褐煤地下气化过程汞析出规律的研究

在褐煤地下气化模型试验的基础上 ,研究了褐煤中汞的赋存形态 ,褐煤地下气化煤气中汞含量的变化及存在形态 ,以及气化工艺的影响 ;分析了地下气化过程中汞的析出及反应机理 .实验结果表明 ,汞在试验褐煤中主要以硫化物结合态和残渣态形式存在 ;褐煤地下气化煤气中汞含量随气化时间的变化而变化 ,且主要以Hg0 (g)的形态存在 ;水蒸汽的存在会降低Hg0 (g)被其它气体氧化为Hg2 (g)的趋势 ;与地面气化及燃煤过程不同 ,煤地下气化产物中 ,气态汞占总汞比例低于 2 0 % ,明显低于地面气化及燃煤     

添加稳定剂对尾矿土中砷形态及转换机制的影响

土壤中As的不同存在形态影响着其毒性、可移动性、生物有效性,且产生不同的环境影响.本研究以粉煤灰、干化污泥、硫酸亚铁、碎花生壳为稳定剂,探讨其对土壤As的稳定化效果以及p H、有机质和阳离子交换量与土壤As形态的关系.结果表明添加稳定剂后,土壤p H及有机质含量上升,残渣态砷含量升高.添加10%粉煤灰、10%干化污泥后,可交换态As、碳酸盐结合态As、铁锰氧化物结合态As、有机结合态As分别下降了34.2%、17.5%、19.9%、53.7%,并转化为残渣态As,其含量增长了1.14%.当同时添加10%粉煤灰、10%干化污泥和1%硫酸亚铁后,土壤中可交换态As、碳酸盐结合态As、铁锰氧化物结合态As、有机结合态As含量的降幅分别为62.3%、55.2%、29.6%、58.2%,残渣态As含量增加8.1%.添加10%粉煤灰、10%干化污泥、1%硫酸亚铁和1%粉碎花生壳后,可交换态As下降最显著,最大降幅为73.3%.施用适量的粉煤灰、干化污泥、硫酸亚铁能使土壤中的可交换态、碳酸盐结合态、铁锰氧化物结合态、有机结合态As的一部分转化为残渣态As,降低其毒性.提高p H,残渣态As含量上升,可交换态As、碳酸盐结合态As、铁锰结合态As、有机结合态As含量下降,As在接近中性的环境中稳定性最好;提高有机质含量,碳酸盐结合态As与残渣态As含量上升,可交换态As、铁锰结合态As、有机结合态As含量下降,有机结合态As含量下降明显;阳离子交换量上升,残渣态As含量上升,可交换态As、碳酸盐结合态As、铁锰结合态As、有机结合态As含量下降.     

镁基膨润土和水泥对砷铅复合污染土壤的钝化效能与机理研究

利用镁基膨润土（MB）和水泥（SN）作为钝化剂修复化工厂砷（As）、铅（Pb）复合污染土壤,探索了两种钝化剂对土壤pH值、有机碳含量（OC）、阳离子交换量（CEC）、浸出毒性及重金属形态分布的影响,结合钝化前后土壤形貌的变化,初步揭示了钝化机理.结果表明,两种钝化剂均可使土壤pH值显著升高,有机碳含量增加,阳离子交换能力增强.钝化30 d后,MB-5对As、Pb的钝化率分别达到67.09%和65.93%;SN-5对As、Pb的钝化率分别达到65.76%和65.04%.经两种钝化剂处理后,Pb的弱酸提取态和可还原态向更加稳定的可氧化态和残渣态转化.MB处理使土壤As由可交换态、可氧化态向无定形铁结合态、结晶性铁结合态转化,SN处理使土壤As向残渣态转化.两种钝化剂均可使土壤的微观形态从片状转变为碎屑状、增加团聚颗粒.与SN相比,MB更能促使土壤As（Ⅲ）向As（V）转化,从而显著降低土壤毒性.     

湖北菱角湖沉积物中重金属垂直分布及形态分析

以湖北省菱角湖沉积物为研究对象,分析沉积物中砷(As)、汞(Hg)、铅(Pb)、镉(Cd)等4种重金属的垂直分布情况,并通过地累积指数(Igeo)法对重金属污染程度进行评价。同时选取污染较为严重的As、Pb进行形态分析,以了解其潜在生态风险。地累积指数结果表明,菱角湖沉积物中Pb为轻度或偏中度污染,As、Hg主要为清洁或轻度污染,Cd为清洁;形态分析表明,As以残渣态为主,不同深度的形态分布基本保持不变,潜在生物有效性较低;Pb以残渣态为主,其次是铁锰氧化结合态,残渣态和铁锰氧化结合态随深度的增加分别增加和减少,潜在危害性增加。     

稳定化处理对矿渣中重金属迁移转化的影响研究

土壤中重金属的不同存在形态会产生不同的环境效应,并直接影响重金属的毒性、迁移性和生物有效性.以石灰、粉煤灰、干化污泥、花生壳为稳定剂,对某金矿区含重金属矿渣进行组合处理;通过重金属形态分析、淋滤试验、植物盆栽试验,探讨矿渣中重金属的迁移转化规律.结果表明,添加稳定剂后,酸性矿渣的pH升高至中性以上,有机质含量显著增加.矿渣中As、Pb、Zn的主要存在形态为残渣态,添加粉煤灰、干化污泥和花生壳使矿渣中可交换态As和有机结合态As含量分别降低了65.6%、87.7%;添加石灰、粉煤灰和花生壳使矿渣中铁锰氧化物结合态As主要向碳酸盐结合态As转化;添加石灰和粉煤灰使矿渣中的可交换态、铁锰氧化物结合态和有机结合态Pb、Zn主要向残渣态Pb、Zn转化.经前期稳定化处理后,矿渣淋滤液中As、Pb、Zn的含量均有不同程度的下降,添加花生壳处理后淋滤液中的As、Pb、Zn含量进一步下降.其中,粉煤灰、干化污泥和花生壳处理后淋滤液中As含量下降最显著,降幅为57.4%;石灰、粉煤灰和花生壳处理后淋滤液中Zn含量下降最显著,降幅为24.9%.添加稳定剂处理矿渣明显有利于植物的萌发与生长,其中添加粉煤灰、干化污泥和花生壳效果最好,香根草的萌发率为76%.     

我国红树林主要分布区表层沉积物砷的分布及形态特征

利用ICP-MS分析了我国红树林主要分布区表层沉积物的As含量和形态,阐明As的分布及其形态特征.结果表明,表层沉积物中w(As)为3.14～19.16 mg/g,平均值为8.14 mg/g.表层沉积物中w(As)与w(Fe),w(Mn),pH,w(有机质),粉粒和黏粒所占比例呈显著或极显著正相关.表层沉积物中的As主要以残渣态存在,其次为有机质-硫化物结合态.在整个研究区域,As的5种形态在总量中的所占比例:可交换离子态为14.40%,碳酸盐结合态为1.41%,铁锰氧化物结合态为2.16%,有机质-硫化物结合态为30.40%,残渣态为50.65%.可交换离子态所占比例与w(有机质)和pH呈极显著正相关.有机质-硫化物结合态所占比例与盐度、黏粒和粉粒所占比例呈显著或极显著正相关.残渣态所占比例与盐度、粉粒和黏粒所占比例呈极显著正相关.      

水泥窑共处置产品中重金属的形态

通过模拟煅烧掺入重金属化学试剂的水泥生料,制备水泥熟料,进而制取水泥净浆. 采用修正的Tessier连续提取法,分别研究了水泥熟料和水泥净浆中各重金属的形态. 结果表明:水泥熟料中Ni,As,Cd和Pb几乎不存在可交换态. 其中,Cr和Cd主要以酸性醋酸钠溶液提取态存在,分别为71.0%和95.1%;Ni主要分布在酸性盐酸羟胺溶液提取态(65.6%)中,在残渣态中的分布也较多(20.3%);Pb主要分布在硫化物结合态(72.7%)中,与硫形成某种化合物固溶于水泥矿物相中;As的硫化物结合态和酸性醋酸钠溶液提取态质量分数较高,分别为35.1%和51.8%. 水泥净浆中各重金属的形态分布与水泥熟料基本一致,表明重金属的主要化学形态分布受水化作用影响不大.      

三峡库区消落区水体-沉积物重金属迁移转化特征

结合三峡水库反季节调度模式,对消落区沉积物中Cu、Pb、Cd、Cr这4种重金属的存在形态及迁移转化特征进行研究.结果表明,不同重金属在消落区沉积物中形态分布各异,Cu主要以有机物及硫化物结合态和残渣态形式存在,Pb主要以碳酸盐结合态、Fe-Mn氧化物结合态及残渣态存在,Cd主要以碳酸盐结合态、Fe-Mn氧化物结合态存在,Cr主要以残渣态存在.伴随着消落过程的进行,汛期出露沉积物的有机质及AVS含量下降、ORP升高、pH值降低,沉积物中可提取态重金属的相对含量显著下降,重金属具有向水体迁移趋势, Cu、Pb、Cd、Cr平均迁移率分别为30.50%、 26.10%、 33.50%和11.77%,4种重金属的迁移性大小依次为Cd>Cu>Pb>Cr.可提取态Cu、Pb、Cd、Cr对重金属迁移贡献率分别为77.15%、 86.09%、 94.86%和32.34%,可提取态是重金属发生迁移的主要部分.研究结果表明, 消落区重金属迁移呈"缓释"特征,三峡水库的反季节调度模式有利于缓解消落区重金属迁移诱导的生态风险,库区水体重金属含量处于较低水平.     

好氧高温堆肥处理对猪粪中重金属形态的影响

用 Tessier 连续提取法研究了好氧高温堆肥处理对猪粪中重金属结合形态变化的影响.结果表明,经过好氧堆肥处理,猪粪中 Pb、Cu、Zn、Ni、Cr、Cd、As 的总浓度升高;碳酸盐结合态 Ni、Zn 的浓度降低,其余 Pb、Cu、Cr、Cd 的浓度都升高;硫化物及有机结合态、残渣态重金属的浓度普遍升高,仅有硫化物及有机结合态 As 和 Zn 的浓度下降;可交换态 Cu、Zn、Cr、As 的浓度显著降低.堆肥处理可以降低可交换态和碳酸盐交换态 Pb、Ni、Cu、Cr、Zn、As 和铁锰氧化物结合态 Pb、Cu、Cr、As 的分配系数,因此可以降低猪粪中重金属的有效性.堆肥处理有利于降低猪粪土地利用中重金属污染的风险.     

巢湖沉积物中重金属的BCR形态分析

以巢湖沉积物为研究对象,利用BCR(European Communities Bureau of Reference)连续提取法分析了沉积物样品中Zn、Cu、Pb、Cd、Mn赋存特征,分为可交换态及碳酸盐结合态、铁锰氧化物结合态、有机物及硫化物结合态和残渣态。结果表明:南淝河入湖区S1采样点五种金属总量都达到最高,兆河入湖区S2采样点金属总量浓度最低。五种金属中锌和锰的质量较高,重金属回收率分别为:锌(93%),铜(92%),铅(90%),镉(92%),锰(93%)。Cu以残渣态为主(54.7%),Zn以铁锰氧化物结合态为主(40.5%),Pb以有机物、硫化物结合态为主(35.3%),Cd和Mn以可交换态及碳酸盐结合态为主,所占比例分布为41.9%、58.6%。研究表明,应用BCR连续提取法有助于确定沉积物中重金属的污染状况和潜在释放能力。     

A life cycle comparison of greenhouse emissions for power generation from coal mining and underground coal gasification

Underground coal gasification (UCG) is an advancing technology that is receiving considerable global attention as an economic and environmentally friendly alternative for exploitation of coal deposits. UCG has the potential to decrease greenhouse gas emissions (GHG) during the development and utilization of coal resources. In this paper, the life cycle of UCG from in situ coal gasification to utilization for electricity generation is analyzed and compared with coal extraction through conventional coal mining and utilization in power plants. Four life cycle assessment models have been developed and analyzed to compare (greenhouse gas) GHG emissions of coal mining, coal gasification and power generation through conventional pulverized coal fired power plants (PCC), supercritical coal fired (SCPC) power plants, integrated gasification combined cycle plants for coal (Coal-IGCC), and combined cycle gas turbine plants for UCG (UCG-CCGT). The analysis shows that UCG is comparable to these latest technologies and in fact, the GHG emissions from UCG are about 28 % less than the conventional PCC plant. When combined with the economic superiority, UCG has a clear advantage over competing technologies. The comparison also shows that there is considerable reduction in the GHG emissions with the development of technology and improvements in generation efficiencies.     

Cost comparison of syngas production from natural gas conversion and underground coal gasification

Underground coal gasification (UCG) is a promising technology to reduce the cost of producing syngas from coal. Coal is gasified in place, which may make it safer, cleaner and less expensive than using a surface gasifier. UCG provides an efficient approach to mitigate the tension between supplying energy and ensuring sustainable development. However, the coal gasification industry presently is facing competition from the low price of natural gas. The technology needs to be reviewed to assess its competiveness. In this paper, the production cost of syngas from an imaginary commercial-scale UCG plant was broken down and calculated. The produced syngas was assumed to be used as feedstock in liquid fuel production through the Fischer-Tropsch process or methanol synthesis. The syngas had a hydrogen (H₂) to carbon monoxide (CO) ratio of 2. On this basis, its cost was compared with the cost of syngas produced from natural gas. The results indicated that the production cost of syngas from natural gas is mainly determined by the price of natural gas, and varied from $24.46 per thousand cubic meters (TCM) to $90.09/TCM, depending on the assumed price range of natural gas. The cost of producing UCG syngas is affected by the coal seam depth and thickness. Using the Harmon lignite bed in North Dakota, USA, as an example, the cost of producing syngas through UCG was between $37.27/TCM and $39.80/TCM. Therefore, the cost of UCG syngas was within the cost range of syngas produced by natural gas conversion. A sensitivity analysis was conducted to investigate how the cost varies with coal depth and thickness. It was found that by utilizing thicker coal seams, syngas production per cavity can be increased, and the number of new wells drilled per year can be reduced, therefore improving the economics of UCG. Results of this study indicate the competitiveness of UCG regarding to natural gas conversion technologies, and can be used to guide UCG site selection and to optimize the operation strategy.     

Sequentially coupled flow-geomechanical modeling of underground coal gasification for a three-dimensional problem

Underground coal gasification (UCG) has been identified as an environmentally friendly technique for gasification of deep un-mineable coal seams in situ. This technology has the potential to be a clean and promising energy provider from coal seams with minimal greenhouse gas emission. The UCG eliminates the presence of coal miners underground hence, it is believed to be a much safer technique compared to the deep coal mining method. The UCG includes drilling injection and production wells into the coal seam, igniting coal, and injecting oxygen-based mix to facilitate coal gasification. Produced syngas is extracted from the production well. Evolution of a cavity created from the gasification process along with high temperature as well as change in pore fluid pressure causes mechanical changes to the coal and surrounding formations. Therefore, simulation of the gasification process alone is not sufficient to represent this complex thermal-hydro-chemical–mechanical process. Instead, a coupled flow and geomechanical modeling can help better represent the process by allowing simultaneous observation of the syngas production, advancement of the gasification chamber, and the cavity growth. Adaptation of such a coupled simulation would aid in optimization of the UCG process while helping controlling and mitigating the environmental risks caused by geomechanical failure and syngas loss to the groundwater. This paper presents results of a sequentially coupled flow-geomechanical simulation of a three-dimensional (3D) UCG example using the numerical methodology devised in this study. The 3D model includes caprock on top, coal seam in the middle, and another layer of rock underneath. Gasification modeling was conducted in the Computer Modelling Group Ltd. (CMG)’s Steam, Thermal, and Advanced processes Reservoir Simulator (STARS). Temperature and fluid pressure of each grid block as well as the cavity geometry, at the timestep level, were passed from the STARS to the geomechanical simulator i.e. the Fast Lagrangian Analysis of Continua in 3 Dimensions (FLAC3D) computer program (from the Itasca Consulting Group Inc.). Key features of the UCG process which were investigated herein include syngas flow rate, cavity growth, temperature and pressure profiles, porosity and permeability changes, and stress and deformation in coal and rock layers. It was observed that the coal matrix deformed towards the cavity, displacement and additional stress happened, and some blocks in the coal and rock layers mechanically failed.     

1980—2007年我国燃煤大气汞、铅、砷排放趋势分析

基于文献调研,对1980—2007年我国汞、铅、砷3种主要燃煤大气重金属排放清单进行归纳,计算了3种重金属的逐年平均排放量,并分析排放量与燃煤量的相关性、单位煤耗大气重金属污染物排放量的变化趋势及原因. 结果表明:1980—2007年我国燃煤大气汞、铅、砷排放量与燃煤量增长趋势基本一致,均呈显著正相关(R2分别为0.911、0.971、0.996),但燃煤大气汞排放量与燃煤量间的相关性却比铅、砷排放量与燃煤量的相关性小很多,这主要是燃煤电厂对汞协同脱除能力比对铅、砷强,以及电厂汞排放所占比例较大所致. 燃煤大气汞排放量在2005年后趋于稳定,而铅、砷排放量在2000年后快速增长,年均增速均超过10%,其中电厂和工业锅炉是重金属排放的重点行业. 在燃煤量不断增长的背景下,单位煤耗的大气汞、铅排放量均呈下降趋势,其中汞排放量在2005—2007年年均降低5.0%,铅排放量在1996—2007年年均降低1.7%. 这与我国主要燃煤行业除尘、脱硫、脱硝等大气污染控制装置对重金属的协同脱除能力不断增强有密切关系.      

Mitigation and adaptation strategies for global change via the implementation of underground coal gasification

Coal is the most abundant hydrocarbon energy source in the world. It also produces a very high volume of greenhouse gases using the current production technology. It is more difficult to handle and transport than crude oil and natural gas. We face a challenge: how can we access this abundant resource and at the same time mitigate global environmental challenges, in particular, the production of carbon dioxide (CO₂)? The editors of this special edition journal consider the opportunity to increase the utilization of this globally abundant resource and recover it in an environmentally sustainable manner. Underground coal gasification (UCG) is the recovery of energy from coal by gasifying the coal underground. This  process produces a high calorific synthesis gas, which can be applied for electricity generation and/or the production of fuels and chemicals. The carbon dioxide emissions are relatively pure and the surface facilities are limited in their environmental footprint. Unused carbon is readily separated and can be geo-sequester in the resulting cavity. The cavity is also being considered as a potential option to mitigate against change impacts of other sources of carbon dioxide (CO₂) emissions. These outcomes mean there is an opportunity to provide developing and developed countries a source of low-cost clean energy. Further, the burning of coal in situ means that the traditional dangers of underground mining and extraction are reduced, a higher percentage of the coal is actually recovered and the resulting cavern creates the potential for a long-term storage solution of the gasification wastes. The process is not without challenges. Ground subsidence and groundwater pollution are two potential environmental impacts that need to be averted for this process to be acceptable. It is essential to advance the understanding of this practice and this special edition journal seeks to share the progress that scientists are making in this dynamic field. The technical challenges are being addressed by researchers around the world who work to resolve and understand how burning coal underground impacts the geology, the surface land, and ground water both in the short and the long term. This special issue reviews the process of UCG and considers the opportunities, challenges, risks, competitive analysis and synergies, commercial initiatives and a roadmap to solutions via the modelling and simulation of UCG. Building and then disseminating the fundamental knowledge of UCG will enhance policy development, best practices and processes that reflect the global desires for energy production with reduced environmental impact.     

Reaction rate constants in simulation of underground coal gasification using porous medium approach

Underground coal gasification (UCG) is an emerging energy technology for a cleaner type of coal extraction method. It avoids current coal mining challenges such as drastic changes to landscapes, high machinery costs, elevated risks to personnel, and post-extraction transport. UCG has a huge potential to provide a clean coal energy source by implementing carbon capture and storage techniques as part of the process. In order to support mitigation strategies for clean coal production and policy development, much research needs to be completed. One component of this information is the need to understand what happens when the coal burns and a subsurface cavity is formed. This paper looks at the efforts to enhance reliable prediction of the size and shape of the cavities. Reactions are one of the most important mechanisms that control the rate of the growth of the cavities. Therefore, modeling the reactions and precise prediction of reaction kinetics can influence the accuracy of a UCG process. The produced syngas composition during UCG is closely linked to the reactions that take place in this process, the permeability of the coal seam, and the temperature distribution. Since the combination of reactions can influence the distributions of the heat and gas components in the coal seam during UCG or even extinguish the combustion, accurate modeling of the reactions is crucial, particularly when all phenomena affecting the reaction rate are considered in a single set of kinetics. In this study, procedures are proposed to estimate the frequency factor and activation energy of the pyrolysis reaction using a single-step decomposition method, the kinetics of the endothermic direction of homogeneous reversible reactions, and the frequency factor of heterogeneous reactions from experiments or literature data. The estimated kinetics is more appropriate for simulation of the UCG process using the porous medium approach. Computer Modelling Group’s CMG-STARS (Steam, Thermal, and Advanced Processes Reservoir Simulator) software is used in this study.     

CaO对烟气中砷的形态和分布的影响

采用热力平衡分析方法研究了在一个大气压下，1300K-400K温度范围里痕量元素砷在煤燃烧过程的形态及分布以及添加剂CaO对砷的形态和分布的影响．为探讨规律，研究的系统只考虑煤中的主量元素和砷．分析结果表明，在煤燃烧和气化的高温区域里，大部分的砷元素蒸发以一氧化砷的形式存在于气相中，随着温度的降低，一氧化砷将发生化学反应生成固相As2O5和As2S2．CaO可以大大地增强砷元素的沉积趋势，烟气中CaO的含量越大，砷酸钙作为稳定相的温度范围越宽。     

On the mitigating environmental aspects of a vertical well in underground coal gasification method

Mitigation and Adaptation Strategies for Global Change - Underground coal gasification (UCG) is an energy production pathway in underground coal deposits with the potential advantage of decreasing...     

煤气化废水处理技术现状及发展趋势

介绍了国内煤气化企业在废水处理上的困境和煤气化废水的水质特点,从预处理、生化处理、深度处理三个方面总结了国内煤气化废水的研究和应用现状,分析了各处理技术对污染物的去除效果和潜在的应用问题,指出目前煤气化废水处理技术的研究大多局限于小型试验并且缺乏对耦合工艺的总体分析,认为物化技术与生化技术的优化组合是未来研究的主题。     

鲁奇煤气化工艺低温煤焦油的组成研究

利用液-液提取分离和制备液相色谱分离相结合的预分离程序、GC-MS结合保留指数的定性方法,分析研究了鲁奇煤气化工艺低温煤焦油的化学组成,推测鉴定出12大类共400余种化合物,并对其中脂肪烃、PAH、NPAH和酚类化合物进行了定量分析,讨论了鲁奇低温煤焦油的组成特点.