jiang Gong Key Laboratory of Material Chemistry for Energy Conversion and Storage Hubei Key Laboratory of Material Chemistry and Service FailureHubei Engineering Research Center for Biomaterials and Medical Protective MaterialsSemiconductor Chemistry CenterSchool of Chemistry and Chemical EngineeringMinistry of EducationHuazhong University of Science and TechnologyWuhan 430074China School of Chemical Engineering and Pharmacy Wuhan Institute of TechnologyWuhan 430073China Collaborative Innovation Center for Advanced Organic Chemical Materials Co-constructed by the Province and Ministry Ministry of Education Key Laboratory for the Synthesis and Application of Organic Functional Molecules and College of Chemistry and Chemical EngineeringHubei UniversityWuhan 430062China School of Physics and Engineering ITMO UniversitySt.Petersburg197101Russia School of Materials Science and Engineering Hubei UniversityWuhan430062China Guangdong Provincial Key Laboratory of Technique and Equipment for Macromolecular Advanced Manufacturing School of Mechanical and Automotive EngineeringKey Laboratory of Polymer Processing EngineeringMinistry of EducationSouth China University of TechnologyGuangzhou 510641China

Developing luminescent metal-organic frameworks(MOFs) capable of high-efficiency Fe^(3+)sensing has aroused great attraction in the fields of biology,chemistry,***,previous solvothermal methods are limited by organic solvent usage,time consuming,high pressure,and high-energy ***,we propose the waste-toMOF strategy towards the scale-up production of La-MOF nanoparticles through the ball milling of recycled poly(-ethylene terephthalate)(PET) bottles and La(NO_(3))_(3)·_(6)H_(2)*** goes on alkaline hydrolysis to form 1,4-benzenedicarboxylic acid sodium salt(Na_(2)BDC) and ethylene glycol by ball ***,BDC reacts with La^(3+)to form *** as-prepared La-MOF crystal nanoparticles possess a rod-like morphology with the size of few hundred ***,La-MOF nanoparticles display high selectivity and sensitivity for Fe^(3+)*** quenching constant and limit of detection are 5.29×10^(3)(mol·L^(-1))^(-1) and 0.147 μmol·L^(-1),respectively,thus surpassing many advanced Fe^(3+) *** to the result of density functional theory,the high Fe^(3+) detection performance of La-MOF is related to the complexing of Fe^(3+)with La-MOF,which leads to the gradual dissociation of the coordination bond between terephthalic acid and La^(3+).It is anticipated that the mechanochemistry milling-based wasteto-MOF strategy provides a new platform for the massive production of functional MOFs in a green manner.

关键词： Metal-organic framework Waste polyester Mechanochemistry milling Fluorescence sensor

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