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SusMat 2023年第1期3卷 137-144页

作者： Chuanfa Li Pengwei Ma Shenghao Lin Zongheng Cen Junlong Huang Yin Cui Shimei Li Shaohong Liu Ruowen Fu Dingcai Wu PCFM Lab School of ChemistrySun Yat-sen UniversityGuangzhouP.R.China Research Center of Medical Sciences Guangdong Provincial People’s HospitalGuangdong Academy of Medical SciencesGuangzhouP.R.China

Lithium-sulfur(Li-S)batteries have been regarded as promising next-generation energy-storage devices owing to their inherently high theoretical energy density.Unfortunately,the poor capacity and cycling life caused by severe polysulfide shuttle effect and sluggish redox kinetics in sulfur cathodes greatly impede the practical application of Li-S batteries.Herein,a new class of nanonetworkstructured carbon decorated with oxygen-vacancy-containing cerium oxide nanoparticles(NSC-CeO_(2−x)),in which carbon skeleton is composed of highly conductive carbon nanotube core welded by hybrid carbon shell,has been developed via one-step heating treatment of hybrid molecular brush and further employed as functional interlayer to modify separator of Li-S battery.Owing to the synergistic effect of the highly active CeO_(2−x)nanoparticles and the threedimensional carbon nanonetwork in enhancing the preservation of the soluble polysulfides and boosting the redox kinetics of sulfur species,the NSC-CeO_(2−x)significantly promotes the electrochemical performance of sulfur cathode.As a result,the as-constructed Li-S batteries exhibit an ultrahigh initial sulfur utilization of 92.9%and an extremely large capacity of 751mA h g^(−1) at a high rate of 5 C.Remarkably,a stable capacity of 728 mA h g^(−1)over 300 cycles at 1 C is also achieved.

关键词： lithium-sulfur batteries nanonetwork-structured carbon oxygen vacancies

Highly efficient removal of ozone by amorphous manganese oxides synthesized with a simple hydrothermal method

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Journal of Environmental Sciences 2023年第12期134卷 96-107页

作者： Hong Zhao Aijie Wang Qiuyan Zhang Chong Han School of Metallurgy Northeastern UniversityShenyang 110819China

Amorphous manganese oxides (MnO_(x)) were synthesized by facile hydrothermal reactions between potassium permanganate and manganese acetate.Synthesis parameters,including hydrothermal time and temperature and molar ratio of precursors,significantly affected the ozone removal performance and structure property of MnO_(x).Amorphous MnO_(x)-1.5,which was prepared at the Mn^(2+)/Mn^(7+)molar ratio of 1.5 under hydrothermal conditions of 120℃ and 2 hr,showed the highest ozone removal rate of 93% after 480 min at the room temperature,RH (relative humidity)=80%and WHSV (weight hourly space velocity)=600 L/(g·hr).The morphology,composition and structure of catalysts were investigated with X-ray diffractometer (XRD),Raman spectra,N_(2) physisorption,field emission scanning electron microscope (FESEM),X-ray photoelectron spectroscopy (XPS),H2temperature-programmed reduction (H_(2)-TPR),O_(2) temperature-programmed desorption (O_(2)-TPD) and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS).It was confirmed that high catalytic activity of amorphous MnOxfor ozone removal was mainly ascribed to its abundant oxygen vacancies,high oxygen mobility and large specific surface area.

关键词： Amorphous manganese oxides Hydrothermal method Ozone Catalytic decomposition oxygen vacancies

Electric-Field-Treated Ni/Co_(3)O_(4) Film as High-Performance Bifunctional Electrocatalysts for Efficient Overall Water Splitting

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Nano-Micro Letters 2022年第9期14卷 160-173页

作者： Junming Li Jun Li Jun Ren Hong Hong Dongxue Liu Lizhe Liu Dunhui Wang National Laboratory of Solid State Microstructures Collaborative Innovation Center of Advanced MicrostructuresJiangsu Provincial Key Laboratory for NanotechnologySchool of PhysicsNanjing UniversityNanjing 210093People’s Republic of China Hangzhou Dianzi University Hangzhou 310018People’s Republic of China

Rational design of bifunctional electrocatalysts for oxygen evolution reaction(OER)and hydrogen evolution reaction(HER)with excellent activity and stability is of great significance,since overall water splitting is a promising technology for sustainable conversion of clean energy.However,most electrocatalysts do not simultaneously possess optimal HER/OER activities and their electrical conductivities are intrinsically low,which limit the development of overall water splitting.In this paper,a strategy of electric field treatment is proposed and applied to Ni/Co_(3)O_(4) film to develop a novel bifunctional electrocatalyst.After treated by electric field,the conductive channels consisting of oxygen vacancies are formed in the Co_(3)O_(4) film,which remarkably reduces the resistance of the system by almost 2×10^(4) times.Meanwhile,the surface Ni metal electrode is partially oxidized to nickel oxide,which enhances the catalytic activity.The electric-field-treated Ni/Co_(3)O_(4) material exhibits super outstanding performance of HER,OER,and overall water splitting,and the catalytic activity is significantly superior to the state-of-the-art noble metal catalysts(Pt/C,RuO_(2),and RuO_(2)‖Pt/C couple).This work provides an effective and feasible method for the development of novel and efficient bifunctional electrocatalyst,which is also promising for wide use in the field of catalysis.

关键词： Bifunctional electrocatalyst Overall water splitting Co_(3)O_(4)film oxygen vacancies Electric field

Photocatalytic Aerobic Oxysulfonylation of Alkynes to Access β-Keto Sulfones Catalyzed by OVs-N-Nb_(2)O_(5)

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Chinese Journal of Chemistry 2022年第22期40卷 2618-2624页

作者： Tao Song Yinpan Zhang Chun Wang Yafei Li Yong Yang CAS Key Laboratory of Bio-based Materials Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesShandong Energy InstituteQingdaoNewEnergyShandongLaboratoryQingdaoShandong266101China Schoolof Chemistry and Materials Science Nanjing Normal UniversityNanjingJiangsu 210023China

Herein,we report a novel heterogeneous photocatalyst for radical-mediated oxidative oxysulfonylation of alkynes toβ-keto sulfones under environmentally benign conditions.The oxygen vacancy-rich semiconductor Nb2O5(labeled as OVs-N-Nb_(2)O_(5))could efficiently catalyze a wide range of alkynes,especially for those bearing electron-deficient substituents or internal alkynes,to their correspondingβ-keto sulfones in good to high yields with good tolerance of diverse functional groups under visible-light illumination.The late-stage modification of steroidal compounds and synthesis of bioactive molecules were also achieved via this procedure,highlighting its potential for practical applications.Meanwhile,the photocatalyst OVs-N-Nb_(2)O_(5) showed outstanding catalytic stability for successive recycles without appreciable loss in activity and selectivity.The critical role of oxygen vacancies on improving reaction activity and selectivity was clearly disclosed via control experiments and theoretical calculation.

关键词： oxygen vacancies Semiconducts Photocatalysis Oxysulfonylation of alkynes β-Keto sulfones

Interfacial processes and mechanisms of synergistic degradation of dichlorobiphenyl by white rot fungi and magnetite nanoparticles

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Science China Earth Sciences 2023年第9期66卷 2057-2065页

作者： Le CHANG Guanghui YU Congqiang LIU Institute of Surface-Earth System Science School of Earth System ScienceTianjin Key Laboratory of Earth Critical Zone Science and Sustainable Development in Bohai RimBohai Coastal Critical Zone National Observation and Research StationTianjin UniversityTianjin 300072China

The rapid increase in the artificial syntheses of organic pollutants has raised widespread concern.However,the mechanisms by which fungi degrade these new organic pollutants in the environment and adapt to environmental stressors remain unclear.In this study,Phanerochaete chrysosporium,a model white rot fungus,was used to explore the interfacial processes and mechanisms for synergistic degradation of 4,4′-dichlorobiphenyl(PCB15)with magnetite nanoparticles.The results showed that after 3 and 5 days of cultivation with Phanerochaete chrysosporium alone,the rates for PCB15 degradation were 32%and 65%,respectively,indicating that the white rot fungus itself was able to degrade the organic pollutant.Moreover,the addition of magnetite nanoparticles significantly enhanced the degradation of PCB15 by Phanerochaete chrysosporium.After cocultivation for 3 and 5 days,the rates for PCB15 degradation increased to 42%and 84%,respectively.Synchrotron radiation-based Fourier transform infrared spectromicroscopy(SR-FTIR)showed that the magnetite particles were tightly adhered to the fungal hyphae and were unevenly distributed on the hyphal surfaces.Furthermore,cocultivation of the fungus and magnetite nanoparticles significantly enhanced the nanozymatic activity of magnetite.A linear regression model provided a significantly negative correlation(r=−0.96,poxygen vacancies on the mineral surfaces rather than the iron valence.Together,these findings increase our understanding of the powerful capabilities of fungi in terms of stress resistance and adaptation to extreme environments and provide new insights into fungal-mediated degradation of organic pollutants for soil remediation in contaminated si

关键词： Magnetite nanoparticles Nanozymes oxygen vacancies White rot fungi X-ray photoelectron spectroscopy Synchrotron radiation based FTIR spectromicroscopy Dichlorobiphenyl

Construction of defect-containing UiO-66/MoSe_(2) heterojunctions with superior photocatalytic performance for wastewater treatment and mechanism insight

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Frontiers of Chemical Science and Engineering 2023年第4期17卷 449-459页

作者： Xiao Han Xiaoxuan Wang Jiafang Wang Yingjie Xie Cuiwei Du Chongfei Yu Jinglan Feng Jianhui Sun Shuying Dong School of Environment Henan Normal UniversityXinxiang 453007China Key Laboratory for Yellow River and Huai River Water Environmental and Pollution Control Ministry of EducationXinxiang 453007China

Metal-organic frameworks are recognized as promising multifunctional materials,especially metal-organic framework-based photocatalysts,which are considered to be ideal photocatalytic materials.Herein,a new type of UiO-66/MoSe_(2) composite was prepared using the solvothermal method.The optimum composite was selected by adjusting the mass ratio of UiO-66 and MoSe_(2).X-ray diffraction analysis showed that the mass ratio influenced the crystal plane exposure rate of the composite,which may have affected its photocatalytic performance.The composite is composed of ultra-thin flower-like MoSe_(2) that wrapped around cubic UiO-66,a structure that increases the abundance of active sites for reactions and is more conducive to the separation of carriers.The photocatalytic properties of the composite were evaluated by measuring the degradation rate of Rhodamine B and the catalyst’s ability to reduce Cr(VI)-containing wastewater under visible light irradiation.Rhodamine B was decolorized completely in 120 min,and most of the Cr(VI)was reduced within 150 min.The photochemical mechanism of the complex was studied in detail.The existence of Mo^(6+)and oxygen vacancies,in addition to the Z-type heterojunction promote the separation of electrons and holes,which enhances the photocatalytic effect.

关键词： UiO-66 MoSe_(2) photocatalysis dye-containing wastewater heavy metal wastewater oxygen vacancies

Electrodeposited 3D hierarchical NiFe microflowers assembled from nanosheets robust for the selective electrooxidation of furfuryl alcohol

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Green Energy & Environment 2023年第3期8卷 874-882页

作者： Biying Liu Man Zhang Yaoyu Liu Yuchen Wang Kai Yan Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology School of Environmental Science and EngineeringSun Yat-sen University135 Xingang Xi RoadGuangzhou510275China

A robust and green strategy for the selective upgrading of biomass-derived platform chemicals towards highly valuable products is important for the sustainable development.Herein,the efficient electrocatalytic oxidation of biomass-derived furfuryl alcohol(FFA)into furoic acid(FurAc)catalyzed by the electrodeposited non-precious NiFe microflowers was successfully reached under the low temperature and ambient pressure.The 3D hierarchical NiFe microflowers assembled from ultrathin nanosheets were controllably synthesized by the electrodeposition method and uniformly grown on carbon fiber paper(CFP).Electrochemical analysis confirmed that NiFe nanosheets more preferred in the selective oxidation of FFA(FFAOR)than oxygen evolution reaction(OER).The linear sweep voltammetry(LSV)in FFAOR displayed a clear decrease towards lower potential,resulting in 30 mV reduction of overpotential at 20 mA cm^(-2) compared with that of OER.The optimal catalyst Ni_(1)Fe_(2) nanosheets exhibited the highest selectivity of FurAc(94.0%)and 81.4%conversion of FFA within 3 h.Besides,the influence of various reaction parameters on FFAOR was then explored in details.After that,the reaction pathway was investigated and rationally proposed.The outstanding performance for FFAOR can be ascribed to the unique structure of 3D flower-like NiFe nanosheets and oxygen vacancies,resulting in large exposure of active sites,faster electron transfer and enhanced adsorption of reactants.Our findings highlight a facile and convenient mean with a promising green future,which is promising for processing of various biomass-derived platform chemicals into value-added products.

关键词： Electrodeposition Microflowers assembled by nanosheets NiOOH oxygen vacancies Electrochemical oxidation Furfuryl alcohol Furoic acid

CeO_(2)and CeO_(2)-based nanomaterials for photocatalytic,antioxidant and antimicrobial activities

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Journal of Rare Earths 2023年第2期41卷 167-181页

作者： Shaidatul Najihah Matussin Mohammad Hilni Harunsani Mohammad Mansoob Khan Chemical Sciences Faculty of ScienceUniversiti Brunei DarussalamJalan Tungku LinkGadongBE 1410Brunei Darussalam

Cerium oxide(CeO_(2)),one of the most significant rare-earth oxides,has attracted considerable interest over the past decades.This is primarily due to the ease in Ce^(3+)/Ce^(4+)redox ability as well as other factors that affect the efficacy of CeO_(2)and CeO_(2)-based materials.CeO_(2)and CeO_(2)-based materials have shown enhanced responses in catalytic and photocatalytic activities for environmental and biological applications.In addition,the formation of Ce^(3+)and oxygen vacancies in CeO_(2)has aided in enhancing CeO_(2)activities.In order to produce oxygen-deficient CeO_(2)and CeO_(2)-based materials,a variety of synthesis methods were used and are highlighted in this review.Therefore,this review compiles and discusses the mechanisms that involve oxygen vacancies,defects,and Ce^(3+)formation for environmental applications,such as photocatalytic dye degradation,photocatalytic CO_(2)reduction,and non-colored pollutants removal.The biological applications of CeO_(2),such as antioxidant enzyme mimetic,antioxidant reactive oxygen species/reactive nitrogen species,and antimicrobial activities,are also discussed.Additionally,future prospects are also suggested for future development and detailed investigations.

关键词： oxygen vacancies oxygen deficient CeO_(2) Ce^(3+)/Ce4^(+) Environmental applications Biological applications Rare earths

oxygen vacancies in ferroelectric perovskites and their regulation from first-principles study

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Oxygen vacancies in ferroelectric perovskites and their regu...

Defective layered Mn-based cathode materials with excellent performance via ion exchange for Li-ion batteries

第十三届全国物理力学学术会议

作者： Q.Yang J.X.Cao Y.C.Zhou Key Laboratory of Low Dimensional Materials and Application Technology of Ministry of Education Xiangtan University

oxygen vacancy(VO)is one of the common and mobile defects,which is believed to play an important role in the electrical properties of ferroelectric materials.In present work,the physical properties of VO were studied with a prototypical ferroelectric perovskite oxide Pt Ti O3(PTO)using density functional theory(DFT)calculation.Meanwhile,we studied the effects of potential regulation means,such as epitaxial strain,on the structural and electronic properties of VO.VO was found to result in a tail-to-tail domain configuration and pinning the domain wall movement.Our results show that VO in ferroelectric epitaxial thin films can be systematically tuned from a strong domain-pinning centre to a non-pinning centre by applying a compressive misfit strain.The formation and migration energies of VO can be enhanced by compressive strain.This suggests that proper strain may solve the VO-induced ferroelectric failure.

关键词： Ferroelectric perovskites oxygen vacancies Domain-pinning centre Leakage current First-principles study

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Journal of Energy Chemistry 2023年第7期82卷 537-546,I0012页

作者： Yongheng Si Kun Bai Yaxin Wang Han Lu Litong Liu Ziyan Long Yujuan Zhao Beijing Key Laboratory for Green Catalysis and Separation Department of ChemistryThe Faculty of Environment and LifeBeijing University of TechnologyBeijing 100124China

Defective layered Mn-based materials were synthesized by Li/Na ion exchange to improve their electrochemical activity and Coulombic efficiency.The annealing temperature of the Na precursors was important to control the P3-P2 phase transition,which directly affected the structure and electrochemical characteristics of the final products obtained by ion exchange.The O3-Li_(0.78)[Li_(0.25)Fe_(0.075)Mn_(0.675)]O_(δ) cathode made from a P3-type precursor calcined at 700℃ was analyzed using X-ray photoelectron spectrometry and electron paramagnetic resonance.The results showed that the presence of abundant trivalent manganese and defects resulted in a discharge capacity of 230 mAh/g with an initial Coulombic efficiency of about 109%.Afterward,galvanostatic intermittent titration was performed to examine the Li^(+) ion diffusion coefficients,which affected the reversible capacity.First principles calculations suggested that the charge redistribution induced by oxygen vacancies(OV_(s))greatly affected the local Mn coordination environment and enhanced the structural activity.Moreover,the Li-deficient cathode was a perfect match for the pre-lithiation anode,providing a novel approach to improve the initial Coulombic efficiency and activity of Mn-based materials in the commercial application.

关键词： Ion exchange Defective cathode materials oxygen vacancies Initial coulombic efficiency DFT calculations