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Phase and chemical state tuning of FeNi oxides for oxygen evolution reaction

Science China chemistry 2024年第8期67卷 2755-2766页

作者： Jiawei Wu Zhouyang Ma Lice Yu Shuli Wang Fulin Yang Ligang Feng school of chemistry and chemical engineering Yangzhou UniversityYangzhou 225002China

Advancing and deploying the Fe Ni-based catalyst,the state-of-the-art pre-electrocatalysts,for oxygen evolution reactions(OER)still suffer from unclear chemical state correlation to the catalytic ability,as evidenced by the variedly reported performance for the different Fe Ni ***,we contributed the phase and redox chemical states tuning of Fe Ni oxides by the surface microenvironment regulation for the OER catalysis that was realized by the urea-assisted pyrolysis and molybdenum-doping technique by integrating molybdenum into the iron–nickel metal-organic *** by the complicated and compromised atmosphere,namely,the oxidation state driven by the Mo doping and reduction ability induced by the urea-assisted pyrolysis,could transfer confined Fe Ni oxides to hybrid phases of Fe_(2)O_(3)and FeNi_(3)alloy,and the resultant compromised chemical states by the charge redistribution imparted very high electrocatalytic performance for OER compared with the control *** insitu Raman spectroscopy and post-XPS analysis confirmed the facile Fe/Ni oxyhydroxide active phase formation resulting from the proper phase and chemical states,and theoretical analysis disclosed the microenvironment regulation resulting in the charge redistribution forming the electron accumulation and depletion sites to accelerate the oxygen-species to oxyhydroxide-species transformation and enhance the electronic state density near the Fermi level by significantly reducing the energy *** work not only showed the importance of surface chemical state tunning that can basically answer the varied performance of Fe Ni catalysts but also revealed an effective approach for fine-tuning their catalytic properties.

关键词： oxygen evolution reaction FeNi-based catalysts urea pyrolysis chemical states charge redistribution

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Fully fluorinated hybrid zeolite imidazole/Prussian blue analogs with combined advantages for efficient oxygen evolution reaction

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Chinese chemical Letters 2024年第6期35卷 222-228页

作者： Jiayu Xu Meng Li Baoxia Dong Ligang Feng school of chemistry and chemical engineering Yangzhou UniversityYangzhou 225002China

Hybrid metal-organic framework(MOF)derivatives play a significant role in the novel catalyst development in energy conversion ***,we demonstrated the low-temperature fully fluorinated zeolitic imidazole framework(ZIF)coupled with a three-dimensional open framework Prussian blue analog(PBA)with combined advantages for electrocatalytic oxygen evolution reaction(OER)in water splitting *** spectroscopic analysis and the electrochemical studies revealed the combined advantages of efficient electronic effect and active site *** of good conductivity improvement by Ndoped carbon derived from ZIF and the high electrochemical surface area and active site exposure from PBA derivatives,good catalytic performance was obtained on the optimal catalyst of Co Ni ZIF/Co Fe-PBAF-300,which required a low overpotential of 250 m V to reach 10 m A/cm^(2)loaded on the glassy carbon electrode,with Tafel slope of 47.4 m V/dec,and very high dynamic and steady *** addition,the multi-component with the mixed structure from highly polar metal fluorides promoted the easy formation of the active phase as revealed by the post-sample *** current results showed a novel composite catalyst materials development from the hybrid MOF derivatives,which would be promising in the electrolysis of water oxidation reactions and energy-relevant catalysis reactions.

关键词： Metal-organic framework Zeolitic imidazole framework Prussian blue analog Fluoridation Multi-component Oxygen evolution reaction

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An effective bimetallic oxide catalyst of RuO_(2)-Co_(3)O_(4) for alkaline overall water splitting

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Nano Research 2024年第5期17卷 3785-3793页

作者： Fangfang Ren Jiayu Xu Ligang Feng College of chemical and Environmental engineering Yancheng Teachers UniversityYancheng 224007China school of chemistry and chemical engineering Yangzhou UniversityYangzhou 225002China

The rational design of effective bifunctional electrocatalysts is of paramount importance for overall water-splitting technology in sustainable energy ***,bimetallic oxide catalysts(RuO_(2)-Co_(3)O_(4))derived from Ru combined MOF-derivatives(MOF=metal-organic framework)were demonstrated effective for overall water splitting in an alkaline solution,owing to the combined merits such as the two-dimensional interconnected network structure,the synergetic coupling effects and increased chemical *** as-prepared RuO_(2)-Co_(3)O_(4) only requires an overpotential of 260 mV for oxygen evolution and 75 mV for hydrogen evolution at 10 mA/cm^(2) in 1 M KOH solution;a low cell voltage of 1.54 V was required to reach the kinetic current density of 10 mA/cm^(2) for the water electrolysis when supporting on glass carbon electrode,and very good stability for 40 h was *** and theoretical results demonstrated the electronic structure optimization of bimetallic RuO_(2)-Co_(3)O_(4) compared to the individual metal oxide,which promoted interface charges redistribution and the d-band center downshift,resulting in increased activity and stability for water-splitting *** work provides a feasible approach for developing bimetallic oxides for application in energy-relevant electrocatalysis reactions.

关键词： ruthenium dioxide cobalt oxide metal-organic frameworks heterostructures overall water splitting

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Mo@PANI-catalyzed oxidative deoximation reaction

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Chinese chemical Letters 2024年第2期35卷 407-410页

作者： Yiyang Zhang Wen Li Zuofeng Hu Xiaobi Jing Lei Yu school of Mechanical engineering Yangzhou UniversityYangzhou 225127China school of chemistry and chemical engineering Yangzhou UniversityYangzhou 225002China yangzhou Yangzi Auto Interior & Exterior Co. Ltd.Yangzhou 225119China

Deoximation is an important transformation in synthetic *** can be employed in protection,characterization and purification of the carbonyls,and in the synthesis of ketones from non-carbonyl *** the field,oxidative deoximation reaction can utilize the driving force caused by the oxidation process so that the reaction can occur under relatively mild ***,we designed and prepared polyaniline-supported molybdenum(Mo@PANI)just by immersing PANI into the EtOH/H_(2)O solution of MoCl_(5).The material was successfully applied as the efficient catalyst for oxidative deoximation reactions,which were performed in ethanol using H_(2)O_(2)as the clean *** substrate scope of the reaction was *** could be applied on heterocycle-containing substrates,making this protocol preferable for pharmaceutical intermediate *** Mo is a necessary trace element for both animals and plants,this method is environment-friendly and is suitable for large-scale *** work as the first example of Mo-catalyzed oxidative deoximation reaction may inspire novel ideas for both catalyst design and synthetic process development.

关键词： Molybdenum Polyaniline Oxidation Deoximation Carbonyl

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Metal-organic framework and its composites modulate macrophage polarization in the treatment of inflammatory diseases

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Chinese chemical Letters 2024年第5期35卷 45-56页

作者： Feifei Wang Hang Yao Xinyue Wu Yijian Tang Yang Bai Hui Chong Huan Pang school of chemistry and chemical engineering Yangzhou UniversityYangzhou 225002China school of Pharmacy Changzhou UniversityChangzhou 213164China State Key Laboratory of Coordination chemistry Nanjing UniversityNanjing 210023China

Metal-organic framework(MOF)is a periodic sexual network structure with large surface area and high porosity,which is assembled by inorganic nodes and organic ligands through coordinate covalent *** have the advantages of controllable pore size and shape,large specific surface area,easy modification and more active *** addition,MOF based nanoenzymes display excellent enzyme catalytic activity due to their special structure and multiple exposed metal active sites,controlling the production of reactive oxygen species(ROS)in cells or the body,and thus regulating the polarization of *** article reviews the mechanism of MOF material regulating macrophage polarization and the function of macrophages with different *** utilizing the excellent properties of MOFs and the advantages of combining them with bioactive materials,we have discovered their excellent applications in the treatment of inflammatory ***,we discussed the current challenges and prospects faced by MOF based composite *** expect that the research in this developing field will play a more important role in combating inflammatory diseases in the field of nanomedicine.

关键词： Metal-organic framework Inflammation Macrophage polarization Reactive oxygen species Nanozyme activity

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Design and preparation of highly crystalline K-intercalated W@PCN:an efficient material for aniline elimination

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Rare Metals 2024年第3期43卷 1337-1342页

作者： Hao-Fei Li Kai-Wen Yu Xiao-Bi Jing Lei Duan Yi-Yang Zhang school of chemistry and chemical engineering Yangzhou UniversityYangzhou225002China school of Mechanical engineering Yangzhou UniversityYangzhou225127China school of Material Science and engineering Huazhong University of Science and TechnologyWuhan430071China school of chemical engineering.and Materials Changzhou Institute of TechnologyChangzhou213032China Department of Basic Courses Army Engineering University of PLANanjing211101China

In this paper,we designed and prepared the polymeric carbon nitride-supported tungsten(W@PCN)*** were employed as the catalysts for photocatalytic oxidation of aniline in *** the process,H_(2)O_(2)was initially generated via the PCN-catalyzed *** by supported tungsten,aniline was oxidized by the in situ generated H_(2)O_(2)to obtain less toxicpoly aniline.

关键词： materials aniline crystalline

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Recent advances in heterogeneous hydrosilylation of unsaturated carbon-carbon bonds

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Chinese chemical Letters 2024年第6期35卷 71-85页

作者： Heng Yang Zhijie Zhou Conghui Tang Feng Chen school of chemistry and chemical engineering Yangzhou UniversityYangzhou 225002China Key Laboratory of Material chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

The hydrosilylation of unsaturated carbon-carbon bonds is one of the most critical reactions in silicone industrial *** homogeneous Speier's catalyst,Karstedt's catalyst,and other noble metal-based catalysts are widely ***,simplifying the separation of the homogeneous catalyst from reaction products and reducing the high cost of precious metals is still *** review describes the recent development of heterogeneous catalysts for alkene,alkyne,and allene hydrosilylations,which can effectively solve problems in homogeneous hydrosilylation.

关键词： Hydrosilylation Heterogeneous catalysis Alkenes Alkynes Silanes

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Low carbon alcohol fuel electrolysis of hydrogen generation catalyzed by a novel and effective Pt–CoTe/C bifunctional catalyst system

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Green Energy & Environment 2024年第4期9卷 758-770页

作者： Yang Zhou Lice Yu Jinfa Chang Ligang Feng Jiujun Zhang school of chemistry and chemical engineering Yangzhou UniversityYangzhou225002JiangsuChina NanoScience Technology Center University of Central FloridaOrlandoFL32826USA College of Sciences&Institute for Sustainable Energy Shanghai UniversityShanghai200444China

Low carbon alcohol fuels electrolysis under ambient conditions is promising for green hydrogen generation instead of the traditional alcohol fuels steam reforming technique,and highly efficient bifunctional catalysts for membrane electrode fabrication are required to drive the electrolysis ***,the efficient catalytic promotion effect of a novel catalyst promoter,CoTe,on Pt is demonstrated for low carbon alcohol fuels of methanol and ethanol electrolysis for hydrogen *** and density functional theory calculation results indicate that the optimized electronic structure of Pt–CoTe/C resulting from the synergetic effect between Pt and CoTe further regulates the adsorption energies of CO and H*that enhances the catalytic ability for methanol and ethanol ***,the good water activation ability of CoTe and the strong electronic effect of Pt and CoTe increased the tolerance ability to the poisoning species as demonstrated by the CO-stripping *** high catalytic kinetics and stability,as well as the promotion effect,were also carefully ***,71.9%and 75.5%of the initial peak current density was maintained after 1000 CV cycles in acid electrolyte for methanol and ethanol oxidation;and a low overpotential of 30 and 35 mV was required to drive the hydrogen evolution reaction in methanol and ethanol solution at the current density of 10 mA cm^(-2).In the two-electrode system for alcohol fuels electrolysis,using the optimal Pt–CoTe/C catalyst as bi-functional catalysts,the cell potential of 0.66 V(0.67 V)was required to achieve 10 mA cm^(-2) for methanol(ethanol)electrolysis,much smaller than that of water electrolysis(1.76 V).The current study offers a novel platform for hydrogen generation via low carbon alcohol fuel electrolysis,and the result is helpful to the catalysis mechanism understanding of Pt assisted by the novel promoter.

关键词： Methanol electrolysis Ethanol electrolysis Cobalt telluride Pt-based electrocatalyst Hydrogen evolution reaction

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Atmospheric fate of typical liquid crystal monomers in the tropospheric gas,liquid,and granular phases

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Journal of Environmental Sciences 2024年第2期136卷 348-360页

作者： Yanru Huo Zexiu An Mingxue Li Jinchan Jiang Yuxin Zhou Ju Xie Jianguo Zhang Maoxia He Environment Research Institute Shandong UniversityQingdao 266237China College of Plant Protection Hebei Agricultural UniversityBaoding 071000China school of chemistry and chemical engineering Yangzhou UniversityYangzhou 225002China Jinan Environmental Research Academy Jinan 250000China

Mineral aerosol particles significantly impact environmental risk prediction of liquid crystal monomers(LCMs).In this work,we investigated the reaction mechanisms and kinetics of three typical LCMs(4-cyano-3,5-difluorophenyl 4-ethylbenzoate(CEB-2F),4-cyano-3-fluorophenyl 4-ethylbenzoate(CEB-F),and 4-cyanophenyl 4-ethylbenzoate(CEB))with ozone(O_(3))in the atmospheric gas,liquid,and particle phases employing density functional theory(DFT).Here,O_(3)is prone to add to the benzene ring without F atom(s)in the selected *** ozonolysis products are aldehydes,carboxylic acids,epoxides,and unsaturated hydrocarbons containing aromatic *** products undergo secondary ozonolysis to generate small molecular compounds such as glyoxal,which is beneficial for generating secondary organic aerosol(SOA).Titanium dioxide(TiO_(2)),an essential component of mineral aerosol particles,has good adsorption properties for LCMs;however,it slightly reduces the reactivity with O_(3).At 298 K,the reaction rate constant of the selected LCMs reacting with O_(3)in the gas and atmospheric liquid phases is(2.74–5.53)×10^(-24)cm^(3)/(mol·sec)and 5.58×10^(-3)–39.1 L/(mol·sec),while CEB-2F reacting with O_(3)on(TiO_(2))_(6)cluster is 1.84×10^(-24)cm^(3)/(mol·sec).The existence of TiO_(2)clusters increases the persistence and long-distance transportability of LCMs,which enlarges the contaminated area of LCMs.

关键词： Liquid crystal monomers(LCMs) Ozonolysis TiO_(2)clusters Adsorption Toxicity assessment

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HZSM-5 zeolites undergoing the high-temperature process for boosting the bimolecular reaction in n-heptane catalytic cracking

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Chinese Journal of chemical engineering 2024年第2期66卷 136-144页

作者： Chenggong Song Zhenzhou Ma Xu Hou Hao Zhou Huimin Qiao Changchang Tian Li Yin Baitang Jin Enxian Yuan school of chemical engineering Changchun University of TechnologyChangchun130012China Department of chemical and Biomolecular engineering North Carolina State UniversityRaleighNC 27606USA school of chemistry and chemical engineering Yangzhou UniversityYangzhou225009China

High-temperature treatment is key to the preparation of zeolite ***,the effects of hightemperature treatment on the property and performance of HZSM-5 zeolites were studied in this work.X-Ray diffraction,N2physisorption,27Al magic angle spinning nuclear magnetic resonance(MAS NMR),and temperature-programmed desorption of ammonia results indicated that the hightemperature treatment at 650℃ hardly affected the inherent crystal and texture of HZSM-5zeolites but facilitated the conversion of framework Al to extra-framework Al,reducing the acid site and enhancing the acid ***,the high-temperature treatment improved the performance of HZSM-5 zeolites in n-heptane catalytic cracking,promoting the conversion and light olefins yield while inhibiting coke *** on the kinetic and mechanism analysis,the improvement of HZSM-5 performance caused by high-temperature treatment has been attributed to the formation of extra-framework Al,which enhanced the acid strength,facilitated the bimolecular reaction,and promoted the entropy change to overcome a higher energy barrier in n-heptane catalytic cracking.

关键词： HZSM-5 n-Heptane Catalytic cracking High-temperature treatment Extra-framework Al

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