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Chinese chemical Letters 2024年第9期35卷 165-168页

作者： Jindong Hao Yufen Lv Shuyue Tian Chao Ma Wenxiu Cui Huilan Yue Wei Wei Dong Yi key laboratory of Catalytic Conversion and clean Energy in Universities of shandong province School of Chemistry and Chemical EngineeringQufu Normal UniversityQufu 273165China Qinghai Provincial key laboratory of Tibetan Medicine Research and CAS key laboratory of Tibetan Medicine Research Northwest Institute of Plateau BiologyXining 810008China Green Pharmaceutical Technology key laboratory of Luzhou City School of PharmacySouthwest Medical UniversityLuzhou 646000China

A simple and additive-free protocol has been developed for the preparation ofβ-keto phosphorodithioates through the three-component reaction of easily available sulfoxonium ylides,P_(4)S_(10),and *** present geminal hydro-phosphorodithiolation reaction was performed at room temperature to construct a series ofβ-keto phosphorodithioates in the absence of any metal reagents,bases,or additives.

关键词： β-Keto phosphorodithioates Phosphorodithiolation Sulfoxonium ylides P_(4)S_(10) Alcohols

Curing Mechanism of Condensed Polynuclear Aromatic Resin and Thermal Stability of Cured Resin

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China Petroleum processing & Petrochemical Technology 2015年第2期17卷 9-16页

作者： Li Shibin Sun Qiqian Wang Yuwei Wu Mingbo Zhang Zailong College of chemical Engineering State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum

In order to improve the thermal stability of condensed polynuclear aromatic(COPNA) resin synthesized from vacuum residue, 1,4-benzenedimethanol was added to cure COPNA resin. The curing mechanism was investigated by proton nuclear magnetic resonance spectrometry, solid carbon-13 nuclear magnetic resonance spectrometry and Fourier transform infrared spectroscopy. Microstructures of the uncured and the cured COPNA resins were studied by scanning electron microscopy and X-ray diffractometry. The thermal stability of COPNA resins before and after curing was tested by thermogravimetric analysis. The element composition of the cured COPNA resin heated at different temperatures was analyzed by an element analyzer. The results showed that the uncured COPNA resin reacted with the cross-linking agent during the curing process, and the curing mechanism was confirmed to be the electrophilic substitution reaction. Compared with the uncured COPNA resin, the cured COPNA resin had a smooth surface, well-ordered and streamlined sheet structure with more crystalline solids, better molecular arrangement and orientation. The weight loss process of the uncured and cured COPNA resins was divided into three stages. Carbon residue of the cured COPNA resin was 41.65% at 600 ℃, which was much higher than 25.02% of the uncured COPNA resin, which indicated that the cured COPNA resin had higher thermal stability.

关键词： condensed polynuclear aromatic resin synthesis vacuum residue curing thermal stability

Cross-metathesis of biomass to olefins:Molecular catalysis bridging the gap between fossil and bio-energy

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Chinese Journal of chemical Engineering 2022年第8期35卷 44-60页

作者： Wenjuan Yan Zhenchao You Kexin Meng Feng Du Shuxia Zhang Xin Jin State key laboratory of Heavy Oil processing Center for Chemical Engineering Experimental TeachingChina University of PetroleumQingdao 266580China

Terminal olefins are important building blocks for the industry of biofuels,oligomers,and lubricants *** industrial processes for production of olefins involving oligomerization of ethylene or cracking of petrochemical waxes have several flaws including low yield and high cost in product ***-metathesis of bio-derived unsaturated fatty esters and olefins with ethylene(ethenolysis),allows the conversion of sustainable waste biomass to various renewable olefins with much safer,less toxic,sustainable,and zero-CO_(2) emission *** our best knowledge,however,a comprehensive summary of key advances in this field(since 2017)is yet to be available,particularly on molecular features of homogeneous and heterogeneous *** paper presents a critical review on molecular structures of metal complex and oxide catalysts for ethenolysis of olefins and *** influence of cationic centers,coordination conditions,nature of ligands,operating conditions on catalyst performances will be systematically discussed along with relevant reaction *** key challenges for rational design of coordinated cationic hybrids have been summarized,which will provide insights to technological advancement of large-scale production of oleochemical-derived olefins.

关键词： Metathesis Catalysts Metal complex Metal oxide Olefins Oleochemicals

The aromatic peptide protected gold nanoclusters with significant Stokes shift:Ligand-mediated two-step FRET

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Nano Research 2023年第10期16卷 12207-12214页

作者： Qi Dai ZhiXiong Zhang Biao Yu Xinyu Li Jingqiu Li Zichun Qi Hua He Fang Huang Xiaojuan Wang State key laboratory of Heavy Oil processing College of Chemical EngineeringChina University of Petroleum(East China)Qingdao 266580China

During the last decade,a great variety of ligand protected gold nanoclusters(AuNCs)have been synthesized,and their broad applications have been intensively *** the spectroscopic properties of AuNCs have been comprehensively explored,the mechanism of the significant Stokes shift(>200 nm)and the specific role played by surface ligands have not been clearly explained *** this study,a series of fluorescent AuNCs with huge Stokes shift(up to 530 nm)were successfully prepared by employing the rationally designed tri-peptides as the protecting ligands,and their spectroscopic properties were systematically *** detailed measurements on the example product,YCY-AuNCs(Tyr-Cys-Tyr liganded AuNCs),showed that the energy absorbed by the tyrosine(~250 nm)can be effectively transferred through the ligand-mediated two-step Förster resonance energy transfer(FRET)process and released as fluorescence emission in the near-infrared fluorescence(NIR)range(~780 nm),which resulted in the significant apparent Stokes *** YCY ligands play a critical role by offering the tyrosine groups(donor of the first FRET pair),generating the dityrosine-like structure on the AuNCs surface(acceptor of the first FRET pair and donor of the second FRET pair),and protecting the cores(acceptor of the second acceptor).The additional ligand exchange experiments and the investigation on the other AuNCs further demonstrated that the sufficient high density of the aromatic groups is also essential to mediate the two-step FRET and achieve the remarkable Stokes *** believe that the aromatic ligand-mediated FRET mechanism not only offers a new theoretical explanation for the huge Stokes shift exhibited in AuNCs,but also provides a general strategy for the construction of new materials with large Stokes shift.

关键词： gold nanoclusters Stokes shift ligand effect aromatic ligands Förster resonance energy transfer(FRET)

Constructing a multifunctional mesoporous composite of metallic cobalt nanoparticles and nitrogen-doped reduced graphene oxides for high-performance lithium-sulfur batteries

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Carbon Energy 2022年第2期4卷 142-154页

作者： Luhai Gai Chenhao Zhao Ya Zhang Zhibiao Hu Qiang Shen key laboratory for Colloid and Interface Chemistry of Education Ministry School of Chemistry and Chemical EngineeringShandong UniversityJinanChina Fujian Provincial key laboratory of clean Energy Materials College of Chemistry&MaterialsLongyan UniversityLongyanChina

Electrochemical properties of lithium-sulfur(Li-S)batteries are mainly hindered by both the insulating nature of elemental sulfur(i.e.,molecular S8)and the shuttling effect or sluggish redox kinetics of lithium polysulfide intermediates(Li_(2)S_(n),3≤n≤8).In this paper,a three-dimensional mesoporous reduced graphene oxide-based nanocomposite,with the embedding of metallic Co nanoparticles and the doping of elemental N(Co/NrGO),and its simply ground mixture with powdered S at a mass ratio of 1:6(Co/NrGO/S)are prepared and used as cathode-/separator-coated interlayers and working electrodes in assembled Li-S cells,*** of the effective cell configurations is to paste composite Co/NrGO onto both the S-loading cathode and separator,showing good cycling stability(1070mAh g^(−1) in the 100th cycle at 0.2 C),highrate capability(835mAh g^(−1),2.0 C),and excellent durability(905mAh g^(−1) in the 250th cycle at 0.5 or 0.2 C).Compared with the experimental results of Co-absent NrGO,electrochemical properties of various Co/NrGO-based cell configurations clearly show multiple functions of Co/NrGO,indicating that the absence of Co/NrGO coatings and/or Co nanoparticles may be inadequate to achieve superior S availability of assembled Li-S batteries.

关键词： high-performance mechanism lithium-sulfur batteries multifunctional three-dimensional mesoporous reduced graphene oxide-based nanocomposite

Activated carbon induced oxygen vacancies-engineered nickel ferrite with enhanced conductivity for supercapacitor application

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Frontiers of chemical Science and Engineering 2023年第12期17卷 2088-2100页

作者： Xicheng Gao Jianqiang Bi Linjie Meng Lulin Xie Chen Liu key laboratory for Liquid-Solid Structural Evolution and processing of Materials(Ministry of Education) School of Materials Science and EngineeringShandong UniversityJinan 250061China

NiFe_(2)O_(4) is a kind of bimetallic oxide possessing excellent theoretical capacity and application prospect in the field of ***,due to the inherent poor conductivity of metal oxides,the performance of NiFe_(2)O_(4) is not ideal in *** vacancies can not only enhance the conductivities of NiFe_(2)O_(4) but also provide better adsorption of OH,which is beneficial to the electrochemical ***,oxygen vacancies engineered NiFe_(2)O_(4)(NiFe_(2)O_(4)‒δ)is obtained through a two-step method,including a hydrothermal reaction and a further heat treatment in activated carbon *** of electron paramagnetic resonance spectra indicate that more oxygen vacancies exist in the treated NiFe_(2)O_(4)‒δthan the original ***-Vis diffuse reflectance spectra prove that the treated NiFe_(2)O_(4)‒δowns better conductivity than the original NiFe_(2)O_(4).As for the electrochemical performances,the treated NiFe_(2)O_(4)‒δperforms a high specific capacitance of 808.02 F∙g^(‒1) at 1 A∙g^(‒1).Moreover,the asymmetric supercapacitor of NiFe_(2)O_(4)‒δ//active carbon displays a high energy density of 17.7 Wh∙kg^(‒1) at the power density of 375 W∙kg^(‒1).This work gives an effective way to improve the conductivity of metal oxides,which is beneficial to the application of metal oxides in supercapacitors.

关键词： nickel ferrite oxygen vacancy high conductivity supercapacitor

Three-in-one LaNiO_(3) functionalized separator boosting electrochemical stability and redox kinetics for high-performance Li-S battery

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Journal of Energy Chemistry 2023年第7期82卷 581-591,I0013页

作者： Weiyu Wang Mingxiu Hou Fangqian Han Di Yu Jie Liu Qian Zhang Fengli Yu Lei Wang Maoshuai He State key laboratory Base of Eco-chemical Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina College of Chemistry and Molecular Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina College of chemical Engineering Qingdao University of Science and TechnologyQingdao 266042ShandongChina Weifang key laboratory of Green processing of Separator for chemical Power Sources School of Chemistry and EngineeringWeifang Vocational CollegeWeifang 261108ShandongChina shandong Engineering Research Center for Marine Environment Corrosion and Safety Protection College of Environment and Safety EngineeringQingdao University of Science and TechnologyQingdao 266042ShandongChina

The lithium-sulfur(Li-S)battery,as one of the energy storage devices,has been in the limelight due to its high theoretical energy ***,the poor redox kinetics and the"shuttle effect"of polysulfides severely restrict the use of Li-S batteries in practical ***,a novel bimetallic LaNiO_(3) functional material with high electrical conductivity and catalytic property is prepared to act as a high-efficiency polysulfide shuttling *** three LaNiO_(3) samples with different physical/chemical characteristics are obtained by controlling the calcination *** conjunction with the high electrical conductivity and excellent catalytic properties of the as-prepared materials,the appropriate chemisorption toward polysulfides offers great potential to enhance electrochemical stability for highperformance Li-S ***,the Li-S cell with the separator modified by such functional material gives a specific capacity of 658 mA h g^(-1) after 500 cycles at a high current density of 2 *** with high sulfur loading of 6.05 mg cm^(-2),the Li-S battery still exhibits an areal specific capacity of 2.81 m A h cm^(-2)after 150 *** work paves a new avenue for the rational design of materials for separator modification in high-performance Li-S batteries.

关键词： Li-S battery Functional separator Catalytic property Electrochemical stability Redox kinetics

Rational design of carbon-based electrocatalysts for enhancing redox reactions in rechargeable metal batteries

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Nano Research 2023年第4期16卷 4246-4276页

作者： Song Chen Qianwu Chen Siyu Ding Yadong Tian Jun Wang Shaoqi Hou Jintao Zhang key laboratory for Colloid and Interface Chemistry(Ministry of Education) School of Chemistry and Chemical EngineeringShandong UniversityJinan 250061China key laboratory for Liquid-Solid Structural Evolution and processing of Materials(Ministry of Education) Shandong UniversityJinan 250061China Country School of Mathematical and Physical Sciences University of Technology SydneyUltimoNew South Wales 2007Australia

Exploitation of the efficient and cost-effective electrode materials is urgently desirable for the development of advanced energy *** the unique features of good electronic conductivity,structure flexibility,and desirable physicochemical property,carbon-based nanomaterials have attracted enormous research attention as efficient electrode *** and microstructure engineering of carbon-based nanomaterials are the keys to regulate the electrocatalytic properties for the specific redox reactions of advanced metal-based ***,the critical roles of carbon-based electrocatalysts for rechargeable metal batteries have not been comprehensively *** the basic introduction on the electronic and microstructure engineering strategies,we summarize the recent advances on the rational design of carbon-based electrocatalysts for the important redox reactions in various metal-air batteries and metal-halogen *** relationships between the composition,structure,and the electrocatalytic properties of carbon-based materials were well-addressed to enhance the battery *** overview of present challenges and opportunities of the carbon-based active materials for future energy-related applications was also discussed.

关键词： carbon-based nanomaterials electronic structure microstructure modulations metal-air batteries metal-halogen batteries

Hybrid hard carbon framework derived from polystyrene bearing distinct molecular crosslinking for enhanced sodium storage

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Carbon Energy 2024年第7期6卷 178-190页

作者： Yuqian Qiu Guangshen Jiang Yanxia Su Xinren Zhang Yuxuan Du Xiaosa Xu Qian Ye Jinbo Zhang Miaohan Ban Fei Xu Hongqiang Wang State key laboratory of Solidification processing Center for Nano Energy MaterialsSchool of Materials Science and EngineeringNorthwestern Polytechnical University and Shaanxi Joint Laboratory of Graphene(NPU)Xi'anChina State key laboratory of Solid Lubrication Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhouChina Shaanxi Yanchang Petroleum(Group)Co. Ltd.Dalian Institute of Chemical Physics Xi'anClean Energy(Chemical)Research InstituteXi'anChina

Exploiting high-performance yet low-cost hard carbon anodes is crucial to advancing the state-of-the-art sodium-ion ***,the achievement of superior initial Coulombic efficiency(ICE)and high Na-storage capacity via low-temperature carbonization remains challenging due to the presence of tremendous defects with few closed ***,a facile hybrid carbon framework design is proposed from the polystyrene precursor bearing distinct molecular bridges at a low pyrolysis temperature of 800℃ via in situ fusion and embedding *** is realized by integrating triazine-and carbonylcrosslinked polystyrene nanospheres during *** triazine crosslinking allows in situ fusion of spheres into layered carbon with low defects and abundant closed pores,which serves as a matrix for embedding the well-retained carbon spheres with nanopores/defects derived from carbonyl ***,the hybrid hard carbon with intimate interface showcases synergistic Na ions storage behavior,showing an ICE of 70.2%,a high capacity of 279.3 mAh g^(-1),and long-term 500 cycles,superior to carbons from the respective precursor and other reported carbons fabricated under the low carbonization *** present protocol opens new avenues toward low-cost hard carbon anode materials for high-performance sodiumion batteries.

关键词： closed pores hybrid hard carbons hypercrosslinking polystyrenes low-temperature carbonization sodium storage

Structural engineering of transition metal-based nanostructured electrocatalysts for efficient water splitting

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Frontiers of chemical Science and Engineering 2018年第4期12卷 838-854页

作者： Yueqing Wang Jintao Zhang key laboratory for Colloid and Interface Chemistry (Ministry of Education) School of Chemistry and Chemical EngineeringShandong University Jinan 250100China

Water splitting is a highly promising approach for the generation of sustainable, clean hydrogen energy. Tremendous efforts have been devoted to exploring highly efficient and abundant metal oxide electrocatalysts for oxygen evolution and hydrogen evolution reactions to lower the energy consumption in water splitting. In this review, we summarize the recent advances on the development of metal oxide electrocatalysts with special emphasis on the structural engineering of nanostructures from particle size, composition, crystalline facet, hybrid structure as well as the conductive supports. The special strategies relay on the transformation from the metal organic framework and ion exchange reactions for the preparation of novel metal oxide nanostructures with boosting the catalytic activities are also discussed. The fascinating methods would pave the way for rational design of advanced electrocatalysts for efficient water splitting.

关键词： water splitting structure engineering metal organic framework ion exchange synergistic effect hybrid structure conductive supports