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Biomass-based production of trimellitic and trimesic acids

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Green Energy & Environment 2024年第8期9卷 1267-1278页

作者： Lin Yuan Yancheng Hu Guangyi Li Fengan Han Aiqin Wang Yu Cong Tao Zhang Feng Wang Ning Li CAS Key Laboratory of Science and technology on Applied Catalysis Dalian Institute of Chemical PhysicsChinese Academy of Sciences university of Chinese Academy of Sciences 19 A Yuquan RoadShijingshan District School of chemical Engineering and technology China University of Mining and Technology State Key Laboratory of Catalysis Dalian National Laboratory for Clean EnergyDalian Institute of Chemical PhysicsChinese Academy of Sciences

The production of industrial chemicals with renewable biomass feedstock holds potential to aid the world in pursuing a carbon-neutral *** and trimesic acids are important commodity chemicals in industry that are prepared by the oxidation of petroleum-derived *** reduce the dependence on the limited oil source,we develop a potential sustainable alternative towards trimellitic and trimesic acids using biomass-based 2-methyl-2,4-pentandiol （MPD）,acrylate and crotonaldehyde as starting *** process for trimellitic acid includes dehydration/D-A reaction of MPD and acrylate,flow aromatization over Pd/C catalyst,hydrolysis and catalytic aerobic oxidation （60%overall yield）.The challenging regioselectivity issue of D-A reaction is tackled by a matched combination of temperature and deep eutectic solvent ChCl/*** can also participate in the reaction,followed by Pd/C-catalyzed decarbonylation/dehydrogenation and oxidation to provide trimesic acid in 54%overall *** cycle assessment implies that compared to conventional fossil process,our biomass-based routes present a potential in reducing carbon emissions.

关键词： Biomass Trimellitic acid Trimesic acid Deep eutectic solvent Dehydration/D-A reaction

Enhanced electrocatalytic CO_(2)reduction to formic acid using nanocomposites of In_(2)O_(3)@C with graphene

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Nano Research 2024年第6期17卷 5031-5039页

作者： Wenxiang Li Shuo Gao Chuanruo Yang Juntao Yang Amjad Nisar Guolei Xiang Junsu Jin Beijing Key Laboratory of Membrane Science and technology Beijing University of Chemical TechnologyBeijing 100029China Nanomaterials Research Group PDPINSTECHIslamabad 44000Pakistan institute of Industrial Chemistry College of ChemistryBeijing University of Chemical TechnologyBeijing 100029China

In_(2)O_(3)is an effective electrocatalyst to convert CO_(2)to formic acid(HCOOH),but its inherent poor electrical conductivity limits the efficient charge transfer during the ***,the tendency of In_(2)O_(3)particles to agglomerate during synthesis further limits the exposure of active *** we address these issues by leveraging the template effect of graphene oxide and employing InBDC as a self-sacrificing template for the pyrolysis synthesis of In_(2)O_(3)@*** resulting In_(2)O_(3)@C/rGO-600 material features In_(2)O_(3)@C nanocubes uniformly anchored on a support of reduced graphene oxide(rGO),significantly enhancing the active sites *** conductive rGO network facilitates charge transfer during electrocatalysis,and the presence of oxygen vacancies generated during pyrolysis,combined with the strong electron-donating ability of rGO,enhances the adsorption and activation of CO_(2).In performance evaluation,In_(2)O_(3)@C/rGO-600 exhibits a remarkable HCOOH Faradaic efficiency exceeding 94.0%over a broad potential window of−0.7 to−1.0 V(*** hydrogen electrode(RHE)),with the highest value of 97.9%at−0.9 V(***)in a ***,the material demonstrates an excellent cathodic energy efficiency of 71.6%at−0.7 V(***).The study underscores the efficacy of uniformly anchoring metal oxide nanoparticles onto rGO for enhancing the electrocatalytic CO_(2)reduction performance of materials.

关键词： In_(2)O_(3)@C nanocomposite electrochemical CO_(2)reduction reduced graphene oxide oxygen vacancy

Design method of extractant for liquid-liquid extraction based on elements and chemical bonds

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Chinese Journal of chemical Engineering 2024年第4期68卷 193-202页

作者： Yuwen Wei Chunling Zhang Yue Zhang Lili Wang Li Xia Xiaoyan Sun Shuguang Xiang institute of Process System Engineering College of Chemical EngineeringQingdao University of Science and TechnologyQingdao 266042China Yantai Guobang chemical Machinery technology Co. Ltd.Yantai 264002China

In the petrochemical industry process, the relative volatility between the components to be separated is close to one or the azeotrope that systems are difficult to separate. Liquid-liquid extraction is a common and effective separation method, and selecting an extraction agent is the key to extraction technology research. In this paper, a design method of extractants based on elements and chemical bonds was proposed. A knowledge-based molecular design method was adopted to pre-select elements and chemical bond groups. The molecules were automatically synthesized according to specific combination rules to avoid the problem of “combination explosion” of molecules. The target properties of the extractant were set, and the extractant meeting the requirements was selected by predicting the correlation physical properties of the generated molecules. Based on the separation performance of the extractant in liquid-liquid extraction and the relative importance of each index, the fuzzy comprehensive evaluation membership function was established, the analytic hierarchy process determined the mass ratio of each index, and the consistency test results were passed. The results of case study based on quantum chemical analysis demonstrated that effective determination of extractants for the analysis of benzene-cyclohexane systems. The results unanimously prove that the method has important theoretical significance and application value.

关键词： Molecular design Element and chemical bonds Molecular simulation Thermodynamics Solvent extraction

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Preparation of bifunctional electrocatalyst by recycling heavy metal ions from wastewater using EDTAD-functionalized MOF as highly efficient adsorbent

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Rare Metals 2024年第10期43卷 5105-5116页

作者： Yue Qian Pei-Xue Fu Rui-Ze Yin Han-Ni Yang Si-Yang Li Wei-Wei Xiong Fen-Fen Zheng Jun-Hao Zhang Ai-Hua Yuan Huan Pang School of Environmental and chemical Engineering Jiangsu University of Science and Technology School of Chemistry and chemical Engineering Yangzhou University

The recovery and subsequent reuse of heavy metal ions from industrial wastewater are crucial for promoting sustainable development,but they also presen significant *** this article,ethylenediaminetetraacetic dianhydride （EDTAD）,which possesses strong metal chelating ability,is covalently attached to MIL-101-NH2（Fe）,resulting in a significant improvement in the removal rate of heavy metal ions in ***,the recovered waste metal ions are transformed into high-performance FeNi3/NiFe2O4@NC dual-functional oxygen evolution reaction （OER） and oxygen reduction reaction （ORR） ***,FeNi3/NiFe2O4@NC exhibits outstanding OER performance,with only a264 mV overpotential at 10 mA·*** functiona theory （DFT） calculations reveal that the synergistic effect of the FeNi3/NiFe2O4@NC heterostructure can enhance conductivity,optimize the free energy of*to OH*during OER reaction,and promote catalytic *** work not only improves the removal rate of heavy metal ions but also obtains high-performance catalysts,while providing a new approach for the treatment and secondary utilization of heavy metal ion wastewater as well as the preparation of low-cost catalysts.

关键词： Bifunctional electrocatalyst Covalently modified MOF Ethylenediaminetetraacetic dianhydride Heavy metals

Hydrogen-bonded organic framework modified separator for simultaneously enhancing the safety and electrochemical performance of Ni-rich lithium-ion battery

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Journal of Energy Chemistry 2024年第9期96卷 72-78页

作者： Chengyu Han Yu Cao Ming Yang Yuhan Wang Di Tang Shaojie Zhang Yiran Jia Yiming Zhang Hern Kim Fusheng Pan Zhongyi Jiang Jie Sun Key Laboratory for Green chemical technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Science and technology on Power Sources Laboratory Tianjin Institute of Power SourcesTianjin 300384China Haihe Laboratory of Sustainable chemical Transformations Tianjin 300192China Quzhou institute for Innovation in Resource chemical Engineering Quzhou 324000ZhejiangChina Department of Energy Science and technology Director Environmental Waste Recycle InstituteYongin 17058Republic of Korea School of Chemistry and chemical Engineering Hainan UniversityHaikou 570228HainanChina

Nickel-rich layered oxide cathode(LiNi_(x)Co_(y)Mn_(1−x−y)O_(2),x>0.5,NCM)shows substantial potential for applications in longer-range electrical ***,the rapid capacity decay and serious safety concerns impede its practical *** work provides a hydrogen-bonded organic framework(HOF)modification strategy to simultaneously improve the electrochemical performance,thermal stability and incombustibility of *** cyanurate(MCA),as a low-cost and reliable flame-retardant HOF,was implemented in the separator modification layer,which can prevent the battery short circuit even at a high *** addition,the supermolecule properties of MCA provide unique physical and chemical microenvironment for regulating ion-transport behavior in *** MCA coating layer enabled the nickel-rich layered oxide cathode with a high-capacity retention of 90.3%after 300 cycles at 1.0 ***,the usage of MCA in lithium-ion batteries(LIBs)affords a simple,low-cost and efficient strategy to improve the security and service life of nickel-rich layered cathodes.

关键词： Hydrogen-bonded organic framework Modified separator Ni-richlayered oxide cathode Thermal runaway Li^(+)transference number

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NiO@Ni nanoparticles embedded in N-doped carbon for efficient photothermal CO_(2) methanation coupled with H_(2)O splitting

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Nano Research 2024年第4期17卷 2283-2290页

作者： Yun Zhou Peng Zheng Fang Wang Fangna Gu Wenqing Xu Qinyang Lu Tingyu Zhu Ziyi Zhong Guangwen Xu Fabing Su institute of Process Engineering Chinese Academy of SciencesBeijing 100190China Key Laboratory on Resources chemicals and Materials of Ministry of Education Shenyang University of Chemical TechnologyShenyang 110142China institute of Industrial Chemistry and Energy technology Shenyang University of Chemical TechnologyShenyang 110142China School of Ecology and Environment Beijing Technology and Business UniversityBeijing 100048China Beijing Key Laboratory of Enze Biomass Fine chemicals College of New Materials and Chemical EngineeringBeijing Institute of Petrochemical TechnologyBeijing 102617China International School of Beijing 10 An Hua Street Shunyi DistrictBeijing 100048China Department of chemical Engineering Guangdong Technion Israel Institute of Technology(GTIIT)Shantou 515063China Technion Israel institute of technology(IIT) Haifa32000Israel

Photothermal carbon dioxide(CO_(2))methanation has attracted increasing interest in solar fuel synthesis,which employs the advantages of photocatalytic H_(2)O splitting as a hydrogen source and photothermal catalytic CO_(2) *** work prepared three-dimensional(3D)honeycomb N-doped carbon(NC)loaded with core–shell NiO@Ni nanoparticles generated in situ at 500℃(NiO@Ni/NC-500).Under the photothermal catalysis(200℃,1.5 W/cm^(2)),the CH_(4) evolution rate of NiO@Ni/NC-500 reached 5.5 mmol/(g·h),which is much higher than that of the photocatalysis(0.8 mmol/(g·h))and the thermal catalysis(3.7 mmol/(g·h)).It is found that the generated localized surface plasmon resonance enhances the injection of hot electrons from Ni to NiO,while thermal heating accelerates the thermal motion of radicals,thus generating a strong photo-thermal synergistic effect on the *** CO_(2) reduction to CH_(4) follows the*OCH *** work demonstrates the synergistic effect of NiO@Ni and NC can enhance the catalytic performance of photothermal CO_(2) reduction reaction coupled with water splitting reaction.

关键词： Ni localized surface plasmon resonance photothermal methanation

Electrocatalytic coupling of anodic nitrogen oxidation and cathodic nitrate reduction for ammonia synthesis from air and water

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Nano Research 2024年第9期17卷 7824-7829页

作者： Aijing Ma Jianzhou Gui Yanmei Huang Yifu Yu State Key Laboratory of Separation Membranes and Membrane Processes Tianjin Key Laboratory of Green Chemical Technology and Process EngineeringSchool of Chemical Engineering and TechnologyTiangong UniversityTianjin 300387China institute of Molecular Plus School of Chemical EngineeringTianjin UniversityTianjin 300072China

Ammonia plays a vital role in present agriculture and industry,and is also regarded as a next-generation clean energy *** development of electrocatalysis raises an opportunity to make ammonia synthesis compatible with intermittent and variable renewable energy sources such as solar and wind ***,the direct ammonia electrosynthesis from N_(2)reduction is still challenging due to the much easier hydrogen evolution competition *** this perspective,we propose a novel strategy for ammonia electrosynthesis from air and water based on the coupling of anodic nitrogen oxidation and cathodic nitrate *** methods for breaking the bottlenecks of anodic nitrogen oxidation and cathodic nitrate reduction are discussed *** that,key issues that need to be considered in the coupled system are proposed for the application of this strategy.

关键词： electrocatalysis nitrogen oxidation nitrate reduction nitrogen fixation ammonia synthesis

A review of ultra-high temperature heat-resistant energetic materials

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Defence technology（防务技术） 2024年第8期38卷 33-57页

作者： Rongzheng Zhang Yuangang Xu Feng Yang Pengcheng Wang Qiuhan Lin Hui Huang Ming Lu School of Chemistry and chemical Engineering Nanjing University of Science and TechnologyNanjing 210094China institute of chemical Materials China Academy of Engineering PhysicsMianyang 621900China

Heat-resistant energetic materials refer to a type of energetic materials that possess a high melting point,high stability and operational safety. By studying the structures of these energetic materials has showed that the thermal stability can be enhanced by introducing amino groups to form intra/inter-molecular hydrogen bonds, constructing conjugate systems and designing symmetrical structures. This article aims to review the physical and chemical properties of ultra-high temperature heat-resistant energetic compounds and provide valuable theoretical insights for the preparation of ultra-high temperature heatresistant energetic materials. We also analyze the selected 20 heat-resistant energetic materials with decomposition temperatures higher than 350℃, serving as templates for the synthesis of various highperformance heat-resistant energetic materials.

关键词： Heat-resistant energetic materials Organic synthesis Conjugated Hydrogen bond Symmetrical structure Stabilization

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Propylene epoxidation coupled with furfural oxidation over Pt(Ⅱ?) TPP porphyrin with molecular oxygen

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Green chemical Engineering 2024年第4期5卷 519-525页

作者： Hong-Qi Li Hai-Yang Yu Yang Li Xiao-Qi He Xian-Tai Zhou Huizhou Research institute Sun Yat-sen University School of chemical Engineering and technology Sun Yat-sen University

The development of green route for preparing propylene oxide (PO) with molecular oxygen is of significance both in academic and industrial. In this work, propylene epoxidation coupled with furfural oxidation catalyzed by platinum meso-tetraphenylporphyrin (Pt (II)TPP) has been developed. Propylene conversion and PO selectivity reached up to 56%and 83%, respectively. Meanwhile, furfural was almost completely converted to furoic *** on operando characterizations and electron paramagnetic resonance (EPR) tests, a mechanism involved high-valent Pt species was proposed. This work is expected to provide a potential application prospects for producing PO and furoic acid simultaneously in chemical industry.

关键词： Propylene Epoxidation Molecular oxygen Furfural Platinum porphyrins