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Electrocatalytic synthesis of C-N coupling compounds from CO_(2) and nitrogenous species

SusMat 2024年第2期4卷 51-74页

作者： Zheng Zhang Danyang Li Yunchuan Tu Jiao Deng Huiting Bi Yongchao Yao Yan Wang Tingshuai Li Yongsong Luo Shengjun Sun Dongdong Zheng Sónia A.C.Carabineiro Zhou Chen Junjiang Zhu Xuping Sun Hubei key laboratory of biomass Fibers and Eco-Dyeing&Finishing College of Chemistry and Chemical EngineeringWuhan Textile UniversityWuhanHubeiChina School of Chemistry and Chemical Engineering Chongqing UniversityChongqingChina i-lab Vacuum Interconnected NanotechWorkstation(Nano-X)Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhouJiangsuChina Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengduSichuanChina College of Chemistry Chemical Engineering and Materials ScienceShandong Normal UniversityJinanShandongChina LAQV-REQUIMTE Department of ChemistryNOVA School of Science and TechnologyUniversidade NOVA de Lisboa2829-516 CaparicaPortugal College of materials Xiamen UniversityXiamenFujianChina

The electrocatalytic synthesis of C-N coupling compounds from CO_(2) and nitrogenous species not only offers an effective avenue to achieve carbon neutral-ity and reduce environmental pollution,but also establishes a route to synthesize valuable chemicals,such as urea,amide,and amine.This innovative approach expands the application range and product categories beyond simple carbona-ceous species in electrocatalytic CO_(2) reduction,which is becoming a rapidly advancing field.This review summarizes the research progress in electrocatalytic urea synthesis,using N_(2),NO_(2)^(-),and NO_(3)^(-)as nitrogenous species,and explores emerging trends in the electrosynthesis of amide and amine from CO_(2) and nitro-gen species.Additionally,the future opportunities in this field are highlighted,including electrosynthesis of amino acids and other compounds containing C-N bonds,anodic C-N coupling reactions beyond water oxidation,and the catalytic mechanism of corresponding reactions.This critical review also captures the insights aimed at accelerating the development of electrochemical C-N coupling reactions,confirming the superiority of this electrochemical method over the traditional techniques.

关键词： C-N coupling CO_(2) reduction electrocatalysis nitrogenous species reaction mechanism

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Modulating p-type doping of two-dimensional material palladium diselenide

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Nano Research 2024年第4期17卷 3232-3244页

作者： Jiali Yang Yu Liu En-Yang Wang Jinbo Pang Shirong Huang Thomas Gemming Jinshun Bi Alicja Bachmatiuk Hao Jia Shu-Xian Hu Chongyun Jiang Hong Liu Gianaurelio Cuniberti Weijia Zhou Mark H Rümmeli Institute for Advanced Interdisciplinary Research(iAIR) University of JinanJinan 250022China Institute for materials Chemistry Leibniz Institute for Solid State and Materials Research Dresden(IFW Dresden)20 Helmholtz StrasseDresden 01069Germany State key lab of Transducer Technology Shanghai Institute of Microsystem and Information TechnologyChinese Academy of SciencesShanghai 200050China College of energy Soochow Institute for Energy and Materials Innovations Soochow UniversitySuzhou 215006China key laboratory of Advanced Carbon materials and Wearable energy Technologies of Jiangsu Province Soochow UniversitySuzhou 215006China School of Integrated Circuits University of Chinese Academy of SciencesBeijing 101408China Institute of Microelectronics of Tianjin Binhai New Area Tianjin 300451China Institute of Microelectronics Chinese Academy of SciencesBeijing 100029China Lukasiewicz Research Network PORT Polish Center for Technology DevelopmentStablowicka 147Wroclaw 54-066Poland School of Mathematics and Physics University of Science and Technology BeijingBeijing 100083China College of electronic information and optical engineering Nankai UniversityTianjin 300350China Centre of Polymer and Carbon materials Polish Academy of SciencesM.Curie Sklodowskiej 34Zabrze 41-819Poland Center for energy and Environmental Technologies VŠB-Technical University of Ostrava17.Listopadu 15Ostrava 70833Czech Republic State key laboratory of Crystal materials Center of Bio&Micro/Nano Functional MaterialsShandong UniversityJinan 250100China Dresden Center for Computational materials Science Technische Universität DresdenDresden 01062Germany Dresden Center for Intelligent materials(GCL DCIM) Technische Universität DresdenDresden 01062Germany Institute for materials Science and Max Bergmann Center of Biomaterials Technische Universität DresdenDresden 01069Germany Center for Advancing Electronics Dresden Technische Universität DresdenDresden 01069Germany

The van der Waals heterostructures have evolved as novel materials for complementing the Si-based semiconductor technologies.Group-10 noble metal dichalcogenides(e.g.,PtS_(2),PtSe_(2),PdS_(2),and PdSe_(2))have been listed into two-dimensional(2D)materials toolkit to assemble van der Waals heterostructures.Among them,PdSe_(2) demonstrates advantages of high stability in air,high mobility,and wide tunable bandgap.However,the regulation of p-type doping of PdSe_(2) remains unsolved problem prior to fabricating p–n junction as a fundamental platform of semiconductor physics.Besides,a quantitative method for the controllable doping of PdSe_(2) is yet to be reported.In this study,the doping level of PdSe_(2) was correlated with the concentration of Lewis acids,for example,SnCl_(4),used for soaking.Considering the transfer characteristics,the threshold voltage(the gate voltage corresponding to the minimum drain current)increased after SnCl_(4) soaking treatment.PdSe_(2) transistors were soaked in SnCl_(4) solutions with five different concentrations.The threshold voltages from the as-obtained transfer curves were extracted for linear fitting to the threshold voltage versus doping concentration correlation equation.This study provides in-depth insights into the controllable p-type doping of PdSe_(2).It may also push forward the research of the regulation of conductivity behaviors of 2D materials.

关键词： two-dimensional(2D)materials Lewis acid treatment p-type doping field-effect transistors transfer characteristic

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Absorption properties and mechanism of lightweight and broadband electromagnetic wave-absorbing porous carbon by the swelling treatment

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International Journal of Minerals,Metallurgy and materials 2024年第7期31卷 1701-1712页

作者： Jianghao Wen Di Lan Yiqun Wang Lianggui Ren Ailing Feng Zirui Jia Guanglei Wu College of materials and Chemistry&Chemical Engineering Chengdu University of TechnologyChengdu 610059China School of materials Science and Engineering Hubei University of Automotive TechnologyShiyan 442002China Institute of materials for energy and Environment State Key Laboratory of Bio-fibers and Eco-textilesCollege of Materials Science and EngineeringQingdao UniversityQingdao 266071China Institute of Physics&Optoelectronics Technology Baoji University of Arts and SciencesBaoji 721016China

Bioderived carbon materials have garnered considerable interest in the fields of microwave absorption and shielding due to their reproducibility and environmental friendliness.In this study,KOH was evenly distributed on biomass Tremella using the swelling induction method,leading to the preparation of a three-dimensional network-structured hierarchical porous carbon(HPC)through carbonization.The achieved microwave absorption intensity is robust at-47.34 dB with a thin thickness of 2.1 mm.Notably,the widest effective absorption bandwidth,reaching 7.0 GHz(11–18 GHz),is attained at a matching thickness of 2.2 mm.The exceptional broadband and reflection loss performance are attributed to the 3D porous networks,interface effects,carbon network defects,and dipole relaxation.HPC has outstanding absorption characteristics due to its excellent impedance matching and high attenuation constant.The uniform pore structures considerably optimize the impedance-matching performance of the material,while the abundance of interfaces and defects enhances the dielectric loss,thereby improving the attenuation constant.Furthermore,the impact of carbonization temperature and swelling rate on microwave absorption performance was systematically investigated.This research presents a strategy for preparing absorbing materials using biomass-derived HPC,showcasing considerable potential in the field of electromagnetic wave absorption.

关键词： biomass hierarchical porous carbon dielectric loss electromagnetic wave absorption

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Multi-Objective Optimization Based on Life Cycle Assessment for Hybrid Solar and biomass Combined Cooling,Heating and Power System

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Journal of Thermal Science 2024年第3期33卷 931-950页

作者： LIU Jiejie LI Yao MENG Xianyang WU Jiangtao key laboratory of Thermo-Fluid Science and Engineering Ministry of EducationXi’an Jiaotong UniversityXi’an710049China

The complementary of biomass and solar energy in combined cooling,heating and power(CCHP)system provides an efficient solution to address the energy crisis and environmental pollutants.This work aims to propose a multi-objective optimization model based on the life cycle assessment(LCA)method for the optimal design of hybrid solar and biomass system.The life-cycle process of the poly-generation system is divided into six phases to analyze energy consumption and greenhouse gas emissions.The comprehensive performances of the hybrid system are optimized by incorporating the evaluation criteria,including environmental impact in the whole life cycle,renewable energy contribution and economic benefit.The non-dominated sorting genetic algorithmⅡ(NSGA-Ⅱ)with the technique for order preference by similarity to ideal solution(TOPSIS)method is employed to search the Pareto frontier result and thereby achieve optimal performance.The developed optimization methodology is used for a case study in an industrial park.The results indicate that the best performance from the optimized hybrid system is reached with the environmental impact load reduction rate(EILRR)of 46.03%,renewable energy contribution proportion(RECP)of 92.73%and annual total cost saving rate(ATCSR)of35.75%,respectively.By comparing pollutant-eq emissions of different stages,the operation phase emits the largest pollutant followed by the phase of raw material acquisition.Overall,this study reveals that the proposed multi-objective optimization model integrated with LCA method delivers an alternative path for the design and optimization of more sustainable CCHP system.

关键词： combined cooling heating and power system solar-biomass multi-objective optimization life cycle assessment optimal design

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Base-free oxidative esterification of 5-hydroxymethylfurfural to furan-2,5-dimethylcarboxylate over n-doped carbon-supported Co/Fe bimetallic catalyst under batch-operation or continuous-flow conditions

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Journal of energy Chemistry 2022年第12期75卷 95-108,I0004页

作者： Weizhen Xie Binglin Chen Wenlong Jia Huai Liu Zheng Li Shuliang Yang Xing Tang Xianhai Zeng Yong Sun Xixian Ke Tianyuan Li Huayu Fang Lu Lin Xiamen key laboratory of Clean and High-valued Applications for biomass Fujian Engineering and Research Center of Clean and High-valued Technologies for BiomassCollege of EnergyXiamen UniversityXiamen 361102FujianChina biomassChem Group Faculty of Chemical EngineeringKunming University of Science and TechnologyKunming 650500YunnanChina key lab for Sport Shoes Upper materials of Fujian Province Fujian Engineering and Research Center for New Functional Fiber Materials(Fujian Huafeng New Material Co.Ltd.Putian Dakai New Material Co.Ltd.)Putian 351144FujianChina

Developing an efficient and easily available catalyst for the selective conversion of biomass-derived 5-hydroxymethylfurfural(HMF)into furan-2,5-dimethylcarboxylate(FDMC),a valuable biomass-based monomer,remains a high demand but formidable challenge.Herein,a facile strategy for the synthesis of N-doped carbon-supported Co/Fe bimetallic catalyst(CoFe-NC)was developed,which provided an outstanding FDMC yield of 93%in a batch reactor(base-free,80℃,2 bar O_(2),4 h).Interestingly,CoFe-NC also gave a high FDMC yield of 91%under continuous-flow conditions for 80 h(5 bar O_(2),80℃,GHSV 1320 h^(-1),LHSV 0.6 h^(-1),base-free).Notably,it is the first time that a non-noble catalyst gave such a high FDMC yield under continuous-flow conditions.The introduction of Fe could greatly improve both the electron intensity of Co-N_(x)species and basicity of the catalyst,which endowed CoFe-NC with improved O_(2)activation capacity and enhanced dehydrogenation activity for the oxidation-esterification of HMF.This work delineates the efficient strategy on the construction of N-doped carbon-supported non-noble catalyst,which might open a new avenue for developing highly efficient catalyst for FDMC production.

关键词： 5-Hydroxymethylfurfural Furan-2,5-dimethylcarboxylate Oxidation-esterification Catalysis Co-N_(x)sites

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Laser-assisted grinding of RB-SiC composites:Laser ablation behavior and mechanism

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Chinese Journal of Aeronautics 2024年第1期37卷 362-376页

作者： Zhigang DONG Wenchao SUN Xintong CAI Feng YANG Yan BAO Renke KANG Dongjiang WU Guangyi MA Fangyong NIU key laboratory for Precision and Non-traditional Machining Technology of the Ministry of Education School of Mechanical EngineeringDalian University of TechnologyDalian 116024China

Laser ablation is an important process during Laser-Assisted Grinding(LAG)of hard and brittle materials.To realize controllable material removal during laser ablation of RB-SiC composites,ablation experiments under different Laser energy Density(LAED)and LAG experiments are conducted.Evolution rules and mechanism of physical phase,ablation morphology and crack characteristics caused by laser irradiation are investigated.The forces of LAG and Conventional Grinding(CG)are compared.The results show that ablation surface changes from slight oxidation to obvious material removal with LAED increasing,and ablation depth increases gradually.The ablation products change from submicron SiO_(2)particles to nanoscale particles and floccule.High LAED promotes SiC decomposition and sublimation,which leads to the increase of C element.The SiC phase forms corrugated shape in recast layer and columnar shape in Heat Affected Zone(HAZ)at 56 J/mm^(2).The cold and heat cycle leads to formation of fishbone crack.For ablation specimen under 30 J/mm^(2),the grinding force can be reduced by a maximum of 39%and brittle damage region is reduced.The material removal and microcrack generated will significantly reduce the hardness and improve machinability,which can promote grinding efficiency.

关键词： RB-SiC Laser Ceramic Composites Grinding

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Towards carbon neutrality of calcium carbide-based acetylene production with sustainable biomass resources

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Green energy & Environment 2024年第6期9卷 1068-1078页

作者： Peng Jiang Guanhan Zhao Hao Zhang Tuo Ji Liwen Mu Xiaohua Lu Jiahua Zhu State key laboratory of materials-oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing211816China

Acetylene is produced from the reaction between calcium carbide(CaC_(2))and water,while the production of CaC_(2) generates significant amount of carbon dioxide not only because it is an energy-intensive process but also the raw material for CaC_(2) synthesis is from coal.Here,a comprehensive biomass-to-acetylene process was constructed that integrated several units including biomass pyrolysis,oxygen-thermal CaC_(2) fabrication and calcium looping.For comparison,a coal-to-acetylene process was also established by using coal as feedstock.The carbon efficiency,energy efficiency and environmental impacts of the bio-based calcium carbide acetylene(BCCA)and coal-based calcium carbide acetylene(CCCA)processes were systematically analyzed.Moreover,the environmental impacts were further evaluated by applying thermal integration at system level and energy substitution in CaC_(2) furnace.Even though the BCCA process showed lower carbon efficiency and energy efficiency than that of the CCCA process,life cycle assessment demonstrated the BCCA(1.873 kgCO_(2eq) kg-prod^(-1))a lower carbon footprint process which is 0.366 kgCO_(2eq) kg-prod^(-1) lower compared to the CCCA process.With sustainable energy(biomass power)substitution in CaC_(2) furnace,an even lower GWP value of 1.377 kgCO_(2eq) kg-prod^(-1) can be achieved in BCCA process.This work performed a systematic analysis on integrating biomass into industrial acetylene production,and revealed the positive role of biomass as raw material(carbon)and energy supplier.

关键词： biomass pyrolysis CO_(2)mitigation Calcium carbide Acetylene Calcium loop

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Catalyst design strategy toward the efficient heterogeneously-catalyzed selective oxidation of 5-hydroxymethylfurfural

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Green energy & Environment 2022年第5期7卷 900-932页

作者： Huai Liu Xing Tang Xianhai Zeng Yong Sun Xixian Ke Tianyuan Li Jiaren Zhang Lu Lin biomassChem Group Faculty of Chemical EngineeringKunming University of Science and TechnologyKunming650500China Xiamen key laboratory of Clean and High-valued Utilization for biomass College of EnergyXiamen UniversityXiamen361102China Fujian Engineering and Research Center of Clean and High-valued Technologies for biomass Xiamen UniversityXiamen361005China key lab for Sport Shoes Upper materials of Fujian Province(Fujian Huafeng New material Co. Ltd.)Putian351144China PetroChina Petrochemical Research Institute Beijing102206China

The selective oxidation of 5-hydroxymethylfurfural(HMF),a versatile bio-based platform molecule,leads to the formation of several intriguing and useful downstream chemicals,such as 2,5-diformylfuran(DFF),5-hydroxymethyl-2-furancarboxylic acid(HMFCA),formyl 2-furancarboxylic acid(FFCA),2,5-furandicarboxylic acid(FDCA) and furan-2,5-dimethylcarboxylate(FDMC).These products have been extensively employed to fabricate novel polymers,pharmaceuticals,sustainable dyes and many other value-added fine chemicals.The heart of the developed HMF oxidation processes is always the catalyst.In this regard,this review comprehensively summarized the established heterogeneous catalyst design strategy for the selective oxidation of HMF via thermo-catalysis.Particular attention has been focused on the reaction mechanism of HMF oxidation over different catalysts as well as enhancing the catalytic performance of the catalyst through manipulating the properties of the support and fabricating of multi-component metal nano-particles and oxides.The current challenges and possible research directions for the catalytic oxidation of HMF in the future are also discussed.

关键词： hydroxymethyl catalyst catalyzed

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Facile Synthesis and Crystal Structure of a Novel Cyanopyridine

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Chinese Journal of Structural Chemistry 2011年第7期30卷 1011-1015页

作者：杨晓慧刘承果周永红崔竞方林小羽 Institute of Chemical Industry of Forestry Products CAF National Engineering lab.for biomass Chemical Utilization key and lab.on Forest Chemical Engineering SFA key lab.of biomass energy and material

The title compound 2-amino-4-（4-hydroxy-3,5-dimethoxyphenyl）-5-methyl-6- phenyl nicotinonitrile, C21H19N3O3, was synthesized via four-component reactions between propiophenone, malononitrile, syringaldehyde and ammonium acetate in ethanol under reflux without catalyst and characterized by IR, 1H NMR, 13C NMR, MS, EA and single-crystal X-ray diffraction. Single-crystal X-ray diffraction analysis shows that the compound is of monoclinic system, space group P21/n with a = 8.4600（17）, b = 17.139（3）, c = 13.408（3） A, β= 107.06（3）°, V= 1858.6（6） A3, Z = 4, Mr = 361.39, F（000） = 760, μ（MoKa） = 0.088 mm^-1 Dc = 1.292 g/cm3, 2 = 0.71073 A, the final R = 0.0751 and wR = 0.0938 for 3333 observed reflections with I〉 2σ（I）. The crystal packing of the title compound is stabilized by intermolecular hydrogen bonds.

关键词： cyanopyridine synthesis crystal structure multi-component reactions

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Bimetallic active site nuclear-shell heterostructure enables efficient dual-functional electrocatalysis in alkaline media

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稀有金属:英文版 2023年第9期42卷 3024-3033页

作者： Yu Cheng Xi Zhou Qin-Min Pan Li-Fang Zhang Yu-Feng Cao Tao Qian School of Chemistry and Chemical Engineering Nantong UniversityNantong226019China Institute of Chemical Industry of Forestry Products Chinese Academy of ForestryKey Lab.of Biomass Energy and MaterialNanjing210000China School of Chemical and Environmental Engineering College of ChemistryChemical Engineering and Material ScienceSoochow UniversitySuzhou215123China Department of Chemical Engineering University of WaterlooWaterlooONN2L 3G1Canada

Hydrogen,as a green and clean next-generation fuel,is a key to achieving the goal of carbon neutrality.Constructing an electrocatalyst with bifunctional hydrogen evolution and oxygen evolution activity in the same electrolyte is a key technology for producing hydrogen via water splitting.Herein,a bimetallic active site catalyst,which possessed an edge-riched MoS_(2)nanoflakes array vertically growing on cubic CoS_(2),forming a nuclear-shell heterogeneous configuration,termed CSC-Mo S_(2)@Co S_(2).was reported The optimal CSC-Mo S_(2)@Co S_(2)-24 possessed good dualfunctional electrocatalytic activity(hydrogen evolution(HER),10 m A·cm^(-2)@241.5 m V and oxygen evolution(OER),10 m A·cm^(-2)@350 m V).Especially,CSC-Mo S_(2)@CoS_(2)-24 exhibited an extremely high mass activity for HER,and only required an overpotential of~550 m V when reaching a large current density of 1422 m A·mg^(-1),which was20.6-fold that of the bulk CoS_(2)(69 m A·mg^(-1)),as well as exhibiting stability of up to 100 h.The good electrocatalytic performance was attributed to the nuclear-shell heterostructure of Mo S_(2)@CoS_(2)hybrid could bring critical synergies,improving efficient mass transfer and electron transfer processes between Co S_(2)and Mo S_(2),which collaboratively promoted the electrocatalytic kinetics.It is foreseeable that the method proposed in this work will have guiding value for the preparation of dual-functional electrocatalysts with multi-interface heterostructures by assembling layered sulfides on cubic sulfides.

关键词： Dual-functional electrocatalysts Nuclearshell cubic heterostructure Edge-riched Bimetallic active site Strong interaction

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