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Nano Research 2024年第1期17卷 372-381页

作者： Zhen Su§ Depeng Li§ Lixin Zhang Si Tian Yuhong Su Xiaoyun Hu Duan Xiong Qingqing Guan key laboratory of oil and Gas fine chemicals ministry of education College of Chemical EngineeringXinjiang UniversityUrumqi 830017China

Smart materials that integrate multi-stimuli response,full reversibility,and dual-visual read-out channel are highly desired for anticounterfeiting and information encryption applications.Herein,we developed a multiresponsive perchlorate terpyridyl Pt(Ⅱ)nano complex which could undergo fully reversible conversion between three forms stimulated by water or formaldehyde molecule due to the extent of Pt–Pt interaction.Meanwhile,a dual-visual channel,i.e.,the colorimetric channel changed from yellow to orange or red and the corresponding luminescent channel from orange to orange-red or red,has also been found.The weak and equivalent strength of ion-dipole interaction and hydrogen bond that generated between formaldehyde/water and Pt(II)salt result in the easy-control reversibility between the three forms.Furthermore,by introducing different polymer matrices,1Cl·ClO_(4)@PMMA(1Cl·ClO_(4):[Pt(tpy)Cl]·ClO4,tpy:2,2':6',2''-terpyridine),PMMA:poly(methyl methacrylate))and 1Cl·ClO4@PVA(PVA:polyvinyl alcohol)are successfully constructed,which exhibit different reversible behaviors since the PMMA and PVA matrix exert different influences on the strength of hydrogen-bond.Those smart Pt(II)salt nanostructures present great potential for high-security-level anticounterfeiting application.

关键词： Pt(II)complex multiresponse reversibility anticounterfeiting information encryption

Discovery and structure-activity relationship studies of novel tetrahydro-β-carboline derivatives as apoptosis initiators for treating bacterial infections

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Journal of Integrative Agriculture 2024年第4期23卷 1259-1273页

作者： Shanshan Su Hongwu Liu Junrong Zhang Puying Qi Yue Ding Ling Zhang Linli Yang Liwei Liu Xiang Zhou Song Yang National key laboratory of Green Pesticide/key laboratory of Green Pesticide and Agricultural Bioengineering Ministry of Education/Center for R&D of Fine ChemicalsGuizhou UniversityGuiyang 550025China

Developing and excavating new agrochemicals with highly active and safe is an important tactic for protecting crop health and food safety.In this paper,to discover the new bactericide candidates,we designed,prepared a new type of1,2,3,4-tetrahydro-β-carboline(THC)derivatives and evaluated the in vitro and in vivo bioactivities against the Xanthomonas oryzae pv.oryzae(Xoo),Xanthomonas axonopodis pv.citri(Xac),and Pseudomonas syringae pv.actinidiae(Psa).The in vitro bioassay results exhibited that most title molecules possessed good activity toward the three plant pathogenic bacteria,the compound A17 showed the most active against Xoo and Xac with EC50 values of 7.27 and 4.89 mg mL^(-1)respectively,and compound A8 exhibited the best inhibitory activity against Psa with EC50value of 4.87 mg mL^(-1).Pot experiments showed that compound A17 exhibited excellent in vivo antibacterial activities to manage rice bacterial leaf blight and citrus bacterial canker,with protective efficiencies of 52.67 and 79.79%at 200 mgmL^(-1),respectively.Meanwhile,compound A8 showed good control efficiency(84.31%)against kiwifruit bacterial canker at 200 mg mL^(-1).Antibacterial mechanism suggested that these compounds could interfere with the balance of the redox system,damage the cell membrane,and induce the apoptosis of Xoo cells.Taken together,our study revealed that tetrahydro-β-carboline derivatives could be a promising candidate model for novel broadspectrum bactericides.

关键词： tetrahydro-β-carboline derivatives antibacterial activity ROS cell apoptosis

Bactericidal bissulfone B7 targets bacterial pyruvate kinase to impair bacterial biology and pathogenicity in plants

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Science China(Life Sciences) 2024年第2期67卷 391-402页

作者： Awei Zhang Haizhen Zhang Ronghua Wang Hongfu He Baoan Song Runjiang Song National key laboratory of Green Pesticide Key Laboratory of Green Pesticide and Agricultural BioengineeringMinistry of EducationCenter for R&D of Fine Chemicals of Guizhou UniversityGuiyang 550025China

The prevention and control of rice bacterial leaf blight(BLB)disease has not yet been achieved due to the lack of effective agrochemicals and available targets.Herein,we develop a series of novel bissulfones and a novel target with a unique mechanism to address this challenge.The developed bissulfones can control Xanthomonas oryzae pv.oryzae(Xoo),and 2-(bis(methylsulfonyl)methylene)-N-(4-chlorophenyl)hydrazine-1-carboxamide(B_(7))is more effective than the commercial drugs thiodiazole copper(TC)and bismerthiazol(BT).Pyruvate kinase(PYK)in Xoo has been identified for the first time as the target protein of our bissulfone B_(7).PYK modulates bacterial virulence via a CRP-like protein(Clp)/two-component system regulatory protein(reg R)axis.The elucidation of this pathway facilitates the use of B_(7)to reduce PYK expression at the transcriptional level,block PYK activity at the protein level,and impair the interaction within the PYK-Clp-reg R complex via competitive inhibition,thereby attenuating bacterial biology and pathogenicity.This study offers insights into the molecular and mechanistic aspects underlying anti-Xoo strategies that target PYK.We believe that these valuable discoveries will be used for bacterial disease control in the future.

关键词： 2-bissulfone-N-phenylhydrazine-1-carboxamide derivatives Xoo antibacterial activities pyruvate kinase regulatory mechanism

Sustainable electrochemical dearomatization for the synthesis of diverse 2,3-functionalized indolines

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Green Synthesis and Catalysis

Green Synthesis and Catalysis 2024年第1期5卷 25-30页

作者： Jun Chen Rong Zhang Caiyan Ma Peng Zhang Yonghong Zhang Bin Wang Fei Xue Weiwei Jin Yu Xia Chenjiang Liu Urumqi key laboratory of Green Catalysis and Synthesis Technology Key Laboratory of Oil and Gas Fine ChemicalsMinistry of Education&Xinjiang Uygur Autonomous RegionState Key Laboratory of Chemistry and Utilization of Carbon Based Energy ResourcesCollege of ChemistryCollege of Future TechnologyXinjiang UniversityUrumqi 830017China

Herein,we achieved a green and efficient dearomatization for the synthesis of 2,3-functionalized polycyclic indolines in an electrochemical way.This avoiding of external oxidants and metals approach allowed various nucleophilic sources(Nu¼anilines,TMSN3 and ROH)to perform the products,representing an environmentally benign means.Additionally,the continuous flow electrosynthesis and synthetic transformations also reveal the strong practicality of electrochemistry in organic synthesis.

关键词： Green synthesis Organic electrochemistry Indole Dearomatization Cyclization

Morphology effect on catalytic performance of ebullated-bed residue hydrotreating over Ni-Mo/Al_(2)O_(3)catalyst:a kinetic modeling study

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Green Chemical Engineering 2024年第1期5卷 60-67页

作者： Zhe Liu Juncong Yuan Zongzhuang Sun Xiang Feng Yibin Liu Huihong Zhu Chong Peng Chaohe Yang State key laboratory of Heavy oil Processing China University of PetroleumQingdao266580China Dalian Research Institute of Petroleum and Petrochemicals SINOPECDalian116045China State key laboratory of fine chemicals Dalian University of TechnologyDalian116024China

Upgrading of vacuum residue is of prime industrial significance due to the increasing demand for light oils.Elucidating the effect of catalyst morphology on vacuum residue hydrotreating performance by kinetic modeling is therefore of great importance.Herein,kinetic analysis of hydrodemetallization(HDM)and hydrodeconradsoncarbon-residue(HDCCR)performances on industrial Ni-Mo/Al_(2)O_(3)catalysts with spherical and cylindrical morphologies in ebullated-bed were evaluated for more than 1600 h.It was found that the percentage of light impurities easier to be removed on spherical catalysts were 78.20%and 39.43%in HDM and HDCCR reactions,respectively,higher than 65.20%and 17.50%on cylindrical catalysts.This suggests that catalyst morphology affects the impurity removal ability and the impurity properties,resulting in better hydrotreating performance of spherical catalysts.This work not only combines catalyst morphology with impurity removal capability through kinetic modeling,but also provides new insights into the design of efficient hydrotreating catalysts.

关键词： Morphology effect Kinetic analysis Vacuum residue Hydrotreating

Electrooxidative trifunctionalization of alkenes with N-chlorosuccinimide and ArSSAr/ArSH to α,β-dichloride arylsulfoxides

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Green Synthesis and Catalysis

Green Synthesis and Catalysis 2024年第2期5卷 131-135页

作者： Guohui Qin Renjie Wang Zhen Cheng Yonghong Zhang Bin Wang Yu Xia Weiwei Jin Chenjiang Liu Urumqi key laboratory of Green Catalysis and Synthesis Technology Key Laboratory of Oil and Gas Fine ChemicalsMinistry of Education&Xinjiang Uygur Autonomous RegionState Key Laboratory of Chemistry and Utilization of Carbon Based Energy ResourcesCollege of ChemistryXinjiang UniversityUrumqi 830017China

An unprecedented electrochemical oxidative trifunctionalization of olefins with diaryl disulfides/aryl thiols and N-chlorosuccinimide in an aqueous system is developed.Two C-Cl bonds,one C-S bond,and one S=O bond are produced simultaneously in one step from simple and commercially available starting materials with clean energy.This tandem methodology features as mild reaction conditions,transition metal and additional oxidant free,broad substrate scope,good functional group compatibility,and gram scale preparation.

关键词： Electrooxidation Alkenes functionalization Vicinal dichlorination Sulfoxidation Tandem reaction

Gelation mechanisms of gel polymer electrolytes for zinc-based batteries

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Chinese Chemical Letters 2024年第5期35卷 97-116页

作者： Mengjun Sun Zhi Wang Jvhui Jiang Xiaobing Wang Chuang Yu Collaborative Innovation Center of Henan Province for Green Manufacturing of fine chemicals Key Laboratory of Green Chemical Media and ReactionsMinistry of EducationSchool of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiang 453007China key laboratory for Yellow River and Huaihe River Water Environment and Pollution Control Ministry of EducationHenan Key Laboratory for Environmental Pollution ControlSchool of EnvironmentHenan Normal UniversityXinxiang 453007China State key laboratory of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic EngineeringHuazhong University of Science and TechnologyWuhan 430074China

Zinc-based batteries(ZBs)have been deemed as a potential substitute for lithium-ion batteries due to its unique advantages of abundant resources,low cost and acceptable energy density.Despite great progress in designing electrode materials has been made,the development of high-performance ZBs still remain challenges,such as the dendrite growth of zinc anode,hydrogen evolution reaction,limited electrochemical stability window,water evaporation and liquid leakage.Gel polymer electrolytes(GPEs),including hydrous GPEs with low content of active water and anhydrous GPEs without the presence of water,are proposed to avoid these problems.Furthermore,employing GPEs is conductive to fabricate flexible devices owing to the good mechanical strength.To date,most of researches focus on discovering new GPEs and exploring its application on flexible or wearable devices.Recent reviews also have outlined the polymer matrixes and advances of GPEs in various battery systems.Given this,herein,we seek to summarize the gelation mechanisms of GPEs,involving physical gel of polymer,chemical crosslinking of polymer and chemical polymerization of monomers.Peculiarly,the preparation methods are also classified.In addition,not only the features and central conundrum of GPEs are analyzed but also the corresponding strategies are discussed,contributing to design GPEs with ideal properties for high-performance ZBs.

关键词： Gelation mechanisms Gel polymer electrolytes Zinc-based batteries Gelation methods

Synthesis of poly(thiourethane-alt-thioester) by alternating ring-opening copolymerization of N-thiocarboxyanhydrides and episulfides

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Science China Chemistry 2024年

作者： Wei Xiong Tianjun Yue Haiwang Lai Chunyan Lü Weimin Ren Hua Lu Beijing National laboratory for Molecular Sciences Center for Soft Matter Science and Engineering Key Laboratory of Polymer Chemistry and Physics of Ministry of Education College of Chemistry and Molecular Engineering Peking University State key laboratory of fine chemicals Dalian University of Technology

Polythiourethanes(PTU) and polythioesters(PTE) derived from renewable sources are emerging sustainable polymers for their excellent degradability and recyclability. However, P(TU-alt-TE) copolymers have been rare and challenging to synthesize.Here, we report the efficient synthesis of novel P(TU-alt-TE) copolymers via the alternating copolymerization of N-thiocarboxyanhydrides(NTA)/episufides(ES) and provide mechanistic insight into the alternating chain propagation process via density functional theory(DFT) calculation. The incorporation of ESs into traditional peptide backbone is capable of adjusting the glass transition temperature below thermal decomposition temperature, which confers better thermal processability by regulating the rigidity of the backbone and the hydrogen bond interaction among the polymer chains. Crosslinked PTUs with tailored properties are accessible by altering the feeding ratio of NTAs and(bifunctional) ESs. Moreover, the thiourethane in the backbone can endow interesting underwater adhesion properties to the materials. Considering the broad scope of NTA and ES monomers, this method is expected to provide a promising and general route to a wide range of P(TU-alt-TE) copolymers with diverse properties.

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Waste to treasure:Reutilization of fluid catalytic cracking coke block as photothermal conversion material for water evaporation

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Particuology 2024年第5期88卷 62-70页

作者： Zhuwei Gao Chengxin Li Jingjing He Zhuo Wang Xinyu Qi Lan He Shihao Wang Zhongxin Liu School of Chemical Engineering and Technology Hainan UniversityHaikou 570228China TJ-YZ School of Network Science Haikou University of EconomicsHaikou 570203China School of Food Science and Engineering Hainan UniversityHaikou 570228China key laboratory of Advanced Materials of Tropical Island Resources of ministry of education Hainan UniversityHaikou 570228China Hainan Provincial key laboratory of fine chemicals Hainan UniversityHaikou 570228China

This study aims to analyze the coking process and propose an effective method for the reutilization of fluid catalytic cracking(FCC)coke block.Herein,we analyzed the basic characteristics and chemical composition of FCC coke blocks.The results showed that the main components were carbon,oxygen,and aluminum,accounting for 60.8%,26.6%,and 11.5%,respectively.Under the conventional catalytic cracking reaction temperature from 500°C to 600°C,the formation of the first aromatic hydrocarbon was particularly important for the formation of coke.The condensation of oil-gas-entrained catalyst particles and their heavy components was the physical cause of coking,while the dehydrogenation condensation reaction of oil-gas heavy components was the chemical factor.In addition,the membrane prepared by powdered coke had excellent photothermal conversion ability,which could be heated to more than 110°C within 360 s under two fixed light intensities.The evaporation rate of photothermal water was 5.89 kg m 2 h−1,which has great industrial application potential.These works provide a novel and effective method of separation membrane for the reutilization of FCC coke blocks.

关键词： Coking process Reutilization of FCC coke Carbonaceous deposition Membrane Photothermal conversion

Facile molybdenum and aluminum recovery from spent hydrogenation catalyst

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Chinese Journal of Chemical Engineering 2024年第5期69卷 72-78页

作者： Zhenhui Lv Jianan Li Dong Xue Tao Yang Gang Wang Chong Peng State key laboratory of fine chemicals School of Chemical EngineeringDalian University of TechnologyDalian 116024China Dalian Research Institute of Petroleum and Petrochemicals SINOPECDalian 116041China

Industrial catalyst waste has emerged as a hazardous pollutant that requires safe and proper disposal after the unloading process.Finding a valuable and sustainable strategy for its treatment is a significant challenge compared to traditional methods.In this study,we present a facile method for the recovery of molybdenum and aluminum contents from spent Mo-Ni/Al_(2)O_(3) hydrogenation catalysts through crystallization separation and coprecipitation.Furthermore,the recovered molybdenum and aluminum are utilized as active metals and carriers for the preparation of new catalysts.Their properties were thoroughly analyzed and investigated using various characterization techniques.The hydrogenation activity of these newly prepared catalysts was evaluated on a fixed-bed small-scale device and compared with a reference catalyst synthesized from commercial raw reagents.Finally,the hydrogenation activity of the catalysts was further assessed by using the entire distillate oil of coal liquefaction as the raw oil,specifically focusing on denitrogenation and aromatic saturation.This work not only offers an effective solution for recycling catalysts but also promotes sustainable development.

关键词： Waste treatment Alumina Hydrogenation Catalyst Crystallization Precipitation