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Removal of kathon by UV-C activated hydrogen peroxide:Kinetics,mechanisms,and enhanced biodegradability assessment

chinese Journal of chemical Engineering 2024年第1期65卷 178-187页

作者： Jinzhi Cui Guiqiao Wang Xing Rong Wensu gao Yaxin Lu Yawen Luo Lichao Zhang Zhongfa cheng Canzhu gao School of Environmental Science and Engineering Shandong UniversityQingdao 266237China Shandong Taihe Technologies Co. Ltd.Zaozhuang 250031China

Kathon(CMI-MI),a mixture of 5-chloro-2-methyl-4-isothiazolin-3-one(CMI)and 2-methyl-4-isothiazolin-3-one(MI),was extensively used in industry as a nonoxidizing biocide or ***,it would show adverse effects on aquatic life when it is discharged into surface *** this study,the removal performance,parameter influence,degradation products and enhancement of subsequent biodegradation of CMI-MI in UV/H_(2)O_(2)system were systematically *** degradation rate of CMI-MI could reach 90%under UV irradiation for 20 min when the dosage of H_(2)O_(2)was 0.3 mmol·L^(–1).The DOC(dissolved organic carbon)mineralization rate of CMI-MI could reach 35%under certain conditions([H_(2)O_(2)]=0.3 mmol·L^(–1),UV irradiation for 40 min).kobs was inversely proportional to the concentration of CMI-MI and proportional to the concentration of H_(2)O_(2).The degradation rate of CMIMI was almost unchanged in the pH range from 4 to *** the presence of CO_(3)^(2-)inhibited the removal rate of CMI-MI,SO_(4)^(2-),Cl^(-),NO_(3)^(-),and NH_(4)^(+) did not interfere with the degradation of CMI-MI in the *** was found that UV/H_(2)O_(2)system had lower energy consumption and more economic advantage compared with UV/PS system by comparing the EEO(electric energy per order)values under the same *** main organic products were identified,namely HCOOH and ch_(3)NH_(2).There’s also the formation of Cl^(-)and SO_(4)^(2-).After UV and UV/H_(2)O_(2)photolysis,the biochemical properties of CMI-MI solution were obviously improved,especially the UV/H_(2)O_(2)treatment effect was better,indicating that UV/H_(2)O_(2)technology is expected to combine with biotechnology to remove CMI-MI effectively and environmentally friendly from wastewater.

关键词： Kathon UV/H_(2)O_(2) Biological degradation Circulating cooling water

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Role of polarization evolution in the hysteresis effect of Pb-based antiferroelecrtics

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chinese chemical Letters 2024年第4期35卷 516-519页

作者： Botao gao He Qi Hui Liu Jun chen Beijing Advanced Innovation Center for Materials Genome Engineering Department of Physical ChemistryUniversity of Science and Technology BeijingBeijing 100083China Shanghai Institute of Ceramics Chinese Academy of SciencesShanghai 201899China Hainan University Haikou 570228China

The electric field-induced irreversible domain wall motion results in a ferroelectric(FE) hysteresis. In antiferroelectrics(AFEs), the irreversible phase transition is the main reason for the hysteresis effects, which plays an important role in energy storage performance. Compared to the well-demonstrated FE hysteresis,the structural mechanism of the hysteresis in AFE is not well understood. In this work, the underlying correlation between structure and the hysteresis effect is unveiled in Pb(Zr,Sn,Ti)O_(3) AFE system by using in-situ electrical biasing synchrotron X-ray diffraction. It is found that the AFE with a canting dipole configuration, which shows a continuous polarization rotation under the electric field, tends to have a small hysteresis effect. It presents a negligible phase transition, a small axis ratio, and electric field-induced lattice changing, small domain switching. All these features together lead to a slim hysteresis loop and a high energy storage efficiency. These results offer a deep insight into the structure-hysteresis relationship of AFEs and are helpful for the design of energy storage material.

关键词： Antiferroelectric Hysteresis effect Structure refinement Perovskite In situ synchrotron radiation

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Ligand modulation of active center to promote lead-free Cs_(2)AgInCl_(6)photocatalytic CO_(2)reduction

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Journal of Energy chemistry 2024年第8期95卷 660-669,I0015页

作者： Baofei Sun Wei chen Yanyi Huang Daofu Wu Heng Luo Faguang Kuang Hongmei Ran Yichen Liu Liqin gao Jinchen Zhou Bo gao Qiang Huang Xiaosheng Tang Key Laboratory of Human Brain Bank for Functions and Diseases of Department of Education of Guizhou Province College of Basic MedicalGuizhou Medical UniversityGuiyang 550025GuizhouChina School of Electromechanical and Automotive Engineering Yantai UniversityYantai 264005ShandongChina State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina College of Optoelectronic Engineering Chongqing University of Posts and TelecommunicationsChongqing 400065China Key Laboratory of Optoelectronic Technology&Systems(Ministry of Education) College of Optoelectronic EngineeringChongqing UniversityChongqing 400044China School of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001HenanChina

Metal halide perovskites(MHP)are potential candidates for the photocatalytic reduction of CO_(2)due to their long photogenerated carrier lifetime and charge diffusion ***,the conventional long-chain ligand impedes the adsorption and activation of CO_(2)molecules in practical ***,a ligand modulation technology is employed to enhance the photocatalytic CO_(2)reduction activity of lead-free Cs_(2)AgInCl_(6)microcrystals(MCs).The Cs_(2)AgInCl_(6)MCs passivated by Oleic acid(OLA)and Octanoic acid(OCA)are used for photocatalytic CO_(2)*** results show that the surface defects and electronic properties of Cs_(2)AgInCl_(6)MCs can be adjusted through ligand *** with the OLA-Cs_(2)AgInCl_(6),the OCA-Cs_(2)AgInCl_(6)catalyst demonstrated a significant improvement in the catalytic yield of CO and ch_(4).The CO and ch_(4)catalytic yields of OCA-Cs_(2)AgInCl_(6)reached 171.88 and34.15μmol g^(-1)h^(-1)which were 2.03 and 12.98 times higher than those of OLA-Cs_(2)AgInCl_(6),and the total electron consumption rate of OCA-Cs_(2)AgInCl_(6)was 615.2μmol g^(-1)h^(-1)which was 3.25 times higher than that of OLA-Cs_(2)AgInCl_(6).Furthermore,in situ diffuse reflectance infrared Fourier transform spectra revealed the enhancement of photocatalytic activity in Cs_(2)AgInCl_(6)MCs induced by ligand *** study illustrates the potential of lead-free Cs_(2)AgInCl_(6)MCs for efficient photocatalytic CO_(2)reduction and provides a ligand modulation strategy for the active promotion of MHP photocatalysts.

关键词： Surface ligand Photocatalysis CO_(2)reduction Lead-free perovskite Reactive mechanism

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A Scalable Pillar Layered Metal-Organic Framework for Natural Gas Purification

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chemical Research in chinese Universities 2024年第4期40卷 675-681页

作者： LU Nan LAN Lan gao Qiang LI Na BU Xian-He School of Materials Science and Engineering Nankai UniversityTianjin300350P.R.China State Key Laboratory of Elemento-Organic chemistry College of ChemistryNankai UniversityTianjin300071P.R.China School of Environmental and chemical Engineering Jiangsu University of Science and TechnologyZhenjiang212003P.R.China

One-step harvest of high-purity methane(ch_(4))from ternary propane/ethane/methane(C_(3)H_(8)/C_(2)H_(6)/ch_(4))mixtures remains a desirable yet challenging goal for natural gas ***,adsorbents either suffer from high capacity and selectivity,or are caught in a dilemma of scalable ***,we demonstrate a scalable pillar layered metal-organic framework Ni-MOF for highly efficient one-step ch_(4)***-MOF exhibits high C_(2)H_(6)and C_(3)H_(8)uptakes of 83.3 and 86.1 cm^(3)/g at 298 K and 100 kPa and remarkable C_(2)H_(6)/ch_(4)(50/50,volume ratio,21.5)and C_(3)H_(8)/ch_(4)(50/50,volume ratio,212.0)***,high C_(2)H_(6)(42.2 cm^(3)/g at 10 kPa)and C_(3)H_(8)(64.7 cm^(3)/g at 5 kPa)capacities in the low-pressure region at 298 K were realized on Ni-MOF,suggesting the strong affinities of Ni-MOF towards C_(2)H_(6)and C_(3)H_(8).Furthermore,the dynamic breakthrough experiments revealed that purifying ch_(4)from natural gas in one-step can be achieved in Ni-MOF with high-purity(>99.8%)and productivity(346.0 cm^(3)/g).Most significantly,the production of Ni-MOF can be scalably synthesized at room temperature,rendering it promising potential for industrial *** combined advantages of exceptional separation performance,scalability,and cycle stability of Ni-MOF pave the way for one-step ch_(4)purification from natural gas.

关键词： Metal-organic framework Adsorption and separation Natural gas purification Scale-up synthesis

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Peracetic acid catalytic activation using Co3O4 nanocluster decorated graphitic carbon nitride for cefapirin degradation in water

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Science china Technological Sciences 2024年第10期67卷 3103-3115页

作者： YIN ShiMei gao YiXuan chEN Long LI Fan LIU XiaoNa QI Fei LIU Wen Beijing Key Lab for Source Control Technology of Water Pollution College of Environmental Science and EngineeringBeijing Forestry University Key Laboratory of Water and Sediment Sciences (Ministry of Education) College of Environmental Sciences and EngineeringPeking University School of Environmental Science and Engineering Taiyuan University of Technology State Environmental Protection Key Laboratory of All Material Fluxes in River Ecosystems Peking University Beijing National Laboratory for Molecular Sciences Peking University

This study innovated cobalt-based catalytic nanocomposites（CCNs） for the heterogeneous activation of peracetic acid（PAA）,a green and efficient advanced oxidation process for removing antibiotics from *** Co3O4catalysts exhibit limited activity due to stable electronic *** overcome this,CCNs were synthesized using a one-step condensation method,incorporating a size control strategy that anchors Co3O4nanoclusters within 4-5 nm onto six-fold cavity of g-C3N4,simultaneously modifying the coordination environment of *** alteration significantly enhances the adsorption energy of PAA and catalytic activity compared to commercial *** improved performance of CCN2,in particular,is attributed to a shift in the cobalt d band center towards the Fermi level,facilitating electron delocalization and transfer,enhancing Co-O bonding,and accelerating PAA ***2's superior activity,with a cefapirin（CFP） degradation kinetic rate constant(k1=0.760 min-1)～11 times that of PAA direct oxidation(k1=0.070 min-1) and～5 times that of commercial Co3O4/PAA system(k1=0.164 min-1),is due to its ability to generate dominant reactive species for antibiotic degradation,including alkoxy radicals(ch3C（=O）OO·),high valence metal(CoⅣ（=O）2+),and singlet oxygen（1O2）,with the latter two being crucial for the degradation *** degradation of CFP involved three mechanisms,including direct oxidation by PAA,decarboxylation,and open-ring reactions at nitrogen *** research provides insights into developing high-activity catalysts for efficient PAA activation and antibiotic removal,leveraging the strategy of shifting the transition metal d band center.

关键词： peracetic acid Co3O4 nanocluster high valence metal singlet oxygen cefapirin

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Siliceous mesocellular foam supported Cu catalysts for promoting non-thermal plasma activated CO_(2) hydrogenation toward methanol synthesis

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Frontiers of chemical Science and Engineering 2024年第7期18卷 55-65页

作者： Yi chen Shaowei chen Yan Shao Cui Quan Ningbo gao Xiaolei Fan Huanhao chen State Key Laboratory of Materials-Oriented chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China School of Environmental Science and Engineering Nanjing Tech UniversityNanjing 211816China School of Energy and Power Engineering Xi’an Jiaotong UniversityXi’an 710049China Department of chemical Engineering School of EngineeringThe University of ManchesterManchester M139PLUK Nottingham Ningbo china Beacons of Excellence Research and Innovation Institute University of Nottingham Ningbo ChinaNingbo 315048China Institute of Wenzhou Zhejiang UniversityWenzhou 325006China

Electrified non-thermal plasma (NTP) catalytic hydrogenation is the promising alternative to the thermal counterparts, being able to be operated under mild conditions and compatible with green electricity/hydrogen. Rational design of the catalysts for such NTP-catalytic systems is one of the keys to improve the process efficiency. Here, we present the development of siliceous mesocellular foam (MCF) supported Cu catalysts for NTP-catalytic CO_(2) hydrogenation to methanol. The findings show that the pristine MCF support with high specific surface area and large mesopore of 784 m2·g−1 and ~8.5 nm could promote the plasma discharging and the diffusion of species through its framework, outperforming other control porous materials (viz., silicalite-1, SiO_(2), and SBA-15). Compared to the NTP system employing the bare MCF, the inclusion of Cu and Zn in MCF (i.e., Cu1Zn1/MCF) promoted the methanol formation of the NTP-catalytic system with a higher space-time yield of methanol at ~275 μmol·g_(cat)^(−1)·h^(−1) and a lower energy consumption of 26.4 kJ^(−1)·mmol_(ch_(3)OH)^(-1) (conversely, ~225 μmol·g_(cat)^(−1)·h^(−1) and ~71 kJ^(−1)·mmol_(ch_(3)OH)^(-1), respectively, for the bare MCF system at 10.1 kV). The findings suggest that inclusion of active metal sites (especially Zn species) could stabilize the CO_(2)/CO-related intermediates to facilitate the surface reaction toward methanol formation.

关键词： non-thermal plasma(NTP)catalysis Cu catalyst CO_(2)hydrogenation methanol siliceous mesocellular foam(MCF)

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Nickel-modified In_(2)O_(3) with inherent oxygen vacancies for CO_(2) hydrogenation to methanol

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Science china chemistry 2024年第5期67卷 1715-1728页

作者： Zixuan Zhou Yuchen Wang Yuanjie Bao Haiyan Yang Jiong Li chunran chang Shenggang Li Peng gao CAS Key Laboratory of Low-Carbon Conversion Science and Engineering Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201210China University of chinese Academy of Sciences Beijing 100049China School of Physical Science and Technology ShanghaiTech UniversityShanghai 201210China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China Shaanxi Key Laboratory of Low Metamorphic Coal Clean Utilization School of Chemistry and Chemical EngineeringYulin UniversityYulin 719000China

Methanol synthesis is one of the most important industrially-viable approaches for carbon dioxide(CO_(2)) utilization, as the produced methanol can be used as a platform chemical for manufacturing green fuels and chemicals. The In_(2)O_(3) catalysts are ideal for sustainable methanol synthesis and have received considerable attention. Herein, Co-, Ni-and Cu-modified In_(2)O_(3) catalysts were fabricated with high dispersion and high stability to improve the hydrogenation performance. The Ni-promoted In_(2)O_(3) catalyst in the form of high dispersion possessed the largest amount of oxygen vacancies and the strongest ability for H_(2) activation, leading to the highest CO_(2) conversion and space time yield of methanol of 0.390 g_(Me OH)g_(cat)^(-1)h^(-1) with ch_(3)OH selectivity of 68.7%. In addition, the catalyst exhibits very stable performance over 120 h on stream, which suggests the promising prospect for industrial applications. Further experimental and theoretical studies demonstrate that surface Ni doping promotes the formation of oxygen defects on the In_(2)O_(3) catalyst, although it also results in lower methanol selectivity. Surprisingly, subsurface Ni dopants are found to be more beneficial for methanol formation than surface Ni dopants, so the Nipromoted In_(2)O_(3)catalyst with a lower surface Ni content at the similar Ni loading can reach higher methanol selectivity and productivity. This work thus provides theoretical guidance for significantly improving the CO_(2) reactivity of In_(2)O_(3)-based catalysts while maintaining high methanol selectivity.

关键词： carbon dioxide hydrogenation methanol synthesis indium oxides Ni doping sites transition metal promoters

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Investigation of oxy-fuel combustion for methane and acid gas in a diffusion flame

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chinese Journal of chemical Engineering 2024年第1期65卷 106-116页

作者： Songling Guo Xun Tao Fan Zhou Mengyan Yu Yufan Wu Yunfei gao Lu Ding Fuchen Wang Institute of Clean Coal Technology East China University of Science and TechnologyShanghai 200237China

Co-combustion of methane(ch4)and acid gas(AG)is required to sustain the temperature in Claus reaction *** this study,oxy-fuel combustion of methane and acid gas has been experimentally studied in a diffusion *** equivalence ratios(ER=1.0,1.5,2.0)and ch_(4)-addition ratios(ch_(4)/AG=0.3,0.5,0.7)were examined and the flame was interpreted by analyzing the distributions of the temperature and species concentration along central ***_(4)-AG diffusion flame could be classified into three sections namely initial reaction,oxidation and complex reaction *** oxidation of ch_(4)and H_(2)S was noted in the first section wherein H_(2)S was preferred and both were mainly proceeding decomposition and partial ***_(2)was formed at oxidation section together with obvious presence of H2 and ***,H2 and CO were inclined to be sustained under fuel rich condition in the complex reaction *** ER and increasing ch4/AG contributed to higher temperature,H_(2)S and ch_(4)oxidation and CO_(2)*** a growing trend for ch_(4)and AG to convert into H_(2),CO and SO_(2)could be *** this factor enhanced the generation of CS2 and COS in the flame inner core by interactions of ch4 and CO_(2)with sulfur *** was formed through the interactions of CO and CO_(2)with sulfur *** CS_(2)production directly relied on reaction of ch_(4)with sulfur *** concentration of COS was greater than CS_(2)since CS_(2)was probably inhibited due to the presence of H_(2).COS and CS_(2)could be consumed by further oxidation or other complex reactions.

关键词： Acid gas Methane Oxy-fuel combustion Oxidation chemical analysis Carbon sulfides

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Remarkably Enhanced Methane Sensing Performance at Room Temperature via Constructing a Self-Assembled Mulberry-Like ZnO/SnO_(2) Hierarchical Structure

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Energy & Environmental Materials 2024年第3期7卷 337-344页

作者： Xun Li Tian Tan Wei Ji Wanling Zhou Yuwen Bao Xiaohong Xia Zhangfan Zeng Yun gao Ministry-of-Education Key Laboratory for the Green Preparation and Application of Functional Materials School of Materials Science&EngineeringHubei UniversityWuhan 430062China School of Artificial Intelligence Hubei UniversityWuhan 430062China

Development of metal oxide semiconductors-based methane sensors with good response and low power consumption is one of the major challenges to realize the real-time monitoring of methane *** this work,a self-assembled mulberry-like ZnO/SnO_(2)hierarchical structure is constructed by a two-step hydrothermal *** resultant sensor works at room temperature with excellent response of~56.1%to 2000 ppm ch_(4)at 55%relative *** is found that the strain induced at the ZnO/SnO_(2)interface greatly enhances the piezoelectric polarization on the ZnO surface and that the band bending results in the accumulation of chemically adsorbed O_(2)^(-)ions close to the interface,leading to significant improvement in the sensing performance of the methane gas sensor at room temperature.

关键词： heterojunction methane sensor oxygen vacancy piezoelectric polarization ZnO/SnO_(2)hierarchical structure

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Investigating the Absorption and Desorption Behavior of Methylene chloride in the Poly(aryl ether ketone) Film with Different Crystallinities

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chinese Journal of Polymer Science 2024年第2期42卷 239-246,I0009页

作者： Hong-Ru Yang Jin-Dong Zhang Dong-Ting gao Gang Liu chun-Hai chen Jia-Nan Yao Center for Advanced Low-Dimension Materials State Key Laboratory for Modification of Chemical Fibers and Polymer MaterialsCollege of Materials Science and EngineeringDonghua UniversityShanghai201620China

Poly(aryl ether keton e)(PAEK) films with different crystallinities were obtained by controlling the cooling rate,which were subjected to the absorption and desorption of methylene chloride(ch_(2)Cl_(2)).We employed attenuated total reflection Fourier transform infrared(ATR-FTIR)spectroscopy analyses to investigate the diffusion behavior of ch_(2)Cl_(2) in PAEK films with different *** to the Fickian diffusion model,the calculated diffu sion coefficients of ch_(2)Cl_(2) in PAEK films were observed to decrease with increasing *** effect of ch_(2)Cl_(2)absorption and desorption on the mechanical properties of PAEK films with different crystallinity was further analyzed using tensile *** tensile tests exhibited that ch_(2)Cl_(2) has two concurrent effects:plasticization and solvent-induced *** scanning calorimetry(DSC) and wide-angle X-ray diffraction(WXRD) techniques further confirmed solvent-induced crystallization *** results would be beneficial to understand the solvent resistance of PAEK materials and consequently provide the practical application conditions of PAEK with a theoretical basis.

关键词： Poly(aryl ether ketone) Diffusion behavior Infrared spectra Solvent-induced crystallization Mechanical properties

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