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钯化学态对g-C_(3)N_(4)光催化还原CO_(2)的影响:单原子态在促进CH4生成中的独特作用
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作者 李钱 唐麒君 +4 位作者 熊珮瑶 陈东之 陈建孟 吴忠标 王海强 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2023年第3期177-190,共14页
化石燃料过度消耗引起的CO_(2)过量排放和能源短缺问题日益突出.利用太阳能和光催化剂将CO_(2)转化成高附加值化学原料,可以同时缓解温室效应与能源短缺,是实现“碳中和”与社会可持续发展的有效途径.目前在光催化剂合成方面已取得巨大... 化石燃料过度消耗引起的CO_(2)过量排放和能源短缺问题日益突出.利用太阳能和光催化剂将CO_(2)转化成高附加值化学原料,可以同时缓解温室效应与能源短缺,是实现“碳中和”与社会可持续发展的有效途径.目前在光催化剂合成方面已取得巨大进步,但由于电荷重组严重,表面反应动力学迟缓,CO_(2)还原效率仍普遍偏低.助催化剂修饰是改善催化剂催化CO_(2)还原效率的有效策略.贵金属是提升催化剂性能最显著的一类助催化剂,然而其资源有限,优格昂贵,将贵金属助催化剂的尺寸减小至单原子,可以最大限度地提高原子利用率,大幅降低成本,显著提升催化剂的催化性能.现有研究在揭示贵金属助催化剂性能提升机制时,主要集中在其对基底材料性质的影响,忽略了单原子态与其它化学价态的区别.因此本文以g-C_(3)N_(4)(CN)纳米片为基底,研究Pd单原子(Pd-SA),PdO_(x),Pd纳米颗粒(Pd-NP)修饰对CN光催化还原CO_(2)性能的影响及性能提升差异显著的内在机制.利用透射电子显微镜、高角度环形暗场扫描透射电子显微镜、X射线光电子能谱、基于同步辐射的X射线吸收谱等手段确定Pd物种在CN表面的存在形态和化学价态.性能测试结果表明,三种形态Pd修饰均可促进CN光催化还原CO_(2)的性能,但提升效果存在显著差异.Pd/CN-SA上的CH_(4)产量约2.25μmol/g,明显高于PdO_(x)/CN(1.08μmol/g),Pd/CN-NP(0.44μmol/g)和CN(0.104μmol/g);Pd修饰后,CN的CH_(4)选择性明显提高,其中Pd/CN-SA的CH_(4)选择性高达73.5%,优于PdO_(x)/CN(67.2%)和Pd/CN-NP(60%).光电性质分析结果表明,Pd修饰有效提升了CN的光吸收性能,显著促进了载流子的迁移与分离,且Pd/CN-NP和PdO_(x)/CN的有效光生电子密度较Pd/CN-SA更高,结果说明样品的光电性质不是影响其光催化还原CO_(2)活性的关键因素.CO_(2)^(-)PPD结果表明,Pd/CN-SA表面具有丰富的中等强度的碱性位(HCO_(3)-),更有利于CO_(2)吸附与活化.H_(+)的产生通常伴随着·OH和·O_(2)^(-)的形成,因此根据电子自旋共振获得的·OH和·O_(2)^(-)产量可推测出,Pd/CN-NP可形成最丰富的H_(+),PdO_(x)/CN次之,Pd/CN-SA最低.H_(2)吸附实验结果表明,在氢溢流效应的影响下,Pd修饰显著促进了CN对H_(2)的吸附,且Pd/CN-SA对H_(2)的吸收量最大,说明H_(2)在Pd-SA表面更易发生解离形成·H,这可能是其CH_(4)产量较高的重要原因.对比了以H_(2)和H_(2)O为还原剂时的CO_(2)光催化还原性能,结果表明,PdO_(x)/CN和Pd/CN-SA的CH_(4)产量分别下降了66.3%和28.6%,Pd/CN-NP的甲烷产量反而提高,说明Pd/CN-NP可能具有较好的·H利用效率,其以H_(2)O为还原剂时的低CH_(4)产量可能受限于·H的形成.为进一步验证该推测,利用DFT模拟研究了H_(2)O分子在Pd/CN-NP,PdO_(x)/CN和Pd/CN-SA表面的吸附解离能,结果表明,H_(2)O分子在Pd/CN-SA表面的活化能最低,最有利于·H的形成.此外,完整的H_(2)O解离反应过程中Pd/CN-NP会释放出0.40 eV能量,Pd/CN-SA与PdO_(x)/CN则需补充额外的能量(0.51和1.47 eV),再次强有力地证明Pd/CN-NP具有较好的·H利用效率.最后,利用原位红外分析了各样品光催化还原CO_(2)反应过程的差异,发现Pd/CN-SA表面的CO_(2)吸附态物种在可见光照射下更容易参与至后续的光催化还原反应中;PdO_(x)/CN和Pd/CN-NP表面的CO_(2)吸附态物种含量足够丰富,但由于它们的光生电子还原能力有限,无法将吸附物种进一步还原;Pd/CN-SA和Pd/CN-NP表面吸附的CO可进一步被还原成甲氧基,但吸附在PdO_(x)/CN表面的CO难以被进一步还原.综上,本文揭示了贵金属Pd的化学价态对CO_(2)还原性能的关键作用,对未来合理设计开发更有效的CO_(2)还原光催化剂具有借鉴意义. 展开更多
关键词 CO_(2)光催化还原 化学价态 Pd g-C_(3)N_(4) H原子利用
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改性钒钛基SCR催化剂的研究进展(英文) 被引量:34
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作者 陈传敏 曹悦 +2 位作者 刘松涛 陈建猛 贾文波 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2018年第8期1347-1365,共19页
钒钛基选择性催化还原催化剂是目前燃煤电厂应用最为广泛的脱硝催化剂.由于传统钒钛基催化剂存在低温脱硝效率低、热稳定性差、单质汞氧化效率低、二氧化硫氧化、氨逃逸、碱金属中毒等问题,人们开始尝试通过对传统SCR催化剂进行改性,以... 钒钛基选择性催化还原催化剂是目前燃煤电厂应用最为广泛的脱硝催化剂.由于传统钒钛基催化剂存在低温脱硝效率低、热稳定性差、单质汞氧化效率低、二氧化硫氧化、氨逃逸、碱金属中毒等问题,人们开始尝试通过对传统SCR催化剂进行改性,以期改善其综合性能.本文从(1)拓宽催化剂的反应温度窗口,尤其是向低温区扩展,(2)提高催化剂的热稳定性,(3)协同氧化单质汞,(4)控制氨逃逸,(5)降低SO_2至SO_3的转化率和(6)提高催化剂抗碱金属中毒性能等方面综述了改性钒钛基SCR催化剂的研究进展,总结了其催化性能和相关影响机理.研究表明,某些金属及非金属的改性可以增加钒钛基SCR催化剂的表面酸度、活性位点及氧化还原性能,非金属的掺杂还可以抑制TiO_2载体由锐钛矿向金红石型转化、增加表面氧空位,从而改善了钒钛基催化剂的低温脱硝性能;硅、钨、钡和稀土金属等的添加也可抑制TiO_2的金红石化过程,锆、钾则改变了钒氧化物的存在形态,抑制其高温聚合,提高了钒钛基催化剂的热稳定性;贵金属、过渡金属、金属氯化物及非金属的改性改变了钒钛基催化剂的汞氧化机制,均可有效促进低氯甚至无氯条件下钒钛基催化剂对单质汞的氧化;贵金属钌及助剂钼添加的钒钛基催化剂可在维持较高脱硝效率的同时,实现单质汞及逃逸氨的高效去除,在SCR尾部将逃逸氨选择性氧化生成无害的氮气和水;被铜、氧化钡、氧化硅等物质改性后,更多的钒以低价态存在,使催化剂的氧化还原性能降低,并抑制了二氧化硫的吸附,从而减少了三氧化硫的生成;由于具有高储氧能力和氧化还原特性,还可降低碱金属的吸附量,铈的掺杂可提高钒钛基催化剂的抗碱金属中毒性能.此外,本文还汇总了包括贵金属(如银、钌)、过渡金属(如锰、铁、铜、锆等)、稀土金属(铈、镨)等金属、金属氯化物(如氯化铜、氯化钙)及非金属(氟、硫、硅等)改性钒钛基SCR催化剂的优缺点.基于前人研究及作者观点,改性组分的掺杂有利于进一步提高钒钛基催化剂的综合性能,具有巨大的发展潜力,也是在现有基础上实现多污染物控制的方法之一. 展开更多
关键词 钒钛基催化剂 选择性催化还原 低温脱硝 汞氧化 逃逸氨 二氧化硫氧化
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A supplementary assessment system of AQI-V for comprehensive management and control of air quality in chemical industrial parks
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作者 Qiaoli Wang Dongping Sheng +7 位作者 chengzhi Wu Deji Jing Nana cheng Xingnong Cai Sujing Li Jingkai Zhao Wei Li jianmeng chen 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2023年第8期114-125,共12页
Volatile organic compounds(VOCs)are the dominant pollutants in industrial parks.However,they are not generally considered as part of the air quality index(AQI)system,which leads to a biased assessment of pollution in ... Volatile organic compounds(VOCs)are the dominant pollutants in industrial parks.However,they are not generally considered as part of the air quality index(AQI)system,which leads to a biased assessment of pollution in industrial parks.In this study,a supplementary assessment system of AQI-V was established by analyzing VOCs characteristics with vehicle-mounted PTR-TOFMS instrument,correlation analysis and the standards analysis.Three hourly and daily scenarios were considered,and the hierarchical parameter setting was further optimized by field application.The hourly and daily assessments revealed the evaluation factors for the discriminability of different air quality levels,practiced value for regional air quality improvement,and the reservation of general dominant pollutants.Finally,the universality testing in ZPIP successfully recognized most of the peaks,with 54.76%,38.39%and 6.85%for O_(3),VOCs and NO_(2) as the dominant pollutant,and reflected the daily ambient air quality condition,togetherwith the dominant pollutant.The AQI-V systemwith VOCs sub-index is essential for air quality evaluation in industrial parks,which can further provide scientific support to control the pollution of VOCs and the secondary pollutant,therefore significantly improve the air quality in local industrial parks. 展开更多
关键词 Air quality index Industrial parks VOCs sub-index AQI-V system Scenario analysis
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Conversion characteristics and mechanism analysis of gaseous dichloromethane degraded by a VUV light in different reaction media 被引量:4
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作者 Jianming Yu Wenji Cai +3 位作者 jianmeng chen Li Feng Yifeng Jiang Zhuowei cheng 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2012年第10期1777-1784,共8页
The photodegradation of gaseous dichloromethane (DCM) by a vacuum ultraviolet (VUV) light in a spiral reactor was investigated with different reaction media and initial concentrations. Through the combination of d... The photodegradation of gaseous dichloromethane (DCM) by a vacuum ultraviolet (VUV) light in a spiral reactor was investigated with different reaction media and initial concentrations. Through the combination of direct photolysis, O3 oxidation and HO. oxidation, DCM was ultimately mineralized into inorganic compounds (such as HC1, CO2, H20, etc.) in the air with relative humidity (RH) of 75%-85%. During the photodegradation process, some small organic acids (including formic acid, acetic acid) were also detected and the intermediates were more soluble than DCM, providing a possibility for its combination with subsequent biodegradation. Based on the detected intermediates and the confirmed radicals, a photodegradation pathway of DCM by VUV was proposed. With RH 75%- 80% air as the reaction medium, the DCM removal followed the second-order kinetic model at inlet concentration of 100-1000 mg/m3. Kinetic analysis showed that the reaction media affected the kinetic constants of DCM conversion by a large extent, and RH 80% air could cause a much lower half-life for its conversion. Such results supported the possibility that VUV photodegradation could be used not only for the mineralization of DCM but also as a pretreatment before biodegradation. 展开更多
关键词 DICHLOROMETHANE VUV photodegradation MECHANISM carbon balance kinetic analysis
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Pollutant toxicology with respect to microalgae and cyanobacteria 被引量:4
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作者 Tao Lu Qi Zhang +4 位作者 Zhenyan Zhang Baolan Hu jianmeng chen Jun chen Haifeng Qian 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2021年第1期175-186,共12页
Microalgae and cyanobacteria are fundamental components of aquatic ecosystems.Pollution in aquatic environment is a worldwide problem.Toxicological research on microalgae and cyanobacteria can help to establish a soli... Microalgae and cyanobacteria are fundamental components of aquatic ecosystems.Pollution in aquatic environment is a worldwide problem.Toxicological research on microalgae and cyanobacteria can help to establish a solid foundation for aquatic ecotoxicological assessments.Algae and cyanobacteria occupy a large proportion of the biomass in aquatic environments;thus,their toxicological responses have been investigated extensively.However,the depth of toxic mechanisms and breadth of toxicological investigations need to be improved.While existing pollutants are being discharged into the environment daily,new ones are also being produced continuously.As a result,the phenomenon of water pollution has become unprecedentedly complex.In this review,we summarize the latest findings on five kinds of aquatic pollutants,namely,metals,nanomaterials,pesticides,pharmaceutical and personal care products(PPCPs),and persistent organic pollutants(POPs).Further,we present information on emerging pollutants such as graphene,microplastics,and ionic liquids.Efforts in studying the toxicological effects of pollutants on microalgae and cyanobacteria must be increased in order to better predict the potential risks posed by these materials to aquatic ecosystems as well as human health. 展开更多
关键词 Aquatic ecotoxicology HERBICIDES Fungicides Algae and cyanobacteria
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Enzyme-electrolytic degradation of dichloromethane: Efficiency, kinetics and mechanism 被引量:3
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作者 Jianming Yu Meng Wu +4 位作者 Yuwei Tang Jiaqi Shi Jun Hu Zhiliang Yu jianmeng chen 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2019年第12期187-194,共8页
Enzymatic electrolysis cell(EEC)has advantages over microbial electrolysis cell(MEC)due to the needless of microbe inoculation and high-efficiency of enzymatic reaction.In this study,an EEC was first applied to achiev... Enzymatic electrolysis cell(EEC)has advantages over microbial electrolysis cell(MEC)due to the needless of microbe inoculation and high-efficiency of enzymatic reaction.In this study,an EEC was first applied to achieve the effective degradation of halogenated organic pollutants and dichloromethane(CH2Cl2)was utilized as a model pollutant.The results indicate that the degradation efficiency of CH2Cl2 after 2 hr reaction in the EEC was almost100%,which was significantly higher than that with enzyme(51.1%)or current(19.0%).The current induced the continuous regeneration of reduced glutathione(GSH),thus CH2Cl2 was degraded under the catalysis of GSH-dependent dehalogenase through stepwise dechlorination,and successively formed monochloromethane(CH3Cl)and methane(CH4).The kinetic result shows that with a current of 15 mA,the maximum specific degradation rate of CH2Cl2(3.77×10-3 hr-1)was increased by 5.7 times.The optimum condition for CH2Cl2 dechlorination was also obtained with pH,current and temperature of 7.0,15 mA and 35°C,respectively.Importantly,this study helps to understand the behavior of enzymes and the fate of halogenated organic pollutants with EEC,providing a possible treatment technology for halogenated organic pollutants. 展开更多
关键词 Enzyme electrode DICHLOROMETHANE KINETICS Reductive dichlorination Reduced glutathione(GSH) REGENERATION
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Photocatalytic activity of TiO2 containing anatase nanoparticles and rutile nanoflower structure consisting of nanorods 被引量:3
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作者 Zhiqiao He Qiaolan Cai +4 位作者 Huiying Fang Gaohua Situ Jianping Qiu Shuang Song jianmeng chen 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2013年第12期2460-2468,共9页
A series of TiO2 with different crystal phases and morphologies was synthesized via a facile hydrothermal process using titanium nbutoxide and concentrated hydrochloric acid as raw materials. The photocatalytic activi... A series of TiO2 with different crystal phases and morphologies was synthesized via a facile hydrothermal process using titanium nbutoxide and concentrated hydrochloric acid as raw materials. The photocatalytic activity of the samples was evaluated by degradation of Methyl Orange in aqueous solution under UV-Visible light irradiation. On the basis of detailed analysis of the characterizing results of high-resolution transmission electron microscopy, X-ray powder diffraction measurements, X-ray photoelectron spectroscopy and Brunauer-Emmett-Teller measurement, it was concluded that the photo-activity of the catalyst is related directly to the 3D morphology and the crystal phase composition. An excellent catalyst should have both a futile 3D flower-like structure and anatase granulous particles. The 3D flower-like structure could enhance light harvesting, as well as the transfer of reactant molecules from bulk solution to the reactive sites on TiO2. In addition, the optimum anatase/rutile phase ratio was found to be 80:20, which is beneficial to the effective separation of the photogenerated electron-hole pairs. 展开更多
关键词 photocatalysis TIO2 anatase nanoparticles rutile nanoflowers simulated solar light illumination.
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Kinetic analysis and bacterium metabolization of α-pinene by a novel identified Pseudomonas sp.strain 被引量:3
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作者 Zhuowei cheng Pengfei Sun +2 位作者 Yifeng Jiang Lili Zhang jianmeng chen 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2012年第10期1806-1815,共10页
Biodegradation has become a popular alternative remediation technology for its economic and ecological advantages. An aerobic bacterium (strain ZW) capable of degrading α-pinene was isolated from a biofilter by a s... Biodegradation has become a popular alternative remediation technology for its economic and ecological advantages. An aerobic bacterium (strain ZW) capable of degrading α-pinene was isolated from a biofilter by a selective enrichment. Based on the 16S rRNA gene analysis and physiochemical properties, this strain was identified as Pseudomonas veronii. Under the optimized condition achieved by the response surface methodology (RSM), as well as pH 6.82, temperature 26.3℃ and NaC1 concentration 1.36%, almost 100% α-pinene could be removed within 45 hr. Enzymatic biodegradation by the crude intracellular enzyme could be described well by the Michaelis-Menten model in which the maximum degradation rate Vraax and the half-saturation constant Km were calculated to be 0.431 mmol/(L.min) and 0.169 mmol/L, respectively. Activity assay of catechol suggested that the strain ZW possessed a catechol- 1,2-dioxygenase and could decompose benzene-ring through ortho ring cleavage. Based on the identified intermediates by GC/MS, a new metabolic pathway was proposed, in which the final metabolites were some simpler organic and inorganic compounds. The present work demonstrated that the strain ZW would have a great application prospect for the remediation of α-pinene-contaminated environment. 展开更多
关键词 Pseudomonas veronii ct-pinene growth conditions kinetics analysis metabolic pathway
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Removal characteristics and kinetic analysis of an aerobic vapor-phase bioreactor for hydrophobic alpha-pinene 被引量:2
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作者 Yifeng Jiang Shanshan Li +2 位作者 Zhuowei cheng Runye Zhu jianmeng chen 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2012年第8期1439-1448,共10页
Biofiltration is considered an effective method to control volatile organic compounds (VOCs) pollution. This study was conducted to evaluate the potential use of a bacterial biofilter packed with wood chips and peat... Biofiltration is considered an effective method to control volatile organic compounds (VOCs) pollution. This study was conducted to evaluate the potential use of a bacterial biofilter packed with wood chips and peat for the removal of hydrophobic α-pinene. When inoculated with two pure degraders and adapted activated sludge, a removal efficiency (RE) of more than 95% was achieved after a start- up period of 11 days. The maximum elimination capacity (EC) of 50 g/(m^3.hr) with RE of 94% was obtained at empty bed retention time (EBRT) of 102 sec. When higher α-pinene concentrations and shorter EBRTs were applied, the REs and ECs decreased significantly due to mass-transfer and biological reaction limitations. As deduced from the experimental results, approximately 74% of ct-pinene were completely mineralized by the consortiums and the biomass yield was 0.60 g biomass/g α-pinene. Sequence analysis of the selected bands excised from denaturing gradient gel electrophoresis revealed that the inoculated pure cultures could be present during the whole operation, and others were closely related to bacteria being able to degrade hydrocarbons. The kinetic results demonstrated that the whole biofiltration for α-pinene was diffusion-limit controlled owing to its hydrophobic characteristics. These findings indicated that this bacterial biofiltration is a promising technology for the remediation of hydrophobic industrial waste gases containing ct-pinene. 展开更多
关键词 BIOFILTERS gaseous α-pinene removal characteristics microbial community kinetic parameters
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Degradation of dichloromethane by an isolated strain Pandoraea pnomenusa and its performance in a biotrickling filter 被引量:2
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作者 Jianming Yu Wenji Cai +1 位作者 Zhuowei cheng jianmeng chen 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2014年第5期1108-1117,共10页
A strain Pandoraea pnomenusa LX-1 that uses dichloromethane (DCM) as sole carbon and energy source has been isolated and identified in our laboratory. The optimum aerobic biodegradation of DCM in batch culture was e... A strain Pandoraea pnomenusa LX-1 that uses dichloromethane (DCM) as sole carbon and energy source has been isolated and identified in our laboratory. The optimum aerobic biodegradation of DCM in batch culture was evaluated by response surface methodology. Maximum biodegradation (5.35 mg/(L.hr)) was achieved under cultivation at 32.8℃, pH 7.3, and 0.66% NaC1. The growth and biodegradation processes were well fitted by Haldane's kinetic model, yielding maximum specific growth and degradation rates of 0.133 hr^-1 and 0.856 hr^-1, respectively. The microorganism efficiently degraded a mixture of DCM and coexisting components (benzene, toluene and chlorobenzene). The carbon recovery (52.80%-94.59%) indicated that the targets were predominantly mineralized and incorporated into cell materials. Electron acceptors increased the DCM biodegradation rate in the following order: mixed 〉 oxygen 〉 iron 〉 sulfate 〉 nitrate. The highest dechlorination rate was 0.365 mg C1-/(hr.mg biomass), obtained in the presence of mixed electron acceptors. Removal was achieved in a continuous biotrickling filter at 56%-85% efficiency, with a mineralization rate of 75.2%. Molecular biology techniques revealed the predominant strain as P. pnomenusa LX-1. These results clearly demonstrated the effectiveness of strain LX-1 in treating DCM-containing industrial effluents. As such, the strain is a strong candidate for remediation of DCM coexisting with other organic compounds. 展开更多
关键词 DICHLOROMETHANE Pandoraea pnomenusa biodegradation characteristics removal performance carbon balance
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Efficient degradation of chlorobenzene in a non-thermal plasma catalytic reactor supported on CeO_2/HZSM-5 catalysts 被引量:9
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作者 Liying Jiang Guofeng Nie +5 位作者 Runye Zhu Jiade Wang jianmeng chen Yubo Mao Zhuowei cheng Willam A.Anderson 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2017年第5期266-273,共8页
Chlorobenzene removal was investigated in a non-thermal plasma reactor using CeO2/HZSM-5catalysts.The performance of catalysts was evaluated in terms of removal and energy efficiency.The decomposition products of chlo... Chlorobenzene removal was investigated in a non-thermal plasma reactor using CeO2/HZSM-5catalysts.The performance of catalysts was evaluated in terms of removal and energy efficiency.The decomposition products of chlorobenzene were analyzed.The results show that CeO2/HZSM-5 exhibited a good catalytic activity,which resulted in enhancements of chlorobenzene removal,energy efficiency,and the formation of lower amounts of by-products.With regards to CO2 selectivity,the presence of catalysts favors the oxidation of by-products,leading to a higher CO2 selectivity.With respect to ozone,which is considered as an unavoidable by-product in air plasma reactors,a noticeable decrease in its concentration was observed in the presence of catalysts.Furthermore,the stability of the catalyst was investigated by analyzing the evolution of conversion in time.The experiment results indicated that CeO2/HZSM-5 catalysts have excellent stability:chlorobenzene conversion only decreased from 78%to 60%after 75 hr,which means that the CeO2/HZSM-5 suffered a slight deactivation.Some organic compounds and chlorinated intermediates were adsorbed or deposited on the catalysts surface as shown by the results of Fourier Transform Infrared(FT-IR) spectroscopy,scanning electron microscope(SEM) and energy dispersive X-ray spectroscopy(EDS) analyses of the catalyst before and after the reaction,revealing the cause of catalyst deactivation. 展开更多
关键词 Non-thermal plasma Catalysis Chlorobenzene Degradation CeO2/HZSM-5
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A visible light-responsive iodine-doped titanium dioxide nanosphere 被引量:1
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作者 Zhiqiao He Liyong Zhan +4 位作者 Fangyue Hong Shuang Song Zhengying Lin jianmeng chen Mantong Jin 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2011年第1期166-170,共5页
I-doped titanium dioxide nanospheres (I-TNSs) were synthesized via a two-step hydrothermal synthesis route, their potential for the efficient utilization of visible light was evaluated. The prepared anatase-phase I-... I-doped titanium dioxide nanospheres (I-TNSs) were synthesized via a two-step hydrothermal synthesis route, their potential for the efficient utilization of visible light was evaluated. The prepared anatase-phase I-TNSs had a bimodal porous size distribution with a Brunauer-Emmett-Teller surface area of 76 m2/g, a crystallite size of approximately 14 nm calculated from X-ray diffraction data, and a remarkable absorption in the visible light region at wavelengths 〉 400 nm. The photocatalytic activity of the samples was evaluated by decoloration of Methyl Orange in aqueous solution under visible light irradiation in comparison to the iodine-doped TiO2 (I-TiO2). The I-TNSs showed higher photocatalytic efficiency compared with I-TiO2 after irradiation for 180 rain even though the latter had a much greater surface area (115 m2/g). It was concluded that the surface area was not the predominant factor determining photocatalytic activity, and that the good crystallization and bimodal porous nanosphere structure were favourable for photocatalysis. 展开更多
关键词 I-doped titanium dioxide NANOSPHERES Methyl Orange visible light
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Synthesis,characterization,and photocatalytic activity of porous La–N–co-doped TiO_2 nanotubes for gaseous chlorobenzene oxidation 被引量:4
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作者 Zhuowei cheng Zhiqi Gu +2 位作者 jianmeng chen Jianming Yu Lingjun Zhou 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2016年第8期203-213,共11页
The photocatalytic oxidation of gaseous chlorobenzene(CB) by the 365 nm-induced photocatalyst La/N–Ti O2, synthesized via a sol–gel and hydrothermal method, was evaluated. Response surface methodology(RSM) was u... The photocatalytic oxidation of gaseous chlorobenzene(CB) by the 365 nm-induced photocatalyst La/N–Ti O2, synthesized via a sol–gel and hydrothermal method, was evaluated. Response surface methodology(RSM) was used to model and optimize the conditions for synthesis of the photocatalyst. The optimal photocatalyst was 1.2La/0.5N–Ti O2(0.5) and the effects of La/N on crystalline structure, particle morphology, surface element content, and other structural characteristics were investigated by XRD(X-ray diffraction), TEM(Transmission Electron Microscopy), FTIR(Fourier transform infrared spectroscopy), UV–vis(Ultraviolet–visible spectroscopy), and BET(Brunauer Emmett Teller). Greater surface area and smaller particle size were produced with the co-doped Ti O2 nanotubes than with reference Ti O2. The removal of CB was effective when performed using the synthesized photocatalyst,though it was less efficient at higher initial CB concentrations. Various modified Langmuir-Hinshelwood kinetic models involving the adsorption of chlorobenzene and water on different active sites were evaluated. Fitting results suggested that competitive adsorption caused by water molecules could not be neglected, especially for environments with high relative humidity. The reaction intermediates found after GC–MS(Gas chromatography–mass spectrometry) analysis indicated that most were soluble, low-toxicity, or both. The results demonstrated that the prepared photocatalyst had high activity for VOC(volatile organic compounds) conversion and may be used as a pretreatment prior to biopurification. 展开更多
关键词 Photocatalysis La/N–Ti O2 Chlorobenzene Conversion efficiency Kinetic analysis
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