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1.
液相化学过程作为二次有机气溶胶(SOA)形成的一种必不可少的途径,引起了学界对大气化学的广泛关注.由于其反应复杂性,反应机制、产物特性及对SOA质量的贡献还没有完全理解.本文选择四乙基愈创木酚(4-ethylguaiacol,EG)为前体物,系统地研究了初始浓度(0.03、0.3和3 mmol·L-1)的EG液相·OH氧化形成的液相二次有机气溶胶(aqSOA)特性的影响.用黑炭-气溶胶质谱(SP-AMS)测定aqSOA产率和氧化特性,气相色谱-质谱联用仪(GC/MS)、离子色谱(IC)测定产物和低分子有机酸.紫外分光光度计(UV-vis)和高效液相色谱测定了类腐殖质(HULIS)等表征光吸光产物的形成.结果表明,不同初始浓度(mmol·L-1)下aqSOA的O/C都表现为随着反应时间延长而升高,分别在0.42~0.61(0.03 mmol·L-1)、0.49~0.84(0.3 mmol·L-1)和0.49~0.63(3 mmol·L-1)之间变化.SP-AMS测定aqSOA组分发现高初始浓度时二聚体(C16H18 O2+,m/z 302)量明显高,说明高浓度下更容易发生聚合反应.UV-vis分析表明,随光氧化反应的进行,250 nm处吸光明显增强,可能是由于250 nm处新的吸光性产物生成所致.反应过程中生成的HULIS浓度不断升高,与UV-vis测定的300~400 nm区域内吸光度增强结论一致,说明水相反应形成了棕色碳.IC检测到产物中含有小分子有机酸:甲酸、乙醇酸和草酸,其中甲酸浓度最高.GC/MS检测到aqSOA中含酮、单聚体和二聚体等,说明发生了官能团化和聚合化过程.  相似文献   

2.
上海市大气环境中有机卤素污染物的来源及分布规律   总被引:7,自引:0,他引:7  
采用中子活化分析和气相色谱分析方法,检测了上海嘉定区2004-12~2005-08期间大气颗粒物和降水样品,分析了可萃取有机卤素(EOX)、可萃取持久性有机卤素(EPOX)、有机氯农药(OCPs)和多氯联苯(PCBs)含量.不同粒径大气颗粒物(TSP、PM10)和降水中EOX月均浓度分别为:1?425.37 ng·m-3、552.78 ng·m-3和815.7 ng·L-1,EPOX月均浓度分别为:21.18 ng·m-3、10.7 ng·m-3和低于检测值,OCPs月均浓度分别为:64.4 pg·m-3、31.00  pg·m-3和7.08 pg·L-1.结果表明,EOCl含量占EOX的 80%~96%,即有机氯是大气环境中有机卤素污染物的主要成分,有机卤素污染物绝大部分是酸不稳定化合物,而且大多数有机卤素是未知结构化合物.发现细颗粒具有元素择优富集效应.大气颗粒物是有机氯农药和多氯联苯的主要载体,有机卤素吸附物以5~8氯取代数的高氯PCBs和DDT及其代谢物组分为主,而降水中则以3~5氯取代数的低氯PCBs和HCH组分为主.  相似文献   

3.
黄山  裴成磊  张莹  宋奇聪  齐吉朋  赵一鸣  王鸣  邵敏 《环境科学》2020,41(12):5362-5370
为探究珠江三角洲城区大气甲醛的垂直分布特征,本研究首次在广州塔上3个不同高度点开展了甲醛的同步观测.在2018年秋季连续32 d使用2,4-二硝基苯肼(DNPH)法采集午间1 h甲醛样品,并通过高效液相色谱(HPLC)进行分析.结果表明,广州塔地面、118 m点和488 m点的甲醛浓度均值分别为(5.10±1.93)、(6.61±2.84)和(5.33±2.55)μg·m-3.3个高度观测点的甲醛浓度均与大气氧化剂Ox存在正相关性(R为0.65~0.75),表明光化学过程是广州市城区甲醛的重要来源.甲醛垂直浓度廓线依据分布形状分为3类,出现频率最高的一类为上下低中间高,发生在边界层对流较为温和、光化学反应活跃的状态下,中高层(118 m)可能受到来自较远处的工业高架源传输影响.根据垂直浓度梯度估算出广州塔点的甲醛垂直柱浓度均值为(11.23±4.80)×1015 molecules·cm-2,比同期卫星提供的甲醛柱浓度低19%,和已有报道值数量级一致.  相似文献   

4.
大气降水同位素的研究对于深入理解地区水循环特征具有重要意义.而基于降水样品实测数据在高纬度寒冷地区的研究尚不多见.本文基于2020年7月—2021年6月一个水文年周期内68个大气降水样品,测定了降水中的δD和δ18O,分析了哈尔滨降水稳定同位素特征及水汽来源.结果表明:①哈尔滨大气降水中δD和δ18O平均值分别为-89.33‰和-12.46‰,具有明显的冬低夏高的特点,年内变化范围均较大,分别为-275.50‰~-3.67‰和-35.68‰~-1.10‰,较全球平均值低67.33‰和8.46‰,较中国平均值低39.33‰和4.46‰.②哈尔滨大气降水线方程为:δD=7.66δ18O+6.29(R2=0.98),斜率和截距与全球的8和10和中国大气降水线的7.9和8.2接近,与东北地区大气降水线的7.20和-2.39相比,斜率差异较小而截距差异明显.③氢氧同位素与气温之间的拟合方程为:δD=0.34T-15.40(R2=0.41, p<0.01),δ18O=2.52T-111.18 (R2=0.38, p<0.01),说明哈尔滨降水同位素具有极显著的温度效应.④过量氘(d-excess)的变化范围为-7.63‰~22.98‰,根据降水量计算得到的加权平均值为10.47‰,说明哈尔滨降水主要以陆地气团为主导;d与气温T之间的拟合关系为:d=-0.19T+11.99(R2=0.13, p<0.01) ,与相对湿度RH之间的拟合关系为:d=0.13RH+0.14 (R2=0.07, p<0.05);⑤哈尔滨大气降水的水汽来源从全年的气团后向模拟结果来看是由大西洋水汽,北冰洋的水汽,太平洋水汽以及局地蒸发四部分组成,并且来自局地蒸发的陆地气团的比例始终占1/2以上.  相似文献   

5.
沉积物中氮磷释放到湖水中会加剧湖泊的富营养化,危害生态安全和人类健康.微生物在氮磷转换中不可或缺,准确分析沉积物中氮磷分布特征和来源以及与微生物的关系是湖泊富营养化管控的重要前提.以太湖为研究区,采集30个表层沉积物样品,测定并分析了粒度、pH、有机质(OM)、溶解性有机碳(DOC)、全磷(TP)、全氮(TN)、硝态氮(NO3--N)和溶解性有机氮(DON)等指标含量及空间分布特征,同时利用营养琼脂(NA)培养基以平板计数法测定好氧细菌(AB)数量.结合主成分分析(PCA)和Pearson相关分析探究了太湖沉积物和AB空间分布特征和来源.采用综合污染指数法和有机污染指数法研究了太湖沉积物污染特征.结果表明,太湖表层沉积物指标平均值如下:AB为9.25×104 CFU ·g-1,平均粒径(MZ)为17.59 μm,pH为7.62,ω(OM)为15.05g ·kg-1,ω(DOC)为71.60mg ·kg-1,ω(TP)为598.13mg ·kg-1,ω(TN)为1113.92 mg ·kg-1,ω(NO3--N)为3.22mg ·kg-1,ω(DON)为22.60mg ·kg-1.综合污染指数(FF)显示太湖中的点位13%为中度污染,87%为重度污染.TN除在湖心区、南部湖区和东太湖西部的部分湖区为轻度污染外,其余区域为中重度污染.除竺山湾为重度污染外,太湖中TP整体上为轻中度污染.有机污染指数(OI)表明,太湖沉积物有机污染较轻,主要与有机氮(ON)污染有关.太湖中DOC、DON、TN和OM主要来源于水生植物的影响,TP和AB主要来源于河流外源输入的影响.研究将为湖泊富营养化治理提供理论支撑,也为进一步研究AB去除沉积物中氮磷污染提供新思路.  相似文献   

6.
硝基多环芳烃是大气细颗粒物中具有致癌效应的一类重要污染物,为探明硝基多环芳烃污染特征与来源,采集南京市14个大气细颗粒样品,利用气相色谱-质谱联用仪(GC-MS)测定硝基多环芳烃浓度,进行分布特征分析,来源识别和健康风险评估.结果表明,南京市大气细颗粒物中2,8-二硝基二苯并噻吩(743 pg·m-3)、2,7-二硝基芴(331 pg·m-3)、9-硝基蒽(326 pg·m-3)、3-硝基荧蒽(217 pg·m-3)和1,8-二硝基芘(193 pg·m-3)为主要的硝基多环芳烃;硝基多环芳烃检出浓度具有明显的季节变化,冬季最高(3082 pg·m-3),秋季其次(1553 pg·m-3),春季最低(1218 pg·m-3).南京市大气细颗粒物中硝基多环芳烃主要来自多环芳烃大气光氧化反应与生物质燃烧,二次生成是硝基多环芳烃的重要来源.当前南京PM2.5中硝基多环芳烃的致癌风险可控,二硝基多环芳烃是致癌风险的主要来源.  相似文献   

7.
合肥市夏季大气颗粒物中微生物群落的高通量测序分析   总被引:1,自引:1,他引:0  
大气颗粒物的组分、来源和时空变化特征等方面已进行了广泛的研究,但对占大气颗粒物25%的生物气溶胶中细菌和真菌等微生物群落的研究较少.本文使用电感耦合等离子体质谱仪(ICP-MS)和离子色谱仪(IC)分别测定了大气颗粒物中痕量元素和水溶性离子的含量,并结合高通量测序和荧光定量PCR分析了合肥市7~9月大气颗粒物PM1.0、PM2.5和PM10中微生物群落组成及其来源.结果表明,不同粒径下细菌群落多样性无显著差异(ANOVA,P>0.05),雨天细菌和真菌群落多样性均高于晴天,所有样品中细菌群落多样性均显著高于真菌群落多样性(ANOVA,P<0.01);大气中细菌的优势菌门为变形菌门(46.19%)、厚壁菌门(33.42%)、拟杆菌门(10.99%)、蓝藻门(3.33%)和放线菌门(2.11%),真菌的优势菌门为子囊菌门(73.23%)、担子菌门(5.78%)、被孢霉菌门(3.41%)和毛霉门(0.10%);通过分析潜在源环境的指示物种,发现土壤、植物叶片和动物粪便是合肥市大气中细菌群落的主要来源,真菌群落的主要来源是植物叶片和土壤;细菌群落主要受K、Pb、Al、Fe、Mg、Ca、Na+、NO2-和风速(WS)影响,而真菌群落的主要影响因素是V、Mn、Sr、NO2-、NO3-、Na+、Cl-、空气质量指数(AQI)和PM10;此外,在细菌和真菌群落分析中鉴定到了不动杆菌属、链球菌属、肠杆菌属、假单胞菌属、代夫特菌属、沙雷氏菌属、木霉属、链格孢属和曲霉属等9种致病菌,它们可以导致人类和其它生物的多种疾病.本文的研究结果有助于揭示大气微生物的各种特性及其影响因素,以及对人类健康的影响,对后续研究和政府相应政策的制定具有重要的参考价值.  相似文献   

8.
碳质气溶胶作为大气气溶胶的重要组成部分,对大气环境质量、人类健康及全球气候变化有着重要的影响.为探究贵阳市花溪城区大气细颗粒物(PM2.5)中碳质气溶胶的变化特征及来源,于2020年不同季节开展大气PM2.5原位观测研究,利用热/光学碳分析仪(DRI Model 2015)测定大气PM2.5的碳质组分.结果表明,观测期间大气ρ(PM2.5)、ρ[总碳质气溶胶(TCA)]、ρ[有机碳(OC)]、ρ[二次有机碳(SOC)]和ρ[元素碳(EC)]的平均值分别为:(39.7±22.3)、(14.1±7.2)、(7.6±3.9)、(4.4±2.6)和(2.0±1.0)μg·m-3,OC/EC的平均值为(3.9±0.8).ρ(PM2.5)、ρ(TCA)、ρ(OC)、ρ(SOC)和ρ(EC)呈现冬季最高[(52.6±28.6)、(17.0±9.6)、(9.1±5.2)、(6.1±3.9)和(2.4±1.2)μg·m-3],夏季最低[(25.1±7.1)、(11.6±3.6)、(6.3±1.9)、(3.7±1.2)和(1.6±0.6)μg·m-3]的季节变化特征.OC/EC季节变化呈现:夏季(4.2±0.8)>冬季(3.8±0.9)>秋季(3.8±0.5)>春季(3.7±0.9),表明花溪城区各季节均存在SOC生成.SOC与OC呈现显著相关(R2=0.9),且随着大气氧化性增强,SOC浓度呈增加趋势.OC与EC各季节均呈现较好相关性,其中秋季最高(R2=0.9),其他3个季节偏低(R2为0.74~0.75),表明二者具有共同来源.通过OC/EC值范围初步判断碳质气溶胶来源于机动车尾气排放、燃煤排放和生物质燃烧排放.为了进一步定量解析主要排放源对碳质气溶胶的贡献,利用PMF模型对碳质气溶胶来源解析,结果表明贵阳市花溪城区碳质气溶胶主要来源为燃煤源(29.3%)、机动车排放源(21.5%)和生物质燃烧源(49.2%).  相似文献   

9.
2007年春节期间北京大气细粒子中正构烷烃的污染特征   总被引:6,自引:4,他引:2  
利用大流量颗粒物采样器分昼夜采集了2007年春节前后大气气溶胶中PM2.5样品,并采用气相色谱-质谱技术对PM2.5样品中的正构烷烃进行了检测和分析.结果表明,春节期间大气细粒子平均浓度全部超过WHO阈值,且夜间平均浓度要高于白天.细粒子中检测出C10~C33的正构烷烃,总浓度为201.7~2 715.6 ng·m-3,夜间正构烷烃的平均总浓度(943.5 ng·m-3)要高于白天(581.1 ng·m-3),除夕前的平均总浓度(1025.5 ng·m-3)要高于除夕后(536.6 ng·m-3).主峰碳为23、 24和25,CPI值为0.9~1.4,平均为1.15,表明春节期间北京大气细粒子中的正构烷烃主要由化石燃料的不完全燃烧产生,%WaxCn的结果表明生物源对气溶胶中正构烷烃的贡献率为8.5%~47%.  相似文献   

10.
基于超声溶剂萃取、固相萃取和超高效液相色谱-质谱联用技术(UPLC-MS/MS),建立了一种适用于城市污水处理厂污水和污泥中2种典型药物(磺胺甲恶唑和卡马西平)及其5种代谢产物的同步分析方法.污水样品添加硫酸酸化、Na2EDTA络合金属离子后经固相萃取富集净化;污泥样品通过甲醇/0.2 mol·L-1柠檬酸溶液(1:1,体积比)超声萃取后经固相萃取富集净化.采用UPLC-MS/MS电喷雾电离源在多反应监测模式下进行目标物的定量分析.结果表明,在优化条件下,7种目标物标准曲线的线性可决系数(R2)均大于0.99,方法回收率为74%~217%,日内与日间相对标准偏差稳定(RSD<20%),污水定量限为0.17~2.42 ng·L-1,污泥定量限为0.20~2.85 μg·kg-1.将该方法成功应用于两家城市污水处理厂样品中,除N-AcSMX外其余6种目标物被检出,其在污水和污泥中的浓度分别为3.92(SMX-DG)~667(LCBZ)ng·L-1和0.41(2OH-CBZ)~2.74(CBZ)μg·kg-1.  相似文献   

11.
Laogang landfill near Shanghai is the largest landfill in China, and receives about 10000 t of daily garbage per day, Samples of topsoil and plants were analyzed to evaluate mercury pollution from the landfill. For topsoil samples, there were significant correlations among total mercury (HgT), combinative mercury (Hgc) and gaseous mercury (HgG), and content of total organic carbon (TOC), but, no significantly relationship was found between Hg content and filling time. Hg content changes in vertical profiles with time showed that the average Hgv of profiles 1992, 1996, and 2000 was similar, but their average HgG was quite different. HgT was significantly correlated with Hgc in profile 1992 and 2000, and Hgv was significantly correlated with Hg6 in profile 1996. HgG/Hgv ratio in profile samples decreased in the order of (HgG,/HgT)1992〉(HgG/HgT)1996〉〉(HgG/HgT)2000. A simple outline of Hg release in landfill could be drawn: with increasing of filling time, degradation undergoes different biodegradation, accordingly, gaseous mercury goes through small, more, and small proportion to total mercury. Distribution of Hg in plants was inhomogeneous, following the order of leaf〉root〉stem. The highest value of leaf may be associated with higher atmospheric Hg from landfill. Ligneous plants (e.g. Phyllostachys glanca, Prunus salicina and Ligustrum lucidum) are capable of enriching more Hg than herbaceous plants.  相似文献   

12.
Phytoremediation is a potential cleanup technology for the removal of heavy metals from contaminated soils.Bidens maximowicziana is a new Pb hyperaccumulator,which not only has remarkable tolerance to Pb but also extraordinary accumulation capacity for Pb.The maximum Pb concentration was 1509.3 mg/kg in roots and 2164.7 mg/kg in overground tissues.The Pb distribution order in the B. maximowicziana was:leaf>stem>root.The effect of amendments on phytoremediation was also studied.The mobility of soil Pb and the Pb concentrations in plants were both increased by EDTA application.Compared with CK(control check),EDTA application promoted translocation of Pb to overground parts of the plant.The Pb concentrations in overground parts of plants was increased from 24.23-680.56 mg/kg to 29.07-1905.57 mg/kg.This research demonstrated that B.maximowicziana appeared to be suitable for phytoremediation of Pb contaminated soil,especially,combination with EDTA.  相似文献   

13.
Decomposition of alachlor by ozonation and its mechanism   总被引:1,自引:0,他引:1  
Decomposition and corresponding mechanism of alachlor, an endocrine disruptor in water by ozonation were investigated. Results showed that alachlor could not be completely mineralized by ozone alone. Many intermediates and final products were formed during the process, including aromatic compounds, aliphatic carboxylic acids, and inorganic ions. In evoluting these products, some of them with weak polarity were qualitatively identified by GC-MS. The information of inorganic ions suggested that the dechlorination was the first and the fastest step in the ozonation of alachlor.  相似文献   

14.
The influence of the nonionic surfactant Tween 80 on pentachlorophenol (PCP) oxidation catalyzed by horseradish peroxidase was studied. The surfactant was tested at concentrations below and above its critical micelle concentration (CMC). Enhancement of PCP removal was observed at sub-CMCs. The presence of Tween 80 in the reaction mixture reduced enzyme inactivation which occurred through a combination of free radical attack and sorption by precipitated products. A simple first-order model was able to simulate time profiles for enzyme inactivation in the presence or absence of Tween 80. At supra-CMCs, the surfactant caused noticeable reductions in PCP removal, presumably through micelle partitioning of PCP which precluded the hydrophobic PCP molecule from interacting with the enzyme.  相似文献   

15.
以三峡大学的校园河道求索溪为研究对象,利用综合水质标识指数法确定求索溪水质类别,分析其水质时空变化规律,并利用对应分析法得出求索溪中不同监测点的主要污染因子.研究结果表明:求索溪整体的综合水质标识指数为7.423,整体水质为劣V类(地表水环境质量标准GB 3838-2002)且黑臭.从时间变化来看,求索溪4月份的水质最差,5月份次之,4、5月份所有监测点的水质都劣于V类且黑臭;8月份水质最好,水质为Ⅳ类;从空间分布来看,8个监测点综合水质标识指数均超过6.0,水质为劣V类,其中6号监测点的水质相对最好,监测点3号的水质相对最差;对应分析法得出求索溪的整体水体污染程度受总氮因子的影响最大,其次为总磷.该研究拟为求索溪及类似校园河道的水环境治理研究提供基础依据和参考.  相似文献   

16.
Effects of chitosan on a submersed plant, Hydrilla verticillata, were investigated. Results indicated that H. venicillata could prevent ultrastructure phytotoxicities and oxidativereaction from polluted water with high chemical oxygen demand (COD). Superoxide dismutase (SOD) activity and malondialdehyde (MDA) contents in H. verticillata treated with 0.1% chitosan in wastewater increased with high COD (980 mg/L) and decreased with low COD (63 mg/L), respectively. Ultrastructural analysis showed that the stroma and grana of chloroplast basically remained normal. However, plant cells from the control experiment (untreated with chitosan) were vacuolated and the cell interval increased. The relict of protoplast moved to the center, with cells tending to disjoint. Our findings indicate that wastewater with high COD concentration can cause a substantial damage to submersed plant, nevertheless, chitosan probably could alleviate the membrane lipid peroxidization and ultrastructure phytotoxicities, and protect plant cells from stress of high COD concentration polluted water.  相似文献   

17.
Removal of cadmium using MnO2 loaded D301 resin   总被引:6,自引:0,他引:6  
MnO2 loaded weak basic anion exchange resin D301 (Anion exchange resin, macroreticular weak basic styrene) as adsorbent has been prepared and applied to the removal of cadmium. The adsorption characteristics have been investigated with respect to effect of pH, equilibrium isotherms, removal kinetic data, and interference of the coexisting ions. The results indicated that the Cd^2+ could be efficiently removed using MnO2 loaded D301 resin in the pH range of 3-8 from aqueous solutions with the co-existence of high concentration of alkali and alkaline-earth metals ions. The saturate adsorption capacity of the Cd^2+ was 77.88 mg/g. The adsorption process followed the pseudo first-order kinetics. The equilibrium data obtained in this study accorded excellently with the Langmuir adsorption isotherm.  相似文献   

18.
The purpose of this study is to understand the effect and mechanism of preventing membrane fouling, by coagulation pretreatment, in terms of fractional component and molecular weight of natural organic matter (NOM). A relatively higher molecular weight (MW) of hydrophobic compounds was responsible for a rapid decline in the ultrafiltration flux. Coagulation could effectively remove the hydrophobic organics, resulting in the increase of flux. It was found that a lower MW of neutral hydrophilic compounds, which could remove inadequately by coagulation, was responsible for the slow declining flux. The fluxes in the filtration of coagulated water and supernatant water were compared and the results showed that a lower MW of neutral hydrophilic compounds remained in the supernatant water after coagulation could be rejected by a membrane, resulting in fouling. It was also found that the coagulated flocs could absorb neutral hydrophilic compounds effectively. Therefore, with the coagulated flocs formed on the membrane surface, the flux decline could be improved.  相似文献   

19.
Acidithiobacillus ferrooxidans ATCC23270 and Acidithiobacillus thiooxidans TM-32 were used for bioleaching of spent refractories of aluminium and copper melting furnaces for their recycling.Firstly,penetration of elements into aluminium melting furnace refractory was investigated and it was found that up to 7 cm from surface was contaminated.Comparison on leaching efficiency by the strains ATCC23270 and TM-32 found that the strain ATCC23270 could treat larger amount of the refractories than the strain TM-32 could do.In the experiment of bioleaching of spent refractory aluminium melting furnace by the strain ATCC23270,high leaching efficiency were obtained on Al,Si,and Ca,and extremely low leaching performance was,however,shown on the rest of elements i.e.,Na,Mn,and Zn.Under the strain TM-32 use,relatively high leaching performance was recognized on Al,Si,Ca,Na,Mn,and Zn.In the experiment of bioleaching for spent refractory copper melting furnace,almost the same leaching trends were shown on Cu,Zn,Al,and Si under the strains ACTT23270 and TM-32 uses.  相似文献   

20.
Zeolite synthesized from fly ash (ZFA) without modification is not efficient for the purification of NH4+ and phosphate at low concentrations that occur in real effluents, despite the high potential removal capacity. To develop an effective technique to enhance the removal efficiency of ammonium and phosphate at low concentrations, ZFA was modified with acid treatment and the simultaneous removal of ammonium and phosphate in a wide range of concentration was investigated. It was seen that when compared with untreated ZFA, only the treatment by 0.01 mol/L of H2SO4 significantly improved the removal efficiency of ammonium at low initial concentrations. The behavior was well explained by the pH effect. Treatment by more concentrated H2SO4 led to the deterioration of the ZFA structure and a decrease in the cation exchange capacity. Treatment by 0.01 mol/L H2SO4 improved the removal efficiency of phosphate by ZFA at all initial P concentrations, while the treatment by concentrated H2SO4 (≥0.9 mol/L) resulted in a limited maximum phosphate immobilization capacity (PIC). It was concluded that through a previous mild acid treatment (e.g. 0.01 mol/L of H2SO4), ZFA can be used in the simultaneous removal of NH4+ and P at low concentrations simulating real effluent.  相似文献   

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