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Hydrodechlorination of trifluoro-trichloroethane to chlorotrifluoroethylene:Revealing the deactivation mechanism and regeneration strategy of Pd-Cu/AC catalyst

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Chinese Journal of Chemical Engineering 2024年第6期70卷 261-268页

作者： Song Tian Yicheng Chen Xiaoyu Wen Bingcheng Li Jian Lu Zile Li Feng Feng Qingtao Wang Qunfeng Zhang Xiaonian Li state key laboratory breeding base of green chemistry synthesis technology Institute of Industrial Catalysis of Zhejiang University of TechnologyHangzhou 310014China state key laboratory of Fluorine&Nitrogen Chemicals Xi'an Modern Chemistry Research InstituteXi'an 710065China

Chlorotrifluoroethylene(CTFE)is a vital fluorinated olefinic monomer produced through the catalytic hydrodechlorination of trichlorotrifluoroethane(CFC-113),an eco-friendly ***,hydrodechlorination catalysts for olefin production often suffer from poor *** Pd/AC catalyst and Pd-Cu/AC catalyst prepared by co-impregnation method exhibited poor stability,Pd-Cu/AC catalyst with CFC-113 conversion dropping to around 37%after 50 h of hydrodechlorination ***-Emmett-Teller,transmission electron microscopy,X-ray photoelectron spectroscopy,and X-ray diffraction of fresh and deactivated Pd/AC catalysts indicate that the deactivation of Pd/AC catalysts is due to high-temperature agglomeration of *** analysis of fresh and deactivated Pd-Cu/AC catalysts using Brunauer-Emmett-Teller,transmission electron microscopy,and thermogravimetric analysis techniques revealed decreased dispersion of active sites,reduced surface area,catalyst aggregation deactivation,and a significant decrease in Cu ***,the results of NH3-TPD revealed that the acid sites of the catalyst increased significantly.X-ray diffraction spectra indicated the formation of new species,basic copper chloride(Cu_(2)(OH)_(3)Cl),during the *** the reaction progressed,these new species agglomerated,leading to a gradual loss of catalyst ***,the deactivated catalyst was successfully reactivated using a simple alkaline washing method.

关键词： CFC-113 Hydrodechlorination Chlorotrifluoroethylene Catalyst deactivation

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Visible-light photoredox-catalyzed carboxylation of aryl epoxides with CO_(2)

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Chinese Chemical Letters 2024年第7期35卷 281-284页

作者： Tian-Yu Gao Xiao-Yan Mo Shu-Rong Zhang Yuan-Xu Jiang Shu-Ping Luo Jian-Heng Ye Da-Gang Yu key laboratory of green chemistry&technology of Ministry of Education College of ChemistrySichuan UniversityChengdu 610064China state key laboratory breeding base of green chemistry-synthesis technology Zhejiang University of TechnologyHangzhou 310014China state key laboratory of Elemento-Organic chemistry Nankai UniversityTianjin 300071China

Herein, we report the first visible-light photoredox-catalyzed carboxylation of aryl epoxides with CO_(2)to synthesize hydroxy acid derivatives. A variety of valuable β-, γ-, δ-, ε–hydroxy acid derivatives are obtained in moderate to high yields under mild conditions. This protocol shows noteworthy functionalgroup compatibility, high chemo-and regioselectivities under transition-metal-free conditions with an inexpensive organo-dye as photosensitizer. Mechanistic studies indicate that the benzylic carbanion is generated as an intermediate via the sequential single electron transfer(SSET) process.

关键词： Carbon dioxide Epoxides Visible-light photoredox catalysis Hydroxy acid Sequential single electron transfer

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Activity promotion of Rh_(1)Ca_(x)/Al_(2)O_(3) single-atom catalyst in 1-octene hydroformylation:a volcano curve exists between Ca adding ratio and catalytic activity

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Science China chemistry 2024年第4期67卷 1187-1192页

作者： Hao Zhang Xingcong Zhang Xilun Wang Qingdi Sun Hao Liu Hongbing Ji Xiaohui He key laboratory of Bioinorganic and Synthetic chemistry of Ministry of Education Fine Chemical Industry Research InstituteSchool of ChemistryIGCMESun Yat-sen UniversityGuangzhou 510275China Huizhou Research Institute Sun Yat-sen UniversityHuizhou 516081China state key laboratory breeding base of green-Chemical synthesis technology Institute of Green Petroleum Processing and Light Hydrocarbon ConversionCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014China

Single-atom catalysts(SACs)are considered the best candidates for olefin hydroformylation due to their combined advantages of homogeneous and heterogeneous *** conventional organo-phosphine modification,Rh SAC is modified by introducing Ca,resulting in a significant increase in activity(maximum~5.7-fold)and ***,a volcano curve between Ca addition ratio and catalytic activity is *** Ca significantly increases activity by decreasing the energy barrier,but excessive Ca decreases activity due to hindering substrate adsorption and reaction.

关键词： hydroformylation bimetallic single-atom catalysts rhodium heterogeneous catalyst

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Layer-by-layer fabrication of montmorillonite coating immobilizing Cu_(2)O nanoparticles for continuously catalyzing glycerol to dihydroxyacetone

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Chinese Journal of Chemical Engineering 2024年第4期68卷 263-275页

作者： Kejin Li Jiahui Liu Dajian Li Xiaolan Chen Chunhui Zhou Research Group for Advanced Materials&Sustainable Catalysis(AMSC) State Key Laboratory Breeding Base of Green Chemistry-Synthesis TechnologyCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310032China Qing Yang Institute for Industrial Minerals Qingyang 242804China Engineering Research Center of Non-metallic Minerals of Zhejiang Province Zhejiang Institute of Geology and Mineral ResourcesHangzhou 310007China

Microreactors are increasingly used for green and safe chemical processes owing to their benefits of superior mass and heat transfer,increased yield,safety,and simplicity of ***,immobilizing catalysts in microreactors remains *** this investigation,a technique for creating Cu_(2)O/montmorillonite catalyst coating,using electrostatic attraction for layer-by-layer self-assembly,was *** montmorillonite film's morphology and thickness could be efficiently regulated by adjusting the degree of exfoliation and surface charge of montmorillonite,alongside layer-by-layer coating *** Cu_(2)O nanoparticles were immobilized using the flow deposition *** resulting Cu_(2)O@montmorillonite-film-coated capillary microreactor successfully transformed glycerol into *** conversion of glycerol and product selectivity could be controlled by adjusting the molar ratio of reactants,temperature,residence time,and Cu_(2)O *** maximum glycerol conversion observed was 47.6%,with a 27%selectivity toward *** study presents a technique for immobilizing montmorillonite-based catalyst coatings in capillary tubing,which can serve as a foundation for the future application of microreactors in glycerol conversion.

关键词： Microreactor Coating Montmorillonite Glycerol Cu_(2)O

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Control of interfacial reaction and defect formation in Gd/Bi_(2)Te_(2.7)Se_(0.3)composites with excellent thermoelectric and magnetocaloric properties

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Chinese Physics B 2024年第8期33卷 474-481页

作者：薛天畅魏平刘承姗李龙舟朱婉婷聂晓蕾赵文俞 state key laboratory of Advanced technology for Materials synthesis and Processing Wuhan University of TechnologyWuhan 430070China

The method to combine thermoelectric(TE)and magnetocaloric(MC)cooling techniques lies in developing a new material that simultaneously possesses a large TE and good MC cooling *** this work,using n-type Bi_(2)Te_(2.7)Se_(0.3)(BTS)as the TE base material and Gd as the second-phase MC material,Gd/BTS composites were prepared by the spark plasma sintering *** the composites,interfacial reaction between Gd and BTS was identified,resulting in the formation of Gd Te,which has a large impact on the electron concentration through the adjustment of defect *** MC/TE composite containing 2.5 wt%Gd exhibited a ZT value of 0.6 at 300 K,essentially retaining the original TE performance,while all the composites largely maintained the excellent MC performance of *** work provides a potential pathway to achieving high performance in MC/TE composites.

关键词： thermo-electro-magnetic energy conversion materials interfacial reaction thermoelectric performance magnetic entropy change

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NaBH4-induced phase transition of CoSe_(2) with abundant Se deficiency for acidic oxygen reduction to hydrogen peroxide

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Rare Metals 2024年第2期43卷 500-510页

作者： Cai-Di Han Yong-Chao Zhang Qian Zhang Jin-Ting Wu Jian Gao Ji-Jun Zou Xiao-Dong Zhu state key laboratory base of Eco-Chemical Engineering College of Chemical Engineering Qingdao University of Science and TechnologyQingdao266042China key laboratory for green Chemical technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin300072China

Electrocatalytic oxygen reduction(ORR)via the 2e−pathway to form H_(2)O_(2) in acidic medium has attracted extensive ***,the low activity,insufficient selectivity and high cost of catalysts have been the ***,CoSe_(2) with abundant Se deficiency was synthesized by a simple hydrothermal method,and the addition of NaBH4-induced CoSe_(2) phase transition from orthorhombic to cubic phase with more Se *** cubic phase CoSe_(2) with abundant Se deficiency can effectively regulate the surface electronic structure with suitable binding energies of*OOH and*O,which shows high activity,selectivity and long-term stability for acidic ORR to H_(2)O_(2).The onset potential is as low as 0.73 V *** hydrogen electrode(RHE),the H_(2)O_(2) selectivity is 84%(0 V ***),and the average electron transfer number is about ***,the H_(2)O_(2) yield measured using a flow cell is as high as 115.92 mmol·gcat.^(−1)·h^(−1) and the Faradaic efficiency is 70%at 0 V ***,which presents high potential in electrocatalytic acidic ORR to H_(2)O_(2) and organic pollutant degradation using the electron-Fenton process.

关键词： Se defected CoSe_(2) Crystal phase transition Electrocatalysis Acidic oxygen reduction Hydrogen peroxide

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Single-atom Zn confined in hierarchical hollow microstructure as an acid/base-resistant microwave absorption materials

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Nano Research 2024年第8期17卷 6785-6794页

作者： Yue Lou Jiao Li Xiaokun Li Zhenyu Zhu Zhan Shi Biao Xu School of chemistry and Chemical Engineering Nanjing University of Science and TechnologyNanjing 210094China state key laboratory of Inorganic synthesis and Preparative chemistry College of ChemistryJilin UniversityChangchun 130012China

Developing acid/base-resistant and low-price microwave-absorbing materials with lighter weight is highly desired for practical applications in extreme ***,we demonstrate the successful synthesis of the N-doped porous carbon(NC)material with hierarchical pore structure by the spray pyrolysis *** large specific surface area(SBET=707.53 m^(2)·g^(−1))of materials enables multiple scattering of incident electromagnetic waves,and N doping greatly enhances the electrical conductivity of the ***,single-atom Zn can adjust the local electronic structure of adjacent sites such as carbon and nitrogen atoms,induce the center of polarization,and thus change the dielectric and electronic properties of the host *** porous carbon coating of single-atom Zn avoids the deterioration of electromagnetic parameters caused by the accumulation of magnetic particles under high-temperature *** the same time,they can also be used in various complex environments,such as acidic and basic ***,NC-1000,with high surface area,low density,and good chemical stability,obtained a minimum reflection loss(RLmin)of−50.5 dB and an effective absorption bandwidth(EAB)exceeding 5.1 GHz at the thickness of 1.9 *** soaking in the strong acid and base solution,the electromagnetic wave absorption performance of the material decreased by<15%.Widely available raw materials and a simple preparation scheme are expected to expedite industrial mass production for this novel type of materials.

关键词： hierarchical hollow microstructure microwave absorption metal-organic framework(MOF) impedance matching singleatom Zn acid/base-resistant

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Controlling hydrogenation of C=C and C=O bonds in cinnamaldehyde using Pt_(1)/Ni and Pt_(1)/Co single-atom alloy catalysts

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Rare Metals 2024年第6期43卷 2859-2868页

作者： Huan-Shi Lan Yi-Da Yang Qing-Di Sun Hao Zhang Ying Zhang Qian He Ran Chen Guo-Yi Bai Xiao-Hui He Hong-Bing Ji School of chemistry and Chemical Engineering Guangxi UniversityNanning 530004China key laboratory of Bioinorganicand Synthetic chemistry of Ministry of Education Fine Chemical Industry Research InstituteSchool of ChemistryIGCMESun Yat-sen UniversityGuangzhou510275China UBFC CNRSENSMMFEMTO-ST Institute25030 Besancon CEDEXFrance College of chemistry and Materials Science Hebei UniversityBaoding 071002China state key laboratory breeding base of green-Chemical synthesis technology Institute of Green Petroleum Processing and Light Hydrocarbon ConversionCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014China

Selective hydrogenation of C=C and C=O bonds in cinnamaldehyde(CAL)to produce desired products is a challenging task due to the complex conjugate system of the two unsaturated functional *** this study,a simple ball milling method is presented for synthesizing Pt-based single-atom alloy catalysts(SAAs)that can function as a control switch for the selective hydrogenation of CAL into highly valuable products.

关键词： alloy hydrogenation conjugate

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Constructing electron-blocking grain boundaries in garnet to suppress lithium dendrite growth

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Journal of Advanced Ceramics 2024年第2期13卷 166-175页

作者： Xing Xiang Zecheng Fang Congkun Du Zhenzhen Zhao Jiajia Chen Yanhua Zhang Huihu Wang Chenhuinan Wei Fei Chen Qiang Shen Hubei Provincial key laboratory of green Materials for Light Industry Hubei University of TechnologyWuhan 430068China Hubei Longzhong laboratory Wuhan University of Technology Xiangyang Demonstration ZoneXiangyang 441000China Collaborative Innovation Center of green Light-weight Materials and Processing Hubei University of TechnologyWuhan 430068China New Materials and green Manufacturing Talent Introduction and Innovation Demonstration base Hubei University of TechnologyWuhan 430068China state key Lab of Advanced technology for Materials synthesis and Processing Wuhan University of TechnologyWuhan 430070China

Li_(7)La_(3)Zr_(2)O_(12)(LLZO)is considered as a promising solid-state electrolyte due to its high ionic conductivity,wide electrochemical window,and excellent electrochemical ***,its application in solid-state lithium metal batteries(SSLMBs)is impeded by the growth of lithium dendrites in LLZO due to some reasons such as its high electronic *** this study,lithium fluoride(LiF)was introduced into Ta-doped LLZO(LLZTO)to modify its grain boundaries to enhance the performance of SSLMBs.A nanoscale LiF layer was uniformly coated on the LLZTO grains,creating a threedimensional continuous electron-blocking network at the grain *** from the electronic insulator LiF and the special structure of the modified LLZTO,the symmetric cells based on LLZO achieved a high critical current density(CCD)of 1.1 mA·cm^(-2)(in capacity-constant mode)and maintained stability over 2000 h at 0.3 mA·cm^(-2).Moreover,the full cells combined with a LiFePO_(4)(LFP)cathode,demonstrated excellent cycling performance,retaining 97.1% of capacity retention after 500 cycles at 0.5 ***,this work provides a facile and effective approach for preparing a modified electrolyte suitable for high-performance SSLMBs.

关键词： solid electrolyte garnet lithium dendrite microstructure solid-state batteries

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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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