Uranium speciation in coal bottom ash investigated via X-ray absorption fine structure and X-ray photoelectron spectra

Similar to chromium contamination, the environmental contamination caused by uranium in radioactive coal bottom ash (CBA) is primarily dependent on the chemical speciation of uranium. However, the relationship between uranium speciation and environmental contamination has not been adequately studied. To determine the relationship between uranium speciation and environmental contamination, X-ray absorption fine structure (XAFS) and X-ray photoelectron spectra (XPS) analyses were performed to determine the uranium speciation in CBA exposed to different chemical environments and simulated natural environments. The leachability of the different forms of uranium in the CBA was studied via a simulated acid rain leaching experiment, and the results showed that 57.0% of the total uranium was leached out as U(VI). The results of a linear combination fit (LCF) of the X-ray absorption near edge structure (XANES) spectrum revealed that in the raw CBA, the uranium mainly occurred as U3O8 (71.8%). However, in the iron-rich particles, the uranium mainly occurred as UO2 (91.9%) after magnetic separation. Magnetite is a ubiquitous ferrous-bearing oxide, and it was effective for the sorption of U(IV). The result of FeSO4 leaching experiment indicated that 96.57% of total uranium was reduced from U(VI) to U(IV) when infiltrated with the FeSO4 solution for 6 months. This result clearly demonstrated the changes in chemical valence of uranium in the coal ash and provided a conceptual principle for preventing uranium migration from ash to the surrounding soil and plants.     

硅基多孔材料的表征及其对SO2的吸附性能

为增强火山灰反应的强度,提高对SO₂的脱除性能,以粉煤灰为原料采用两步水热合成法制备硅基多孔材料,并对制备的材料进行表征.结果表明:硅基多孔材料整体呈无序形态,主要成分为水化硅酸钙和CaCO₃,属于无定型的非晶相物质;由C、O、Si、Na、Ca等元素构成,主要以SiO₃2-、CO₃2-的形式存在;呈蜂窝和玻璃纤维的网状结构,内部空隙发达,比表面积较大,且存在有大量的吸附水和结合水.利用固定床反应器测定了硅基多孔材料对SO₂的吸附性能,在入口ρ（SO₂）为1 200 mg/m3、吸附温度为50℃、SO₂含氧量为9%、粒度为200目（0.075 mm）的条件下,SO₂的吸附量可达24.87 mg/g,脱硫率可达100%,与钙基吸附剂相比吸附量提高了74%;将吸附SO₂后的硅基多孔材料在700℃下焙烧3 h,可以继续吸附SO₂,重复使用率可达72.24%.由于SO₂在脱除过程中存在一定的化学反应,含氧量的增加能够提高其对SO₂的吸附量.研究显示,硅基多孔材料脱除SO₂的过程是由物理吸附和化学反应相结合的结果,其中由于制备的硅基多孔材料具有较大的比表面积和较为丰富的孔结构,有利于物理吸附;同时,在两步法制备硅基多孔材料的过程中使火山灰反应得到增强也同样提高了SO₂与硅基多孔材料的化学反应,进而增强了化学吸附的效果.      

助剂对医疗垃圾焚烧飞灰浸出液中重金属电渗析分离的影响

通过医疗垃圾焚烧飞灰电渗析实验,比较了去离子水及助剂柠檬酸铵(0.25 mol/L)/氨水(1.25%)、葡萄糖酸钠的添加对重金属移除的影响,并比较了电渗析处理前后重金属形态的改变。结果表明:2种助剂的添加明显提高了重金属的移除率,且柠檬酸铵/氨水的效果优于葡萄糖酸钠;以柠檬酸铵/氨水作为助剂时,Pb、Zn、Cd、Cu、Cr 5种重金属的移除率分别达到11.1%、42.3%、56.7%、38.7%、7.5%;除了Cu外,Pb、Zn、Cd和Cr等4种重金属大都以负价态向阴极侧迁移;在葡萄糖酸钠为助剂时,5种重金属的大部分则均迁移到阳极侧;在去离子水及柠檬酸铵/氨水、葡萄糖酸钠等助剂作用下,飞灰中Cl的移除率均达到97%左右;电渗析几乎全部移除了飞灰中可交换态的重金属,同时部分碳酸盐态重金属被移除,残灰中重金属的铁锰氧化态、有机络合态或残余态的比例明显升高。     

污泥包裹飞灰热解炭中重金属稳定性研究:铁盐添加剂的作用

在污泥包裹飞灰中添加不同比例的铁盐后进行热解,依据HJ/T 300—2007《固体废物浸出毒性浸出方法——醋酸缓冲溶液法》,研究了铁盐对污泥包裹飞灰热解炭中重金属的稳定效果,确定了基于热解炭最终处置目标的最经济的铁盐添加量和最大飞灰包裹量。结果表明:添加混合铁盐可以增加污泥包裹飞灰热解炭中重金属的稳定性,随着铁盐添加量增加,重金属的浸出浓度先减小后增加。综合经济性和稳定性,确定最适宜的铁盐添加量为1.5%。添加铁盐可增加污泥的飞灰包裹量,在Fe添加量为1.5%,热解温度500℃的条件下,污泥对飞灰的最大包裹量是1∶2,此条件下的产物热解炭可以进入生活垃圾填埋场处置。     

固定源飞灰中PCDD/Fs的时间变化特性分析

对河北省某生活垃圾焚烧厂(固定源)飞灰中二恶英(PCDD/Fs)含量随时间的变化特性进行了分析,并结合美国、欧盟和国内排放标准限值和3种常见垃圾(医疗垃圾、生活垃圾和工业危险废弃物)以及PCDDs/PCDFs比值,分析了焚烧飞灰中PCDD/Fs特征。结果表明:2014年10月—2015年11月PCDD/Fs的TEQ变化范围为0.00322~0.671μg I-TEQ/kg,同时O8CDD(5.020%~34.19%)、2,3,7,8-T4CDF(0.764%~9.696%)和1,2,3,7,8-P5CDF(0.273%~8.575%)均在PCDD/Fs浓度中占据主要贡献率,2,3,4,7,8-P5CDF(12.12%~68.53%)在PCDD/Fs毒性当量中占据主要贡献率,并且均低于美国、欧盟和国内排放标准限值,同时发现PCDDs/PCDFs TEQ比值与焚烧垃圾类型存在一定关系;本研究样品中PCDD/Fs的合成机理符合从头反应的理论。     

高铝粉煤灰脱硅反应工艺优化及机理探讨

为探究高铝粉煤灰脱硅最佳工艺条件及了解其脱硅过程物相转化机理,通过正交试验研究了w(NaOH)(10%~30%)、灰碱比(质量比,取1∶0.3~1∶2.0)、时间(1.0~4.0 h)和温度(90~150 ℃)对脱硅效率及铝硅比(质量比)的影响. 结果表明:w(NaOH)为20%、灰碱比为1∶0.5、反应时间为2.0 h、反应温度为120 ℃是粉煤灰脱硅反应的最佳条件;在最佳条件下铝硅比由原灰的1.23升至2.02以上,脱硅效率达38.6%.反应温度、灰碱比、碱液浓度、时间对脱硅率的影响依次减弱. 通过定量X射线衍射(XRD)分析了脱硅前后物相的变化,当温度高于120 ℃时,有大量方钠石形成,并且方钠石生成量(X)与铝硅比(Y)呈显著负相关,有Y=-0.012 8X+2.03 (R2=0.930,P<0.01). 由扫描电镜(SEM)对粉煤灰脱硅前后的表观形貌变化观察可知,粉煤灰在脱硅过程中非晶态SiO₂部分溶解,从而进一步证实了方钠石的生成是影响脱硅效率的关键因素.      

除尘器灰斗电加热器供配电节能降耗方案优化

对目前广泛使用的除尘器灰斗电加热器的供配电系统进行了分析,提出了电控设备投资更省、供配电系统运行更节能经济的优化方案,并通过工程实例进行了分析验证。     

H_4SiW_(12)O_(40)/TiO_2/空心微珠光催化降解联苯胺

采用复合型光催化剂H_4SiW_(12)O_(40)/TiO_2/空心微珠(cenospheres)光催化降解联苯胺,考察了联苯胺降解效果的影响因素,并运用FTIR和GS-MS技术分析了联苯胺光催化降解过程的主要中间产物,探讨了联苯胺可能的降解路径。实验结果表明:以125 W中压汞灯为光源,在溶液pH为6.3,初始联苯胺质量浓度为10 mg/L的条件下光反应240 min,联苯胺降解率达78%,比Ti_O2/空心微珠提高了24百分点;H_4SiW_(12)O_(40)/TiO_2/空心微珠光催化降解联苯胺符合表观一级动力学特征,且反应速率常数随初始联苯胺质量浓度的增加而减小;H_4SiW_(12)O_(40)/TiO_2/空心微珠具有较好的稳定性,易于分离,可重复利用;联苯胺光催化降解过程的主要中间产物为4-氨基联苯、4-氨基苯酚、对苯二酚和1,4-苯醌。     

生活垃圾焚烧飞灰中重金属浸出影响研究

通过浸出液pH测定、全量测定以及(HJ/T 299-2007)硫酸硝酸法和(HJ/T 300-2007)醋酸缓冲溶液法浸提,对生活垃圾焚烧飞灰中重金属浸出特性进行了实验研究.结果表明浸出pH条件、飞灰中重金属含量以及重金属分布形态是影响浸出浓度的主要因素.相比于硫酸硝酸法,醋酸缓冲溶液法重金属提取效率明显较高,尤其是铜锌镉铬.垃圾焚烧飞灰潜在环境风险较大,在填埋处理及综合利用时应充分考虑其浸出特性.     

Valuable utilisation of spray dryer ash and its performance in structural concrete

This paper focuses on the valuable utilisation of spray dryer ash (SDA) and investigates its performance in concrete for structural applications. Based on the challenges associated with the disposal of coal combustion products (including SDA) and the economic costs linked to cement production, this research seeks to provide an environmentally friendly and more cost-effective concrete product by utilising SDA in partial replacement of cement in concrete. With the exception of a relatively high-sulphur content, SDA exhibits very useful properties that are closely related to Class C fly ash and Portland cement.

Experimental tests were carried out to determine the effect of SDA replacement of Portland cement (ranging from 0 to 50% replacement) on the compressive strength, bond strength, freeze-thaw performance and corrosion resistance of concrete. The addition of SDA in non-air entrained concrete provided a general increase in its strength with optimal limits ranging between 25 and 35% replacement. The addition of SDA produced a negligible effect on the freeze-thaw durability of the concrete (air entrained). Results for corrosion performance were not as definitive, but indicate that the use of SDA does not significantly change the likelihood of reinforcing bar corrosion.