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Chinese Chemical Letters 2024年第4期35卷 17-30页

作者： Li Li Fanpeng Chen Bohang Zhao Yifu Yu Department of Chemistry School of ScienceInstitute of Molecular PlusTianjin UniversityTianjin 300072China

Converting CO_(2) into value-added chemicals and fuels through various catalytic methods to lower the atmospheric CO_(2) concentration has been developed to be a crucial means to alleviate the energy shortage and ameliorate the ever-fragile environment status. However, the complexity of the CO_(2) conversion reaction and the strong reduction conditions lead to the inevitable structural evolution, making it difficult for the prior design of suitable catalytic materials. Herein, to guide the rational design of efficient catalysts,we will be centered on the thermal, electro, and photo-induced structural evolution and Active species identification during the CO_(2) conversion, including the in situ/operando characterization techniques monitoring the activation, steady, and deactivation stage of the catalysts as well as the inherent restructuring mechanism towards Active species. Besides, the future challenges and opportunities on the merits of combining the structural evolution with the adsorbed intermediates recognized by ultra-fast spectroscopic techniques, simultaneously, the combination of theoretical simulation and the results of in situ experiments will also be addressed. This review can not only guide the identification of real Active species, but also provide an approach to design the specific Active species towards CO_(2) conversion, rather than only focusing on activity, for the purpose of practical industrial application.

关键词： CO_(2) Structural evolution Active species In situ Operando

Degradation of Organic Compounds by Active species Sprayed in a Dielectric Barrier Corona Discharge System

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Plasma Science and Technology 2009年第2期11卷 211-215页

作者：李杰宋玲刘强屈广周李国锋吴彦 Institute of Electrostatics and Special Power Dalian University of Technology School of Environmental and Biological Science and Technology Dalian University of Technology Key Laboratory of Industrial Ecology and Environmental Engineering MOE

Investigation was made into the degradation of organic compounds by a dielectric barrier corona discharge （DBCD） system. The DBCD, consisting of a quartz tube, a concentric high voltage electrode and a net wrapped to the external wall （used as ground electrode）, was introduced to generate Active species which were sprayed into the organic solution through an aerator fixed on the bottom of the tube. The effect of four factors-the discharge voltage, gas flow rate, solution conductivity, and pH of wastewater, on the degradation efficiency of phenol was assessed. The obtained results demonstrated that this process was an effective method for phenol degradation. The degradation rate was enhanced with the increase in power supplied. The degradation efficiency in alkaline conditions was higher than those in acid and neutral conditions. The optimal gas flow rate for phenol degradation in the system was 1.6 L/min, while the solution conductivity had little effect on the degradation.

关键词： dielectric barrier corona discharge （DBCD） Active species organic compound degradation wastewater treatment

Strong interface interaction and internal electric field promote electron transfer of Bi_(2)O_(2)S/NiFe_(2)O_(4) heterojunction for photocatalytic antibiotic degradation

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Journal of Materials Science & Technology 2023年第27期158卷 145-155页

作者： Shaoxuan Pang Yilin Dong Dongyu Xu Qiuwen Wang Weihong Gao Lijun Zhang Kang Wang Guangming Zhang Longyi Lv Yuguo Xia Zhijun Ren Pengfei Wang School of Energy and Environmental Engineering Hebei University of TechnologyTianjin 300401China Tianjin Key Laboratory of Clean Energy and Pollutant Control Tianjin 300401China School of Chemistry and Chemical Engineering National Engineering Research Center for Colloidal MaterialsShandong UniversityJinan 250100China

Heterojunction photocatalysts have shown considerable activities for organic pollutants degradation.However,the faint connection interface and inferior charge shift efficiency critically block the property of heterojunction photocatalysis.Herein,Bi_(2)O_(2)S/NiFe_(2)O_(4) nanosheets heterojunction with ultrastrong inter-face interaction and high internal electric field are designed by an in-situ growth method.Tentative and theoretical consequences prove that the interfacial interaction and internal electric field not only act as the electron flow bridge but also decrease the electrons shift energy obstacle,thus speeding up electrons transfer and achieving effective spatial electron-hole separation.Therefore,a large amount of·O_(2)^(-)and holes as Active species were generated.Remarkably,Bi_(2)O_(2) S/NiFe_(2)O_(4) establishes a considerably boosted photocatalytic performance for tetracycline degradation(0.032 min^(-1)),which is about 14.2-fold and 7.8-fold of the pristine BOS and NFO,respectively.This work provides a promising motivation for modulating charge transfer by interface control and internal electric field to boost photocatalytic performance.

关键词： Bi_(2)O_(2)S/NiFe_(2)O_(4) S-scheme heterojunction Ultrastrong interface interaction Internal electric field Active species Photocatalytic degradation

One-pot synthesis of Fe/Cu-SSZ-13 catalyst and its highly efficient performance for the selective catalytic reduction of nitrogen oxide with ammonia

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Journal of Environmental Sciences 2021年第2期33卷 306-316页

作者： Jie Wan Jiawei Chen Ru Zhao Renxian Zhou Energy Research Institute Nanjing Institute of TechnologyNanjing 211167China Institute of Catalysis Zhejiang UniversityHangzhou 310028China

Series of Fe/Cu-SSZ-13 catalysts with different Fe loading content were synthesized by simple one-pot strategy.The obtained catalysts were subjected to selective catalytic reduction(SCR)of NO x with NH 3 and were characterized by various techniques.The results show that Fe 0.63/Cu 1.50-SSZ-13 catalyst with proper Fe content exhibits excellent catalytic activity with widest operation temperature window from 160 to 580℃,excellent hydrothermal stability as well as good resistance to sulfur poisoning when compared with Cu-SSZ-13,signifying its great potential for practical applications.Further characterizations reveal that the synthesized Fe/Cu-SSZ-13 catalysts present typical chabazite(CHA)structure with good crystallinity,while isolated Cu^2+and monomeric Fe 3+are revealed as the predominant copper and iron species.At low temperatures,isolated Cu^2+species act as primary active sites for SCR reaction,while monomeric Fe^3+species provide sufficient active sites for sustain the SCR activity at high temperature.Moreover,Fe over doping would lead to the damage of zeolite structure,destruction of isolated Cu^2+site,as well as the formation of highly oxidizing Fe2O3,thus causing deterioration of catalytic performances.

关键词： NH3-SCR Fe/Cu-SSZ-13 One-pot synthesis Active species

Cerium(Ⅳ)oxide nanocomposites:Catalytic properties and industrial application

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Journal of Rare Earths 2021年第2期39卷 129-139页

作者： Samira Bagheri Ibrahim Khalil Nurhidayatullaili Muhd Julkapli Nanotechnology and Catalysis Research Centre(NANOCAT) Institute for Advanced StudiesLevel 3Block AUniversity of Malaya50603 Kuala LumpurMalaysia

This review article provides a new insight on the application of cerium oxide(CeO_(2))-metal oxide nanocomposites as catalyst with enhanced reducibility and improved oxygen(O_(2))storage capacity,especially in the varying chemical reaction processes including combustion,oxidation,epoxidation and redox.The CeO_(2)-metal oxide interaction plays an important role in controlling particle size,O_(2) availability and coke resistance properties of the catalyst.Strong metal oxide-CeO_(2) interaction also assists in generating small and highly dispersed particles,resists sintering of catalyst particles during the catalysis process,and consequently improves the O_(2) availability of the catalyst.Indeed,CeO_(2) not only provides an active support to heterogeneous catalyst,but also creates a new active site at the metal-support interface to produce stronger nanoparticle bonding through the surface O_(2) vacancy.This consequently produces a heterogeneous catalytic system with promising reaction rate and catalytic stability in many industrial applications such as CO_(2) hydrogenation,CO oxidatio n,biodiesel productio n,gas reduction,photocatalytic and methane steam reforming.

关键词： Interface Composition Synergistic effect Active species Physiochemical Rare earths

Fabrication of Z-Scheme WO3/KNbO3 Photocatalyst with Enhanced Separation of Charge Carriers

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Chemical Research in Chinese Universities 2020年第5期36卷 901-907页

作者： ZHENG Xiuzhen HAN Huijuan YE Xiangju MENG Sugang ZHAO Shuangshuang WANG Xiangxiang CHEN Shifu College of Chemistry and Materials Science Huaibei Notmal UniversityHuaihei 235000P.R.China State Key Laboratory of Photocatalysis on Energy and Environment Fuzhou UniversityFuzhou 350116P.R.China College of Chemistry and Material Engineering Anhui Science and Technology UniversityFengyang 233100P.R.China

Z-Schemc photocatalysts as a research locus pertomi strong redox capability and high photocatalytic peribnnance.WO3/KNbO3 photocatalysts were fabricated by ball milling method,and performed higlier photocatalytic activity in liquid degradation(rhodamine B,methylene blue and bisphenol A),compared with WO3 or KNbO3 monomer.This is due to that Z-scheme heterojunction is lonned between WO3 and KNbO3,and the holes photo-excited in valence band of KNbO?are quickly combined with the electrons in conduction band of WO3.The electrons accumulated in conduction band of KNbO3 show high reducibility,thereby reducing O2 to·O 2-,and the holes in valence band of WO3 show high oxidative to oxidize H2O to·OH,respectively.Furthermore,it is proved by means of electron spin resonaiice(ESR)spectra,terephthalic acid photolumiiiescence probing technique(TA・PL),and UV-Vis absorption spectra of nitroblue tetrazolium.This work indicates that the iabrication of Z-scheme structure can improve the photocatalytic activity by efficiently separating the photogenerated electrons and holes in the photocatalytic reaction system,which is helpful to deeply understand the migration mechanism of photoexcited cairier(band-band transfer and Z-scheme transfer)in heterojunction photocatalysts.

关键词： WO3/KNbO3- Z-Scheme Photogenerated electron and hole Photocatalytic degradation Active species

Preliminary study of an open-air water-contacting discharge for direct nitrogen fixation

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Plasma Science and Technology 2021年第3期23卷 93-101页

作者：舒展汪传奇 Insaf HOSSAIN 陈强李婉莲王晋琪刘鹏飞熊青 State Key Laboratory of Power Transmission Equipment and System Security and New Technology Chongqing UniversityChongqing 400044People's Republic of China Shenzhen Research Institute of Xiamen University Institute of Electromagnetics and AcousticsFujianProvincial Key Laboratory of Plasma and Magnetic ResonanceKey Laboratory of Electromagnetic Wave Science and Detection TechnologyXiamen UniversityXiamen 361005People's Republic of China

Efficient nitrogen fixation through a reactive plasma process attracts intense interest due to the environmental issues induced by the conventional Haber–Bosch method. In this work, we present a direct and simple fixation routine without any catalysts for nitrogen in open air using an atmospheric-pressure pin-to-solution plasma electrolytic system. Nitrate, nitrite, and ammonia as the nitrogen-derived chemicals in solution were analyzed as indicators under various discharge conditions to estimate the energy efficiency of this process. The results show that the nitrogen fixation process was much more efficient by the pin-positive discharge compared to the negative one. N chemicals preferred to be formed when the solution was of negative polarity. It was also found that, with the help of solution circulation, the energy efficiency was enhanced compared to that of static liquid. However, an inverse trend was observed with the increase of the discharge current. Further study by optical emission spectroscopy indicates the important roles of active N2* and water vapour and their derived species near the plasma–water interface in the fixation process.

关键词： nitrogen fixation air-water discharge energy efficiency Active species plasma-water interface

Nanoceria Supported Gold Catalysts for CO Oxidation

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Chinese Journal of Chemistry 2018年第7期36卷 639-643页

作者： Zhao Jin Yang-Yang Song Xin-Pu Fu Qi-Sheng Song Chun-Jiang Jia Key Laboratory for Colloid and interface Chemistry Key Laboratory of Special Aggregated Materials School of Chemistry and Chemical Engineering Shandong University Jinan Shandong 250100 China

Two types of CeO2 nanocubes （average size of 5 and 20 nm, respectively） prepared via the hydrothermal process were selected to load gold species via a deposition-precipitation （DP） method. Various measurements, including X-ray diffraction （XRD）, Raman spectra, high resolution transmission electron microscopy （HRTEM）, in situ diffuse reflectance infrared Fourier transform spectroscopy （in situ DRIFTS）, and temperature-programmed reduction by hydrogen （H2-TPR）, were applied to characterize the catalysts. It is found that the sample with ceria size of 20 nm （Au/CeO2-20） was covered by well dis ersed both Au^3＋ and Au^δ＋（0〈δ〈1）. For the other sample with ceria size of 5 nm （Au/CEO2-5）, Au^3＋ is the dominant gold species. Au/CeO2-20 performed better catalytic activity for CO oxidation because of the strong CO adsorption of Au^δ＋ in the catalysts. The catalytic activity of Au/CeO2-5 was improved due to the transformation of Au^3＋ to Au^δ＋. Based on the CO oxidation and in situ DRIFTS results, Au^δ＋ is likely to play a more important role in catalyzing CO oxidation reaction.

关键词： gold catalysts nanoceria CO oxidation Active species

Contrasting Behaviours of AC and DC Excited Plasmas in Contact with Liquid

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Plasma Science and Technology 2013年第8期15卷 768-775页

作者：柳晶晶胡晓 Department of Mechanical and Electrical Engineering Guangzhou University

A comparative study of the needle-to-liquid plasma in the continuous mode with DC and AC excitations is detailed in this paper. All plasmas studied here are shown to be glow discharges. This study is based on measurements of several key parameters, including electrical energy, optical emission intensities of Active species, rotational and vibrational temperatures, and temperatures of the needle and liquid electrodes. AC plasmas can produce 1.2～5 times higher excited state Active species than DC plasmas under the same dissipated power. AC excited liquid plasmas have the highest energy utilization efficiency among the three systems （AC excited plasmas, DC excited plasmas with water anode and DC excited plasmas with water cathode）; most of the energy is used to produce useful species rather than to heat the electrodes and plasmas.

关键词： electrical energy Active species rotational temperature vibrational temperature energy use efficiency

Atmospheric Pressure Plasma Jet in Organic Solution:Spectra,Degradation Effects of Solution Flow Rate and Initial pH Value

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Plasma Science and Technology 2014年第12期16卷 1126-1134页

作者：陈秉岩朱昌平陈龙威费峻涛高莹文文单鸣雷任兆杏 Department of Mathematics and Physics Hohai University College of Energy and Electrical Engineering Hohai University Jiangsu Key Laboratory of Power Transmission and Distribution Equipment Technology Institute of Plasma Physics Chinese Academy of Sciences College of Mechanical and Electrical Engineering Hohai University

The organic compounds of p-nitrophenol （PNP） solution was treated by the Active species generated in a stirred reactor by an atmospheric pressure plasma jet （APPJ）. The emission intensities of hydroxyl （OH）, oxygen （O）, nitric oxide （NO）, hydrogen （H） and molecular （N2） were measured by optical emission spectroscopy （OES）. The relations between the flow rates of the PNP solution and degradation, the degradation effects and initial pH value of the solution were also investigated. Experimental results show that there exist intense emissions of O （777.1 nm）, N（337.1 nm）, OH （306-310 nm） and NO band （200-290 nm） in the region of plasma. Given the treatment time and gas flow rate, the degradation increased as a function of discharge energy and solution flow rate, respectively. The solution flow rate for the most efficient degradation ranged from 1.414 m/s to 1.702 m/s, and contributed very little when it exceeded 2.199 m/s. This indicates the existence of diffusion-controlled reactions at a low solution flow rate and activation- controlled reactions at a high solution flow rate. Moreover, increasing or decreasing the initial pH value of neutral PNP solution （pH=5.95） could improve the degradation efficiency. Treated by APPJ, the PNP solutions with different initial pH values of 5.95, 7.47 and 2.78 turned more acidic in the end, while the neutral solution had the lowest degradation efficiency. This work clearly demonstrates the close coupling of Active species, photolysis of ultraviolet, the organic solution flow rate and the initial pH value, and thus is helpful in the study of the mechanism and application of plasma in wastewater treatment.

关键词： atmospheric pressure plasma jet Active species organic solution degradation,optical emission spectroscopy （OES）