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Symmetry dependent activation and reactivity of peroxysulfates on FeS_(2)(001)surface

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Science Bulletin 2024年第2期69卷 154-158页

作者： Cancan Ling Meiqi Li Hao Li Xiufan Liu Guangming Zhan Hongwei Sun Chuan Liang Yaling Li Bing Zhou Jincai Zhao Lizhi Zhang School of Environmental Science and Engineering Shanghai Jiao Tong UniversityShanghai 200240China Key Laboratory of pesticide&Chemical Biology of Ministry of Education Institute of Environmental&Applied ChemistryCentral China Normal UniversityWuhan 430079China

Heterogeneous peroxysulfates-based advanced oxidation processes(AOPs)have garnered significant attention for purifying organic wastewater since they offer many advantages like low cost,safe storage,facile activation and reactive species participation[1].Nonradical and radical pathways have been proposed to be involved in peroxysulfates activation.

关键词： activation radical reactivity

Synergy of heterogeneous Co/Ni dual atoms enabling selective C-O bond scission of lignin coupling with in-situ N-functionalization

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Journal of Energy Chemistry 2024年第5期92卷 16-25页

作者： Baoyu Wang Jinshu Huang Hongguo Wu Ximing Yan Yuhe Liao Hu Li National Key Laboratory of Green pesticide Key Laboratory of Green Pesticide&Agricultural BioengineeringMinistry of EducationState-Local Joint Laboratory for Comprehensive Utilization of BiomassCollege of Pharmacy&Center for R&D of Fine ChemicalsGuizhou UniversityGuiyang 550025GuizhouChina Guangxi Key Laboratory of Green Chemical Materials and Safety Technology Beibu Gulf UniversityQinzhou 535011GuangxiChina Guangzhou institute of Energy Conversion Chinese Academy of SciencesGuangzhou 510640GuangdongChina

Selective cleavage of Csp^(2)-OCH_(3)bond in lignin without breaking other types of C-O bonds followed by N-functionalization is fascinating for on-purpose valorization of biomass.Here,a Co/Ni-based dual-atom catalyst CoNiDA@NC prepared by in-situ evaporation and acid-etching of metal species from tailor-made metal–organic frameworks was efficient for reductive upgrading of various lignin-derived phenols to cyclohexanols(88.5%–99.9%yields),which had ca.4 times higher reaction rate than the single-atom catalyst and was superior to state-of-the-art heterogeneous catalysts.The synergistic catalysis of Co/Ni dual atoms facilitated both hydrogen dissociation and hydrogenolysis steps,and could optimize adsorption configuration of lignin-derived methoxylated phenols to further favor the Csp^(2)-OCH_(3)cleavage,as elaborated by theoretical calculations.Notably,the CoNi_(DA)@NC catalyst was highly recyclable,and exhibited excellent demethoxylation performance(77.1%yield)in real lignin monomer mixtures.Via in-situ cascade conversion processes assisted by dual-atom catalysis,various high-value N-containing chemicals,including caprolactams and cyclohexylamines,could be produced from lignin.

关键词： Biomass conversion Heterogeneous catalysis Lignin Dual-atom catalyst Selective C-ocleavage

Morpho-cultural, Pathogenicity and Molecular Characterization of Phyllosticta capitalensis Inciting Cavendish Banana Freckle Disease in Hainan

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Plant Diseases and Pests 2024年第3期15卷 5-7页

作者： Yanxiang QI Hong ZHAO Zhaojing ZHANG Yanfei OUYANG Xin ZHANG Environment and Plant Protection institute Chinese Academy of Tropical Agricultural SciencesHaikou 571101China State 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 College of Plant Science and Technology of Huazhong Agricultural University Wuhan 430070China

[Objectives]The study was to identify the casual agent of freckle disease on Cavendish banana in Hainan Province,China.[Methods]Fungal isolates were isolated from affected leaf tissues and identified by the morphological features,molecular identification and pathogenicity test.[Results]The fungus isolated from affected leaf tissues was identified as Phyllosticta capitalensis based on the morphological properties of the colony and spore,coupled with sequence analyses of the internal transcribed spacer(ITS)region and the large subunit(LSU)rDNA gene.Koch s postulates were fulfilled by successfully re-isolating the pathogen from the artificial inoculated leaves.[Conclusions]P.capitalensis is a new pathogen responsible for Cavendish banana freckle disease in Hainan.

关键词： Phyllosticta capitalensis Cavendish banana Freckle disease

Unveiling the geometric site dependent activity of spinel Co_(3)O_(4)for electrocatalytic chlorine evolution reaction

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Journal of Energy Chemistry 2024年第5期92卷 95-103页

作者： Linke Cai Yao Liu Jingfang Zhang Qiqi Jia Jiacheng Guan Hongwei Sun Yu Yu Yi Huang Key Laboratory of pesticide&Chemical Biology of Ministry of Education Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction of Ministry of EducationCollege of ChemistryCentral China Normal UniversityWuhan 430079HubeiChina Key Laboratory of Green Chemical Engineering Process of Ministry of Education Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of EducationHubei Key Laboratory of Novel Reactor and Green Chemical TechnologySchool of Chemical Engineering&PharmacyWuhan Institute of TechnologyWuhan 430205HubeiChina College of Materials Science and Engineering Fuzhou UniversityFuzhou 350108FujianChina School of Chemistry and Chemical Engineering Anhui UniversityHefei 230601AnhuiChina

Spinel cobalt oxide(Co_(3)O_(4)),consisting of tetrahedral Co^(2+)(CoTd)and octahedral Co^(3+)(CoOh),is considered as promising earth-abundant electrocatalyst for chlorine evolution reaction(CER).Identifying the catalytic contribution of geometric Co site in the electrocatalytic CER plays a pivotal role to precisely modulate electronic configuration of active Co sites to boost CER.Herein,combining density functional theory calculations and experiment results assisted with operando analysis,we found that the Co_(Oh) site acts as the main active site for CER in spinel Co_(3)O_(4),which shows better Cl^(-)adsorption and more moderate intermediate adsorption toward CER than CoTd site,and does not undergo redox transition under CER condition at applied potentials.Guided by above findings,the oxygen vacancies were further introduced into the Co_(3)O_(4) to precisely manipulate the electronic configuration of Co_(Oh) to boost Cl^(-)adsorption and optimize the reaction path of CER and thus to enhance the intrinsic CER activity significantly.Our work figures out the importance of geometric configuration dependent CER activity,shedding light on the rational design of advanced electrocatalysts from geometric configuration optimization at the atomic level.

关键词： Chlorine evolution reaction Geometry effects Active chlorine Electronic configuration optimization Spinel oxides

Tumor-targeted self-assembled micelles reducing PD-L1 expression combined with ICIs to enhance chemo-immunotherapy of TNBC

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Chinese Chemical Letters 2024年第2期35卷 305-310页

作者： Hongda Zhu Kai Ma Rui Ruan Chaobo Yang Aqin Yan Jing Li Qi Yu Hongmei Sun Mingxing Liu Hongmei Zheng Jing Gao Xiaofang Guan Zhu Dai Yao Sun Cooperative Innovation Center of Industrial Fermentation (Ministry of Education & Hubei Province) Key Laboratory of Fermentation Engineering (Ministry of Education)National “111” Center for Cellular Regulation and Molecular PharmaceuticsSchool of Food and Biological EngineeringHubei University of TechnologyWuhan 430068China Hubei Cancer Hospital Tongji Medical CollegeHuazhong University of Science and TechnologyWuhan 430079China National Key Laboratory of Green pesticide College of ChemistryCentral China Normal UniversityWuhan 430079China Key Laboratory of Medical Optics Suzhou Institute of Biomedical Engineering and TechnologyChinese Academy of SciencesSuzhou 215163China Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science Ministry of EducationQingdao University of Science and TechnologyQingdao 266000China

Immune checkpoint inhibitors(ICIs)therapy targeting programmed cell death ligand 1(PD-L1)and programmed death protein 1(PD-1)had exhibited significant clinical benefits for cancer treatment such as triple negative breast cancer(TNBC).However,the relatively low anti-tumor immune response rate and ICIs drug resistance highlight the necessity of developing ICIs combination therapy strategies to improve the anti-tumor effect of immunotherapy.Herein,the immunomodulator epigallocatechin gallate palmitate(PEGCG)and the immunoadjuvant metformin(MET)self-assembled into tumor-targeted micelles via hydrogen bond and electrostatic interaction,which encapsulated the therapeutic agents doxorubicin(DOX)-loaded PEGCG-MET micelles(PMD)and combined with ICIs(anti-PD-1 antibody)as therapeutic strategy to reduce the endogenous expression of PD-L1 and improve the tumor immunosuppressive microenvironment.The results presented that PMD integrated chemotherapy and immunotherapy to enhance antitumor efficacy in vitro and in vivo,compared with DOX or anti-PD-1 antibody for the therapy of TNBC.PMD micelles might be a potential candidate,which could remedy the shortcomings of antibody-based ICIs and provide synergistic effect to enhance the antitumor effects of ICIs in tumor therapy.

关键词： Immunotherapy Tumor-targeted Self-assembled micelles Metformin Reducing PD-L1 expression TNBC

Establishment of a system for screening and identification of novel bactericide targets in the plant pathogenic bacterium Xanthomonas oryzae pv. oryzae using Tn-seq and SPR

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Journal of Integrative Agriculture 2024年第5期23卷 1580-1592页

作者： Chaoyue Pang Ling Jin Haoyu Zang Damalk Saint-Claire SKoklannou Jiazhi Sun Jiawei Yang Yongxing Wang Liang Xu Chunyan Gu Yang Sun Xing Chen Yu Chen School of Plant Protection Anhui Agricultural UniversityHefei 230036China institute of Plant Protection and Agro-Products Safety Anhui Academy of Agricultural SciencesHefei 230031China Anhui Province Laboratory for Green pesticide Development and Application School of Plant ProtectionAnhui Agricultural UniversityHefei230036China Hefei Research Center State Key Laboratory for Biology of Plant Diseases and Insect PestsHefei 230036China Key Laboratory of Integrated Crop Pest Management of Anhui Province School of Plant ProtectionAnhui Agricultural University Hefei230036China Shandong Vicome Greenland Chemical Co. Ltd.Jinan 250204China

Xanthomonas spp. cause severe bacterial diseases. However, effective strategies for prevention and management of these diseases are scarce. Thus, it is necessary to improve the efficiency of control of diseases caused by Xanthomonas. In this study, Xanthomonas oryzae pv. oryzae(Xoo), which causes rice bacterial leaf blight, has been studied as a representative. A transposon insertion library of Xoo, comprising approximately 200,000 individual insertion mutants, was generated. Transposon sequencing data indicated that the mariner C9 transposase mapped at 35.7–36.4% of all potential insertion sites, revealing 491 essential genes required for the growth of Xoo in rich media. The results show that, compared to the functions of essential genes of other bacteria, the functions of some essential genes of Xoo are unknown, 25 genes might be dangerous for the Xanthomonas group, and 3 are specific to Xanthomonas. High-priority candidates for developing broad-spectrum, Xanthomonas-specific, and environment-friendly bactericides were identified in this study. In addition, this study revealed the possible targets of dioctyldiethylenetriamine using surface plasmon resonance(SPR) in combination with high performance liquid chromatography–mass spectrometry(HPLC–MS). The study also provided references for the research of some certain bactericides with unknown anti-bacterial mode of action. In conclusion, this study urged a better understanding of Xanthomonas,provided meaningful data for the management of bacterial leaf blight, and disclosed selected targets of a novel bactericide.

关键词： rice bacterial leaf blight Xanthomonas essential genes Tn-seq dioctyldiethylenetriamine

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单分子结中的有机自由基

Science China Materials 2024年第3期67卷 709-728页

作者：张雅琦邱仁慧屈恺张成 J.Fraser Stoddart 陈洪亮 Stoddart institute of Molecular Science Department of ChemistryZhejiang UniversityHangzhou 310021China Zhejiang-Israel Joint Laboratory of Self-Assembling Functional Materials ZJU-Hangzhou Global Scientific and Technological Innovation CentreZhejiang UniversityHangzhou 311215China Department of Chemistry and Innovation Center of pesticide Research China Agricultural UniversityBeijing 100193China Department of Chemistry The University of Hong KongHong Kong SAR 999077China School of Chemistry University of New South WalesSydneyNSW 2052Australia Beijing National Laboratory for Molecular Sciences Beijing 100871China

空气稳定有机自由基的发现引起了人们对探究其在分子电子学和自旋电子学中应用的兴趣.这些自由基具有独特的开壳层电子结构,因而表现出特殊的电学特性.由于其较弱的旋轨耦合特性,也使得其成为自旋电子学的重要研究对象.此外,自由基还可... 详细信息

空气稳定有机自由基的发现引起了人们对探究其在分子电子学和自旋电子学中应用的兴趣.这些自由基具有独特的开壳层电子结构,因而表现出特殊的电学特性.由于其较弱的旋轨耦合特性,也使得其成为自旋电子学的重要研究对象.此外,自由基还可以通过二聚、分子识别和机械互锁等分子间相互作用来构筑超分子器件.本文综述了空气稳定有机自由基在电子学及自旋电子学中的应用,通过详述其卓越的电磁性能来拓展启发分子设计的多样性.本综述还概述了超分子自由基的制备方法和相关性质的研究进展,拓宽了单分子研究的范围.此外,自由基介导的单分子反应是一个新兴的研究方向,本文也对该领域的未来发展方向进行了展望.通过阐明空气稳定有机自由基的应用潜力,本文将有望对分子电子学和自旋电子学的研究产生一定的指导意义.

关键词： air-stable radicals molecular electronics spintronics supramolecular devices

Invasion of fall armyworm led to the succession of maize pests in Southwest China

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Journal of Integrative Agriculture 2024年第4期23卷 1300-1314页

作者： Zezheng Fan Yifei Song Shengyuan Zhao Kongming Wu Agricultural Information institute Chinese Academy of Agricultural SciencesBeijing 100081China Guangdong Laboratory for Lingnan Modern Agriculture Guangzhou 510642China State Key Laboratory for Biology of Plant Diseases and Insect Pests Institute of Plant ProtectionChinese Academy of Agricultural SciencesBeijing 100193China

The invasive fall armyworm Spodoptera frugiperda(J.E.Smith)invaded Asia in 2018,colonizing the tropical and southern subtropical regions as well as migrating with the monsoons into Northeast Asia during spring and summer.This has resulted in widespread infestations,with significant impacts on maize production in various Asian countries.Previous studies have shown that the invasion of this pest can alter the species relationships of maize pests,but the actual impact on maize pest management is still unclear.This study investigated the changes in maize pest occurrence and pesticide use in the annual breeding areas of S.frugiperda in Yunnan Province and the Guangxi Zhuang Autonomous Region of China during 2017-2021,based on surveys and interviews with small farmers in maize production.The results showed that S.frugiperda has emerged as the dominant species among maize pests after invasion and colonization,replacing traditional pests such as Ostrinia furnacalis,Spodoptera litura,Agrotis ypsilon,and Rhopalosiphum maidis.The variety of pesticides used for maize pest control has changed from chlorpyrifos,lambda-cyhalothrin,and acetamiprid to emamectin benzoate-based pesticides with high effectiveness against S.frugiperda.Furthermore,the frequency of maize pest chemical applications has increased from an average of 5.88 to 7.21 times per season,with the amounts of pesticides used in summer and autumn maize being significantly higher than in winter and spring maize,thereby increasing application costs by more than 35%.The results of this study clarified the impact of S.frugiperda invasion on maize pest community succession and chemical pesticide use in tropical and south subtropical China,thereby providing a baseline for modifying the regional control strategies for maize pests after the invasion of this relatively new pest.

关键词： Spodoptera frugiperda annual breeding region sweet waxy corn economic evaluation

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单分子结中的有机自由基（英文）

Science China Materials 2024年

作者：张雅琦邱仁慧屈恺张成 J.Fraser Stoddart 陈洪亮 Zhejiang-Israel Joint Laboratory of Self-Assembling Functional Materials ZJU-Hangzhou Global Scientific and Technological Innovation Centre Zhejiang University Department of Chemistry The University of Hong Kong Stoddart institute of Molecular Science Department of Chemistry Zhejiang University Beijing National Laboratory for Molecular Sciences Beijing 100871 China Department of Chemistry and Innovation Center of pesticide Research China Agricultural University School of Chemistry University of New South Wales

空气稳定有机自由基的发现引起了人们对探究其在分子电子学和自旋电子学中应用的兴趣.这些自由基具有独特的开壳层电子结构,因而表现出特殊的电学特性.由于其较弱的旋轨耦合特性,也使得其成为自旋电子学的重要研究对象.此外,自由基还可...

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