甲烷13C同位素比值表征温度对甲烷生成途径的影响

采用测试气相碳同位素比值的方法比较了中温厌氧降解和高温厌氧降解过程中甲烷（CH₄）生成途径的差异,表征了生活垃圾厌氧消化过程CH₄生成途径的演变,并结合气液相化学组分和产甲烷菌荧光原位杂交（FISH）分析对同位素表征结果进行了验证.中温（35℃）条件下,垃圾降解初期甲烷¹³C同位素比值（δ¹³CH₄）下降至-69.5‰,表明此阶段CH₄主要产生自CO₂还原途径;随着垃圾降解进入快速产CH₄阶段,δ¹³CH₄值相应迅速上升至-23.8‰,说明乙酸发酵逐渐成为CH₄生成的主要途径,FISH实验结果也发现此阶段以乙酸发酵型产甲烷菌Methanosarcinaceae为主;当产CH₄速率逐渐减小进入稳定期时,δ¹³CH₄值迅速降低至-55‰后相对稳定,说明乙酸发酵途径的比例减小,并且维持在较稳定的水平.高温（55℃）条件下,δ¹³CH₄值始终维持在约-70‰,表明甲烷主要由CO₂还原作用生成,在快速产CH₄阶段,乙酸氧化和CO₂还原作用是CH₄生成的重要途径.     

Methane dehydroaromatization over Mo-modified H-MFI for gas to liquid catalysts

For direct gas to liquid (GTL),a novel process producing energy sources for methane dehydroaromatization is needed.Supporting MoO3 on H-MFI zeolite shows the high catalytic capacity and a selective activity for dehydroaromatization of methane to benzene at 973 K in a fixed bed reactor.On the other hand,deactivation by coke on the active sites in all the catalysts is formed during the reaction.H2 co-feed suppressed the deactivation,which is probably due to the decrease in coking amount.Mo K-edge X-ray absorption fine structure (XAFS) results showed the formation of dispersed Mo2C species with low crystallinity after dehydroaromatization.Mo L-edge XANES (X-ray absorption near-edge structure) indicated the formation of active Mo species including Mo2C and Mo-oxycarbide (MoOxCy),where the red-ox state should be independent in the absence/presence of H2.It is concluded that Mo-oxycarbide species act as highly active species,and their stability affected the durable activity in the presence of H2.     

水热处理泔脚脱油与产物消化性能变化

水热预处理泔脚废物,测定生物化学甲烷势(BMP),研究废物脱油、水解和消化性能的变化.结果表明,预处理加速废物的溶解和有机物的水解.随着反应温度升高,产物pH 降低,SCOD 和VFA浓度显著升高.150℃、 60 min预处理后,可浮油含量增加并达到较好的分离效果,消化过程在4～6 d内完成,降解速率提高1倍.170℃预处理后4 d生物气产量最高,继续提高温度会降低产物甲烷势.能量衡算分析表明,优化预处理能耗合理.     

含水率对生活垃圾甲烷化过程的影响

采用批式实验,通过分析产气量和气、液相组成的变化,比较了含水率分别在35%、65%～70%（田间持水率）、 80%和>95%（饱和含水率）的条件下,不同食物类废物和纤维素类废物含量的典型法国生活垃圾和中国生活垃圾以及纤维素类废物厌氧产甲烷过程的差异.结果表明,对于含易腐有机物的生活垃圾,提高含水率能够削弱VFA等中间产物对水解酸化和甲烷化的抑制作用：典型法国生活垃圾大量产甲烷所需的含水率不应低于80%,而有机物含量更高的典型中国生活垃圾直至含水率达到96%时,反应体系内快速产甲烷过程才能得以进行;同时,提高生活垃圾的含水率也有利于加速其厌氧产甲烷过程和提高甲烷的最终产量,含水率>95%的法国生活垃圾反应体系的最终甲烷产量是含水率为80%时产量的1.6倍.而对于纤维素类废物,提高含水率则能改善水分在水解和酸化过程中的可获得性,从而增大甲烷化的底物可获得量,含水率>95%的纤维素类废物反应体系的甲烷最终产量是含水率为65%时产量的3.8倍.     

污水厂出水DOM的分级及三卤甲烷生成势研究

研究目的在于调查寒冷季节城市污水处理厂出水中天然有机物化学组分分级,探讨各分级组分与消毒副产物生成潜能间之关系。采集污水厂二级出水,以三种不同树脂把污水厂出水中有机物分离成六类不同组分,其中A水厂含量最高的物质为亲水酸性物质(33%)而B水厂的疏水性中性物质含量最多约占总有机物的64%。从总体来看两水厂的疏水性物质含量大于亲水性物质含量,疏水性物质的三卤甲烷生成势也较大,是水体中消毒副产物的主要前驱物质。疏水性有机物质较多,代表受生活污水污染严重,得知该城市污水主要受民生污染较多。     

NH3/CH4混合气体爆炸极限试验研究及动力学分析

为了预防化工场所合成氨工艺中混合气体爆炸事故,利用爆炸极限测试仪和CHEMKIN软件,研究了 NH3和CH4混合气体的爆炸极限和动力学过程.通过分析NH3和CH4混合气体的爆炸极限和爆炸传播火焰特征,以及爆炸过程中温度、压力和关键自由基·H和·OH的变化规律,探讨了不同体积分数的NH3对CH4爆炸极限的影响.结果表明:NH3的存在使混合气体的爆炸下限上升,在某种程度上抑制了 CH4爆炸,且体积分数越大,抑制作用越明显;爆炸下限时的火焰经历了半圆形向指尖形的转变,NH3体积分数越大,爆炸火焰颜色越亮;NH3主要通过影响CH4爆炸链式反应的关键自由基·H和·OH来抑制CH4爆炸.所得结论为有效预防NH3/CH4混合爆炸事故提供了理论依据.     

节水灌溉模式对稻田CH4排放规律的影响

基于水稻节水灌溉技术和密闭静态箱技术田间原位采集甲烷气样,试验研究了水稻节水控制灌溉模式对稻田CH₄排放规律的影响.结果表明,控制灌溉稻田CH₄排放呈现明显的下午极大值型日变化,CH₄排放高峰主要出现在下午13:00,淹水处理CH₄排放峰值在1 d中各个时刻的出现具有一定的随机性.控制灌溉稻田CH₄排放呈现明显的单峰型季节排放规律,排放高峰发生在分蘖前期,比淹水处理提前了10 d.所以,控制灌溉模式在水稻返青期后的水分调控及生产性用水等水管理措施对稻田CH₄排放的影响至关重要.控制灌溉水稻全生育期的稻田CH₄排放总量为24.46 g·m^-2,比淹水稻田减少了39%,平均排放率为7.96 mg·(m²·h)^-1,但返青期和分蘖前期的CH₄平均排放率比淹水稻田高,在以后的各个生育阶段均低于淹水稻田.     

呼吸型填埋场覆盖层技术研究Ⅰ：热动力自充氧装置构建

填埋场最终覆盖层（以下简称＂覆盖层＂）中的氧气含量是影响甲烷氧化效果的重要因素.本研究基于空气热力学原理提出了一种呼吸型覆盖层技术,构建了利用垃圾堆体与外界环境的温差而实现覆盖层自充氧的热动力自充氧装置,并优化了其空气/氧气充气效率.结果表明,导气管路内空气流速（v）与温差（ΔT）呈线性关系（v=0.0281ΔT-0....     

Seasonal variation effects on the formation of trihalomethane during chlorination of water from Yangtze River and associated cancer risk assessment

For the system of water samples collected from Yangtze River,the effects of seasonal variation and Fe(III) concentrations on the formation and distribution of trihalomethanes (THMs) during chlorination have been investigated.The corresponding lifetime cancer risk of the formed THMs to human beings was estimated using the parameters and procedure issued by the US EPA.The results indicated that the average concentration of THMs (100.81 μg/L) in spring was significantly higher than that in other seasons,which ...     

Emissions of C2 – C12 hydrocarbons in the Hsuehshan tunnel, Taiwan

The concentrations of 56 hydrocarbons from C2 to C12 were measured simultaneously in the southbound bore, the northbound bore and the exhaust air shafts of the Hsuehshan tunnel near Yilan, Taiwan for 12 days during 2007 and 2008. A total of 60 integrated air samples were collected using stainless steel canisters and analyzed using GC/FID and GC/MS. The five most abundant species in all samples were ethylene, acetylene, isopentane, propylene and toluene. The exit/entrance ratios of total non-methane hydrocarbons (NMHC) concentration were 7.8 and 4.8 for the southbound and northbound bores, respectively. Furthermore, the exhaust from the vertical shafts affects air quality in the neighborhood. The most abundant species of emission rate (ER) was toluene (21.93–42.89 mg/sec), followed by isopentane, ethylene, propylene and 1-butene, with ER ranging from 2.50 to 9.31 mg/sec. The species in the three exhaust air shafts showed that the reactivities of these emissions are similar to those of vehicle emissions. Notably, the control of emissions in the vertical shafts of the vehicle tunnel will be important in the future.