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Chinese Journal of Structural Chemistry 2021年第12期40卷 1647-1654,1554页

作者：任惠东李康明易阳杰王曼叶姣胡艾希陈云欧晓明李建明 College of Chemistry and Chemical Engineering Hunan UniversityChangsha 410082China National Pesticide Creation Engineering Technology Research Center Hunan Research Institute of Chemical Industry Co.Ltd.Changsha 410007China

Four novel 2-methoxyimino phenylacetate derivatives containing 1,3,4-oxadiazole ring were designed and synthesized from the key intermediate of Trifloxystrobin or Azoxystrobin via intermediate derivatization and active structure splicing.The chemical structures of the target compounds were confirmed by]H NMR,13C NMR and elemental analysis.The crystal structure of methyl(E)-2-(methoxyimino)-2-(2-(((5-((4-methoxyphenoxy)methyl)-1,3,4-oxadiazol-2-yl)thio)methyl)phenyl)acetate(Al)was determined by single-crystal X-ray diffraction.Compound A1 belongs to triclinic system,space group Pi with two molecules in each unit cell.The benzene ring plane C(2)-C(3)-C(4)-C(5)-C(6)-C(7)and oxazole ring plane are nearly parallel with the dihedral angle of 6.4°.The benzene ring plane C(12)-C(13)-C(14)-C(15)-C(16)-C(17)and oxazole ring plane are not perpendicular with the dihedral angle of 49.4°.The crystal of compound Al is stabilized by π-π stacking interactions.The fungicidal activities of the target compounds against four plant pathogenic fungi in vitro were tested,and some of them had good activities.The DFT calculation was carried out to study the structure-activity relationship of the title derivatives using Gasian 09 and Multiwfii 3.6.

关键词： 2-methoxyimino phenylacetate derivatives synthesis crystal structure fungicidal activities DFT calculation

High active amorphous Co(OH)_(2) nanocages as peroxymonosulfate activator for boosting acetaminophen degradation and DFT calculation

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Chinese Chemical Letters 2021年第5期32卷 1814-1818页

作者： Juanjuan Qi Juzhe Liu Fengbin Sun Taobo Huang Jun Duan Wen Liu The Key Laboratory of Resources and Environmental Systems Optimization Ministry of EducationCollege of Environmental Science and EngineeringNorth China Electric Power UniversityBeijing 102206China The Key Laboratory of Water and Sediment Sciences Ministry of EducationCollege of Environmental Sciences and EngineeringPeking UniversityBeijing 100871China School of Chemistry and Beijing Advanced Innovation Center for Biomedical Engineering Beihang UniversityBeijing 100191China State Environmental Protection Key Laboratory of All Material Fluxes in River Ecosystems Peking UniversityBeijing 100871China

Acetaminophen(ACE)is commonly used in analgesic and antipyretic drug,which is hardly removed by traditional wastewater treatment processes.Herein,amorphous Co(OH)_(2)nanocages were explored as peroxymonosulfate(PMS)activator for efficient degradation of ACE.In the presence of amorphous Co(OH)_(2)nanocages,100%of ACE removal was reached within 2 min with a reaction rate constant k_(1)=3.68 min 1 at optimum pH 5,which was much better than that of crystallineβ-Co(OH)_(2)and Co_(3)O_(4).Amorphous materials(disorder atom arrangement)with hollow structures possess large specific surface area,more reactive sites,and abundant vacancies structures,which could efficiently facilitate the catalytic redox reactions.The radicals quenching experiment demonstrated that SO_(4)^(·-)radicals dominated the ACE degradation rather than^(·)OH radicals.The mechanism of ACE degradation was elucidated by the an alysis of degradation in termediates and theoretical calculation,indicating that the electrophilic SO_(4)^(·-)and^(·)OH tend to attack the atoms of ACE with high Fukui index(f).Our finding highlights the remarkable advantages of amorphous materials as heterogeneous catalysts in sulfate radicals-based AOPs and sheds new lights on water treatment for the degradation of emerging organic contaminants.

关键词： Amorphous Co(OH)_(2) Peroxymonosulfate(PMS) Acetaminophen(ACE) Intermediates DFT calculation

Efficient removal of polybrominated diphenyl ethers from soil washing effluent by dummy molecular imprinted adsorbents: Selectivity and mechanisms

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Journal of Environmental Sciences 2023年第7期129卷 45-57页

作者： Yao Ma Jinfan Chen Xiaodong Du Chunsheng Xie Jiangmin Zhou Xueqin Tao Zhi Dang Guining Lu School of Environment and Energy South China University of TechnologyGuangzhou 510006China Guangdong Provincial Key Laboratory of Environmental Health and Land Resource Zhaoqing UniversityZhaoqing 526061China College of Life and Environmental Sciences Wenzhou UniversityWenzhou 325035China College of Resources and Environment Zhongkai University of Agriculture and EngineeringGuangzhou 510225China The Key Laboratory of Pollution Control and Ecosystem Restoration in Industry Clusters Ministry of EducationGuangzhou 510006China Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling South China University of TechnologyGuangzhou 510006China

Surfactant enhanced elution is an effective method for removing hydrophobic organic pollutants from soils.The key to the development of leaching technology is selective removal of targeted pollutants in soil washing effluent and recycling of surfactant solutions.In this study,a molecular imprinting technique was applied to selectively sorb polybrominated diphenyl ethers(PBDEs)in soil washing effluent.The novel molecular imprinted polymers(MIPs)using different template molecules were synthesized by precipitation polymerization.Adsorption behaviors andmechanisms ofMIPs were studied through experiments and theoretical calculations.The results show that 4-bromo-4'-hydroxybiphenyl and toluene can be effective imprinting molecule for MIPs synthesis.The maximal adsorption capacity of selected dummy molecular imprinted polymer(D1-MIP)was 1032.36μmol/g,and that of part molecular imprinted polymer(P-MIP)was 981.13μmol/g.Their imprinting factors in 5 PBDEs adsorption ranged from 2.13 to 5.88,the recovery percentage of Triton X-100 can reach 99.09%,confirming the feasibility of reusing surfactant.Various PBDEs could be removed by MIPs,and Quantitative Structure Property Relationship analysis revealed that PBDEs’molecular volume,planarity,polarity,and hydrophobicity have major influences on their adsorption performance.DFT calculation revealed that Van derWaals force and hydrogen bonding played important roles during selective adsorption.These results can provide effective theoretical guidance for surfactant enhanced soil elution in practical engineering applications.

关键词： Molecular imprinting Selective adsorption Polybrominated diphenyl ethers Triton X-100 DFT calculation

Tuning Active Metal Atomic Spacing by Filling of Light Atoms and Resulting Reversed Hydrogen Adsorption-Distance Relationship for Efficient Catalysis

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Nano-Micro Letters 2023年第10期15卷 151-162页

作者： Ding Chen Ruihu Lu Ruohan Yu Hongyu Zhao Dulan Wu Youtao Yao Kesong Yu Jiawei Zhu Pengxia Ji Zonghua Pu Zongkui Kou Jun Yu Jinsong Wu Shichun Mu State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070People’s Republic of China NRC(Nanostructure Research Centre) Wuhan University of TechnologyWuhan 430070People’s Republic of China

Precisely tuning the spacing of the active centers on the atomic scale is of great significance to improve the catalytic activity and deepen the understanding of the catalytic mechanism,but still remains a challenge.Here,we develop a strategy to dilute catalytically active metal interatomic spacing(d_(M-M))with light atoms and discover the unusual adsorption patterns.For example,by elevating the content of boron as interstitial atoms,the atomic spacing of osmium(d_(Os-Os))gradually increases from 2.73 to 2.96?.More importantly,we find that,with the increase in dOs-Os,the hydrogen adsorption-distance relationship is reversed via downshifting d-band states,which breaks the traditional cognition,thereby optimizing the H adsorption and H_2O dissociation on the electrode surface during the catalytic process;this finally leads to a nearly linear increase in hydrogen evolution reaction activity.Namely,the maximum dOs-Os of 2.96?presents the optimal HER activity(8 mV@10 mA cm^(-2))in alkaline media as well as suppressed O adsorption and thus promoted stability.It is believed that this novel atomic-level distance modulation strategy of catalytic sites and the reversed hydrogen adsorption-distance relationship can shew new insights for optimal design of highly efficient catalysts.

关键词： Electrocatalysis DFT calculation Interstitial filling Hydrogen evolution Structure–activity relationships

Experimental and theoretical insight into carbamazepine degradation by chlorine-based advanced oxidation processes:Efficiency,energy consumption,mechanism and DBPs formation

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Journal of Environmental Sciences 2024年第5期139卷 72-83页

作者： Chunwei Liu Zuo Tong How Yue Ju Li Feng Xuefeng Ren Mohamed Gamal El-Din Key Laboratory ofCoal Processing and Efficient Utilization of Ministry of Education School of Chemical Engineering and TechnologyChina University of Mining and TechnologyJiangsu 221116China Department of Civil and Environmental Engineering University of AlbertaEdmonton T6G 1H9AlbertaCanada School of Environment and Spatial Informatics China University of Mining and TechnologyJiangsu 221116China Key Laboratory of Agro-Forestry Environmental Processes and Ecological Regulation ofHainan Province School of Ecology and EnvironmentHainan UniversityHainan 570228China

Chlorine has been widely used in different advanced oxidation processes(AOPs)for micropollutants removal.In this study,different chlorine-based AOPs,namely medium pressure(MP)UV/chlorine,low pressure(LP)UV/chlorine,and in-situ chlorination,were compared for carbamazepine(CBZ)removal efficiency,energy consumption,and disinfection by-products(DBPs)formation.All three processes could achieve nearly 100%CBZ removal,while the reaction time needed by in-situ chlorination was double the time required by UV/chlorine processes.The energy consumed per magnitude of CBZ removed(EE/O)of MP UV/chlorine was 13 times higher than that of LP UV/chlorine,and relative to that of in-situ chlorination process.Accordingly,MP and LP UV/chlorine processes generated one to two orders of magnitude more hydroxyl radicals(^(·)OH)and reactive chlorine species(RCS)than in-situ chlorination.Besides,RCS were the dominant reactive species,contributing to 78.3%,75.6%,and 71.6% of CBZ removal in MP,LP UV/chlorine,and in-situ chlorination,respectively.According to the Gibbs free energy barriers between CBZ and RCS/^(·)OH calculated based on density functional theory(dft),RCS had more reaction routes with CBZ and showed lower energy barrier in the main CBZ degradation pathways like epoxidation and formation of iminostilbene.When applied to secondary wastewater effluent,UV/chlorine and in-situ chlorination produced overall DBPs ranging from 104.77 to 135.41μg/L.However,the production of chlorate during UV/chlorine processes was 15 times higher than that during in-situ chlorination.

关键词： UV/chlorine In-situ chlorination Energy efficiency Role of reactive species DFT calculation Disinfection by-products

Synthesis of Skipped Aminodienes by a Ni-Catalyzed Ring-Opening/Cross-Coupling Reaction of Vinylaziridines with Multifunctional Organoboronic Acids

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Chinese Journal of Chemistry 2023年第22期41卷 3003-3011页

作者： Lu Zhang Qingfeng Du Yicong Luo Yuanlin Wang Feng Gao Yong Ye Wanbin Zhang Green Catalysis Center College of ChemistryZhengzhou University100 Kexue RoadZhengzhouHenan 450001China Frontiers Science Center for Transformative Molecules School of Chemistry and Chemical EngineeringShanghai Jiao Tong University 800 Dongchuan RoadShanghai 200240China

Skipped dienes are of great importance but remain challenging to synthesize because of the presence of a sp hybrid carbon between the two alkenes.Herein,we have developed the first nickel-catalyzed regio-,(E)-stereo-and linear-selective ring-opening/cross-coupling reaction of vinylaziridines with organoboronic acids under mild conditions to construct various skipped aminodienes.The reaction exhibits wide functional-group compatibility,and could be adapted for the introduction of skipped aminodiene functionality into bioactive molecules.

关键词： DFT calculation Multifunctional organoboronic acids Ni-catalyzed Ring-opening Skipped aminodiene

High‑Quality Epitaxial N Doped Graphene on SiC with Tunable Interfacial Interactions via Electron/Ion Bridges for Stable Lithium‑Ion Storage

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纳微快报:英文版 2023年第11期15卷 185-204页

作者： Changlong Sun Xin Xu Cenlin Gui Fuzhou Chen Yian Wang Shengzhou Chen Minhua Shao Jiahai Wang School of Chemistry and Chemical Engineering Guangzhou UniversityGuangzhou 510006People’s Republic of China Department of Chemical and Biological Engineering The Hong Kong University of Science and TechnologyClear Water BayKowloonHong KongPeople’s Republic of China

Tailoring the interfacial interaction in SiCbased anode materials is crucial to the accomplishment of higher energy capacities and longer cycle lives for lithium-ion storage.In this paper,atomic-scale tunable interfacial interaction is achieved by epitaxial growth of high-quality N doped graphene(NG)on SiC(NG@SiC).This well-designed NG@SiC heterojunction demonstrates an intrinsic electric field with intensive interfacial interaction,making it an ideal prototype to thoroughly understand the configurations of electron/ion bridges and the mechanisms of interatomic electron migration.Both density functional theory(dft)analysis and electrochemical kinetic analysis reveal that these intriguing electron/ion bridges can control and tailor the interfacial interaction via the interfacial coupled chemical bonds,enhancing the interfacial charge transfer kinetics and preventing pulverization/aggregation.As a proof-of-concept study,this well-designed NG@SiC anode shows good reversible capacity(1197.5 mAh g^(−1)after 200 cycles at 0.1 A g^(−1))and cycling durability with 76.6%capacity retention at 447.8 mAh g^(−1)after 1000 cycles at 10.0 A g^(−1).As expected,the lithium-ion full cell(LiFePO_(4)/C//NG@SiC)shows superior rate capability and cycling stability.This interfacial interaction tailoring strategy via epitaxial growth method provides new opportunities for traditional SiC-based anodes to achieve high-performance lithium-ion storage and beyond.

关键词： SiC Heterojunction Interfacial engineering Lithium-ion battery DFT calculation

One-pot molten salt method for constructing CdS/C_(3)N_(4) nanojunctions with highly enhanced photocatalytic performance for hydrogen evolution reaction

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Journal of Environmental Sciences 2022年第2期34卷 244-257页

作者： Weijia Zhao Hongyun Niu Yongliang Yang Hongzhou Lv Jungang Lv Yaqi Cai State Key Laboratory of Environmental Chemistry and Ecotoxicology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China Institute of Environment and Health Jianghan UniversityWuhan 430056China Procuratoral Technology and Information Research Center Supreme People's ProcuratorateBeijing 100726China Institute of Environment and Health Hangzhou Institute for Advanced StudyUniversity of Chinese Academic SciencesHangzhou 310024China

The construction of heterojunction photocatalysts for efficiently utilizing solar energy has attracted considerable attention to solve the energy crisis and reduce environmental pollution.In this study,we use the energy released from an easily-occurred exothermic chemical reaction to serve as the drive force to trigger the formation of Cd S and C_(3)N_(4) nanocomposites which are successfully fabricated with cadmium nitrate and thiourea without addition of any solvents and protection of inert gas at initial temperature,a little higher than the melting point of thiourea.The as-prepared Cd S/C_(3)N_(4) materials exhibit high efficiency for photocatalytic hydrogen evolution reaction(HER)with the HER rate as high as 15,866μmol/(g·hr)under visible light irradiation(λ>420 nm),which is 89 and 9 times those of pristine C_(3)N_(4) and Cd S,respectively.Also,the apparent quantum efficiency(AQE)of Cd S/C_(3)N_(4)–1:2–200–2(Cd S/C_(3)N_(4)–1:2–200–2 means the ratio of Cd to S is 1:2 and the reaction temperature is set at 200℃ for two hours)reaches 3.25%atλ=420±15 nm.After irradiated for more than 24 hr,the HER efficiencies of Cd S/C_(3)N_(4) do not exhibit any attenuation.The DFT calculation suggests that the charge difference causes an internal electric field from C_(3)N_(4) pointing to Cd S,which can more effectively promote the transfer of photogenerated electrons from Cd S to C_(3)N_(4).Therefore,most HER should occur on C_(3)N_(4) surface where photogenerated electrons accumulate,which largely protects Cd S from photo-corrosion.

关键词： One-pot molten salt method Cd S/C_(3)N_(4)nanojunctions Photocatalytic hydrogen evolution reaction Anti-photo-corrosion DFT calculation

Insights into the confinement effect on isobutane alkylation with C_(4) olefin catalyzed by zeolite catalyst:A combined theoretical and experimental study

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Chinese Journal of Chemical Engineering 2022年第7期35卷 174-184页

作者： Shuo Li Jianlin Cao Xiang Feng Yupeng Du De Chen Chaohe Yang Wenhua Wang Wanzhong Ren College of Chemistry&Chemical Engineering Yantai UniversityYantai 264005China State Key Laboratory of Heavy Oil Processing School of Chemical EngineeringChina University of PetroleumQingdao 266580China Department of Chemical Engineering Norwegian University of Science and TechnologyTrondheim 7491Norway

Elucidating the confinement effect harbours tremendous significance for isobutane alkylation with C_(4) olefin.Herein,the confinement effect over zeolite catalysts was elucidated by combining DFT calculations,experiments(using the novel Beta zeolite exposing only external surfaces(Beta-E)and conventional Beta-I zeolite with both external and internal surfaces)and multi-techniques(e.g.,TGA-DTG,HRTEM,SEM and XRD).It is found that the main active sites for C_(4) alkylation reaction are located on internal surface rather than external surface.On the external surface,the hydride transfer reaction does not occur because the H-shared intermediate cannot be formed without the confinement effect.Moreover,the external surface has stronger selectivity for C_(4) olefin adsorption than isobutane,leading to enhanced oligomerization reactions.Therefore,the suitable micropore with confinement effect is essential for zeolite-catalyzed C_(4) alkylation.The atomic-scale insights of this work are of great referential importance to the design of highly effective zeolite catalyst.

关键词： C_(4)alkylation Surface Zeolite Catalysis DFT calculation

A robust and transparent nanosilica-filled silicone rubber coating with synergistically enhanced mechanical properties and barrier performance

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Journal of Materials Science & Technology 2023年第20期151卷 219-226页

作者： Shiyao Du Hui Yan Zihe Liu Ao Tang Ying Li Institute of Metal Research Chinese Academy of SciencesShenyang 110016China School of Materials Science and Engineering University of Science and Technology of ChinaShenyang 110016China Shenyang National Laboratory for Materials Science Northeastern UniversityShenyang 110819China

Implantable electronic devices(IEDs)are widely used by human beings to achieve medical treatment and diagnosis nowadays.However,ideal encapsulation of IEDs is still far from perfect as full prevention of body fluid diffusion into the coating remains unsolved.Herein,we develop a high-performance composite coating for IED encapsulation by introducing SiO_(2) nanoparticles into silicone rubber,which synergistically enhances mechanical properties and improves barrier performance.By fabricating composite coatings with different nanosilica contents,3%nanosilica is proved to be an optimal additive content with an excellent combination of improved fracture strength(from 2.5 MPa to 4.5 MPa),increased coating resistance(from 10^(4) to 10^(9) cm^(2))and ideal coating uniformity.Mechanical and electrochemical characterizations subsequently confirm substantially enhanced mechanical properties and barrier performance of the composite coating,which effectively resist crack propagation and impede penetrations of water and chloride ions through the coating.Theoretical calculations further uncover that modified SiO_(2) particles with enriched methyl groups endow a strong bridging effect to interact with silicone rubber monomer,which,together with anti-agglomeration property of methyl groups,contributes to a pronounced improvement in mechanical performance of nanosilica-filled silicone rubber.Benefitting from the enhanced mechanical and barrier properties,the as-fabricated nanosilica-filled silicone rubber demonstrates superior protection for the encapsulated circuits with a significantly improved lifetime(709.1 h)compared to that of circuits coated by pure silicone rubber(472.8 h)and bare circuit boards(1 h),which offers great values for packaging material design in future IED encapsulation.

关键词： Organic coatings Implantable electronic devices Nanosilica DFT calculation Mechanical property