Simulation of the Effect of an Increase in Methane on Air Temperature

The infrared radiative effect of methane was analyzed using the 2D, interactive chemical dynamical radiative SOCRATES model of the National Center for Atmospheric Research. Then, a sensitivity experi ment, with the methane volume mixing ratio increased by 10%, was carried out to study the influence of an increase of methane on air temperature. The results showed that methane has a heating effect through the infrared radiative process in the troposphere and a cooling effect in the stratosphere. However, the cooling effect of the methane is much smaller than that of water vapor in the stratosphere and is negligible in the mesosphere. The simulation results also showed that when methane concentration is increased by 10%, the air temperature lowers in the stratosphere and mesosphere and increases in the troposphere. The cooling can reach 0.2 K at the stratopause and can vary from 0.2-0.4 K in the mesosphere, and the temperature rise varies by around 0.001-0.002 K in the troposphere. The cooling results from the increase of the infrared radiative cooling rate caused by increased water vapor and O3 concentration, which are stimulated by the increase in methane in most of the stratosphere. The infrared radiation cooling of methane itself is minor. The depletion of O3 stimulated by the methane increase results indirectly in a decrease in the rate of so- lar radiation heating, producing cooling in the stratopause and mesosphere. The tropospheric warming is mainly caused by the increase of methane, which produces infrared radiative heating. The increase in H2O and O3 caused by the methane increase also contributes to a rise in temperature in the troposphere.

A numerical simulation study on active species production in dense methane-air plasma discharge

Recently, low-temperature atmospheric pressure plasmas have been proposed as a potential type of ＇reaction cartier＇ for the conversion of methane into value-added chemicals. In this paper, the multi-physics field coupling software of COMSOL is used to simulate the detailed discharge characteristics of atmospheric pressure methane-air plasma. A two-dimensional axisymmetric fluid model is constructed, in which 77 plasma chemical reactions and 32 different species are taken into account. The spatial density distributions of dominant charged ions and reactive radical species, such as ＋ ＋ ＋ ＋ CH4, CH3,N2,02, H, O, CH3, and CH2, are presented, which is due to plasma chemical reactions of methane/air dissociation （or ionization） and reforming of small fragment radical species. The physicochemical mechanisms of methane dissociation and radical species recombination are also discussed and analyzed.

Comparison on Determination Results of Methane and Total Hydrocarbons by Glass Syringe Method and Air Bag Method

Samples at different setting time were determined by glass syringe method and air bag method, and their results were analyzed. The results showed that concentrations of methane and total hydrocarbons obviously declined with the prolonging of setting time by glass syringe method, and recovery rate of sample declined to 60% after 8 h. In air bag method, analysis results of methane and total hydrocarbons were stabler, and recovery rate of sample was 93% after 8 h.

Experimental investigation on microstructure behavior of premixed methane-air flame-flow interaction in a semi-vented chamber

To explore the premixed methane-air flame microstructure behavior and the flame-flow interaction, the premixed methane/air flame was studied in a semi-vented chamber. A high speed camera and schlieren images methods were used to record the processes of interaction between rare- faction wave and flame. Meanwhile, a pressure sensor was utilized to catch the pressure variation in the process of flame propagation. The experiment results showed that the interference of rarefaction wave on flame caused the flame front structure change, which led to the flame transition from lami- nar to turbulent quickly. The rarefaction wave intervened in the flame by turning the flame front sur- face into dentiform structure. The violent turbulent combustion began to appear in part of the flame front and spreaded to the whole flame front surface. The rarefaction also decreased the flame propa- gation speed.

Laminar Diffusion Flames of Methane in a Co-annular Jet of Oxygen-Enriched Air

Oxygen rich combustion is a mean to increase the energy efficiency and to contribute to CO2 capture. Influence of oxygen enriched air on the stability of methane flames from non premixed laminar jets has been investigated experimentally. The burner consists of two coaxial jets： methane flowing out of the inner, oxidizer from the outer. The flame behavior is studied according to the proportion of oxygen in the oxidizer jet, the oxidizer and the methane jets velocities. The flame is either anchored to the burner, lifted, stationary or not or blown-out. The addition of oxygen produces a decrease of the lift height, a reduction of the length of the reaction zone and an increase in the soot emission. These results have been reported into diagrams of stability where the flame configurations are connected to the competition between the dynamic effect of the injection velocity and the chemical effect of oxygen addition.

Modeling Methane Emissions from Paddy Rice Fields under Elevated Atmospheric Carbon Dioxide Conditions

Abstract Methane （CH4） emissions from paddy rice fields substantially contribute to the dramatic increase of this greenhouse gas in the atmosphere. Due to great concern about climate change, it is necessary to predict the effects of the dramatic increase in atmospheric carbon dioxide （CO2） on CH4 emissions from paddy rice fields. CH4MOD 1.0 is the most widely validated model for simulating CH4 emissions from paddy rice fields exposed to ambient CO2 （hereinafter referred to as aCO2）. We upgraded the model to CH4MOD 2.0 by： （a） modifying the description of the influences of soil Eh and the water regime on CH4 production; （b） adding new features to reflect the regulatory effects of atmospheric CO2 upon methanogenic substrates, soil Eh during drainages, and vascular CH4 transport; and （c） adding a new feature to simulate the influences of nitrogen （N） addition rates on methanogenic substrates under elevated CO2 （hereinafter referred to as eCO2） condition. Validation with 109 observation cases under aC02 condition showed that CHaMOD 2.0 possessed a minor systematic bias in the prediction of seasonally accumulated methane emissions （SAM）. Validation with observations in free-air CO2 enrichment （FACE） experiments in temperate and subtropical climates showed that CH4MOD 2.0 successfully simulated the effects of eCO2 upon SAM from paddy rice fields incorporated with various levels of previous crop residues and/or N fertilizer. Our results imply that CH4MOD 2.0 provides a potential approach for estimating of the effects of elevated atmospheric CO2 upon CHa emissions from regional or global paddy rice fields with various management practices in a changing climate.

Atmospheric Methane over the Past 2000 Years from a Sub-tropical Ice Core, Central Himalayas

A high-resolution 2ooo-year methane record has been constructed from an ice core recovered at 7200 m a.s.1, on the Dasuopu Glacier in the central Himalayas. This sub-tropical methane record reveals an increasing trend in the concentration of methane during the industrial era that is similar to observations from polar regions. However, we also observed the differences in the atmospheric methane mixing ratio between this monsoon record and those from polar regions during pre-industrial times. In the time interval o N 1850 A.D., the average methane concentration in the Dasuopu ice core was 782±40 ppbv and the maximum temporal variation exceeded 200 ppbv. The difference gradient of methane concentration in Dasuopu ice core with Greenland and Antarctica cores are 66±40 ppbv and 107±40 ppbv, respectively. This suggests that the tropical latitudes might have acted as a major global methane source in preindustrial times. In addition, the temporal fluctuation of the pre-industrial methane records suggests that monsoon evolution incorporated with high methane emission from south Asia might be responsible for the relatively high methane concentration observed in the Dasuopu ice core around A.D. 800 and A.D. 1600. These results provide a rough understanding of the contribution of tropical methane source to the global methane budget and also the relationship betweenatmospheric methane and climate change.

RANS Simulation of Methane Diffusion Flame： Comparison of Two Chemical Kinetics Mechanisms

Turbulent non-premixed combustion of gaseous fuels is of importance for many technical applications, especially for the steel and refractory industry. Accurate turbulent flow and temperature fields are of major importance in order to predict details on the concentration fields. The performances of the GRI-Mech 3.0 and the Jones and Lindstedt mechanisms are compared. Detailed chemistry is included with the GRI-Mech 3.0 and J-L kinetic mechanisms in combination with the laminar flamelet combustion model. The combustion system selected for this comparison is a confined non-premixed methane flame surrounded by co-flowing air The simulation results are compared with experimental data of Lewis and Smoot （2001）.

LaMnO_(3)(La_(0.8)Sr_(0.2)MnO_(3))Perovskites for Lean Methane Combustion:Effect of Synthesis Method

The effect of the preparation method on the properties of LaMnO3 and La0.8Sr0.2MnO3 perovskite was studied. Materials were prepared by four methods: sol-gel, chemical combustion, solvothermal and spray pyrolysis and characterized. The effect of the synthesis method on the texture, acid-base character of the surface, reducibility with hydrogen, oxygen desorption, surface composition and catalytic activity for combustion of lean methane was studied. It was found that synthesis method affects physicochemical properties of obtained materials-solvothermally produced materials exhibit well-developed surface area, presence of reactive oxygen species on surface and high catalytic activity for CH4 combustion. Generally, LaMnO3 and La0.8Sr0.2MnO3 perovskites show catalytic activity for lean CH4 combustion comparable or higher than the activity of 0.5 wt.% Pt/Al2O3 but lower than 1 wt.% Pd/Al2O3.

2022年8月北黄海北部溶解甲烷分布、海-气交换通量及影响因素

科学评估陆架边缘海溶解甲烷(CH_(4))的分布及海-气交换通量对于认识陆架边缘海CH_(4)的释放对大气CH_(4)的区域性贡献具有重要意义。基于2022年8月的现场调查数据和资料,研究北黄海北部海水溶解CH_(4)的分布、海-气交换通量及影响因素。结果表明:研究海域溶解CH_(4)浓度为4.0~63.3 nmol/L,饱和度为168%~2 360%,高值区位于鸭绿江口附近海域,随着离岸距离的增加表层海水溶解CH_(4)浓度迅速降低。鸭绿江等陆源冲淡水的输入耦合海水及沉积物有机质的降解致使近岸海域海水CH_(4)升高;陆源冲淡水与海水混合过程中海水CH_(4)的氧化消耗也是控制CH_(4)浓度和分布不容忽视的重要过程。离岸海域海水及沉积物有机质厌氧降解耦合黄海冷水团的作用使得底层海水溶解CH_(4)浓度高于表层海水。研究海域海-气CH_(4)交换通量为18.4~578.8μmol/(m^(2)·d),是大气CH_(4)的源;鸭绿江口附近海域海-气CH_(4)交换通量高于离岸海域。由此可见,受陆源冲淡水输入的影响研究海域溶解CH_(4)浓度和海-气交换通量具有显著的区域性差异,且变幅高于世界其他海域;加强河口以及近海调查研究对于准确评估陆架边缘海CH_(4)的排放,明确CH_(4)排放源项的构成及制定CH_(4)减排的有效措施至关重要。

甲烷-空气预混区外含钾细水雾抑爆特性研究

为了解含钾细水雾在综合管廊燃气泄漏场景下的抑爆能力,采用自制的爆炸试验系统,开展含添加剂细水雾位于甲烷-空气爆炸区域外的抑爆试验,分析纯水及草酸钾、碳酸钾、氯化钾3种含钾化合物细水雾对9.5%甲烷-空气爆炸超压与过火范围的影响。研究结果表明:纯水细水雾的临界抑爆雾化质量浓度区间为320~480 g/m^(3);含草酸钾条件下超压下降率随质量分数增加呈现正态累积分布函数(NormalCDF)变化,最佳抑爆质量分数为10%;当雾化质量浓度为480 g/m^(3)、雾滴D32为61.7μm、化合物质量分数为10%时,对应抑爆能力均大于纯水细水雾条件,其中,含草酸钾抑爆能力最强,其次为碳酸钾与氯化钾,峰值超压下降率较纯水细水雾条件分别提高2.32、1.88与1.53倍,过火范围分别缩减46.7%、40%与13.3%。相较于碳酸钾与氯化钾条件,爆炸气体预混区域外含草酸钾细水雾能够吸收更多的爆炸热量、消耗更多的活性自由基。

环境空气监测用氮中甲烷气体标准物质质量评估

为了解和掌握当前环境空气非甲烷总烃监测所使用的氮中甲烷气体标准物质的质量状况,通过对全国范围内开展环境空气非甲烷总烃监测的实验室中的99家进行使用情况调查,发现共涉及35家制造商。选择其中使用占比较高的10家,另外再随机选取6家,通过匿名采购等方式获取31瓶氮中甲烷气体标准物质。经两家测试单位分别测试后,采用归一化偏差(E_(n))法和相对偏差法两种方法评价所选标准物质的量值准确性和监测适用性,同时依照相关国家计量技术规范评估其证书完整性和规范性。结果显示,两种方法的评价结果一致。16家制造商中,14家的27瓶气体标准物质定值准确,2家的4瓶气体标准物质定值不准确;9家证书相对完整、规范,其余7家普遍存在缺少标准物质唯一标识等问题,部分制造商甚至存在涉嫌冒用证书、证书中的定值浓度超出认定范围等问题。鉴于氮中甲烷气体标准物质是保障非甲烷总烃监测结果准确性、可比性和可溯源性的重要基础,且制造商数量众多,建议使用者加强标准物质质量评估工作,并审查其所附证书的规范性。

燃煤锅炉燃烧利用矿井乏风甲烷改造经济性及运行影响分析

为处理矿井大流量乏风中的超低浓度甲烷,拟采用将乏风作为锅炉二次风进行处理利用。对此类工程改造的锅炉引风、投资运行成本、项目改造收益、锅炉效率影响进行了分析。结果表明,矿井乏风甲烷利用工程改造减小了原来锅炉烟气的产生量,且烟气量改变很小,无需对锅炉侧进行改造。管道及保温材料的采购与安装是此类改造工程的主要投资部分。该类项目的主要收益为乏风处理的碳汇补贴收益。乏风流速越低,工程投资成本变高,但运行成本变低,有助于项目的长周期盈利。绘制了不同输运长度下乏风总量与瓦斯绝对涌出量的20年期盈利平衡曲线。提出了优化矿井侧及二次风侧的乏风输送系统,并对乏风温度、湿度等因素对锅炉效率的影响进行了分析。对矿井乏风利用项目的立项及可行性分析提供了指导。

AIRS反演青藏高原对流层大气甲烷分布特征

利用AIRS反演结果与瓦里关大气本底站甲烷浓度观测资料进行了对比分析,并对2003~2015年青藏高原对流层大气甲烷浓度的分布变化特征进行研究分析.结果表明:AIRS反演资料与瓦里关观测资料具有一致的月、年、季度变化趋势和分段变化特征.青藏高原甲烷浓度沿羌塘高原东缘——三江源西北地区一线,东南高、西北低,随高度上升呈现显著降低趋势,高原中部偏南地区甲烷浓度变率最大且异常敏感.2003~2015年青藏高原甲烷浓度持续上升,秋季最快、冬季最慢,年增长速度为5.2nmol/(mol?a),2013~2015期间小于全球增速;季节变化为典型单峰分布,夏季最高,春季最低,随着高度上升季节变化更为明显.

煤层气和压缩空气储能复合的矿区综合能源系统优化运行模型

由于缺乏有效的回收工序和利用手段,矿区大部分低浓度煤层气被直接排空,造成严重资源浪费和温室效应。同时,间歇随机波动的可再生能源渗透率增加导致电力系统安全经济运行面临严峻挑战。该文集矿区低浓度煤层气资源和压缩空气储能优势于一体,提出煤层气和压缩空气储能复合的矿区型综合能源系统结构。采用变压吸附工艺提纯低浓度煤层气资源,回收提纯过程具有余压的废气资源作为压缩空气储能进气源。利用地下废弃矿道分别作为压缩空气储气库和煤层气储气库,形成余压利用型压缩空气储能系统。利用储能压缩热和煤层气发电余热资源,通过矿区热、电、储联合运行方式与可再生能源互补调节。基于该结构建立系统模型,以系统运行成本、风电消纳和碳排放为目标建立多目标优化模型。通过算例将是否考虑变压吸附的矿区综合能源系统进行对比,结果表明,所提出的系统具有良好的经济性、风电消纳能力和减碳能力。

两型甲烷/空气燃气发生器设计与仿真研究

飞行器热喷流干扰风洞试验需研制稳定可靠工作的甲烷/空气燃气发生器为其提供高温燃气。对燃气发生器进行结构设计,采用同轴直流式和同轴离心预混式两种喷注器结构,并利用数值模拟方法获得其稳态燃烧场,考察两种类型甲烷/空气火炬点火器的燃烧性能和燃烧室热载。结果表明,两种喷注结构条件的火炬点火器均可以满足设计要求,但同轴直流喷注方式燃烧性能表现更好,采用同轴直流式喷注方式比预混喷注方式的燃气温度及组分均匀度更高。

罐采样—转移气袋进样—气相色谱法测定环境空气中非甲烷总烃

建立罐采样—转移气袋进样—气相色谱法测定环境空气中非甲烷总烃的方法。通过校准曲线、空白实验、检出限、样品稳定性实验、正确度和精密度的验证,该方法校准曲线的相关系数大于0.999 4,检出限为0.04 mg/m^(3),低、中、高浓度标准气体的测定结果相对误差不大于4.00%,相对标准偏差不大于4.00%。该方法具有检出限低、准确度好等优点,经实际样品检测分析后表明该方法完全适用于环境空气中非甲烷总烃的测定。

密闭管道内非连续分布甲烷/空气爆炸特性

在长度900 mm、截面为100 mm×100 mm的矩形密闭管道内开展预混气体非连续分布对甲烷/空气爆炸影响的试验研究。通过分段通入甲烷体积分数为9.5%的预混气体,形成甲烷/空气-空气和甲烷/空气-空气-甲烷/空气两种非连续分布模式。研究发现,随着空气区域缩短,火焰传播距离、火焰尖端速度和爆炸超压均增大。特别是在甲烷/空气-空气-甲烷/空气分布中,当中间空气区域小于500 mm时,火焰会穿越并引发二次爆炸,且其超压随空气区域减小而增加。研究结果可为天然气爆炸事故防控提供理论支持。

煤矿乏风中超低浓度甲烷燃烧特性研究及机理敏感性分析

在国家“双碳”目标背景下,煤矿风排瓦斯中甲烷的减排日益重要;乏风氧化燃烧技术是目前乏风中甲烷减排利用的一个重要方向。基于甲烷燃烧详细化学动力学机理GRI-MECH 3.0,针对乏风瓦斯的气氛特点,开展了着火点、绝热火焰温度、点火延迟时间等燃烧特性的研究;基于敏感性分析方法,得到对反应温度有重要影响的基元反应过程。研究表明:乏风瓦斯着火点和甲烷浓度、停留时间有关,当乏风甲烷浓度小于等于0.4%时,着火点快速升高,大于0.4%时着火点变化不大;气体停留时间越长,乏风着火点越低,当停留时间是1 s时,常规乏风瓦斯的自燃温度在680℃~800℃。乏风瓦斯的最高火焰温度和甲烷浓度呈线性递增关系,在起始着火温度基础上,甲烷浓度每升高0.1%,火焰温度升高约23℃。900℃条件下不同浓度乏风瓦斯点火延迟时间几乎相同,但完全反应时间却随着浓度增加而缩短。表观气速对乏风中甲烷的转化率影响较为显著,700℃引燃温度条件下0.5%CH4的乏风进气流速需控制在1.31 m/s以内。最后基于温度敏感性,探讨了关键的基元反应。

青藏高原东北部更尕海7—9月水-气界面CH_(4)、N_(2)O交换通量变化及其影响因素

为了解青藏高原浅水草型湖泊水-气界面CH_(4)与N_(2)O通量的交换机制,以青藏高原东北部的更尕海为例,分别在2021年7月、8月、9月采用漂浮静态箱-气相色谱仪法对其水-气界面CH_(4)、N_(2)O交换通量进行连续、定点观测,并结合流域气象、湖泊水环境探讨其影响因素。结果表明:(1)更尕海水-气界面CH_(4)交换通量平均值为0.557 mg(/m^(2)·h),整体表现为源;N_(2)O交换通量平均值为-0.100μg(/m^(2)·h),整体表现为弱汇。(2)在空间上,受水生植物分布差异影响,更尕海黄苔分布区为水-气界面CH_(4)排放的热点区域,其次为狐尾藻分布区,无植被分布区最低。N_(2)O交换通量的变化受污染负荷的影响,粪便排放区是N_(2)O排放的热点区域。(3)在时间上,CH_(4)交换通量的变化则受温度影响,CH_(4)排放峰值主要出现于15:00时;N_(2)O交换通量的变化与沉水植物的光合作用有关。沉水植物光合作用向水体释放O_(2)并使pH升高,从而抑制了沉积物中的反硝化作用与微生物活性,使得湖泊整体表现为N_(2)O的“汇”。(4)相较于中国东部湖泊,青藏高原气压低,使得水体DO含量相对较低,减弱了水体对CH_(4)的氧化作用,还降低了水体中CH_(4)的溶解度,导致青藏高原湖泊CH_(4)排放通量显著高于中国东部湖泊。而青藏高原湖泊受人类活动的干扰较小,外源性污染较轻,造成该区域N_(2)O排放通量显著低于中国东部湖泊。