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Phosphine/Benzocyclone-based Neutral Nickel Catalysts for Ethylene Polymerization and Copolymerization with Polar Monomers

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chinese Journal of Polymer Science 2024年第2期42卷 202-212,I0007页

作者： Fei Wang Li pan Vladislav A.Tuskaev Svetlana ch.Gagieva Yue-Sheng Li Tianjin Key Lab of Composite&Functional Materials School of Material Science and EngineeringTianjin UniversityTianjin300072China Department of chemistry Lomonosov Moscow State UniversityRussian Federation InstitutionLeninskie Gory 1Moscow119991Russian Federation A N Nesmeyanov Institute of Organoelement Compounds Russian Academy of SciencesVavilova st.28Moscow119991Russian Federation

The efficient copolymerization of olefin with polar monomers using nickel-based catalysts presents a longstanding challenge. In this contribution, three phosphine-benzocyclone ligands and corresponding neutral nickel catalysts(Ni1: Ar = Ph;Ni2: Ar = 2-(C_(6)H_(5))C_(6)H_(4);Ni3: Ar = 2-[2',6'-(Me O)_(2)-C_(6)H3]C_(6)H_(4)) were prepared and applied for the ethylene polymerization and copolymerization with polar monomers without any cocatalyst. The bulky substituent groups in complexes Ni2 and Ni3 contributed to high catalytic activities(up to 7.24×10^(6) and 9.04×10^(6)g·mol Ni^(-1)·h^(-1), respectively), and produced high-molecular-weight polyethylene(Mw up to 545.7 k Da). Complex Ni3 exhibited high activities for ethylene polymerization at the level of 10^(6) g·mol Ni^(-1)·h^(-1) across a wide range from 30 ℃ to 120 ℃, exhibiting excellent high temperature tolerance. These nickel complexes were also effectively employed in the copolymerization of ethylene with methyl acrylate, ethyl acrylate, butyl acrylate and lauryl acrylate, producing copolymers with high molecular weights(Mw up to 80.5 k Da) and high polar monomer incorporation(up to 8.2 mol%). Microstructure analyses revealed that the introduction of large sterically hindered substituents facilitated the incorporation of polar functional units into the polymer backbone. This study demonstrates the potential of these nickel-based catalysts for efficient copolymerization of olefin with polar monomers.

关键词： Neutral nickel catalyst Ethylene polymerization Copolymerization Polar acrylate monomers

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Thermodynamic and Economic Analysis of a Conceptual System Combining Sludge Gasification,SOFC,Supercritical CO_(2)Cycle,and Organic Rankine Cycle

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Journal of Thermal Science 2024年第4期33卷 1491-1508页

作者： LV Jiayang WANG chizhong chEN Heng pan Peiyuan XU Gang ZHANG Guoqiang School of Energy Power and Mechanical EngineeringNorth China Electric Power UniversityBeijing102206China

In order to reduce the environmental impact of conventional sludge treatment methods and to utilize the energy in sludge more effectively,a coupled system based on sewage sludge gasifier(SSG),solid oxide fuel cells(SOFC),supercritical CO_(2)cycle(S-CO_(2)),and organic Rankine cycle(ORC)is *** clean syngas obtained from sludge gasification is mixed with ch4 and then first utilized by the fuel *** exhaust gas from the fuel cell is fully combusted in the afterburning chamber and then enters the bottom cycle system consisting of S-CO_(2)&ORC to generate *** understand the performance of the system,thermodynamic and economic analyses were conducted to examine the project's *** thermodynamics as well as the economics of the coupled system were analyzed to arrive at the following conclusions,the power production of the system is 37.34 MW;the exergy efficiency is 55.62%,and the net electrical efficiency is 61.48%.The main exergy destruction is the gasifier and SOFC,accounting for 62.45%of the total exergy *** takes only6.13 years to repay the construction investment in the novel system,and the project obtains a NPV of 17723820USD during 20 years *** above findings indicate that the new coupled system has a better performance in terms of energy utilization and economy.

关键词： sewage sludge gasifier SOFC supercritical CO_(2)cycle organic Rankine cycle multi-system coupling

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Significant contribution of carbonyls to atmospheric oxidation capacity(AOC)during the winter haze pollution over North china Plain

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Journal of Environmental Sciences 2024年第5期139卷 377-388页

作者： Xue Yang Gen Zhang Guang pan Guolan Fan Houyong Zhang Xuan Ge Mingyue Du School of Municipal and Environmental Engineering Shandong Jianzhu UniversityJi’nan 250101China State Key Laboratory of Severe Weather&Key Laboratory of Atmospheric chemistry of china Meteorological Administration Chinese Academy of Meteorological SciencesBeijing 100081China Shandong Jinan Ecological Environment Monitoring Center Ji’nan 250101China

Atmospheric carbonyl compounds play significant roles in the cycling of radicals and have exhibited surprisingly high levels in winter that were well correlated to particulate matter,for which the reason have not been clearly *** we measured carbonyl compounds and other trace gasses together with PM_(2.5)over urban Jinan in North china Plain during the *** higher carbonyl concentrations(average:14.63±4.21 ppbv)were found during wintertime haze pollution,about one to three-times relative to those on nonhaze days,with slight difference in chemical composition except formaldehyde(HchO).HchO(3.68 ppbv),acetone(3.17 ppbv),and acetaldehyde(ch_3chO)(2.83 ppbv)were the three most abundant species,accounting for~75% of the total carbonylson both haze and non-haze *** from observational-based model(OBM)with atmospheric oxidation capacity(AOC)indicated that AOC significantly increased with the increasing carbonyls during the winter haze *** photolysis have supplied key oxidants such as RO_(2) and HO_(2),and thereby enhancing the formation of fine particles and secondary organic aerosols,elucidating the observed haze-carbonyls *** variation with carbonyls exhibiting peak values at early-noon and night highlighted the combined contribution of both secondary formation and primary diesel-fuel sources.1-butene was further confirmed to be the major precursor for *** study confirms the great contribution of carbonyls to AOC,and also suggests that reducing the emissions of carbonyls would be an effective way to mitigate haze pollution in urban area of the NCP region.

关键词： Carbonyls Haze Observation-based model Source apportionment Atmospheric oxidation capacity

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miR319-TCPs-TGA9/TGA10/ROXY2 regulatory module controls cell fate specification in early anther development in Arabidopsis

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Science china(Life Sciences) 2024年第4期67卷 839-842页

作者： Jinyuan Tao Zijie pan Wenwen Kong Beixin Mo Xuemei chen Yu Yu Guangdong Provincial Key Laboratory for Plant Epigenetics Longhua Bioindustry and Innovation Research InstituteCollege of Life Sciences and OceanographyShenzhen UniversityShenzhen 518060China Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province College of Optoelectronic EngineeringShenzhen UniversityShenzhen 518060China School of Life Sciences Peking-Tsinghua Joint Center for Life SciencesPeking UniversityBeijing 100871China

Dear Editor,The process of anther development is generally conserved across plant species(Ma,2005).Many protein-coding genes and noncoding RNAs have been identified to participate in early anther development in Arabidopsis(Walbot and Egger,2016).mi R319 is one of the most ancient and conserved mi RNA families in land plants(chávez Montes et al.,2014).

关键词： Arabidopsis miR319 ancient

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Synthesis,characterization of Polyethylene Ionomers and Their Antibacterial Properties

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chinese Journal of Polymer Science 2024年第8期42卷 1077-1084页

作者： Jia-Jia Wu Fei Wang Peng-Qi Wan Li pan chun-Sheng Xiao Zhe Ma Yue-Sheng Li Tianjin Key Lab Composite&Functional Materials School of Materials Science and EngineeringTianjin UniversityTianjin 300350China Key Lab Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Owing to its high production volume and wide range of application s,polyethylene has gained a great deal of attention,but its low surface energy and non-polar nature have limited its application in some important *** this study,ethylene/11-iodo-1-undecene copolymers were prepared and used as the intermediates to afford a series of imidazolium-based ionomers bearing methanesulfonate(ch_(3)SO_(3)^(-)),trifluoromethanesulfonate(CF_(3)SO_(3)^(-)),or bis(trifluoromethane)sulfonimide(Tf_(2)N^(-))*** tensile test results showed that the stress-at-break(7.8-25.6 MPa)and the elongation-at-break(445%-847%)of the ionomers could be adjusted by changing the counterion species and the ionic group *** importantly,the ionomers exhibited marvelous antibacterial activities against Staphylococcus aureus(***)and Escherichia coli(***).The ionomers bearing Tf_(2)N^(-)exhibited antibacterial activities>99%against both *** and *** when ionic content reached 9.1%.The imidazolium-based ionomers prepared in this work demonstrated excellent comprehensive properties,especially highefficient and broad-spectrum antibacterial ability,exhibiting the potential fo r the application as the antibacterial materials in packaging,medical,and other fields.

关键词： Polyethylene Ionomer Polymerization catalysis Imidazolium Antibacterial material

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Heteroatom Structural Engineering Enables Ethenylene-Bridged Bisisoindigo-Based Copolymers to Exhibit Unique n-Type Transistor Performance

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CCS chemistry 2024年第2期6卷 473-486页

作者： Yuchai pan Weifeng Zhang Yankai Zhou Xuyang Wei Hao Luo Jinbei Wei Liping Wang Gui Yu Beijing National Laboratory for Molecular Sciences CAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190 School of chemical Sciences University of Chinese Academy of SciencesBeijing 100049 School of Material Science and Engineering University of Science and Technology BeijingBeijing 100083

Herein,we report three novel electron-deficient aromatics,ethenylene-bridged bisisoindigos 3,3′-((3E,3′E)-((E)-ethene-1,2-diyl)bis(1-(4-decyltetradecyl)-2-oxoind-oline-6-yl-3-ylidene))bis(1-(4-decyltetradecyl)-1,3-dihydro-2H-pyrrolo[2,3-b]pyridin-2-one)(NCCN),3,3′-((3E,3′E)-((E)-ethene-1,2-diyl)bis(1-(4-decyltetradecyl)-7-fluoro-2-oxoindoline-6-yl-3-ylidene))bis(1-(4-decyltetradecyl)-1,3-dihydro-2H-pyrrolo[2,3-b]pyridin-2-one)(NFFN),and(3E,3″E)-6,6″-((E)-ethene-1,2-diyl)bis(1,1′-bis(4-decyltetradecyl)-[3,3′-bipyrrolo[2,3-b]pyridinylidene]-2,2′(1H,1′H)-dione)(NNNN),and their derived donor–acceptor(D–A)copolymers,namely poly[3,3′-((3E,3′E)-((E)-ethene-1,2-diyl)bis(1-(4-decyltetradecyl)-2-oxoindoline-6-yl-3-ylidene))bis(1-(4-decyltetradecyl)-1,3-dihydro-2H-pyrrolo[2,3-b]pyridin-2-one-6-yl)]-alt-[5,6-difluoro-4,7-di[(thiophen-2-yl)-5-yl)]benzo[c][1,2,5]thiadiazole](PNCCN-FBT),poly[3,3′-((3E,3′E)-((E)-ethene-1,2-diyl)bis(1-(4-decyltetradecyl)-7-fluoro-2-oxoindoline-6-yl-3-ylidene))bis(1-(4-decyltetradecyl)-1,3-dihydro-2H-pyrrolo[2,3-b]pyridin-2-one-6-yl)]-alt-[5,6-difluoro-4,7-di[(thiophen-2-yl)-5-yl)]benzo[c][1,2,5]thiadiazole](PNFFNFBT),and poly[(3E,3″E)-6′,6‴-((E)-ethene-1,2-diyl)bis(1,1′-bis(4-decyltetradecyl)-[3,3′-bipyrrolo[2,3-b]pyridinylidene]-2,2′(1H,1′H)-dione-6-yl)]-alt-[5,6-difluoro-4,7-di[(thiophen-2-yl)-5-yl)]benzo[c][1,2,5]thiadiazole](PNNNN-FBT),in which 5,6-difluoro-4,7-di(thiophen-2-yl)benzo[c][1,2,5]thiadiazole(FBT)acts as the electron-donating *** ethenylene-bridging unit reduces the steric hindrance of the three *** of heteroatoms,such as fluorine and sp2-nitrogen atoms,endows them with multiple ch···F,ch···N,and N···S intramolecular hydrogen bonds/nonbinding interactions,resulting in increasing backbone planarity from NCCN,NFFN,to NNNN,and thus from PNCCN-FBT,PNFFN-FBT,to *** found that all copolymers formed an improved molecular packing in the 1-chloronaphthalene(CN)-processed thin film compared with the 1,2-d

关键词： D-A copolymers bisisoindigos heteroatom structural engineering n-type field-effect transistors electron mobilities

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Improving hydrogen evolution reaction efficiency through lattice tuning

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Nano Research 2024年第7期17卷 5907-5913页

作者： Zipeng Zhao Haotian Liu Wenpei Gao Praveen Kolla Wang Xue Zeyan Liu Jinghua Guo Sanjeev Mukerjee Xiaoqing pan Qingying Jia Xiangfeng Duan Yu Huang Department of Materials Science and Engineering University of CaliforniaLos AngelesCalifornia 90095USA Department of chemical Engineering and Materials Science University of CaliforniaIrvineCalifornia 92697USA Materials Science and Engineering North Carolina State UniversityRaleighNorth Carolina 27695USA Department of chemistry and chemical Biology Northeastern UniversityBostonMassachusetts 02115USA Department of chemistry and Biochemistry University of CaliforniaLos AngelesCalifornia 90095USA Advanced Light Source Lawrence Berkeley National LaboratoryBerkeleyCalifornia 94720USA Department of chemistry and Biochemistry University of CaliforniaSanta CruzCalifornia 95064USA Department of Physics and Astronomy University of CaliforniaIrvineCalifornia 92697USA California Nanosystems Institute University of CaliforniaLos AngelesCalifornia 90095USA

The intermittent nature of renewable energy sources sets a requirement for efficient energy storage to mitigate the conflict between energy supply and *** is a promising choice for energy storage due to its high energy ***,the conversion of electrical energy to chemical energy stored in hydrogen through water electrolysis suffers from low efficiency,and the electricity cost dominates the total cost of hydrogen ***,we report the study of improving the hydrogen evolution reaction activity of Pt-based catalysts by building a nanoscale surface NiO and Pt interface,further optimizing the performance via tuning the lattice parameter of the core of nanoparticles,which can be achieved by varying the dealloying annealing *** optimized PtCuNi-O/C and PtNi-O/C catalysts are demonstrated to be one of the best catalysts,with a mass activity(MA)of 9.1 and 8.7 mA/μgPt,which is 9.9-fold and 9.5-fold of that of Pt/C,respectively.

关键词： lattice tuning Pt-based catalyst hydrogen evolution reaction electrocatalysis

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Regulated reaction pathway of CO2 photoreduction into ch4 by metal atom pair sites

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Rare Metals 2024年第9期43卷 4620-4627页

作者： Dong-Po He Guang-Bing Huang Jun Hu Yang Wu Xiao-Dong Li Qing-Xia chen Shan Zhu Wen-Sheng Yan Jun-Fa Zhu Yang pan Xing-chen Jiao Key Laboratory of Synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan University Hefei National Research Center for Physical Sciences at Microscale National Synchrotron Radiation LaboratoryUniversity of Science and Technology of China Max Planck Institute of Microstructure Physics State Grid Anhui Electric Power Research Institute

The carbon dioxide （CO2） reduction process involves complex protonation, making the resulting product often unpredictable. To achieve the desired product, it is crucial to manipulate the reaction steps. Herein, we build the metal atom pair sites for selective CO2photoreduction into methane. As a prototype, Ni atom pair sites loaded on the Mo S2nanosheets were synthesized and verified by highresolution transmission electron microscopy （HRTEM）,X-ray photoelectron spectroscopy （XPS） and X-rayabsorption near edge structure spectra （XANES）. In-situ Fourier transform infrared spectroscopy （FTIR） monitors the*chO group, a crucial intermediate in ch4production,during CO2photoreduction on the Ni-Mo S2nanosheets,whereas this monitoring is not observed for the Mo S2nanosheets. Also, theoretical calculations disclose that over the Ni-Mo S2nanosheet slab, the formation energy of*chO intermediates is determined to be lower （0.585 e V） than the desorption energy of*CO intermediates for CO production（0.64 e V）, implying the higher selectivity of ch4production. Accordingly, the Ni-Mo S2nanosheets demonstrate a methane formation rate of 27.21μmol·g-1·h-1, coupled with an impressive electron selectivity of 94.2%.

关键词： Nanosheets

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Extreme drought with seasonal timing consistently promotes ch_(4) uptake through inconsistent pathways in a temperate grassland, china

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Journal of Arid Land 2024年第6期16卷 768-778页

作者： ZHANG Wenwen pan Yue WEN Fuqi FU Juanjuan HAO Yanbin HU Tianming YANG Peizhi College of Grassland Agriculture Northwest A&F UniversityYangling 712100China Binzhou Institute of Technology Weiqiao-UCAS(University of Chinese Academy of Sciences)Science and Technology ParkBinzhou 256606China College of Life Sciences University of Chinese Academy of SciencesBeijing 100049China

Methane(ch_(4))is a potent greenhouse gas that has a substantial impact on global warming due to its substantial influence on the greenhouse *** extreme precipitation events,such as drought,attributable to global warming that caused by greenhouse gases,exert a profound impact on the intricate biological processes associated with ch_(4) ***,the timing of extreme drought occurrence emerges as a pivotal factor influencing ch_(4) uptake,even when the degree of drought remains ***,it is still unclear how the growing season regulates the response of ch_(4) uptake to extreme *** an effort to bridge this knowledge gap,we conducted a field manipulative experiment to evaluate the impact of extreme drought on ch_(4) uptake during early,middle,and late growing stages in a temperate steppe of Inner Mongolia Autonomous Region,*** result showed that all extreme drought consistently exerted positive effects on ch_(4) uptake regardless of seasonal ***,the magnitude of this effect varied depending on the timing of season,as evidenced by a stronger effect in early growing stage than in middle and late growing ***,the pathways of ch_(4) uptake were different from seasonal *** drought affected soil physical-chemical properties and aboveground biomass(AGB),consequently leading to changes in ch_(4) *** structural equation model showed that drought both in the early and middle growing stages enhanced ch_(4) uptake due to reduced soil water content(SWC),leading to a decrease in NO_(3)–-N and an increase in pmoA ***,drought in late growing stage primarily enhanced ch_(4) uptake only by decreasing *** results suggested that seasonal timing significantly contributed to regulate the impacts of extreme drought pathways and magnitudes on ch_(4) *** findings can provide substantial implications for understanding how extreme droughts affect ch_(4) uptake and improve the prediction of

关键词： extreme climate greenhouse gas methane methanotrophs soil inorganic nitrogen

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Synthesis and Spectrophotometric Studies of 2-(5-Carboxy-1,3,4-triazolylazo)-5-diethylamino Aniline

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chinese chemical Letters 2000年第10期11卷 861-862页

作者： pan, FY Ge, ch Liang, HD Taizhou Teachers Coll Dept Chem Zhejiang 317000 Peoples R China

In this paper, 2-(5-carboxy-1,3,4-triazolylazo)-5-diethylamino aniline(CTZAN) was prepared the protonation behaviour of this reagent is reported. Its structure was identified.

关键词： synthesis triazolylazo spectrophotometry protonation behaviour

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