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可见光辐射下新型可循环石墨烯-铁酸铋杂化催化剂高效光催化降解氨氮(英文) 被引量:13
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作者 邹丛阳 刘守清 +3 位作者 申哲民 张园 蒋妮姗 纪文超 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2017年第1期20-28,共9页
近年来,本课题组利用简单的一步水热法,将石墨烯和铁酸锰、铁酸镍进行掺杂,先后制备出石墨烯铁酸锰和活性炭铁酸镍纳米光催化材料,并发现在可见光辐射作用下,这两种光催化剂均能利用可见光能量催化分解过氧化氢产生活性因子,从而有效地... 近年来,本课题组利用简单的一步水热法,将石墨烯和铁酸锰、铁酸镍进行掺杂,先后制备出石墨烯铁酸锰和活性炭铁酸镍纳米光催化材料,并发现在可见光辐射作用下,这两种光催化剂均能利用可见光能量催化分解过氧化氢产生活性因子,从而有效地降解氨.基于此,本文采用简单的水热法成功制备出新型的高效多相石墨烯铁酸铋(rG-BiFeO_3)催化剂,并尝试在不添加H_2O_2的条件下进行光降解氨氮实验.结果表明,该复合光催化剂仍可接受可见光辐射,在rG和BiFeO_3的协同作用下高效地光分解氨氮.由X射线衍射结果计算出rG-BiFeO_3的平均粒径约为18.5 nm.通过清晰的rG-BiFeO_3的透射电镜图可以观察到,BiFeO_3纳米颗粒物较均匀地分散在r G的二维表面上.对比BiFeO_3和rG-BiFeO_3的傅里叶变换红外光谱可以发现,rG和BiFeO_3之间可能形成了化学键.拉曼光谱结果表明,相对于纯的GO,rG-BiFeO_3拉曼谱线的D带和G带发生了蓝移,表明石墨烯铁酸铋复合材料中的GO被充分还原成石墨烯.对比BiFeO_3和rG-BiFeO_3的紫外-可见漫反射光谱发现,rG-BiFeO_3的漫反射光谱发生了红移,表明rG-BiFeO_3光催化材料对可见光的响应程度进一步提高.比表面积测定表明,BiFeO_3的比表面积为21.0 m^2/g,而rG-BiFeO_3催化剂的比表面积则增加到48.6 m^2/g,说明rG-BiFeO_3的吸附性能将得到很大提高.可见光催化反应结果表明,在不添加H2O2,p H=11的条件下,0.2 g rG-BiFeO_3对50 mg/L NH_3-N的降解率达到91.2%.动力学研究表明,BiFeO_3光催化剂氧化氨氮反应遵循一级反应动力学规律.另外,由于BiFeO_3纳米材料本身具有一定的弱磁性,所以BiFeO_3和r G的复合材料也具有一定的磁性,较易回收.催化剂经过7次循环使用后,仍然具有很高的光催化活性.根据已有文献报道,吸附在催化剂表面的氨氮被氧化的路径有两条:(1)氨在被氧化为NH_2,NH和N_2H_x+y(x+y=0,1,2)等一系列中间产物后,最终被分解为氮气;(2)氨被氧化为中间产物HONH_2,最终分解为硝酸盐和亚硝酸盐.本文利用紫外-可见分光光度计对rG-BiFeO_3光降解体系下的氨溶液进行了全波长扫描,在206和211 nm处未检测到任何吸光度,从而排除了氨氮最终分解产物为硝酸盐和亚硝酸盐的可能性.这意味着rG-BiFeO_3可见光降解氨体系符合第一种氧化路径.进一步的机理研究表明,反应过程中石墨烯与铁酸铋之间的协同作用所产生的空穴、超氧阴离子自由基和羟自由基共同将NH_3直接氧化成N_2,其中羟基自由基在整个氧化分解过程中起着最主要的作用. 展开更多
关键词 石墨烯-铁酸铋 光催化剂 可见光 氨去除
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可见光辐射下富勒烯[60]–氧化铁复合催化剂的制备及光芬顿法降解有机污染物研究(英文) 被引量:7
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作者 邹丛阳 孟则达 +4 位作者 纪文超 刘守清 申哲民 张园 蒋妮姗 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2018年第6期1051-1059,共9页
采用简单的可升级的化学浸渍法,将Fe_2O_3掺杂到富勒烯[60](C_(60))上,制得C_(60)-Fe_2O_3纳米复合材料.采用了粉末X射线衍射、X射线光电子能谱(XPS)、扫描电镜、高分辨透射电镜、紫外-可见吸收光谱、拉曼光谱和傅里叶变换红外光谱,对... 采用简单的可升级的化学浸渍法,将Fe_2O_3掺杂到富勒烯[60](C_(60))上,制得C_(60)-Fe_2O_3纳米复合材料.采用了粉末X射线衍射、X射线光电子能谱(XPS)、扫描电镜、高分辨透射电镜、紫外-可见吸收光谱、拉曼光谱和傅里叶变换红外光谱,对其进行了表征.结果发现,XPS数据中,Fe2p_(3/2)和Fe2p_(1/2)的XPS特征峰分别位于结合能710.9和724.1 eV处,对应Fe_2O_3的Fe^(3+).富勒烯颗粒均匀分散在Fe_2O_3纳米颗粒表面,Fe_2O_3纳米颗粒的平均尺寸大约为20–30 nm;Fe_2O_3对于可见光只有微弱的吸收,而制备出的C_(60)-Fe_2O_3纳米复合材料对于可见光有较强的吸收响应.本文将C_(60)-Fe_2O_3纳米复合光催化材料用于光催化降解50 mL,20mg/l MB和50 mL,10 mg/L苯酚实验.结果发现,在双氧水存在下和可见光(>420 nm)辐射条件下,C_(60)-Fe_2O_3对上述有机污染物均有较好的降解效果.通过测定上述有机物的削减程度,评估了C_(60)-Fe_2O_3催化剂的光催化活性,通过改变实验条件,得到可见光/C_(60)-Fe_2O_3/双氧水体系的最佳光催化降解条件:在pH值为3.06~10.34的范围内,投加0.02 g催化剂,5 mol/L双氧水.结果表明,在最佳条件下,亚甲基蓝在80min内脱色率能达到98.9%,矿化率能达到71%.浸出实验的结果表明,C_(60)-Fe_2O_3复合光催化剂中的铁浸出量可以忽略不计.经过5次循环使用后,C_(60)-Fe_2O_3复合光催化剂仍具有较高的光催化活性.为了进一步验证C_(60)-Fe_2O_3复合光催化剂的应用广泛性,本文在可见光/C_(60)-Fe_2O_3/双氧水体系下,开展了降解RhB,MO和苯酚的试验,结果发现,该催化剂它们也具有高的降解效果.机理研究发现,C_(60)-Fe_2O_3复合光催化剂的高效催化能力可归因于C_(60)和Fe_2O_3的协同效应:在可见光辐射下,由于C_(60)具有独特的光敏性特征,能够接收电子并把它们转移到Fe_2O_3的Fe3d轨道,并通过一系列反应,达到Fe^(3+)/Fe^(2+)循环平衡.利用活性组分捕集实验,对光催化反应过程中的主要活性氧化剂进行了区分.结果表明,羟基自由基在整个过程中发挥了最主要的作用. 展开更多
关键词 C60-Fe2O3 多相光催化 光-芬顿 可见光 活性成份的捕获
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Adsorption behavior of phosphate on Lanthanum(Ⅲ) doped mesoporous silicates material 被引量:18
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作者 Jianda Zhang zhemin shen +4 位作者 Wenpo Shan Ziyan Chen Zhijian Mei Yangming Lei Wenhua Wang 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2010年第4期507-511,共5页
A series of lanthanum doped meosoporous MCM-41(LaxM41,x is Si/La molar ratio) was prepared by sol-gel method.The surface structure of the materials was investigated with X-ray diffraction and N2 adsorption/desorption ... A series of lanthanum doped meosoporous MCM-41(LaxM41,x is Si/La molar ratio) was prepared by sol-gel method.The surface structure of the materials was investigated with X-ray diffraction and N2 adsorption/desorption technique.The content of La in the materials was determined by ICP.It was found that the La content of La25M41,La50M41 and La100M41 was 7.53%,3.89% and 2.32%,respectively.The phosphate adsorption capacities increased with increasing amount of La incorporation.With 0.40 g La25M41 99.7% phosphate could be removed.The effects of Si/La molar ratio,LaxM41 dose,pH,initial concentration of phosphate solution,co-ions on phosphate adsorption were also evaluated.The phosphate adsorption kinetics of LaxM41 could be well-described by the pseudo second-order model,and Langmuir isotherm fit equilibrium data much better than the Freundlich isotherm. 展开更多
关键词 硅酸盐材料 磷酸盐溶液 镧(Ⅲ) 吸附行为 LANGMUIR 介孔 掺杂 溶胶凝胶法
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Utilization of Dredged River Sediment in Preparing Autoclaved Aerated Concrete Blocks
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作者 Kai Zhang Qunshan Wei +5 位作者 Shuai Jiang zhemin shen Yanxia Zhang Rui Tang Aiwu Yang Christopher WKChow 《Journal of Renewable Materials》 SCIE EI 2022年第11期2989-3008,共20页
In this study,the dredged river sediment,soft texture and fine particles,is mixed with other materials and transformed into eco-friendly autoclaved aerated concrete(hereinafter referred to as AAC)blocks.The results in... In this study,the dredged river sediment,soft texture and fine particles,is mixed with other materials and transformed into eco-friendly autoclaved aerated concrete(hereinafter referred to as AAC)blocks.The results indicated the bricks produced under the conditions of 30%–34%dredged river sediment,24%cement,10%quick lime,30%fly ash,2%gypsum and 0.09%aluminum powder with 0.5 water to material ratio,2.2 MPa autoclave pressure and 6 h autoclave time,the average compressive strength of 4.5 MPa and average dry density of 716.56 kg/m³were obtained,the two parameters(strength&density)both met the requirement of national industry standard.At the same time,the contents of dredged river sediment,cement,lime,fly ash,gypsum and aluminum powder were 15%,48%,20%,15%,2%and 0.09%,respectively,and the non-AAC block made of 0.5 water to material ratio,the average compressive strength of 3.1 MPa and average dry density of 924.19 kg/m³were obtained,the two parameters(strength&density)also met the requirement of national industry standard.In addition,the AAC block’s phase composition and morphology were micro-analyzed by SEM and XRD,the main substances in AAC block were found to be tobermorite and CSH,Among them,the chemical bond between Si-O-Si and Al-O-Al is broken,Al-O-Si is regenerated,Al substituted tobermorite with better strength is formed,and the compressive strength of AAC is further improved. 展开更多
关键词 Autoclaved aerated concrete dredged river sediment compressive strength FROST-RESISTANCE moisture content MICROSTRUCTURE
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Evaluation of 1,4-naphthoquinone derivatives as antibacterial agents:activity and mechanistic studies
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作者 Zhizhuo Liu zhemin shen +3 位作者 Shouyan Xiang Yang sun Jiahua Cui Jinping Jia 《Frontiers of Environmental Science & Engineering》 SCIE EI CSCD 2023年第3期49-61,共13页
The diverse and large-scale application of disinfectants posed potential health risks and caused ecological damage during the 2019-nCoV pandemic,thereby increasing the demands for the development of disinfectants base... The diverse and large-scale application of disinfectants posed potential health risks and caused ecological damage during the 2019-nCoV pandemic,thereby increasing the demands for the development of disinfectants based on natural products,with low health risks and low aquatic toxicity.In the present study,a few natural naphthoquinones and their derivatives bearing the 1,4-naphthoquinone skeleton were synthesized,and their antibacterial activity against selected bacterial strains was evaluated.In vitro antibacterial activities of the compounds were investigated against Escherichia coli and Staphylococcus aureus.Under the minimum inhibitory concentration(MIC)of≤0.125μmol/L for juglone(1a),5,8-dimethoxy-1,4-naphthoquinone(1f),and 7-methyl-5-acetoxy-1,4-naphthoquinone(3),a strong antibacterial activity against S.aureus was observed.All 1,4-naphthoquinone derivatives exhibited a strong antibacterial activity,with MIC values ranging between 15.625 and 500μmol/Land ECso values rangingbetween10.56 and248.42μmol/L.Most of the synthesized compounds exhibited strong antibacterial activities against S.aureus.Among these compounds,juglone(la)showed the strongest antibacterial activity.The results from mechanistic investigations indicated that juglone,a natural naphthoquinone,caused cell death by inducing reactive oxygen species production in bacterial cells,leading to DNA damage.In addition,juglone could reduce the self-repair ability of bacterial DNA by inhibiting RecA expression.In addition to having a potent antibacterial activity,juglone exhibited low cytotoxicity in cell-based investigations.In conclusion,juglone is a strong antibacterial agent with low toxicity,indicating that its application as a bactericidal agent may be associated with low health risks and aquatic toxicity. 展开更多
关键词 1 4-naphthoquinone derivatives ANTIBACTERIAL Actionmechanism RECA
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Design and Testing of a Novel Piezoelectric-Driven Microvibration Hammerhead
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作者 Zhiyong Guo zhemin shen +3 位作者 Weidong Liu Zhiqiang Zhang Lifeng Zhang Xuhao Wang 《Nanomanufacturing and Metrology》 EI 2023年第1期79-87,共9页
A novel microvibration hammerhead consists of a piezoelectric actuator and a double cross-shape compliant mechanism(DCCM)is presented in this paper.The output force of the piezoelectric actuator can be detected in rea... A novel microvibration hammerhead consists of a piezoelectric actuator and a double cross-shape compliant mechanism(DCCM)is presented in this paper.The output force of the piezoelectric actuator can be detected in real time by an insideinstalled pressure sensor.A theoretical model including the stiffness,first natural frequency,and stress of the DCCM and the displacement output of the piezoelectric actuator are established,and then they are further analyzed using the finite element analysis method.The effects of the beam thickness on the static and dynamic properties are deeply analyzed and compared.A prototype micro hammering system is constructed by integrating the microvibration hammerhead assembly and controlling system.Various experiments are also carried out to verify the basic performance of the micro hammering system. 展开更多
关键词 PIEZOELECTRIC Flexure hinge Micro hammering
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Long-term joint effect of nutrients and temperature increase on algal growth in Lake Taihu,China 被引量:9
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作者 Chun Ye zhemin shen +3 位作者 Tao Zhang Maohong Fan Yangming Lei Jianda Zhang 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2011年第2期222-227,共6页
To study how global warming and eutrophication affect water ecosystems,a multiplicative growth Monod model,modified by incorporating the Arrhenius equation,was applied to Lake Taihu to quantitatively study the relatio... To study how global warming and eutrophication affect water ecosystems,a multiplicative growth Monod model,modified by incorporating the Arrhenius equation,was applied to Lake Taihu to quantitatively study the relationships between algal biomass and both nutrients and temperature using long-term data.To qualitatively assess which factor was a limitation of the improved model,temperature variables were calculated using annual mean air temperature (AT),water temperature (WT),and their average temperature (ST),while substrate variables were calculated using annual mean total nitrogen (TN),total phosphorus (TP),and their weighted aggregate (R),respectively.The nine fitted curves showed that TN and AT were two important factors influencing algal growth;AT limited growth as algal photosynthesis is mainly carried out near the water surface;N leakage of phytoplankton and internal phosphorus load from sediment explains why TN was the best predictor of peak biomass using the Monod model.The fitted results suggest that annual mean algal biomass increased by 0.145 times when annual mean AT increased by 1.0°C.Results also showed that the more eutrophic the lake,the greater the effect AT had on algal growth.Subsequently,the long-term joint effect of annual temperature increase and eutrophication to water ecosystems can be quantitatively assessed and predicted. 展开更多
关键词 水体富营养化 藻类生长 平均温度 共同作用 Arrhenius方程 太湖 Monod模型 年平均气温
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Removal of phosphate by Fe-coordinated amino-functionalized 3D mesoporous silicates hybrid materials 被引量:4
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作者 Jianda Zhang zhemin shen +2 位作者 Zhijian Mei Shanping Li Wenhua Wang 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2011年第2期199-205,共7页
Phosphate removal from aqueous waste streams is an important approach to control the eutrophication downstream bodies of water.A Fe(III) coordinated amino-functionalized silicate adsorbent for phosphate adsorption was... Phosphate removal from aqueous waste streams is an important approach to control the eutrophication downstream bodies of water.A Fe(III) coordinated amino-functionalized silicate adsorbent for phosphate adsorption was synthesized by a post-grafting and metal cation incorporation process.The surface structure of the adsorbent was characterized by X-ray diffraction,N2 adsoropion/desoprotion technique,and Fourier transform infrared spectroscopy.The experimental results showed that the adsorption equilibrium data were well fitted to the Langmuir equation.The maximum adsorption capacity of the modified silicate material was 51.8 mg/g.The kinetic data from the adsorption of phosphate were fitted to pseudo second-order model.The phosphate adsorption was highly pH dependent and the relatively high removal of phosphate fell within the pH range 3.0-6.0.The coexistence of other anions in solutions has an adverse effect on phosphate adsorption;a decrease in adsorption capacity followed the order of exogenous anions:F > SO2-4 > NO-3 > Cl-.In addition,the adsorbed phosphate could be desorbed by NaOH solutions.This silicate adsorbent with a large adsorption capacity and relatively high selectivity could be utilized for the removal of phosphate from aqueous waste streams or in aquatic environment. 展开更多
关键词 磷酸盐吸附 硅酸盐材料 杂化材料 氨基 除铁 LANGMUIR方程 功能化 傅里叶变换红外光谱
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Temperature sensitivity of organic compound destruction in SCWO process 被引量:2
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作者 Yaqin Tan zhemin shen +4 位作者 Weimin Guo Chuang Ouyang Jinping Jia Weili Jiang Haiyun Zhou 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2014年第3期512-518,共7页
To study the temperature sensitivity of the destruction of organic compounds in supercritical water oxidation process(SCWO), oxidation effects of twelve chemicals in supercritical water were investigated. The SCWO rea... To study the temperature sensitivity of the destruction of organic compounds in supercritical water oxidation process(SCWO), oxidation effects of twelve chemicals in supercritical water were investigated. The SCWO reaction rates of different compounds improved to varying degrees with the increase of temperature, so the highest slope of the temperature-effect curve(imax) was defined as the maximum ratio of removal ratio to working temperature. It is an important index to stand for the temperature sensitivity effect in SCWO. It was proven that the higher imax is, the more significant the effect of temperature on the SCWO effect is. Since the high-temperature area of SCWO equipment is subject to considerable damage from fatigue, the temperature is of great significance in SCWO equipment operation. Generally, most compounds(imax > 0.25) can be completely oxidized when the reactor temperature reaches 500℃. However, some compounds(imax > 0.25) need a higher temperature for complete oxidation, up to 560℃. To analyze the correlation coefficients between imax and various molecular descriptors, a quantum chemical method was used in this study. The structures of the twelve organic compounds were optimized by the Density Functional Theory B3LYP/6-311G method, as well as their quantum properties. It was shown that six molecular descriptors were negatively correlated to imax while other three descriptors were positively correlated to imax. Among them, dipole moment had the greatest effect on the oxidation thermodynamics of the twelve organic compounds. Once a correlation between molecular descriptors and imax is established, SCWO can be run at an appropriate temperature according to molecular structure. 展开更多
关键词 超临界水氧化 温度敏感性 有机化合物 氧化过程 分子描述符 量子化学方法 密度泛函理论 氧化作用
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Relationship between reaction rate constants of organic pollutants and their molecular descriptors during Fenton oxidation and in situ formed ferric-oxyhydroxides
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作者 Lijuan Jia zhemin shen Pingru Su 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2016年第5期257-264,共8页
Fenton oxidation is a promising water treatment method to degrade organic pollutants. In this study, 30 different organic compounds were selected and their reaction rate constants(k) were determined for the Fenton oxi... Fenton oxidation is a promising water treatment method to degrade organic pollutants. In this study, 30 different organic compounds were selected and their reaction rate constants(k) were determined for the Fenton oxidation process. Gaussian09 and Material Studio software sets were used to carry out calculations and obtain values of 10 different molecular descriptors for each studied compound. Ferric-oxyhydroxide coagulation experiments were conducted to determine the coagulation percentage. Based upon the adsorption capacity,all of the investigated organic compounds were divided into two groups(Group A and Group B). The percentage adsorption of organic compounds in Group A was less than 15%(wt./wt.)and that in the Group B was higher than 15%(wt./wt.). For Group A, removal of the compounds by oxidation was the dominant process while for Group B, removal by both oxidation and coagulation(as a synergistic process) took place. Results showed that the relationship between the rate constants(k values) and the molecular descriptors of Group A was more pronounced than for Group B compounds. For the oxidation-dominated process,EHOMOand Fukui indices(f(0)_x, f(-)_x, f(+)_x) were the most significant factors. The influence of bond order was more significant for the synergistic process of oxidation and coagulation than for the oxidation-dominated process. The influences of all other molecular descriptors on the synergistic process were weaker than on the oxidation-dominated process. 展开更多
关键词 反应速率常数 分子描述符 氢氧化物 有机污染物 三价铁 有机化合物 STUDIO软件 原位
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