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Ligand-controlled niH-catalyzed regiodivergent hydroalkylation of 2-alkenylazaarenes

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Science China Chemistry 2024年第6期67卷 1935-1940页

作者： ya-Ping shao Zhuo-Min Chi y.ng-Min Liang State Key Laboratory of Applied Organic Chemistry School of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou730000China

A nickel-hydride(ni H)-catalyzed migratory and nonmigratory hydroalkylation reaction of 2-alkenyl azaarenes with alkyl iodines has been established through strategic modulation of n-or P-donor *** method enables the synthesis of diverseβ-orγ-branched aromatic *** mild regiodivergent protocols exhibit wide substrate scope,excellent functional tolerance,and great reaction yield with remarkable ***,deuterium labeling studies reveal ni H-catalyzed interrupted chain-walking mode as the mechanism behind remotedβ-selective hydroalkylation reaction—an interesting phenomenon mediated through aromatic imine directing groups.

关键词： niH regiodivergent hydroalkylation azaarenes interrupted chain-walking

Crystalline-amorphous M@Mn_x(M=Co,Fe,ni)encapsulated in nitrogen-doped carbon for enhanced efficient and durable hydrogen evolution reaction

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Rare Metals 2024年第4期43卷 1547-1556页

作者： y.ng y.ng Xiao-Chuan Duan shao-Hui Guo Xian-Ming Zhang College of Materials Science and Engineering College of ChemistryKey Laboratory of Interface Science and Engineering in Advanced MaterialsTaiyuan University of TechnologyYuci030600China

Developing earth-abundant electrocatalysts for hydrogen evolution reaction(HER)is important for the sustainable energy ***,efficient and stable heterocatalysts consisting of crystalline-amorphous M@Mn_(x)(M=Co,Fe,ni)encapsulated in n-doped carbon layers supported with n-doped graphene sheets(denoted as M@Mn_(x)@nC-nG)are synthesized by facile hydrothermal reaction and nitridation *** the nitriding process,metal ions in M(tzbc)_2(H_(2)O)_4(tzbc=4-(1H-1,2,4-triazol-1-yl)benzoic acid)complexes are reduced to crystalline M cores,accompanied by the formation of amorphous Mn_(x)shells;the tzbc ligands are insitu carbonized to form outermost n-doped carbon(nC)layers that connect with inner Mn_(x)via M-n-C motifs inherited from the complex precursors and inhibit the transition of Mn_(x)from amorphous to crystalline *** Co@Con_(x)@nC-nG catalyst exhibits excellent HER activity with small overpotentials of 45 and 64 mV at a cathode current density of 10 mA·cm^(-2)and low Tafel slopes of 40 and 85 mV·dec^(-1)in 0.5 mol·L^(-1)H_(2)SO_4 and1.0 mol·L^(-1)KOH electrolytes,*** Co@Con_(x)@nC-nG retains 97%of the initial overpotential after 100,000 s in both acidic and alkaline *** outstanding HER performance originates from the crystalline-amorphous Co@Con_(x)that redistributes electrons around the heterointerfaces,facilitating the conversion process of H^(+)/H_(2)O to hydrogen and thereby promoting HER *** outermost nC layers serve as the armor of Co@Con_(x),and graphene nanosheets act as carriers of egg-like Co@Con_(x)@nC and conduction paths for electron shuttles,ensuring stable and continuous electrocatalytic hydrogen production.

关键词： Hydrogen evolution reaction Electrocatalysts Iron group metals Heterojunction Crystalline-amorphous structure

Atomically Dispersed Zinc Active Sites Efficiently Promote the Electrochemical Conversion of n2 to nH3

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Energy & Environmental Materials 2024年第03期7卷 179-185页

作者： y.njiao Wei Xinyu Wang Mengjie Sun Min Ma Jian Tian Minhua shao School of Materials Science and Engineering Shandong University of Science and Technology Department of Chemical and Biological Engineering The Hong Kong University of Science and Technology Energy Institute and Chinese National Engineering Research Center for Control & Treatment of Heavy Metal PollutionThe Hong Kong University of Science and Technology

At present,the research on highly active and stable nitrogen reduction reaction catalysts is still challenging work for the electrosynthesis of ammonia （nH3）.Herein,we synthesized atomically dispersed zinc active sites supported on n-doped carbon nanosheets （Zn/nC nSs） as an efficient nitrogen reduction reaction catalyst,which achieves a high ammonia yield of46.62μ***-0.85 V （vs RHE） and Faradaic efficiency of 95.8%at-0.70 V （vs RHE）.In addition,Zn/nC nSs present great stability and selectivity,and there is no significant change in nH3rate and Faradaic efficiencies after multiple *** structural characterization shows that the active center in the nitrogen reduction reaction process is the Zn-n4sites in the *** calculation confirms that Zn/nC with Zn-n4configuration has a lower energy barrier for the formation of*nnH intermediate compared with pure n-doped carbon nanosheets （n-C nSs）,thus promoting the hydrogenation kinetics in the whole nitrogen reduction reaction process.

关键词： electrocatalysis nitrogen reduction single-atom catalyst Zn–n4

CFD-DEM simulation of high density particles fluidization behaviors in 3D conical spouted beds

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Particuology 2024年第5期88卷 266-281页

作者： Lin Jiang Mofan Qiu Rongzheng Liu Bing Liu youlin shao Malin Liu Institute of nuclear and new Energy Technology Collaborative Innovation Center of Advanced Nuclear Energy TechnologyTsinghua UniversityBeijing 100084China

The spouted bed has been used in the coating process of high-density.nuclear fuel *** particle fluidization behaviors in pseudo-2D and 3D spouted beds were simulated and *** effects of four independent variables(cone angle,particle density,inlet gas velocity,and particle loading)on particle fluidization behaviors in the 3D spouted bed were investigated *** cone angle effect on fluidization mechanism was studied quantitatively first time.A new fluidization quality index was proposed based on the particle entrainment principle,and an extreme value was obtained when the cone angle was 60°,considered to be the optimum value for the 3D conical spouted *** was indicated the gas–solid contact efficiency can be kept up if the gas velocity was proportional to ρ_(p)^(0.65) and n_(p)^(0.78) when the particle density or loading was *** results will be useful for geometry and operation parameters design of the 3D conical spouted bed and helpful for developing the fluidization mechanism of high-density particles.

关键词： Spouted bed High-density particle CFD-DEM Fluidization quality index Particle loading

A Survey on an Emerging Safety Challenge for Autonomous Vehicles:Safety of the Intended Functionality

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Engineering 2024年第2期33卷 17-34页

作者： Hong Wang Wenbo shao Chen Sun Kai y.ng Dongpu Cao Jun Li Tsinghua Intelligent Vehicle Design and Safety Research Institute School of Vehicle and MobilityTsinghua UniversityBeijing 100084China CogDrive Lab Department of Mechanical and Mechatronics EngineeringUniversity of WaterlooWaterlooON N2L3G1Canada College of Mechanical and Vehicle Engineering Chongqing UniversityChongqing 400044China

As the complexity of autonomous vehicles(AVs)continues to increase and artificial intelligence algorithms are becoming increasingly ubiquitous,a novel safety concern known as the safety of the intended functionality(SOTIF)has emerged,presenting significant challenges to the widespread deployment of *** focuses on issues arising from the functional insufficiencies of the AVs’intended functionality or its implementation,apart from conventional safety *** the systems engineering standpoint,this study offers a comprehensive exploration of the SOTIF landscape by reviewing academic research,practical activities,challenges,and perspectives across the development,verification,validation,and operation *** research encompasses system-level SOTIF studies and algorithm-related SOTIF issues and ***,it encapsulates practical SOTIF activities undertaken by corporations,government entities,and academic institutions spanning international and Chinese contexts,focusing on the overarching methodologies and practices in different ***,the paper presents future challenges and outlook pertaining to the development,verification,validation,and operation phases,motivating stakeholders to address the remaining obstacles and challenges.

关键词： Safety of the intended functionality Autonomous vehicles Artificial intelligence Uncertainty Verification Validation

LncRnA pol-lnc78 as a ceRnA regulates antibacterial responses via suppression of pol-miR-n199-3p-mediated SARM down-regulation in Paralichthys olivaceus

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Zoological Research 2024年第1期45卷 25-35页

作者： Xian-Hui ning Bing Han ye Peng shao-Wu y.n College of Marine Science and Engineering Nanjing Normal UniversityNanjingJiangsu 210023China CAS Key Laboratory of Experimental Marine Biology Center for Ocean Mega-ScienceInstitute of OceanologyChinese Academy of SciencesQingdaoShandong 266071China Co-Innovation Center for Marine Bio-Industry Technology of Jiangsu Province LianyungangJiangsu 222005China

Long non-coding RnAs(lncRnAs)function as key modulators in mammalian immunity,particularly due to their involvement in lncRnA-mediated competitive endogenous RnA(ceRnA)*** their recognized significance in mammals,research on lncRnAs in lower vertebrates remains *** the present study,we characterized the first immune-related lncRnA(pol-lnc78)in the teleost Japanese flounder(Paralichthys olivaceus).Results indicated that pol-lnc78 acted as a ceRnA for pol-miR-n199-3p to target the sterile alpha and armadillo motif-containing protein(SARM),the fifth discovered member of the Toll/interleukin 1(IL-1)receptor(TIR)adaptor *** ceRnA network regulated the antibacterial responses of flounder via the Toll-like receptor(TLR)signaling ***,SARM acted as a negative regulator and exacerbated bacterial infection by inhibiting the expression of inflammatory cytokines IL-1βand tumor necrosis factor-α(TnF-α).Pol-miR-n199-3p reduced SARM expression by specifically interacting with the 3’untranslated region(UTR),thereby promoting SARM-dependent inflammatory cytokine expression and protecting the host against bacterial ***,pol-lnc78 sponged pol-miR-n199-3p to ameliorate the inhibition of SARM *** infection,the negative regulators pol-lnc78 and SARM were significantly down-regulated,while pol-miR-n199-3p was significantly up-regulated,thus favoring host antibacterial *** findings provide novel insights into the mechanisms underly.ng fish immunity and open new horizons to better understand ceRnA crosstalk in lower vertebrates.

关键词： LncRnA SARM miRnA ceRnA Antibacterial response

Effect of Frequency on Degradation in BOPP Films Under Repetitively Pulsed Voltage

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CSEE Journal of Power and Energy Systems 2024年第3期10卷 1280-1290页

作者： Chuansheng Zhang yu Feng Fei Kong Bangdou Huang Cheng Zhang Tao shao Beijing International S&T Cooperation Base for Plasma Science and Energy Conversion Institute of Electrical EngineeringChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Operating conditions of film capacitors are complex,and the problem of film insulation failure caused by repetitively pulsed voltage is becoming ever *** of the film under repetitively pulsed voltage cannot be accurately evaluated by the average breakdown electric *** this paper,the effects of pulsed electric field and pulse repetition frequency on the breakdown in biaxially oriented polypropylene(BOPP)films are *** phases of BOPP degradation are proposed based on the voltage amplitude,i.e.,maintenance(M),decline(D),and near-zero(n).Evolution of the BOPP film from degradation to breakdown at different frequencies is ***,transition of discharge mode and elemental composition of the film are *** results show continuous heat generation under repetitive microsecond pulses is the dominant factor for degradation of BOPP *** number of applied pulses and the repetitive stressing time decrease exponentially with increase of *** research can be contributed to the safe and reliable operation of capacitors.

关键词： Aging breakdown film capacitor polypropylene repetitive pulse

Growth of Ag/g-C_(3)n_(4) nanocomposites on nickel foam to enhance photocatalytic degradation of formaldehyde under visible light

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Journal of Environmental Sciences 2024年第3期137卷 432-442页

作者： Ze Wang Zhi Huang Jiang yu Xiao shao Weidong Peng Jie yu y.ny.ng Jiang Department of Environmental Science and Engineering College of Architecture and EnvironmentSichuan UniversityChengdu 610065China Institute of new Energy and Low Carbon Technology Sichuan UniversityChengdu 610065China School of Agriculture and Environment University of Western AustraliaPerth 6907Western AustraliaAustralia yibin Institute of Industrial Technology Sichuan UniversityYibin 644000China

Formaldehyde is a pollutant that significantly affects the indoor air ***,conventional remediation approaches can be challenging to deal with low-concentration formaldehyde in an indoor *** this study,Photocatalysts of Ag/graphitic carbon nitride(g-C_(3)n_(4))/ni with 3D reticulated coral structure were prepared by thermal polymerization and liquid phase photo-deposition,using nickel foam(nF)as the *** demonstrated that when the Ag concentration was 3%,and the relative humidity was 60%,the ni/Ag/g-C_(3)n_(4)showed the maximum degradation rate of formaldehyde at 90.19%under visible light irradiation,and the formaldehyde concentration after degradation was lower than the Hygienic standard stated by the Chinese *** porous structure of ni/Ag/g-C_(3)n_(4)and the formation of Schottky junctions promoted the Adsorption efficiency and degradation of formaldehyde,while the nickel foam carrier effectively promoted the desorption of degradation ***,the degradation rate was only reduced by3.4%after 16 recycles,the three-dimensional porous structure extended the lifetime of the *** study provides a new strategy for the degradation of indoor formaldehyde at low concentrations.

关键词： Graphitic carbon nitride(g-C_(3)n_(4)) nickel foam(nF) Ag Formaldehyde Photocatalysis

Tuning synergy between nickel and iron in Ruddlesden-Popper perovskites through controllable crystal dimensionalities towards enhanced oxygenevolving activity and stability

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Carbon Energy 2024年第6期6卷 113-123页

作者： Haijuan Zhang Daqin Guan yuxing Gu Hengyue Xu Chunchang Wang Zongping shao youmin Guo School of Materials Science and Technology Anhui UniversityHefeiAnhuiChina Department of Building and Real Estate The Hong Kong Polytechnic UniversityHung HomHong KongChina WA School of Mines:Minerals Energy and Chemical EngineeringCurtin UniversityPerthWestern AustraliaAustralia State Key Laboratory of Materials-Oriented Chemical Engineering Nanjing Tech UniversityNanjingJiangsuChina Tsinghua Shenzhen International Graduate School Tsinghua UniversityShenzhenGuangdongChina

ni-Fe-based oxides are among the most promising catalysts developed to date for the bottleneck oxygen evolution reaction(OER)in water ***,understanding and mastering the synergy of ni and Fe remain ***,we report that the synergy between ni and Fe can be tailored by crystal dimensionality of ni,Fe-contained Ruddlesden-Popper(RP)-type perovskites(La_(0.125)Sr_(0.875))n+1(ni_(0.25)Fe_(0.75))nO3n+1(n=1,2,3),where the material with n=3 shows the best OER performance in alkaline *** X-ray absorption spectroscopy spectra before and after OER reveal that the material with n=3 shows enhanced ni/Fe-O covalency to boost the electron transfer as compared to those with n=1 and n=*** experimental investigations demonstrate that the Fe ion is the active site and the ni ion is the stable site in this system,where such unique synergy reaches the optimum at n=***,as n increases,the proportion of unstable rock-salt layers accordingly decreases and the leaching of ions(especially Sr^(2+))into the electrolyte is suppressed,which induces a decrease in the leaching of active Fe ions,ultimately leading to enhanced *** work provides a new avenue for rational catalyst design through the dimensional strategy.

关键词： crystal dimensionalities oxygen evolution reaction Ruddlesden-Popper perovskites synergy