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Ca_(2)MnO_(4)-layered perovskite modified by NaNO_(3)for chemical-looping oxidative dehydrogenation of ethane to ethylene

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Chinese Journal of Chemical Engineering 2024年第4期68卷 53-64页

作者： Weixiao Ding Kun Zhao Shican Jiang Zhen Huang Fang He college of chemistry and bioengineering Guilin University of TechnologyGuilin 541006China Guangzhou Institute of Energy conversion Chinese Academy of SciencesGuangzhou 510640China School of chemistry and Chemical Engineering Nanjing University of Science and TechnologyNanjing 210094China

Chemical-looping oxidative dehydrogenation(CL-ODH)is a process designed for the conversion of alkanes into olefins through cyclic redox reactions,eliminating the need for gaseous O_(2).In this work,we investigated the use of Ca_(2)MnO_(4)-layered perovskites modified with NaNO_(3) dopants,serving as redox catalysts(also known as oxygen carriers),for the CL-ODH of ethane within a temperature range of 700-780℃.Our findings revealed that the incorporation of NaNO_(3) as a modifier significantly-nhanced the selectivity for-thylene generation from Ca_(2)MnO_(4).At 750℃and a gas hourly space velocity of 1300 h^(-1),we achieved an-thane conversion up to 68.17%,accompanied by a corresponding-thylene yield of 57.39%.X-ray photoelectron spectroscopy analysis unveiled that the doping NaNO_(3) onto Ca_(2)MnO_(4) not only played a role in reducing the oxidation state of Mn ions but also increased the lattice oxygen content of the redox ***,formation of NaNO_(3) shell on the surface of Ca_(2)MnO_(4) led to a reduction in the concentration of manganese sites and modulated the oxygen-releasing behavior in a step-wise *** modulation contributed significantly to the enhanced selectivity for ethylene of the NaNO_(3)-doped Ca_(2)MnO_(4) *** findings provide compelling evidence for the potential of Ca_(2)MnO_(4)-layered perovskites as promising redox catalysts in the context of CL-ODH reactions.

关键词： Chemical-looping oxidative dehydrogenation Ethane Ethylene NaNO_(3)-doped Ca_(2)MnO_(4)redox catalyst Layered perovskites

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Engineering single-atom Mn on nitrogen-doped carbon to regulate lithium-peroxide reaction kinetics for rechargeable lithium-oxygen batteries

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Journal of Energy chemistry 2024年第7期94卷 199-207页

作者： Yaling Huang Yong Liu Yang Liu Chenyang Zhang Wenzhang Li Jie Li School of chemistry and Chemical Engineering Central South UniversityChangsha 410083HunanChina School of Minerals Processing and bioengineering Central South UniversityChangsha 4003HunanChina

Precision engineering of catalytic sites to guide more favorable pathways for Li_(2)O_(2) nucleation and decom-position represents an enticing kinetic strategy for mitigating overpotential,enhancing discharge capac-ity,and improving recycling stability of Li-O_(2) *** this work,we employ metal-organic frameworks(MOFs)derivation and ion substitution strategies to construct atomically dispersed Mn-N_(4) moieties on hierarchical porous nitrogen-doped carbon(Mn SAs-NC)with the aim of reducing the over-potential and improving the cycling stability of Li-O_(2) *** porous structure provides more chan-nels for mass transfer and exposes more highly active sites for electrocatalytic reactions,thus promoting the formation and decomposition of Li_(2)O_(2).The Li-O_(2) batteries with Mn SAs-NC cathode achieve lower overpotential,higher specific capacity(14290 mA h g^(-1) at 100 mAg^(-1)),and superior cycle stability(>100 cycles at 200 mA g^(-1))compared with the Mn NPs-NC and *** functional theory(DFT)cal-culations reveal that the construction of Mn-N_(4) moiety tunes the charge distribution of the pyridinic N-rich vacancy and balances the affinity of the intermediates(LiO_(2) and Li_(2)O_(2)).The initial nucleation of Li_(2)O_(2) on Mn SAs-NC favors the O_(2)-→LiO_(2)→Li_(2)O_(2) surface-adsorption pathway,which mitigates the overpoten-tials of the oxygen reduction(ORR)and oxygen evolution reaction(OER).As a result,Mn SAs-NC with Mn-N_(4) moiety effectively facilitates the Li_(2)O_(2) nucleation and enables its reversible *** work establishes a methodology for constructing carbon-based electrocatalysts with high activity and selectivity for Li-O_(2)batteries.

关键词： Single-atom Mn MOFs-oriented architecture Rechargeable Li-O_(2)battery N-doped carbon Density functional theory calculation

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Fabrication of CuFe_(2)O_(4)/Bi_(12)O_(17)Cl_(2) photocatalyst with intrinsic p-n junction for highly efficient bisphenol A degradation

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Journal of Environmental Sciences 2024年第2期136卷 547-558页

作者： Yong Wang Cheng Liu Haoyun Hu Qiujun Lu Haiyan Wang Chenxi Zhao Fuyou Du Ningli Tang Guangxi Key Laboratory of Electrochemical and Magnetochemical Functional Materials College of Chemistry and BioengineeringGuilin University of TechnologyGuilin 541004China college of Biological and Environmental Engineering Changsha UniversityChangsha 410022China

The construction and application of novel highly efficient photocatalysts have been the focus in the field of environmental pollutant *** this work,a novel CuFe_(2)O_(4)/Bi_(12)O_(17)Cl_(2)photocatalysts were synthesized by simple hydrothermal and chemical precipitation *** fabricated CuFe_(2)O_(4)/Bi_(12)O_(17)Cl_(2)composite exhibited much higher photocatalytic activity than pristine CuFe_(2)O_(4)and Bi_(12)O_(17)Cl_(2)in the removal of bisphenol A(BPA)under visible-light illumination,which ascribed to the intrinsic p-n junction of CuFe_(2)O_(4)and Bi_(12)O_(17)Cl_(2).The photocatalytic degradation rate of BPA on CuFe_(2)O_(4)/Bi_(12)O_(17)Cl_(2)with an optimized CuFe_(2)O_(4)content(1.0 wt.%)reached 93.0%within 30 *** capture experiments of active species confirmed that the hydroxyl radicals(·OH)and superoxide radicals(·O_(2)^(-))played crucial roles in photocatalytic BPA degradation ***,the possible degradation mechanism and pathways of BPA was proposed according to the detected intermediates in photocatalytic reaction process.

关键词： Bi_(12)O_(17)Cl_(2) CuFe_(2)O_(4) Heterojunction Bisphenol A Photocatalytic degradation

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covalent organic frameworks/carbon nanotubes composite with cobalt(II)pyrimidine sites for bifunctional oxygen electrocatalysis

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Nano Materials Science 2024年第4期6卷 419-427页

作者： Zhuangzhuang Wu Lijuan Feng Zhe Lu Xinxin Yu Yuzhen Zhao Junming Luo Shaolei Wang Xinlong Tian Qi Chen State Key Laboratory of Marine Resource Utilization in South China Sea School of Marine Science and Engineering Hainan University Key Laboratory of Polyoxometalate and Reticular Material chemistry of Ministry of Education School of Chemistry Northeast Normal University School of bioengineering Zhuhai Campus of Zunyi Medical University

With characteristics and advantages of functional composite materials, they are commendably adopted in numerous fields especially in oxygen electrocatalysis, which is due to the significant synergies between various components. Herein, a novel bifunctional oxygen electrocatalyst（co-CNT@coF-Pyr） has been synthesized through in-situ growth of covalent organic frameworks（coFs） layers on the outer surface of highly conductive carbon nanotubes（CNTs） followed by coordination with co（II）. For electrocatalytic OER, co-CNT@coF-Pyr reveals a low overpotential（438 mV） in alkaline electrolyte（1.0 M aqueous solution of KOH） with a current density of 10 mA cm-2, which is comparable to most discovered coF-based catalysts. For electrocatalytic ORR, coCNT@coF-Pyr exhibits a low H2O2yield range（9.0 %–10.1 %） and a reaction pathway close to 4e-（n =3.82–3.80） in alkaline electrolyte（0.1 M aqueous solution of KOH） within the test potential range of 0.1–0.6 V ***, which is superior to most reported coF-based catalysts. Hence, this research could not only offer an innovative insight into the construction of composites, but also facilitate the practical application of renewable fuel cells, closed water cycle, and rechargeable metal-air batteries.

关键词： Oxygen electrocatalysis covalent organic frameworks Carbon nanotubes composite materials

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Carbene-catalyzed enantioselective seleno-Michael addition as access to antimicrobial active Se-containing heterocycles

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Science China chemistry 2024年第7期67卷 2199-2205页

作者： Hongyan Long Sha Zhao Chunyan Jian Xiuli Wu Fengfei Lu Minghong Liao Fengrui Che Xingxing Wu Yonggui Robin Chi State Key Laboratory of Green Pesticide Key Laboratory of Green Pesticide and Agricultural BioengineeringMinistry of EducationGuizhou UniversityGuiyang 550025China School of chemistry Chemical Engineeringand BiotechnologyNanyang Technological UniversitySingapore 637371Singapore

Organoseleniums exhibit a diverse set of biological activities that are pivotal for drug discovery and are widely explored in synthetic chemistry and material *** many transformations have been developed for non-enantioselective C–Se bond formations,the catalyst-controlled stereoselective preparation of chiral organoseleniums continues to be of considerable *** particular,there are limited studies on the enantioselective seleno-Michael addition reactions to access chiral selenium functional ***,we disclose a carbene-catalyzed highly enantioselective nucleophilic C–Se bond construction through formal[3+3]annulations between selenocarboxamides and bromoenals,affording seleno-thiazinone products with good yields and excellent *** choice of a weak inorganic base was pivotal to suppressing the unproductive racemization and decomposition of the selenium ***,the catalytically generated chiral selenium-containing heterocyclic products feature remarkable antimicrobial activities that could serve as promising lead scaffolds for further agrochemical development.

关键词： seleno-Michael addition organocatalysis N-heterocyclic carbene seleno-heterocycles antimicrobial activity

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Hydrazone derivatives in agrochemical discovery and development

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Chinese Chemical Letters 2024年第3期35卷 104-113页

作者： Ya Wang Shengxin Guo Lijiao Yu Wei Zhang Zhenchao Wang Yonggui Robin Chi Jian Wu National Key Laboratory of Green Pesticide Key Laboratory of Green Pesticide and Agricultural BioengineeringMinistry of EducationGuizhou UniversityHuaxi DistrictGuiyang 550025China Division of chemistry&Biological chemistry School of Physical&Mathematical SciencesNanyang Technological UniversitySingapore 637371Singapore

As a common active substructure,hydrazone has attracted increasing attention and is considered essential for pesticide *** has been widely regarded as a potential insecticidal,antibacterial,antifungal,antiviral,and herbicidal *** this review,we highlight the pesticide versatility of hydrazone fragments and provide a comprehensive summary of the biological activity,structure-activity relationship analysis(SARs),and primary mechanism of their *** profile is expected to give valuable information for discovering new pesticides.

关键词： Hydrazone Agrochemicals Biological activity Structure-activity relationship Preliminary mechanism

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Highly efficient nitrogen fixation over S-scheme heterojunction photocatalysts with enhanced active hydrogen supply

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National Science Review 2024年第05期 315-325页

作者： Tong Bao Yamin Xi Chaoqi Zhang Peiyang Du Yitong Xiang Jiaxin Li Ling Yuan Chengzhong Yu Chao Liu School of chemistry and Molecular Engineering East China Normal University Australian Institute for bioengineering and Nanotechnology The University of Queensland

Photocatalytic N2fixation is a promising strategy for ammonia（NH3） synthesis;however,it suffers from relatively low ammonia yield due to the difficulty in the design of photocatalysts with both high charge transfer efficiency and desirable N2adsorption/activation ***,an S-scheme coSx/ZnS heterojunction with dual active sites is designed as an efficient N2fixation *** coSx/ZnS heterojunction exhibits a unique pocket-like nanostructure with small ZnS nanocrystals adhered on a single-hole coSxhollow *** the heterojunction,the ele ctronic interaction between ZnS and coSxcreates electron-deficient Zn sites with enhanced N2chemisorption and electron-sufficient co sites with active hydrogen supply for N2hydrogenation,cooperatively reducing the energy barrier for *** combination with the promoted photogenerated electron-hole separation of the S-scheme heterojunction and facilitated mass transfer by the pocket-like nanostructure,an excellent N2fixation performance with a high NH3yield of 1175.37 μmol g-1h-1is *** study provides new insights into the design of hetero junction photocatalysts for N2fixation.

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Access to Axially Chiral Aryl Aldehydes via Carbene-Catalyzed Nitrile Formation and Desymmetrization Reaction

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Research 2024年第3期2024卷 715-721页

作者： Yuanlin Cai Ya Lv Liangzhen Shu Zhichao Jin Yonggui Robin Chi Tingting Li National Key Laboratory of Green Pesticide Key Laboratory of Green Pesticide and Agricultural BioengineeringMinistry of EducationGuizhou UniversityGuiyang 550025China School of chemistry Chemical Engineeringand BiotechnologyNanyang Technological UniversitySingapore 637371Singapore.

An approach utilizing N-heterocyclic carbene for nitrile formation and desymmetrization reaction is developed. The process involves kinetic resolution, with the axially chiral aryl monoaldehydes obtained in moderate yields with excellent optical purities. These axially chiral aryl monoaldehydes can be conveniently transformed into functionalized molecules, showing great potential as catalysts in organic chemistry.

关键词： chemistry. aldehydes chiral

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MnS–MnO heterogeneous nanocube@N,S-doped carbon as a highly efficient bifunctional water splitting electrocatalyst

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Rare Metals 2024年第5期43卷 1977-1988页

作者： Xue-Qian Wang Xiang-Ying Ma Wang-Zhi Wu Hui-Bing He Nan-Nan Wang Ren-Ji Zheng Shao-Jian Ma Yan-Qiu Zhu Pei-Kang Shen Jin-Liang Zhu School of Resources Environment and MaterialsState Key Laboratory of Featured Metal Materials and Life-Cycle Safety for Composite StructuresCollege of Chemistry and Chemical EngineeringGuangxi UniversityNanning 530004China School of chemistry and Chemical Engineering Guangxi MinzuUniversity Nanning 530006 China School of Minerals Processing and bioengineering Central South UniversityChangsha 410083China

A stable,efficient,and economical bifunctional electrolytic catalyst would be incredibly beneficial for the development of hydrogen production by electrocatalytic water *** this study,we synthesized a novel MnS–MnO heterogeneous nanocube@N,S-doped carbon(MnS–MnO@NSC).MnS–MnO nanocubes possess rich heterogeneous interfaces and plentiful catalytic active sites to promote electrochemical reactions,while the N,S-doped carbon shell possesses excellent conductivity and catalytic properties and protects the ***–MnO@NSC exhibited excellent electrochemical properties as an effective bifunctional electrocatalyst for the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)in KOH *** the HER,the overpotential was as low as 124 mV at a current density of 10 mA·cm^(-2)while in the OER,it was only 340 mV at 100 mA·cm^(-2)under the same *** addition,a MnS–MnO@NSC||MnS–MnO@NSC electrolyzer exhibited almost comparable activity and higher steadiness than those exhibited by the state-of-the-art Pt/C||RuO_(2)/C system for full water splitting in KOH solution.

关键词： Manganese sulfide Manganese oxide Doped carbon Heterogeneous nanocube Water splitting

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Rh(Ⅲ)-Catalyzed sequential ring-retentive/-opening [4+2]annulations of 2H-imidazoles towards full-color emissive imidazo[5,1-a]isoquinolinium salts and AIE-active non-symmetric 1,1-biisoquinolines

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Chinese Chemical Letters 2024年第10期 239-243页

作者： Peiyan Zhu Yanyan Yang Hui Li Jinhua Wang Shiqing Li Guangxi Key Laboratory of Electrochemical and Magneto-Chemical Functional Materials College of Chemistry and Bioengineering Guilin University of Technology

Rhodium-catalyzed C4aryl-H activation and ring-retentive annulation of 2H-imidazoles with internal alkynes to build imidazo[5,1-a]isoquinolinium salts with high yields and broad scope has been *** novel salts serve as new full-color emissive fluorophores （433-633 nm）,just by simply modifying the substituents on C3 and C4 positions of isoquinoline ***,these salts can undergo ring-opening C5aryl-H activation/annulation with a different alkyne to form non-symmetric and AIE-active1,1-biisoquinolines,where NH4OAc plays an indispensable role that accounts for Hofmann elimination and imine formation,leading to an unprecedented imine dance:cyclic imine→N-alkenyl imine→NH ***15N labelling experiments indicate that the 2ndannulation includes two pathways:N-exchange（major） and N-retention （minor）.

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