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Metallaphotoredox-Catalyzed Three-Component Couplings for Practical Synthesis of Ureas and Carbamates

Chinese Journal of Chemistry 2024年第3期42卷 264-270页

作者： Ernest Koranteng Zhen-Cao Shu yi-yin liu Qian Yang Bin Shi Qiang-Xian Wu Fen Tan Liang-Qiu Lu Wen-Jing Xiao Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction Ministry of EducationCollege of ChemistryCentral China Normal University152 Luoyu RoadWuhanHubei430079 China Wuhan Youji Industries Co. LtdNo.1 2nd Chemical Rd.WuhanHubei430082 China Hubei Key Laboratory of Purification and Application of Plant Anti-cancer Active Ingredients School of Chemistry and Life SciencesHubei University of EducationWuhanHubei430205 China State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhouGansu730000 China School of Chemistry and Chemical Engineering Henan Normal UniversityXinxiangHenan453007 China Wuhan Institute of Photochemistry and Technology WuhanHubei430082 China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai200032 China

Ureas are widely used in drugs,materials and catalysts because of their diamide structure,which can form strong hydrogen ***,it is of great scientific significance to develop efficient and green methods for the synthesis of urea compounds,especially unsymmetrical ***,we have disclosed novel and highly efficient three-component coupling reactions of organic halides,sodium cyanate and amines enabled by nickel/photoredox dual catalysis for the preparation of unsymmetrical *** reaction features simple and safe operations,broad substrate scopes,and product *** allows the facile synthesis of N-aryl/vinyl ureas from readily available,user-friendly feedstocks under mild conditions(27 examples,36%—98%yields).In addition,this method is further derived to alcohols as nucleophiles to synthesize a series of carbamates(15 examples,40%—95%yields).The mechanism experiment shows that the isocyanate produced by the coupling of halide and sodium cyanate may be the key intermediate in this reaction.

关键词： Cross-coupling Nickel Photoredox catalysis Three-component reaction Ureas Carbamates

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Attaining synergetic equilibrium of electrical conductivity and tensile strength in GQDs@GN/Cu composites through multi-scale intragranular and intergranular reinforcements

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Rare Metals 2024年第1期43卷 366-379页

作者： Shuang-yin Zhang Liang liu Rui Bao Jian-Hong yi Sheng-Da Guo Faculty of Materials Science and Engineering Kunming University of Science and TechnologyKunming 650093China Key Laboratory of Advanced Materials of Yunnan Province Kunming University of Science and TechnologyKunming 650093China Faculty of Materials Metallurgy and Chemistry Jiangxi University of Science and TechnologyGanzhou 341000China

The configuration and quality of reinforcements, as well as the robustness of interfacial bonding,holding a critical significance in determining the concurrence between electrical conductivity and mechanical strength in metal matrix composites. In this study, citric acid was employed as the precursor for synthesizing multiscale carbon nanomaterials(graphene quantum dots and graphene, abbreviated as GQDs and GN). The GQDs@GN/Cu composites were fabricated through a segmented ball milling process in conjunction with subsequent spark plasma sintering(SPS). The intragranular GQDs and intergranular GQDs@GN had synergistically reinforced Cu composites through Orowan strengthening, load transfer strengthening and refinement strengthening. Furthermore,the robust interface bonding between GQDs@GN and Cu effectively mitigated interfacial impedance stemming from electron-boundary scattering. The yield strength and ultimate tensile strength of the GQDs@GN/Cu composites were recorded as 270 and 314 MPa, respectively, representing an improvement of 92 and 28% over pure Cu, while maintaining electrical conductivity at a level comparable to that of pure Cu. This study advances the understanding of the possibility of realizing a synergistic compatibility between electrical conductivity and mechanical strength in Cu composites.

关键词： Cu matrix composites Interface bonding Mechanical property Graphene quantum dots(GQDs) Electrical conductivity

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Hydrogen and nitrogen absorption properties of Ce-added Zr_(2)(Fe_(1-x)Ni_(x)) alloys

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Journal of Rare Earths 2024年第6期42卷 1136-1141,I0005页

作者： Kai yin Xiaopeng liu State Key Laboratory of Advanced Materials for Smart Sensing GRINM Group Co.Ltd.Beijing10088China GRIMAT Engineering Institute Co. Ltd.Beijing101407China General Research Institute of Nonferrous Metals Beijing100088China

To improve the nitriding resistance of Zr_(2)Fe alloy,the Ce-added Zr_(2)(Fe_(1-x)Ni_(x))(x=0,0.15,0.3,0.5)alloys were prepared by magnetic levitation melting *** effects of Ni substitution for Fe on the phase structure,hydrogen and nitrogen absorption properties of the alloys were investigated by X-ray diffraction,scanning electron microscopy and p-c isotherm *** experimental results show that Ni substitution can effectively inhibit the formation of both α-Zr and ZrFe_(2) phases and promote the formation of C16 structure Zr_(2)(Fe,Ni)phase,causing Ni-substituted alloys to exhibit low nitrogen absorption rate and *** 623 K under 0.5 MPa nitrogen pressure,the nitrogen absorption capacity of Ce-added Zr_(2)(Fe_(0.5)Ni_(0.5))alloy reaches to 0.8 mL/g,much lower than that of Zr_(2)Fe alloy(1.5 mL/g).Ni substitution decreases the crystal cell volume of the C_(16)Zr_(2)(Fe,Ni)phase,resulting in an increase in the hydrogen absorption equilibrium *** 623 K under 0.05 MPa hydrogen pressure,the hydrogen absorption capacity decreases from 1.46 wt%of Zr_(2)Fe alloy to 1.41 wt%of Ce-added Zr_(2)(Fe_(0.5)Ni_(0.5))alloy.

关键词： Zr_(2)Fe alloy Ce Pressure-composition isotherm Hydrogen absorption Nitrogen absorption Rare earths

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Lipase and photodecarboxylase coexpression: A potential strategy for alkane-based biodiesel production from natural triglycerides

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Chinese Journal of Chemical Engineering 2024年第3期67卷 238-246页

作者： Yong-yi Zeng Xin-yi Xu Jin-Xuan Xie Wen-Li Chen Lan liu Xin-Jian yin Bi-Shuang Chen School of Marine Sciences Sun Yat-Sen UniversityZhuhai 519080China Southern Marine Science and Engineering Guangdong Laboratory(Zhuhai) Zhuhai 519080China

Alkane-based biodiesel is considered the next generation of biodiesel owing to its potential environmental benefits and the fact that it exhibits much higher specific caloric values than traditional ***,the formidable obstacle impeding the commercialization of this cutting-edge fuel alternative lies in the cost associated with its *** this study,an engineered strain Escherichia coli(***)showcasing harmonized coexpression of a lipase(from Thermomyces lanuginosus lipase,TLL)and a fatty acid photodecarboxylase(from Chlorella variabilis,CvFAP)was first constructed to transform triglycerides into *** potential of *** BL21(DE3)/pRSFDuet-1-TLL-CvFAP for alkane synthesis was evaluated with tripalmitin as a model substrate under various process *** a comprehensive examination of the reaction parameters,the scope of the biotransformation was expanded to‘real’substrates(vegetable oils).The results showed that bioderived oils can be transformed into alkanes with high yields(0.80-10.20 mmol·L^(-1))under mild conditions(35℃,pH 8.0,and 36 h)and blue light *** selected processes were performed on an increased lab scale(up to 100 ml)with up to 24.77 mmol·L^(-1) tripalmitin,leading to a yield of 18.89 mmol·L^(-1) *** the employment of a method for efficiently producing alkanes under mild conditions and a simple procedure to isolate alkanes from the reaction system,the utilization of sustainable biomass as a fundamental feedstock emerges as the primary solution to lower the cost of alkane-based ***,this study proposes a readily implementable and highly effective approach for alkane-based biodiesel production.

关键词： Alkane-based biodiesel Renewable biomass Co-overexpression Lipase Photodecarboxylase

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Chemoselective and Living/Controlled Polymerization of Alkenyl Methacrylates by the Phosphonium Ylide/Organoaluminum Lewis Pairs

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Chinese Journal of Polymer Science 2024年第2期42卷 159-167,I0005页

作者： Zhi-Kang Chen Wu-Chao Zhao yi-Ling Zhao Cong-Lei liu liu-yin Jiang Yue-Tao Zhang Hong-Ping Zhu State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China State Key Laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun130012China

Chemoselective,living/controlled polymerizations of allyl methacrylate(AMA) and vinyl methacrylate(VMA) with/without methyl methacrylate(MMA) by using the phosphonium ylide/organoaluminum based Lewis pairs(LPs) have been *** P-ylide-2/AIMe(BHT)_(2)(Pylide-2=Ph_(3)P=CHMe and BHT=2,6-iBu_(2)-4-MeC_(6)H_(2)O) was demonstrated to be superior by which homopolymers PAMAs(M_(n)=27.6-111.5kg/mol and ■=1.14-1.25) and PVMAs(M_(n)=28.4-78.4 kg/mol and ■=1.12-1.18) and block copolymers PMMA-b-PAMA,PAMA-b-PVMA,PAMA-bPMMA,PMMA-b-PAMA-b-PMMA,PAMA-b-PMMA-b-PAMA,and PAMA-b-PVMA-b-PAMA were *** the polymerizations,all of the monomers were reacted by the conjugated ester vinyl groups leaving intactly the nonconjugated acryloxy *** pendant acryloxy groups attached to the main chain enable further to post-functionalization by the AIBN-induced radical "thiol-ene" reaction using PhCH_(2)*** thiolether side group-containing polymers PAMA-SCH_(2)Ph and PAMA-SCH_(2)Ph-b-PMMA-b-PAMA-SCH_(2)Ph were thus prepared.

关键词： Phosphonium ylide Alkenyl methacrylate Chemoselectivity Living/controlled polymerization Post-functionalization

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In-situ embedded ultrafine Bi_(12)O_(17)Br_(2)nanotubes in MOF-derived hierarchical porous carbon for enhanced photocatalytic CO_(2)conversion to CO

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Journal of Materials Science & Technology 2024年第4期171卷 47-53页

作者： Xing Sun Mengxia Ji yi Zhang Qingzeng Xing Zihan liu Nianhua liu Emmanuel Nkudede Huaming Li Sheng yin Jiexiang Xia School of Chemistry and Chemical Engineering Institute for Energy ResearchJiangsu UniversityZhenjiang 212013China Key Laboratory of Comprehensive and Highly Efficient Utilization of Salt Lake Resources Qinghai Provincial Key Laboratory of Resources Chemistry of Salt LakesQinghai Institute of Salt LakesChinese Academy of SciencesXining 81008China

Increasing the utilization efficiency of photogenerated electrons is highly recognized as one of the ef-ficient approaches to boost the photocatalytic CO_(2)conversion ***,ZIF-67-derived porous carbon(PC)material was employed for the construction of PC@ultrafine Bi_(12)O_(17)Br_(2)nanotubes(PC@BOB NTs)composites through a facile solvothermal synthesis in order to optimize the use of excited elec-trons in the BOB *** characterization results revealed that the introduction of PC material achieved a faster charge separation rate in the PC@BOB composites,ensuring more photogener-ated electrons participate in the CO_(2)adsorption and activation ***,the pore structures of ZIF-67-derived PC material provided abundant confined spaces for the enrichment of CO_(2)***-ter 5 h of Xenon lamp irradiation,PC@BOB composites exhibited obviously increased photocatalytic CO_(2)reduction activity in the pure *** the addition amount of PC was 5 wt%,the PC@BOB-2 com-posite showed the highest CO evolution rate of 359.70μmol/g,which was 2.95 times higher than that of the pure BOB *** work provides some independent insights into the applications of Metal-Organic Framework(MOF)-derived hierarchical porous structures to strengthen the CO_(2)enrichment,as well as the excited charge utilization efficiency,thus achieving a high solar-to-fuel conversion efficiency.

关键词： Bi_(12)O_(17)Br_(2)nanotubes Hierarchical porous structure CO_(2)enrichment Charge separation CO_(2)photoreduction

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Photoredox Catalysis Unlocks the Nickel-Catalyzed Cyanation of Aryl Halides under Benign Conditions

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CCS Chemistry 2022年第5期4卷 1577-1586页

作者： Yue Jia yi-yin liu Liang-Qiu Lu Shi-Han liu Hong-Bin Zhou Yu Lan Wen-Jing Xiao CCNU-uOttawa Joint Research Centre Key Laboratory of Pesticide&Chemical BiologyMinistry of EducationCollege of ChemistryCentral China Normal UniversityWuhan 430079 School of Chemistry and Chemical Engineering Chongqing UniversityChongqing 400030 Province College of Chemistry Institute of Green CatalysisZhengzhou UniversityZhengzhou 450001 State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032

The transition-metal-catalyzed cyanations of aryl halides are among the most used methods for synthesizing aryl *** tremendous advances,cyanating an aryl halide in a facile and benign fashion has generally been *** challenge in this significant transformation is the strong affinity of cyanide for metals,which hampers oxidative addition(OD)and reductive elimination(RE)making organometallic catalysis ***,we demonstrate for the first time that photoredox-nickel-catalyzed cyanations of aryl halides are readily enabled by visible light,in which Ni(Ⅱ)species are transiently oxidized to Ni(Ⅲ)species,thereby facilitating subsequent cyanide transfer and *** this dual catalysis strategy,we cyanated aryl and alkenyl halides at room temperature in a highly benign manner(30 examples,53-93% yield)by avoiding the use of air-sensitive ligands,Ni(0)precursors,and hypertoxic cyanation reagents,while also limiting excess metal *** studies were also used to help understand the present transformation.

关键词： nickel catalysis photoredox catalysis visible light cyanation reaction aryl nitrile

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Grain boundary engineering for enhancing intergranular damage resistance of ferritic/martensitic steel P92

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Nuclear Science and Techniques 2024年第5期35卷 186-199页

作者： Lei Peng Shang-Ming Chen Jing-yi Shi Yong-Jie Sun yi-Fei liu yin-Zhong Shen Hong-Ya He Hui-Juan Wang Jie Tian State Key Laboratory of Particle Detection and Electronics University of Science and Technology of ChinaHefei 230026China School of Nuclear Science and Technology University of Science and Technology of ChinaHefei 230027China School of Materials Engineering Shanghai University of Engineering Science333 Long Teng RoadShanghai 201620China Experimental Center of Engineering and Material Science University of Science and Technology of ChinaHefei 230026China

Ferritic/martensitic(F/M)steel is widely used as a structural material in thermal and nuclear power ***,it is susceptible to intergranular damage,which is a critical issue,under service *** this study,to improve the resistance to intergranular damage of F/M steel,a thermomechanical process(TMP)was employed to achieve a grain boundary engineering(GBE)microstructure in F/M steel *** TMP,including cold-rolling thickness reduction of 6%,9%,and 12%,followed by austenitization at 1323 K for 40 min and tempering at 1053 K for 45 min,was applied to the as-received(AR)P92 *** prior austenite grain(PAG)size,prior austenite grain boundary character distribution(GBCD),and connectivity of prior austenite grain boundaries(PAGBs)were *** to the AR specimen,the PAG size did not change *** fraction of coincident site lattice boundaries(CSLBs,3≤Σ≤29)and Σ3^(n) boundaries along PAGBs decreased with increasing reduction ratio because the recrystallization fraction increased with increasing reduction *** PAGB connectivity of the 6%deformed specimen slightly deteriorated compared with that of the AR ***,potentiodynamic polarization studies revealed that the intergranular damage resistance of the studied steel could be improved by increasing the fraction of CSLBs along the PAGBs,indicating that the TMP,which involves low deformation,could enhance the intergranular damage resistance.

关键词： Grain boundary engineering Ferritic/martensitic steel Prior austenite grain boundary character distribution Grain boundary connectivity Intergranular damage resistance

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A stable staggered-grid finite-difference scheme for acoustic modeling beyond conventional stability limit

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Petroleum Science 2024年第1期21卷 182-194页

作者： Jing-yi Xu Yang liu National Key Laboratory of Petroleum Resources and Engineering China University of Petroleum(Beijing)Beijing 102249China China University of Petroleum(Beijing) Karamay CampusKaramay 834000XinjiangChina

Staggered-grid finite-difference(SGFD)schemes have been widely used in acoustic wave modeling for geophysical *** improved methods are proposed to enhance the accuracy of numerical ***,these methods are inevitably limited by the maximum Courant-Friedrichs-Lewy(CFL)numbers,making them unstable when modeling with large time sampling intervals or small grid *** solve this problem,we extend a stable SGFD scheme by controlling SGFD dispersion relations and maximizing the maximum CFL ***,to improve modeling stability,we minimize the error between the FD dispersion relation and the exact relation in the given wave-number region,and make the FD dispersion approach a given function outside the given wave-number area,thus breaking the conventional limits of the maximum CFL ***,to obtain high modeling accuracy,we use the SGFD scheme based on the Remez algorithm to compute the FD *** addition,the hybrid absorbing boundary condition is adopted to suppress boundary reflections and we find a suitable weighting coefficient for the proposed *** derivation and numerical modeling demonstrate that the proposed scheme can maintain high accuracy in the modeling process and the value of the maximum CFL number of the proposed scheme can exceed that of the conventional SGFD scheme when adopting a small maximum effective wavenumber,indicating that the proposed scheme improves stability during the modeling.

关键词： Acoustic wave Staggered-grid finite-difference(SGFD) modeling Courant-friedrichs-lewy(CFL)number Stability

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Modelling analysis embodies drastic transition among global potential natural vegetations in face of changing climate

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Forest Ecosystems 2024年第2期11卷 184-192页

作者： Zhengchao Ren Lei liu Fang yin Xiaoni liu School of Earth Science and Resources Chang’an UniversityXi’an710054China Research Center of Ecological Construction and Environmental Conservation in Gansu Province Gansu Agricultural UniversityLanzhou730070China State Key Laboratory of Tibetan Plateau Earth System Environment and Resources(TPESER)Institute of Tibetan Plateau ResearchChinese Academy of SciencesBeijing100101China School of Land Engineering Chang’an UniversityXi’an710054China College of Pratacultural Science Gansu Agricultural UniversityLanzhou730070China

Potential natural vegetation(PNV)is a valuable reference for ecosystem renovation and has garnered increasing attention ***,there is limited knowledge on the spatio-temporal distributions,transitional processes,and underlying mechanisms of global natural vegetation,particularly in the case of ongoing climate *** this study,we visualize the spatio-temporal pattern and inter-transition procedure of global PNV,analyse the shifting distances and directions of global PNV under the influence of climatic disturbance,and explore the mechanisms of global PNV in response to temperature and precipitation *** achieve this,we utilize meteorological data,mainly temperature and precipitation,from six phases:the Last Inter-Glacial(LIG),the Last Glacial Maximum(LGM),the Mid Holocene(MH),the Present Day(PD),2030(20212040)and 2090(2081–2100),and employ a widely-accepted comprehensive and sequential classification sy–stem(CSCS)for global PNV *** find that the spatial patterns of five PNV groups(forest,shrubland,savanna,grassland and tundra)generally align with their respective ecotopes,although their distributions have shifted due to fluctuating temperature and ***,we observe an unexpected transition between tundra and savanna despite their geographical *** shifts in distance and direction of five PNV groups are mainly driven by temperature and precipitation,although there is heterogeneity among these shifts for each ***,the heterogeneity observed among different global PNV groups suggests that they may possess varying capacities to adjust to and withstand the impacts of changing *** spatio-temporal distributions,mutual transitions and shift tendencies of global PNV and its underlying mechanism in face of changing climate,as revealed in this study,can significantly contribute to the development of strategies for mitigating warming and promoting re-vegetation in degraded regions worldwide.

关键词： Potential natural vegetation Global warming Vegetation classification Predicted model CSCS

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