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翻译李晓静 环科131 1304200028随着我国核电发展方针由“适度发展”调整为“积极发展”,我国核电建设将进入快车道。根据新能源发展规划的数据,未来10年,全国核电装机复合增长率将达15%,远高于全国电力总装机约5%的复合增长率。到2020年,我国核电装机容量将达到8000万kW,届时我国天然铀(U)的年需要量将达到7000 t以上。可以预见,伴随我国核电事业的跨越式发展,铀的需求激增,铀矿山勘探、开采冶炼的规模和力度也随之极大提高。然而,由此产生的巨量铀尾矿也给当地环境带来潜在的危害及安全隐患。由于铀兼具重金属化学毒性与辐射危害,1 mg天然铀的放射性相当于24.79 mBq,在自然堆放过程中不仅会产生氡污染问题4,也可能在降水条件下使铀尾矿中的残余铀释放到环境中。我国在铀矿石的浸出研究方面开展了大量工作,多旨在为了提高冶炼技术与效率。在尾矿的生态效应方面,国内外也有不少工作在开展,其中不乏关于固废中金属迁移性方面的研究。然而,针对铀尾矿的生态环境效应的浸出研究鲜见报道。铀尾矿在长时间的自然堆放中,尤其是在自然风化及雨水的作用下,残留的铀究竟能否再次析出释放到环境中,且以何种形态释放,关乎环境安全与公众健康,正是本研究所努力探讨的两个内容。With the development of Chinas nuclear power policy changed from moderate development to positive development, the construction of nuclear power in China will enter the fast lane. According to data from new energy development plan, the next 10 years, the national nuclear power installed compound growth rate of 15%, far higher than the national electric power generating compound growth rate of about 5%. By 2020, Chinas nuclear power installed capacity will reach 80 million kW, when Chinas natural uranium (U) annual requirement will reach more than 7000 tons. Predictably, along with the leapfrog development of the nuclear power in China, the surge in demand of uranium, the scale of the uranium mine exploration, mining, smelting and strength has been greatly improved. However, the huge amount of uranium tailings resulting local environment but also to the potential hazards and safety risks. Since uranium has chemical toxicity of heavy metals and radiation hazard, radioactive 1g of natural uranium equivalent 24.79 mBq , not only produces in the process of natural stacked radon pollution, may under the condition of the precipitation of uranium tailings residual uranium released into the environment. Our research in the leaching of uranium ore done a lot of work, much aimed to improve smelting technology and efficiency. In terms of the ecological effect of tailings, there are many works carried out in both at home and abroad, there is no lack of among them about metal migration in solid waste. However, the ecological environment effects of leaching research for uranium tailings rarely reported. Uranium tailings in natural piled up for a long time, especially under the effect of natural weathering and rain, residual uranium precipitated again whether we can release into the environment , and in what form to release, relating to environmental safety and public health, is two efforts to explore the contents of this Institute. 1 样品及其来源铀尾矿为2010年10月采自韶关某大型铀矿区的尾矿坝表层,其铀的含量为472.5 mg/kg。为了研究尾矿粒径对铀迁移释放的影响,用孔径分别为0.45 mm、0.9 mm、2 mm和6 mm的4种尼龙标准筛将铀尾矿筛分成5种粒径,分别进行试验:小于0.45 mm,0.450.9 mm,0.92 mm,26 mm和大于6 mm。其中,粒径大于6 mm的尾矿所占份额最大(34.27%),其余粒度的尾矿按质量百分比从大到小依次为:26 mm(25.30%),小于0.45 mm(20.52%),0.92 mm(10.76%)和0.450.9 mm(9.15%)。1.Sample and its sourceUranium tailings for October 2010 from a large uranium deposit area, the tailings dam surface of shaoguan, its uranium content of 472.5 mg/kg. To study the effect of particle size on the migration of uranium tailings release, with a diameter of 0.45 mm and 0.9 mm respectively, 2 mm and 6 mm of 4 kinds of nylon standard sieve sieve the uranium tailings is divided into five kinds of particle size to tested: less than 0.45 mm, 0.45 0.9 mm, 0.9 2 mm, 2 6 mm and greater than 6 mm. Wherein the particle size greater than 6 mm tailings largest share (34.27%), a percentage of the remaining tailings size descending order of quality: 2 6 mm (25.30%), less than 0.45 mm (20.52%) , 0.9 2 mm (10.76%) and 0.45 0.9 mm (9.15%).2 仪器及主要试剂滤出液中的U由环境保护部华南环境科学研究所的电感耦合等离子体质谱仪(ICP-MS,美国PE公司,型号:Elan6100 DRC-e)测量。U标准试剂(100 mgmL-1, 125 mL)产自美国的IV公司。实验用水均采用一级超纯水,为美国Millipore公司Milli-Q超纯水机制备,电阻率始终保持在18.25 Mcm。滤出液的电极电位及pH值由电位酸度计(德国Sartorius公司,型号:PB-10)测定;滤出液的电导率由电导率仪(美国Eutech Instruments公司,型号:ECTestr 11+)测量。所有实验中涉及到的器具和瓶罐均用15%硝酸(体积分数)浸泡过夜后,用自来水反复冲洗干净后,再用超纯水冲洗3次,晾干备用。2.Instruments and ReagentsU-filtrate by the Ministry of Environmental Protection, South China Institute of Environmental Sciences inductively coupled plasma mass spectrometry (ICP-MS, US PE firm, Model: Elan6100 DRC-e) measurement. U standard reagent (100 g - 125 mL-1 selection, mL) of IV company from the United states. The experimental water is using a class of ultra pure water, for the United States Milli-Q company Millipore ultra pure water preparation, the resistivity is always maintained at 18.25 M - cm. Leaching liquid of electrode potential and pH by potential acidity meter (Germany Sartorius, models: PB - 10) measurement. Leaching liquid conductivity by conductivity meter (American Eutech Instruments company, models: ECTestr 11 +) measurement. All experiments related to the instruments and bottles are made of 15% nitric acid (volume fraction) soaked overnight, rinse with tap water after repeatedly and then ultrapure water three times, dry and set aside.3 实验方法本研究共设置了5个平行实验装置。每个实验装置按1 kg的铀尾矿设计,主要由直径为20 cm的布氏漏斗、内衬滤膜、导管、软管和夹子等构成,见图1。装置暴露于实验室室温条件下,每周期淋浸一次。淋浸方式为:先用喷壶将800 ml的淋滤剂(本实验全部为pH 6 左右的去离子水)在尾矿表面均匀地喷淋5 min,之后浸泡55 min,此过程中夹子始终呈关闭状态,800 ml的淋滤剂恰好能将尾矿泡在水中。浸泡过程结束后,打开夹子,将滤液导出到烧杯中,等装置中的水完全滤出后,测量滤出液体积,并将夹子关闭,继续在实验室室温条件下放置7 d。第8 d,又开始新的淋浸过程,即7 d为一周期,以此循环往复。滤出液再经普通滤纸过滤后,测量滤出液的pH、电极电位及电导率,并用ICP-MS分析滤液中的铀含量。5个平行实验装置的淋浸时长通过计时器记录确保完全统一。3.The experimental methodThis research provided five parallel experimental device. Each experimental device is designed according to 1 kg of uranium tailings, which mainly consists of a diameter of 20 cm of the funnel, lined with filter membrane, pipe, hose and clip, etc., shown in Figure 1. Device exposed to laboratory at room temperature under the condition of every cycle leaching leaching. Cream dip way: first with 800 ml of water to watering the leaching agent (in this experiment are all about pH 6 deionized water) is uniformly sprayed 5 min in the tailings surface, after soaking 55 min, this procedure was always clip closed, 800 ml of tailings leaching agent can just soak in water. After the soaking process, open the clamp, the filtrate export into a beaker, such as the water in the device completely filter out after measuring strain the liquid product, and the clamp closed, place 7 d continue to room temperature in the laboratory. Article 8 d, and start a new leaching leaching process, namely 7 d is a cycle, this cycle. The filtrate was then by ordinary filter paper, measuring filtrate of pH, electrode potential and conductivity, and the filtrate was analyzed by ICP-MS in the uranium content. 5 parallel experimental apparatus with a long time pass through the timer record to ensure complete unity.4 实验结果及讨论4.1 粒径大于6 mm的铀尾矿该部分铀尾矿约占三分之一,是铀尾矿的主要组分。其浸滤浓度-电导率曲线见图2。电导率变化区间0.0590.156 mscm-1。电导率曲线与铀滤出浓度曲线变化趋势大致相符,说明铀尾矿中除残余铀是浸滤过程的主要析出元素外,其他元素的析出也很明显。由于该尾矿粒径较大,颗粒比表面积较小,铀的析出过程缓慢且具有较大波动。铀的滤出初始浓度约为40 mgL-1,除第13周铀浓度超过铀矿冶辐射防护和环境保护规定(GB 23727-2009)的排放限值外,其他周次的铀滤出浓度皆达标。浸滤到22周时,滤液pH变化区间5.17.2,电极电位Eh变化区间0.0030.116 V。铀是变价元素,有+3,+4,+5,+6四种价态,其中+4和+6价化合物稳定。铀价态的变化,受溶液的pH和Eh影响很大.4.Experiment results and discussions4.1Diameter larger than 6mm uranium tailingsThis part of uranium tailings is about 1/3, which is the main component of uranium tailings. The conductivity curve of leaching concentration is shown in Figure 2. Conductivity changes range 0.059 0.156 ms cm-1. Filtered out conductivity curve with uranium concentration curve trends broadly in line, indicating that, in addition to residual uranium tailings leaching process of uranium is the main element of the precipitation, the precipitation of other elements is obvious. Due to large

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