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Photoinduced generation of alkyl and phthalimide nitrogen radicals from n-hydroxyphthalimide esters for the synthesis of benzophenone-type bioisosteres

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Science China Chemistry 2024年第10期67卷 3389-3396页

作者： Fei Li Jianyang Dong Huijuan Liao Jiayi Dang xuechen Zhou Yuying wang Chenya wang Qin Jiang Gang Li Dong xue Key Laboratory of Applied Surface and Colloid Chemistry Ministry of Education and School of Chemistry and Chemical EngineeringShaanxi Normal UniversityXi’an 710119China

n-Hydroxyphthalimide(nHPI)esters have emerged as powerful sources of alkyl radicals generated by single-electron transfer,but homolysis of nHPI ester to produce an alkyl radical and a phthalimide nitrogen radical is still in its *** this study,we developed a light-induced method for generation of alkyl and phthalimide nitrogen radicals from nHPI esters and subsequent reactions of the radicals with[1.1.1]propellane and aryl aldehydes for rapid generation of bicycle[1.1.1]pentane *** method does not require metals or photosensitizers,features a broad substrate scope(90 examples)and excellent functional group tolerance,and can be used for the functionalization of structurally complex.natural products and *** investigations indicate that the reaction involves photoinduced homolytic cleavage of the Cs_(2)CO_(3)-nHPI ester complex to produce alkyl and phthalimide nitrogen radicals and subsequent hydrogen atom transfer between the phthalimide nitrogen radical and the aldehyde to generate an acyl radical.

关键词： phthalimide nitrogen radicals aryl aldehydes hydrogen atom transfer bicycle[1.1.1]pentane ketones bioisosteres

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n-acetylcysteine ameliorates erectile dysfunction in rats with hyperlipidemia by inhibiting oxidative stress and corpus cavernosum smooth muscle cells phenotypic modulation

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Asian Journal of Andrology 2024年第1期26卷 99-106页

作者： Wei Ding Jun-Hong Fan Li-Ren Zhong nan-xiong wang Lu-Hao Liu Hai-Bo Zhang Li wang Ming-Qiang wang Bing-Lin He An-Yang Wei Department of Urology The First Affiliated Hospital of Guizhou University of Traditional Chinese MedicineGuiyang 550002China Department of Urology Guangdong Provincial People's HospitalGuangdong Academy of Medical SciencesGuangzhou 510000China Department of Urology Nanfang HospitalSouthern Medical UniversityGuangzhou 510000China Department of Urology Shenzhen Immigration Inspection General Station HospitalShenzhen 518000China Department of Organ Transplantation The Second Affiliated Hospital of Guangzhou Medical UniversityGuangzhou 510000China Department of Endocrinology The First Affiliated Hospital of Guizhou University of Traditional Chinese MedicineGuiyang 550002China

Hyperlipidemia is a major risk factor for erectile dysfunction(ED).Oxidative stress and phenotypic modulation of corpus cavernosum smooth muscle cells(CcSMCs)are the key pathological factors of ED.n-acetylcysteine(nAC)can inhibit oxidative stress;however,whether nAc can alleviate pathological variations in the corpus cavernosum and promote erectile function recovery in hyperlipidemic rats remains unclear.A hyperlipidemia model was established using 27 eight-week-old male Sprague-Dawley(SD)rats fed a high-fat and high-cholesterol diet(hyperlipidemic rats,HR).In addition,9 male SD rats were fed a normal diet to serve as controls(nC).HR rats were divided into three groups:HR,HR+normal saline(nS),and HR+nAC(n=9 for each group;nS or nAc intraperitoneal injections were administered daily for 16 weeks).Subsequently,the lipid profiles,erectile function,oxidative stress,phenotypic modulation markers of ccsMCs,and tissue histology were *** experimental results revealed that erectile function was significantly impaired in the HR and HR+nS groups,but enhanced in the HR+nAC *** lipid levels,over-activated oxidative stress,and multi-organ lesions observed in the HR and HR+nS groups were improved in the HR+nAC ***,the HR group showed significant phenotypic modulation of CCSMCs,which was also inhibited by nAC *** report focuses on the therapeutic effect of nAc in restoring erectile function using a hyperlipidemic rat model by preventing CcSMC phenotypic modulationand attenuating oxidativestress.

关键词： erectile dysfunction hyperlipidemia n-acetylcysteine oxidative stress henotypic modulation

Effect of(Cr,V)_(2)(C,n)on the Microstructure and Mechanical Properties of WC-10Co Cemented Carbides

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Journal of Wuhan University of Technology(Materials Science) 2024年第5期39卷 1138-1148页

作者： LI xiangkun wang Lu YE Jinwen School of Materials Science and Engineering Sichuan UniversityChengdu 610065China

WC-10Co cemented carbides with finer WC and narrower grain size distributions are produced by using(Cr,V)_(2)(C,n)as grain growth *** a result,with the increase of(Cr_(0.9),V_(0.1))_(2)(C,n)and(V_(0.9),Cr_(0.1))_(2)(C,n),the grains size of WC and mean free path of Co phase decrease,and adjacency of WC *** and homogenization of grains enhance the transverse rupture strength(TRS)and the ***,the deflection and bridging of cracks keep the fracture toughness at a respectable *** WC-10Co-0.6(Cr_(0.9),V_(0.1))_(2)(C,n)-0.025(V_(0.9),Cr_(0.1))_(2)(C,n)cemented carbides exhibit excellent comprehensive mechanical properties with the TRS of 4602.6 MPa,hardness of 1835 kg/mm^(2),and fracture toughness of 10.39 MPa·m^(1/2),***,the large pores are caused by excess n larger than 0.03 wt%and deteriorates the mechanical *** provide a new approach to WC-Co cemented carbides preparation with a narrow grain size distribution by adding novel grain growth inhibitors.

关键词： (Cr,V)_(2)(C,n) nutrient content WC grains size microstructure mechanical properties

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A stable implicit nodal integration-based particle finite element method(n-PFEM)for modelling saturated soil dynamics

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Journal of Rock Mechanics and Geotechnical Engineering 2024年第6期16卷 2172-2183页

作者： Liang wang xue Zhang Jingjing Meng Qinghua Lei Department of Earth Sciences ETH ZürichZürich8092Switzerland Department of Civil Engineering and Industrial Design University of LiverpoolLiverpoolL693BXUK Department of Civil Environmental and Natural Resources EngineeringLuleåUniversity of TechnologyLuleå97187Sweden Department of Earth Sciences Uppsala UniversityUppsala75105Sweden

In this study,we present a novel nodal integration-based particle finite element method(n-PFEM)designed for the dynamic analysis of saturated *** approach incorporates the nodal integration technique into a generalised Hellinger-Reissner(HR)variational principle,creating an implicit PFEM *** mitigate the volumetric locking issue in low-order elements,we employ a node-based strain smoothing *** discretising field variables at the centre of smoothing cells,we achieve nodal integration over cells,eliminating the need for sophisticated mapping operations after re-meshing in the *** express the discretised governing equations as a min-max optimisation problem,which is further reformulated as a standard second-order cone programming(SOCP)***,pore water pressure,and displacements are simultaneously determined using the advanced primal-dual interior point ***,our numerical model offers improved accuracy for stresses and pore water pressure compared to the displacement-based PFEM *** experiments demonstrate that the n-PFEM efficiently captures both transient and long-term hydro-mechanical behaviour of saturated soils with high accuracy,obviating the need for stabilisation or regularisation techniques commonly employed in other nodal integration-based PFEM *** work holds significant implications for the development of robust and accurate numerical tools for studying saturated soil dynamics.

关键词： Particle finite element method nodal integration Dynamic saturated media Second-order cone programming(SOCP)

Iron-nickel alloy particles with n-doped carbon “armor” as a highly selective and long-lasting catalyst for the synthesis of nbenzylaniline molecules

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nano Research 2024年第4期17卷 2308-2319页

作者： Gang wang Longchao Sun Wanyi Liu Haijuan Zhan Shuxian Bi College of Chemistry and Chemical Engineering Ningxia UniversityYinchuan 750021China

A scalable strategy for the convenient and rapid preparation of nitrogen-doped carbon-coated iron-based alloy catalysts was *** controlling the type and amount of metal salts in the precursor,various types of nitrogen-doped carbon-coated alloy catalysts can be prepared in a targeted ***_(2)ni2@Cn materials with small particle sizes and relatively homogeneous basic sites showed promising results in the n-alkylation reaction of benzyl alcohol with aniline(optimum yield:99%).It is worth noting that the catalyst can also be magnetically separated and recovered after the reaction,and its performance can be regenerated through simple ***,it was confirmed by kinetic experiments that the activation of C–H at the benzyl alcohol benzylic position is the rate-determining step(RDS).According to density flooding theory calculations,Fe_(2)ni2@Cn catalysts require less energy than other materials(Fe@Cn and ni@Cn)for the RDS(dehydrogenation reaction)*** n-alkylation reactions are more easily carried out on Fe_(2)ni2@Cn catalysts,which may be the reason for the best catalytic activity of Fe-ni alloy *** carbon-coated alloy materials will show great potential in more types of heterogeneous catalysis.

关键词： iron-nickel alloy catalyst n-alkylation reaction magnetic separation reaction path dehydrogenation reaction

Effect of tillage state of paddy soils with heavy metal pollution on the nosZ gene of n_(2)O reductase

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Journal of Environmental Sciences 2024年第3期137卷 469-477页

作者： Liping Jiang Shiguang Liu Shanyun wang Libo Sun Guibing Zhu Key Laboratory of Drinking Water Science and Technology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China School of Environmental and Civil Engineering Jiangnan UniversityWuxi 214122China

Paddy soils are an important source of atmospheric nitrous oxide(n_(2)O).However,numerous studies have focused on n_(2)O production during the soil tillage period,neglecting the n_(2)O production during the dry fallow *** this study,we conducted an incubation experiment using the acetylene inhibition technique to investigate n_(2)O emission and reduction rates of paddy soil profiles(0-1 m)from Guangdong Province and Jinlin Province in China,with different heavy-metal pollution *** abundance and community structures of denitrifying bacteria were determined via quantitative-PCR and Illumina MiSeq sequencing of nosZ,nirK,and nirS *** results showed that the potential n_(2)O emission rate,n_(2)O production rate,and denitrification rate have decreased with increasing soil vertical depth and heavy-metal *** importantly,we found that the functional gene type of n_(2)O reductase switched with the tillage state of paddy soils,which cladeⅡnos Z genes were the dominant gene during the tillage period,while cladeⅠnos Z genes were the dominant gene during the dry fallow *** heavy-metal pollution has less effect on the niche differentiation of the nos Z *** n_(2)O emission rate was significantly regulated by the genus Bradyhizobium,which contains both n_(2)O reductase and nitrite reductase *** findings suggests that the nos Z gene of n_(2)O reductase can significantly impact the n_(2)O emission from paddy soils.

关键词： Pappy soils n_(2)O reductase nosZ gene Heavy-metal pollution

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Regulating metal-acid double site balance on mesoporous SiO2-Al2O3 composite oxide for supercritical n-decane cracking

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Petroleum Science 2024年第4期21卷 2881-2891页

作者： Liu-Ling Chen Jun Zhang Chun-Guang Li Li-Qun Fei Bo wang Chen-Qi Zhang Yi Jiao Jian-Li wang Institute of new Energy and Low-Carbon Technology Sichuan University Engineering Research Center of Combustion and Cooling for Aerospace Power Ministry of Education School of Chemical Engineering Sichuan University State Key Laboratory of Industrial Vent Gas Reuse Southwest Institute of Chemical Co. Ltd Science and Technology on Scramjet Laboratory Beijing Power Machinery Research Institute

The balance between metal and acid sites directly affects the preparation of high-performance cracking catalysts with high heat sink and low ***,how to control acid-metal sites balance and its relationship with cracking performance are reported *** this work,a series of Pt/Al2O3-SiO2dual sites catalysts with different metal to acid active sites ratio(CM/CSA) were constructed by ethanolassisted impregnation method and the impact on n-decane cracking under supercritical conditions was systematically and deeply *** results showed that the conversion and carbon deposition increased gradually with varied CM/CSAand reached the balance at CM/CSAof *** proper ratio CM/CSA（0.13） can balance the deep dehydrogenation coking over metal active sites and high heat sink of cracking over acid active sites,the chemical heat sink reaches amazing 1.75 MJ/kg and carbon deposition is only22.03 mg/cm2at 750℃.Meanwhile,the few metal sites at low CM/CSAand the few strong acid sites at high CM/CSAare the main factors limiting the cracking *** CM/CSAlimit the activation of C-H bond and deep dehydrogenation of coking precursor,resulting in relative low cracking activity and carbon deposition,while high CM/CSAlimit the activation of C-C bond and increase the deep *** this contribution,design and construction of metal-acid dual sites can not only provide the technical solution for the preparation of high heat sink and low coking cracking catalyst,but also deepen the understanding of the cracking path of hydrocarbon fuel.

关键词： Metal-acid dual sites balance Catalytic cracking Hydrocarbon fuels Chemical heat sink Carbon deposition

Co/n co-doped flower-like carbon-based phase change materials toward solar energy harvesting

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Aggregate 2024年第1期5卷 321-330页

作者： xiao Chen Lei wang Yan Gao Yang Li xiaowei Zhang Yu Jiang Ge wang Institute of Advanced Materials Beijing Normal UniversityBeijingChina Beijing Advanced Innovation Center for Materials Genome Engineering Beijing Key Laboratory of Function Materials for Molecule and Structure ConstructionSchool of Materials Science and EngineeringUniversity of Science and Technology BeijingBeijingChina

The photothermal conversion capacity of pristine organic phase change materials(PCMs)is inherently insufficient in solar energy *** upgrade their photothermal conversion capacity,we developed bimetallic zeolitic imidazolate framework(ZIF)derived Co/n co-doped flower-like carbon(Co/n-FLC)-based composite PCMs toward solar energy harvesting.3D interconnected carbon framework with low interfacial thermal resistance,abundant carbon defects and high content of nitrogen doping,excellent localized surface plasmon resonance(LSPR)effect of Co nanoparticles,and light absorber Co_(3)ZnC in Co/n-FLC synergistically upgrade the photothermal capacity of(polyethylene glycol)PEG@Co/n-FLC composite PCMs with an ultrahigh photothermal conversion efficiency of 94.8%under 0.16 W/cm^(2).Uniformly anchored Co and Co_(3)ZnC nanoparticles in carbon framework guarantee excellent photon capture *** carbon nanotubes(CnTs)in 2D carbon nanosheets further accelerate the rapid transport of phonons by constructing cross-connected heat transfer ***,PEG@Co/n-FLC exhibits a thermal energy storage density of 100.69 J/g and excellent thermal stability and durable ***,PEG@Co/n-FLC composite PCMs are promising candidates to accelerate the efficient utilization of solar energy.

关键词： bimetallic ZIF Co/n co-doped carbon phase change materials photothermal conversion thermal energy storage

Flat Zn deposition at battery anode via an ultrathin robust interlayer

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nano Research 2024年第9期17卷 8104-8111页

作者： Yizhou wang Jianyu Chen Zibo Chen Qian He Zhengnan Tian Jin Zhao Yanwen Ma Husam n.Alshareef Materials Science and Engineering King Abdullah University of Science and Technology(KAUST)Thuwal 23955-6900Saudi Arabia State Key Laboratory of Organic Electronics and Information Displays(KLOEID)and Jiangsu Key Laboratory for Biosensors Institute of Advanced Materials(IAM)Nanjing University of Posts and TelecommunicationsNanjing 210023China Suzhou Vocational Institute of Industrial Technology Suzhou 215104China

Rechargeable aqueous zinc(Zn)ion batteries(AZIBs)using low-cost and safe Zn metal anodes are considered promising candidates for future grid-scale energy storage systems,but the Zn dendrite problem severely hinders the further prospects of *** Zn depositing behaviors toward horizontal alignment is highly effective and thus has received huge ***,such a strategy is usually based on previous substrate engineering,which requires complex preparation or expensive ***,it is essential to develop a novel solution that can realize horizontally aligned Zn flake deposition via easy operation and low ***,we report an ultrathin and robust Kevlar membrane as the interlayer to mechanically suppress Zn dendrite *** to the randomly distributed flaky dendrites in the control group,the deposited Zn sheets would grow into parallel alignment with the existence of such *** the dendrites are effectively suppressed,Zn||Cu asymmetric,Zn||Zn symmetric,and Zn||MnO_(2)full batteries using Kevlar interlayer deliver significantly improved cycling ***,the Zn||MnO_(2)pouch cell using a Kevlar interlayer delivers stable cycling performance and shows stable operation during multi-angle *** believe this work provides a new possibility for regulating Zn deposition from a crystallographic perspective.

关键词： Zn metal anodes Zn dendrites aqueous Zn ion batteries dendrite suppression (002)crystal plane