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国家自然科学基金(21221004)

作品数:11 被引量:147H指数:7
相关作者:李俊华拜冰阳乔琦郝吉明张彭义更多>>
相关机构:清华大学中国环境科学研究院北京师范大学更多>>
发文基金:国家自然科学基金国家高技术研究发展计划国家重点基础研究发展计划更多>>
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反硝化型甲烷厌氧氧化的研究进展被引量:10
2015年
反硝化型甲烷厌氧氧化(denitrifying anaerobic methane oxidation,DAMO)即甲烷厌氧氧化耦合反硝化,是指在厌氧条件下以甲烷作为电子供体,NO2-/NO3-作为电子受体的反硝化过程。甲烷是一种温室气体,其引起的温室效应是等物质量CO2的20~30倍。DAMO过程利用甲烷代替常规碳源进行脱氮,有利于减少温室效应,并改善氮循环。研究发现,Candidatus Methylomirabilis oxyfera细菌和Candidatus Methanoperedens nitroreducens古菌是参与DAMO过程的2类主要功能微生物,前者通过内部好氧机制耦合亚硝酸盐还原与甲烷的厌氧氧化,后者则通过逆向产甲烷途径耦合硝酸盐还原与甲烷的厌氧氧化。本文详细阐述了M.oxyfera细菌和M.nitroreducens古菌细胞内代谢途径,着重总结了甲烷、NO2-/NO3-、反应器构型、温度等因素对DAMO性能的影响。并对DAMO实际应用方面的研究现状做了调研。在DAMO功能微生物作用机制、快速富集及影响因素的进一步深入研究的基础上,推进DAMO污水脱氮工艺的应用是未来的主要研究热点和发展方向。
范秋香吴箐常佳丽梁鹏张潇源张传义黄霞
关键词:污水脱氮反硝化速率影响因素
我国西南地区氮饱和马尾松林土壤和植物^(15)N自然丰度对长期氮施加的响应被引量:3
2015年
我国快速增长的氮沉降可能造成森林生态系统的氮饱和,进而导致一系列严重的环境后果.为了深入研究氮沉降对我国森林生态系统的影响,进而评价和预测森林生态系统的氮状态,本研究选取我国西南地区典型的马尾松林生态系统,对土壤和植物的15N自然丰度(δ15N)进行了测定,探讨用15N富集因子(εp/s)作为氮状态指标的可行性.对该马尾松林连续7 a施加NH4NO3或Na NO3的控制实验结果表明,长期的高氮输入显著增加了土壤和植物的δ15N.同时,该生态系统对不同形态的氮输入有不同的响应,即在NH+4沉降下δ15N显著高于NO-3沉降下的值.15N富集因子与氮沉降量、净硝化速率和淋溶量均呈显著的正相关关系,特别是本研究与之前研究的所有马尾松林的15N富集因子与氮沉降量之间线性相关,表明15N富集因子可用来表征氮状态.由于在相同氮沉降的情况下,NH+4的效应强于NO-3,建议我国在未来控制氮氧化物排放的同时也应当重视氨的排放控制.
刘文静康荣华张婷朱婧段雷
关键词:马尾松林N沉降
锰负载量对活性炭载锰氧化物的结构及催化分解臭氧性能的影响(英文)被引量:16
2014年
将高锰酸钾与活性炭(AC)原位氧化还原制备的活性炭载锰氧化物(MnOx/AC)用作臭氧分解的催化剂.采用扫描电镜、X射线光电子能谱、X射线衍射、电子自旋共振波谱、拉曼光谱以及程序升温还原研究了设计Mn负载量对负载锰氧化物性质(形貌、氧化态和晶体结构)的影响.结果表明, Mn负载量由0.44%增至11%,负载锰氧化物在活性炭表面由疏松的地衣状变为堆叠的纳米球状体,负载层的厚度由-180 nm增加至-710 nm,结构由氧化态+2.9到+3.1的低结晶β-MnOOH生长为由氧化态+3.7到+3.8的δ-MnO2结晶. MnOx/AC室温催化分解低浓度臭氧的活性与负载锰氧化物的形貌及含量密切相关. Mn负载量为1.1%的MnOx/AC具有疏松的地衣状形貌,催化分解臭氧的性能最高, Mn负载量为11%的MnOx/AC具有紧密的堆积结构,因而表现出最低的催化臭氧分解活性.
王鸣晓张彭义李金格姜传佳
关键词:锰氧化物臭氧分解活性炭
模拟氮沉降对内蒙古克氏针茅草原N2O排放的影响被引量:20
2016年
随着工农业和社会的快速发展,我国成为全世界氮沉降最高的国家之一,温带草原地区的氮沉降水平局部可能超过3g·(m^2·a)^(-1).为研究氮沉降对我国典型草原生态系统氮循环的影响,在内蒙古太仆寺旗的克氏针茅草原,对土壤氧化亚氮(N_2O)的排放进行了为期1 a测定;同时,对该天然草地施加Na NO_3^-N以模拟氮沉降增加,进行了6个水平:CK(对照)、N_2[2g·(m^2·a)^(-1)]、N5[5 g·(m^2·a)^(-1)]、N10[10 g·(m^2·a)^(-1)]、N_25[25 g·(m^2·a)^(-1)]和N50[50 g·(m^2·a)^(-1)]的野外控制实验.结果表明,在自然氮沉降条件下,该生态系统N_2O的排放主要取决于土壤含水量和土壤温度,通过参数拟合估计全年N_2O-N排放量为0.10 g·(m^2·a)^(-1),约为当地氮沉降量的3%.而提高氮沉降可以显著提高N_2O的排放,特别是在高氮处理下(N_25和N50),N_2O的年排放量与模拟氮沉降量呈线性关系.我国温带典型草原较高的温室气体N_2O排放值得关注.
杨涵越张婷黄永梅段雷
关键词:N2O排放温带草原克氏针茅氮沉降温室气体
Efectiveness of national air pollution control policies on the air quality in metropolitan areas of China被引量:23
2014年
Understanding the effectiveness of national air pollution controls is important for control policy design to improve the future air quality in China. This study evaluated the effectiveness of major national control policies implemented recently in China through a modeling analysis. The sulfur dioxide (SO2) control policy during the llth Five Year Plan period (2006-2010) had succeeded in reducing the national SO2 emission in 2010 by 14% from its 2005 level, which correspondingly reduced ambient SO2 and sulfate (SO42-) concentrations by 13%-15% and 8%-10% respectively over east China. The nitrogen oxides (NOx) control policy during the 12th Five Year Plan period (2011-2015) targets the reduction of the national NOx emission in 2015 by 10% on the basis of 2010. The simulation results suggest that such a reduction in NOx emission will reduce the ambient nitrogen dioxide (NO2), nitrate (NO3-), 1-hr maxima ozone (03) concentrations and total nitrogen deposition by 8%, 3%-14%, 2% and 2%--4%, respectively over east China. The application of new emission standards for power plants will further reduce the NO2, NO3-, 1-hr maxima 03 concentrations and total nitrogen deposition by 2%-4%, 1%-%, 0-2% and 1%-2%, respectively. Sensitivity analysis was conducted to evaluate the inter-provincial impacts of emission reduction in Beijing-Tianjin-Hebei and the Yangtze River Delta, which indicated the need to implement joint regional air pollution control.
Shuxiao WangJia XingBin ZhaoCarey JangJiming Hao
NH_3 selective catalytic reduction of NO: A large surface TiO_2 support and its promotion of V_2O_5 dispersion on the prepared catalyst被引量:3
2016年
A titania support with a large surface area was developed, which has a BET surface area of 380.5 m^2/g, four times that of a traditional titania support. The support was ultrasonically impregnated with 5 wt% vanadia. A special heat treatment was used in the calcination to maintain the large surface area and high dispersion of vanadium species. This catalyst was compared to a common V2O5-TiO2 catalyst with the same vanadia loading prepared by a traditional method. The new catalyst has a surface area of 117.7 m^2/g, which was 38% higher than the traditional V2O5-TiO2 catalyst. The selective catalytic reduction(SCR) performance demonstrated that the new catalyst had a wider temperature window and better N2 selectivity compared to the traditional one. The NO conversion was 80% from 200 to 450 °C. The temperature window was 100 °C wider than the traditional catalyst. Raman spectra indicated that the vanadium species formed more V-O-V linkages on the catalyst prepared by the traditional method. The amount of V-O-Ti and V=O was larger for the new catalyst. Temperature programmed desorption of NH3, temperature programmed reduction by H2 and X-ray photoelectron spectroscopy results showed that its redox ability and total acidity were enhanced. The results are helpful for developing a more efficient SCR catalyst for the removal of NOx in flue gases.
刘欣李俊华李想彭悦王虎江晓明王兰武
关键词:DENITRIFICATIONTITANIADISPERSIBILITY
Gas-to-particle conversion of atmospheric ammonia and sampling artifacts of ammonium in spring of Beijing被引量:11
2015年
PM2.5 and gaseous pollutants(SO2,HNO2,HNO3,HCl,and NH3) were simultaneously collected by Partisol- Model 2300 Sequential Speciation Sampler with denuder-filter pack system in the spring of 2013 in Beijing.Water-soluble inorganic ions and gaseous pollutants were measured by Ion Chromatography.Results showed that the concentrations of NH3,NH+ 4and PM2.5 had similar diurnal variation trends and their concentrations were higher at night than in daytime.The results of gas-to-particle conversion revealed that [NH3]:[NH+4] ratio was usually higher than 1; however,it was less than 1 and the concentration of NH+4 increased significantly during the haze episode,indicating that NH3 played an important role in the formation of fine particle.Research on the sampling artifacts suggested that the volatilization loss of NH+4 was prevalent in the traditional single filter-based sampling.The excess loss of HNO3 and HCl resulted from ammonium-poor aerosols and semivolatile inorganic species had severe losses in the clean day,whereas the mass of NH+ 4was usually overestimated during the single filter-based sampling due to the positive artifacts.Correlation analysis was used to evaluate the influence of meteorological conditions on the volatilization loss of NH+4.It was found that the average relative humidity and temperature had great effects on the loss of NH+4.The loss of NH+4 was significantly under high temperature and low humidity,and tended to increase with the increasing of absorption of gaseous pollutants by denuder.The total mass of volatile loss of NH+4,NO- 3and Cl- could not be ignored and its maximum value was 12.17 μg m-3.Therefore it is important to compensate sampling artifacts for semivolatile inorganic species.
WEI LianFangDUAN JingChunTAN JiHuaMA YongLiangHE KeBinWANG ShuXiaoHUANG XiaoFengZHANG YuanXun
关键词:AMMONIUM
Synthesis of three-dimensional ordered mesoporous MnO_2 and its catalytic performance in formaldehyde oxidation被引量:19
2016年
Three-dimensional(3D)ordered mesoporous MnO2 was prepared using KIT-6 mesoporous molecular sieves as a hard template.The material was used for catalytic oxidation of HCHO.The material has high surface areas and the mesoporous characteristics of the template,with cubic symmetry(ia3d).It consists of a β-MnO2 crystalline phase corresponding to pyrolusite,with a rutile structure.Transmission electron microscopy and X-ray photoelectron spectroscopy showed that the 3D-MnO2 catalyst has a large number of exposed Mn4+ ions on the(110)crystal plane surfaces,with a lattice spacing of 0.311 nm; this enhances oxidation of HCHO.Complete conversion of HCHO to CO2 and H2O was achieved at 130 °C on 3D-MnO2; the same conversions on α-MnO2 and β-MnO2 nanorods were obtained at 140 and 180 °C,respectively,under the same conditions.The specific mesoporous structure,high specific surface area,and large number of surface Mn4+ ions are responsible for the catalytic activity of 3D-MnO2 in HCHO oxidation.
拜冰阳乔琦李俊华郝吉明
关键词:FORMALDEHYDE
Progress in research on catalysts for catalytic oxidation of formaldehyde被引量:38
2016年
Formaldehyde(HCHO)is carcinogenic and teratogenic,and is therefore a serious danger to human health.It also adversely affects air quality.Catalytic oxidation is an efficient technique for removing HCHO.The development of highly efficient and stable catalysts that can completely convert HCHO at low temperatures,even room temperature,is important.Supported Pt and Pd catalysts can completely convert HCHO at room temperature,but their industrial applications are limited because they are expensive.The catalytic activities in HCHO oxidation of transition-metal oxide catalysts such as manganese and cobalt oxides with unusual morphologies are better than those of traditional MnO2,Co3O4,or other metal oxides.This is attributed to their specific structures,high specific surface areas,and other factors such as active phase,reducibility,and amount of surface active oxygens.Such catalysts with various morphologies have great potential and can also be used as catalyst supports.The loading of relatively cheap Ag or Au on transition-metal oxides with special morphologies potentially improves the catalytic activity in HCHO removal at room temperature.The preparation and development of new nanocatalysts with various morphologies and structures is important for HCHO removal.In this paper,research progress on precious-metal and transition-metal oxide catalyst systems for HCHO oxidation is reviewed; topics such as oxidation properties,structure–activity relationships,and factors influencing the catalytic activity and reaction mechanism are discussed.Future prospects and directions for the development of such catalysts are also covered.
拜冰阳乔琦李俊华郝吉明
关键词:FORMALDEHYDE
Effects of pH on photochemical decomposition of perfluorooctanoic acid in different atmospheres by 185 nm vacuum ultraviolet被引量:2
2014年
Perfluorooctanoic acid (PFOA), a persistent organic pollutant, receives increasing concerns due to its worldwide occurrence and resistance to most conventional treatment processes. The photochemical decomposition by 185 nm vacuum ultraviolet (VUV) is one of the efficient methods for PFOA decomposition. The effects of pH on PFOA decomposition in nitrogen atmosphere or oxygen atmosphere were investigated. At its original pH (4.5) of PFOA aqueous solution, PFOA decomposed efficiently both in nitrogen and in oxygen atmosphere. However, when the pH increased to 12.0, PFOA decomposition was greatly inhibited in oxygen atmosphere, while it was greatly accelerated in nitrogen atmosphere with a very short half-life time (9 rain). Furthermore, fluorine atoms originally contained in PFOA molecules were almost completely transformed into fluoride ions. Two decomposi- tion pathways have been proposed to explain the PFOA decomposition under different conditions. In acidic and neutral solutions, PFOA predominantly decomposes via the direct photolysis in both atmospheres; while in the alkaline solution and in the absence of oxygen, the decomposition of PFOA is mainly induced by hydrated electrons.
Yuan WangPengyi Zhang
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