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Doublecarbohelicene:facile synthesis,chiroptical properties,isomerization study,and lasing application

Science China Chemistry 2025年第1期68卷 233-240页

作者： Peipei Liu Yantong Li Meng-Xiang Wu Hao Kang Xiao-Li Zhao Lin Xu Linlin Liu Xiaodong Li Junfeng Fang Zhiwei Fang Ya Cheng Hai-Bo Yang Huakang Yu Xueliang Shi State Key Laboratory of Petroleum Molecular&Process Engineering Shanghai Key Laboratory of Green Chemistry and Chemical ProcessesSchool of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062China School of Physics and Optoelectronics South China University of TechnologyGuangzhou 510640China School of Physics and Electronic Science Engineering Research Center of Nanophotonics&Advanced InstrumentMinistry of EducationEast China Normal UniversityShanghai 200241China State Key Laboratory of Precision Spectroscopy School of Physics and Electronic ScienceEast China Normal UniversityShanghai 200241China Institute of Polymer Optoelectronic Materials&Devices State Key Laboratory of Luminescent Materials&DevicesSouth China University of TechnologyGuangzhou 510640China

Double carbohelicenes have attracted considerable attention due to their aesthetic structures,distinctπ-conjugation extension,inherent chirality,and intriguing optical and electronic ***,the concise de novo synthesis of a new double[5]carbohelicene 1 together with its chiroptical properties,isomerization process and lasing application is presented.1 was synthesized by a simple protocol involving the formation of a 6,6′-bipentacene as the key *** is worth noting that1 existed as two diastereomers 1-PP/MM and 1-PM,which were successfully isolated and unambiguously confirmed by Xray *** optical resolution of the racemic 1-PP/MM was successfully achieved by chiral-phase highperformance liquid chromatography(HPLC),and 1-PP and 1-MM were characterized by circular ***,it was found that 1-PP/MM could be completely isomerized to 1-PM upon heating,and the detailed thermodynamics and kinetics of the isomerization process were systematically investigated.1-PM exhibited deep-red luminescence with emission maximum at 723 nm and fluorescence quantum yield as high as 32.95%.Consequently,we can showcase the lasing application of 1-PM by doping with epoxy resin to assemble a bottle microlaser spontaneously,which the lasing wavelength is 796.6 nm at a threshold of 0.8 m J cm^(-2).We believe that our studies,including the facile synthesis methodology,detailed isomerization studies,and lasing application,will shed some light on the design and synthesis of novel carbohelical systems with more functions.

关键词： double carbohelicene optical resolution organic laser isomerization X-ray diffraction

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Carbon nanofiber catalysts containing high-entropy metal phosphides with low-content Ru for highly efficient hydrogen evolution reaction

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Rare Metals 2025年第1期44卷 324-335页

作者： Peng Wang Jie Zheng Xue-Hao Li Wen-Bo Cui Jin-Hua Liu Yong Wan Jun Zhang Yusuke Yamauchi Zhong-Li Wang Mang Niu Yun-Ze Long Shandong Key Laboratory of Medical and Health Textile Materials College of PhysicsQingdao UniversityQingdao 266071China Industrial Research Institute of Nonwovens and Technical Textiles Shandong Center for Engineered Nonwovens(SCEN)College of Textiles ClothingQingdao UniversityQingdao 266071China State Key Laboratory of Bio-Fibers and Eco-textiles Institute of Biochemical EngineeringCollege of Materials Science and EngineeringQingdao UniversityQingdao 266071China School of Chemical Engineering and Australian Institute for Bioengineering and Nanotechnology(AIBN) The University of QueenslandBrisbaneQLD 4072Australia Department of Chemical and Biomolecular Engineering Yonsei UniversitySeoul 03722Republic of Korea Department of Materials Process Engineering Graduate School of EngineeringNagoya UniversityNagoya 464-8603Japan Tianjin Key Laboratory of Applied Catalysis Science and Technology School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China

High-entropy metal phosphide(HEMP)has considerable potential as an electrocatalyst owing to its beneficial properties,including high-entropy alloy synergy as well as the controllable structure and high conductivity of ***,electrospinning and in situ phosphating were employed to prepare three-dimensional(3D)networks of self-supporting HEMP nanofibers with varying degrees of phosphate *** characterizations via X-ray diffraction and X-ray photoelectron spectroscopy,as well as density functional theory calculations,demonstrate that the introduction of phosphorus(P)atoms to HEMP carbon nanofibers mediates their electronic structure,leads to lattice expansion,which in turn enhances their catalytic performance in the hydrogen evolution reaction(HER).Moreover,the formation of metal-P bonds weakens metal-metal interaction and decreases the free energy of hydrogen adsorption,contributing to the exceptional activity observed in the HEMP *** measurements demonstrate that the HEMP-0.75 catalyst with an ultralow loading of 1.22 wt%ruthenium(Ru)exhibits the highest HER catalytic activity and stability in a 1 M KOH electrolyte,achieving a minimal overpotential of 26 mV at a current density of 10 mA·cm^(-2)and Tafel slope of 50.9 mV·dec^(-1).

关键词： High-entropy metal phosphide Electrospinning Hydrogen evolution reaction Self-supporting carbon nanofibers

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A rechargeable and portable hydrogen storage system grounded on soda water

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Chinese Chemical Letters 2025年第3期36卷 305-310页

作者： Lingyun Shen Shenxiang Yin Qingshu Zheng Zheming Sun Wei Wang Tao Tu State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering School of Chemistry and Chemical EngineeringNingxia UniversityYinchuan 750021China Shanghai Key Laboratory of Molecular Catalysts and Innovative Materials Department of ChemistryFudan UniversityShanghai 200438China Frontiers Science Center for Transformative Molecules Shanghai Key Laboratory for Molecular Engineering of Chiral DrugsSchool of Chemistry and Chemical Engineering and Zhangjiang Institute for Advanced StudyShanghai Jiao Tong UniversityShanghai 200240China Departments of Pharmacology and Toxicology and Chemistry and Biochemistry University of ArizonaTucsonAZ 85721United States State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

The bicarbonate-formate(HCO_(3)−–HCO_(2)−)interconversion provides a promising cycle for a conveniently accessible hydrogen storage system via reversible dehydrogenation and hydrogenation *** catalytic systems often use organic solvents,tedious optimization as well as manipulation of pH values,solvent,pressure and various ***,we present an operational,robust,safe and cost-effective catalytic system for hydrogen storage and *** have established a unique catalytic system with two different solid organometallic assemblies(NHC-Ru and NHC-Ir)that facilitate the reversible transformation between sodium formate and bicarbonate in aqueous solutions collaboratively and ***,the NHC-Ru catalyst is privileged for the hydrogenation of sodium bicarbonate,whereas the NHC-Ir component enables the dehydrogenation of sodium formate,all in a single reaction *** sets this system apart is its *** H_(2)discharging and recharging is simply regulated by heating the mixture with or without H_(2).Remarkably,this process requires no extra additives or supplementary ***,the reversible hydrogen storage system is durable and can be reused for over 30 cycles without a discernible decline in activity and *** strategic paradigm in this study shows significant practical potential in hydrogen fuel cell applications.

关键词： Dehydrogenation Hydrogen storage Hydrogenation N-Heterocyclic carbene Soda water

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Uniform deposition of ultra-thin TiO_(2) film on mica substrate by atmospheric pressure chemical vapor deposition: Effect of precursor concentration

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Chinese Journal of Chemical engineering 2023年第8期60卷 99-107页

作者： Ming Liu Ying Li Rui Wang 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&Environmental Engineering China University of Mining and Technology-BeijingBeijing 100083China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China

The performance of pearlescent pigment significantly affected by the grain size and the roughness of deposited film. The effect of TiCl_(4) concentration on the initial deposition of TiO_(2) on mica by atmospheric pressure chemical vapor deposition(APCVD) was investigated. The precursor concentration significantly affected the deposition and morphology of TiO_(2) grains assembling the film. The deposition time for fully covering the surface of mica decreased from 120 to 10 s as the TiCl_(4) concentration increased from 0.38%to 2.44%. The grain size increased with the TiCl_(4) concentration. The AFM and TEM analysis demonstrated that the aggregation of TiO_(2) clusters at the initial stage finally result to the agglomeration of fine TiO_(2) grains at high TiCl_(4) concentrations. Following the results, it was suggested that the nucleation density and size was easy to be adjusted when the TiCl_(4) concentration is below 0.90%.

关键词： Chemical vapor deposition TiO_(2)thin film Nucleation reaction Precursor concentration Pearlescent pigment

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Progress and Perspectives of Hollow Multishelled Structures

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Chinese Journal of Chemistry 2022年第10期40卷 1190-1203页

作者： Jiangyan Wang Mei Yang Dan Wang State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Hollow multishelled structure(HoMs)has drawn tremendous attention due to its abundant attractive properties and promising ***,for a long time,the limited synthesis method hindered the development of *** sequential templating approach developed by our group,has greatly enriched its composition and'structure *** progress in HoMS synthesis promotes the discovery of its characteristics as well as widens its application ***,the recently explored temporal-spatial ordering characteristic of HoMS has shown great promise in drug delivery and cascade catalysis application ***,we summarize the current development progress of HoMS in the aspects of both synthesis and application,with a focus discussion on how to shape its application performance by manipulating its composition and structure *** addition,we discuss the current challenges and providethe future potentials holdingfor HoMs.

关键词： Hollow multishelled structure Sequential templating approach Temporal-spatial ordering Catalysis Structure-activity relationships

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Synthesis of methanol via CO_(2) hydrogenation catalyzed by La_(2)O_(2)CO_(3)/Cu catalysts

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Nano Research 2025年第2期18卷 153-163页

作者： Jun He Chenglong Yu Zhijuan Zhao Bo Guan Bin Zhang Yanru Zhang Longbo Zhang Yanyan Wang Ying Wang Yahui Wu Jia Guo Yang Li Tianbin Wu Qingli Qian Hongxing Wang Buxing Han Beijing National Laboratory for Molecular Sciences Key Laboratory of Colloid and Interface and ThermodynamicsCenter for Carbon Neutral ChemistryInstitute of ChemistryChinese Academy of SciencesBeijing 100190China College of Chemical Engineering and Materials Science Tianjin University of Science and TechnologyTianjin 300457China School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049China Center for Physicochemical Analysis Measurements Institute of ChemistryChinese Academy of SciencesBeijing 100190China Shanghai Key Laboratory of Green Chemistry and Chemical Processes State Key Laboratory of Petroleum Molecular and Process EngineeringSchool of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062China

The development of efficient Cu-based heterogeneous catalysts for CO_(2) hydrogenation to methanol has been an appealing *** by the concept of inverse catalysts,a series of La_(2)O_(2)CO_(3)/Cu nanorod composites with varying Cu contents(denoted as LOC/Cu-x,where x stands for the mass ratio of La and Cu in the catalysts)were prepared by combining coprecipitation and calcination *** composition-dependence of catalytic activity and selectivity were observed when different LOC/Cu-x(x=0.1,0.2,0.5,1,3 and 5)were used to catalyze the CO_(2) *** predominant product shifted from methane to methanol with the increasing Cu *** highest reaction rate(13.3 mmol·gCu^(-1)·h^(-1))and methanol selectivity(85.5%)were achieved when LOC/Cu-1 was tested at 200℃.The LOC was not active for the reaction,while the Cu itself displayed poor catalytic *** Cu–LOC interactions significantly affected the nature of the catalysts,including mutual electron transfer,crystal structure,morphology,porosity,surface Cu valence and capability of adsorbing the reactant gases,etc.,which account for the outstanding behavior of the LOC/Cu-1 *** work provides a new strategy for the design and optimization of Cu-based catalysts.

关键词： CO_(2)hydrogenation methanol heterogeneous catalysts Cu-La_(2)O_(2)CO_(3)(LOC)interaction

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Preparation of Biobased Porous Hydrogels by Citric Acid Grafted Polyacrylic Acid for Rare Earth Elements Separation

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Palpu Chongi Gisul/Journal of Korea Technical Association of the Pulp and Paper Industry 2025年第2期57卷 29-45页

作者： He, Bo Xiang, Wenchao Li, Wenjing He, Ming Yang, Liangrong Yang, Chao Yang, Guihua State Key Laboratory of Green Papermaking and Resource Recycling Qilu University of Technology China State Key Laboratory of Petroleum Molecular & Process Engineering CAS Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences China School of Chemical Engineering University of Chinese Academy of Science China State Key Laboratory of Petroleum Molecular & Process Engineering CAS Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences China School of Chemical & Environmental Engineering China University of Mining & Technology China State Key Laboratory of Green Papermaking and Resource Recycling Qilu University of Technology China State Key Laboratory of Petroleum Molecular & Process Engineering CAS Key Laboratory of Green Process and Engineering Institute of Process Engineering Chinese Academy of Sciences China School of Chemical Engineering University of Chinese Academy of Science China State Key Laboratory of Green Papermaking and Resource Recycling Qilu University of Technology China

Rare earth elements (REEs) are essential for advanced technologies such as energy, electronics, and aerospace. Efficient separation of REEs is critical for the full utilization of natural limited resources. To obtain biobased absorbents with large adsorption capacity, high selectivity, and good reusability, a larger surface area and functionalized surface of absorbents are required. In this work, the porous PAA-CA (citric acid-grafted polyacrylic acid) hydrogels were prepared using a high internal phase emulsion templating method. The physical and chemical properties of PAA-CA were characterized by FTIR, XPS, and SEM. The influence of pH, temperature, initial concentration, and contact time on the adsorption capacity of Pr3+ (light REE) and Er3+ (heavy REE) was investigated and analyzed. The results show that PAA-CA hydrogels exhibited good adsorption performance with a better adsorption capacity for Er3+ of around 400 mg/g. The adsorption process was pH-dependent, with optimal adsorption at pH = 3–7. Kinetic studies revealed that the adsorption followed a pseudo-second-order model, while thermodynamic analyses confirmed the process was spontaneous and endothermic. PAA-CA exhibited good selectivity for Er3+ in a binary ion system, especially containing K+ or Fe3+. Furthermore, the hydrogels retained high adsorption capacities across 10 adsorption-desorption cycles, highlighting their excellent reusability. These results suggest that porous PAA-CA hydrogels are promising materials for the selective recovery of REEs from aqueous solutions. © 2025 Korean Technical Assoc. of the Pulp and Paper Industry. All rights reserved.

关键词： Grafting (chemical)

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ZnO HoMS@ZIF-8 Nanoreactors for Efficient Enrichment and Photoreduction of Atmospheric CO_(2)

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CCS Chemistry 2024年第12期6卷 3065-3076页

作者： Yanze Wei Juan Li Decai Zhao Yasong Zhao Qinghua Zhang Lin Gu Jiawei Wan Dan Wang State Key Laboratory of Biochemical Engineering Institute of Process EngineeringChinese Academy of SciencesBeijing 100190 Key Laboratory of Biopharmaceutical Preparation and Delivery Chinese Academy of SciencesBeijing 100190 University of Chinese Academy of Sciences Beijing 100049 Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190

The ultimate goal of photocatalytic CO_(2)reduction is to efficiently convert atmospheric CO_(2)into value-added products by designing hierarchical photocatalysts that combine effective harvesting and accelerate activation capabilities of CO_(2)*** this work,we demonstrated direct air-level CO_(2)reduction by hollow multishell structure(HoMS)nanoreactors with zeolitic imidazolate framework-8(ZIF-8)-modified ZnO heteroshells,which offers a promising solution to optimize the mass transfer process via selective sieving and effective enrichment of CO_(2)molecules from the atmospheric ***,heteroshells with ZIF-8 matrix act as pumps that effectively capture CO_(2)molecules,while the cavities serve as tanks to hold these molecules,thus significantly enhancing the transfer kinetics for CO_(2)*** periodic shell-cavity configuration allows the nanoreactor to effectively gather CO_(2)molecules near the catalytic sites,thus increasing conversion opportunities for activated ***,the surface atomic steps on the ZnO/ZIF-8 heterointerfaces with staggered geometry expedite charge transfer and adsorption efficiency,which synergistically boosts the CO_(2)-CO yield up to 3.7μmol/h under CO_(2)flow and 0.7μmol/h under atmospheric conditions with almost complete CO ***,the HoMS nanoreactors offer a potential strategy for solving the“last mile”challenge in practical CO_(2)valorization.

关键词： hollow multishelled structures atmospheric CO_(2)photoreduction ZnO ZIF-8 heterointerface

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The manipulation of rectifying contact of Co and nitrogen-doped carbon hierarchical superstructures toward high-performance oxygen reduction reaction

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Carbon Energy 2024年第9期6卷 338-349页

作者： Jing Li Tingyu Lu Yu Fang Guangyao Zhou Mingyi Zhang Huan Pang Jun Yang Yawen Tang Lin Xu Jiangsu Key Laboratory of New Power Batteries School of Chemistry and Materials ScienceJiangsu Collaborative Innovation Center of Biomedical Functional MaterialsNanjing Normal UniversityNanjingJiangsuChina College of Science Jinling Institute of TechnologyNanjingJiangsuChina Key Laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationSchool of Physics and Electronic EngineeringHarbin Normal UniversityHarbinHeilongjiangChina School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhouJiangsuChina State Key Laboratory of Multiphase Complex Systems Center of MesoscienceInstitute of Process EngineeringChinese Academy of SciencesBeijingChina

Rational design and construction of oxygen reduction reaction(ORR)electrocatalysts with high activity,good stability,and low price are essential for the practical applications of renewable energy conversion devices,such as metal-air *** modification through constructing metal/semiconductor Schottky heterointerface represents a powerful strategy to enhance the electrochemical ***,we demonstrate a concept of Schottky electrocatalyst composed of uniform Co nanoparticles in situ anchored on the carbon nanotubes aligned on the carbon nanosheets(denoted as Co@N-CNTs/NSs hereafter)toward *** experimental findings and theoretical simulation testify that the rectifying contact could impel the voluntary electron flow from Co to N-CNTs/NSs and create an internal electric field,thereby boosting the electron transfer rate and improving the intrinsic *** a consequence,the Co@N-CNTs/NSs deliver outstanding ORR activity,impressive long-term durability,excellent methanol tolerance,and good performance as the air-cathode in the Zn-air *** design concept of Schottky contact may provide the innovational inspirations for the synthesis of advanced catalysts in sustainable energy conversion fields.

关键词： Co-based electrocatalysts oxygen reduction reaction rectifying contact Zn-air batteries

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Graph convolutional network soft sensor for process quality prediction

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Journal of process Control 2023年第1期123卷 12-25页

作者： Jia, Mingwei Xu, Danya Yang, Tao Liu, Yi Yao, Yuan Institute of Process Equipment and Control Engineering Zhejiang University of Technology Hangzhou310023 China State Key Laboratory of Synthetical Automation for Process Industries Northeastern University Shenyang110819 China Department of Chemical Engineering National Tsing Hua University Hsinchu30013 Taiwan

The nonlinear time-varying characteristics of the process industry can be modeled using numerous data-driven soft sensor methods. However, the intrinsic relationships among the variables, especially the localized spatial–temporal correlations that shed light on model behavior, have received little attention. In this study, a soft sensor based on a graph convolutional network is constructed by introducing the concept of graph to process modeling. The focus is on obtaining localized spatial–temporal correlations that aid in comprehending the intricate interactions among the variables included in the soft sensor. The model is trained by considering the regularization terms and it learns distinctive localized spatial–temporal correlations in an end-to-end manner. Furthermore, long-term dependence is established via temporal convolution. Thus, both the localized spatial–temporal correlations and time-series properties are captured. The feasibility of the proposed soft sensor is illustrated using two fermentation processes. The localized spatial–temporal correlations of this case study are visualized, and they demonstrate that the soft sensor is not a black-box model;instead, it is consistent with process knowledge. © 2023 Elsevier Ltd

关键词： Convolution

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