Techno-economic-environmental evaluation of a combined tri and dry reforming of methane for methanol synthesis with a high efficiency CO2 utilization

Production of methanol, as a green energy, from syngas is coming into focus. However, natural gas based methanol plants, which are used steam reforming of methane for syngas production, have a high CO₂ emission resulting in the global warming. In this study, a novel process for methanol synthesis is proposed to reduce CO₂ emission. In this regard, natural gas and flue gas are fed to a parallel-series system with tri and dry reforming of methane for syngas production with the optimized stoichiometric number. Then, the produced syngas is converted to methanol in a reactor. Finally, the produced methanol is purified by two distillation towers. The proposed method is compared to a referenced method in the view of technological, economic and environmental metrics. The techno-economic-environmental analysis of the processes reveals that not only the proposed method, as compared to the referenced one, increases CO₂ conversion from 20.93% to 99.22%, but also it is more economical and environmentally friendly. In addition, the global warming potential of the proposed method is almost 60% lower than that for the referenced method due to the lower CO₂ emission. Therefore, the proposed method can save above MUS$ 8 a year by CO₂ capture.     

Effect of nitrogen on deflagration characteristics of hydrogen / methane mixture

In order to study the influence of nitrogen on the deflagration characteristics of premixed hydrogen/methane, the explosion parameters of premixed hydrogen/methane within various volume ratios and different dilution ratios were studied by using a spherical flame method at room temperature and pressure. The results are as follows: The addition of nitrogen makes the upper limit of explosion of hydrogen/methane premixed gas drop, and the lower limit rises. For explosion hazard (F-number), hydrogen/methane premixed fuel with a hydrogen addition ratio of 10% has the lowest risk, and nitrogen has a greater impact on the dangerous degree of hydrogen and methane premixed gas whose hydrogen addition ratio does not exceed 30%. In terms of flame structure, the spherical flame was affected by buoyancy instability as the percentage of nitrogen dilution increased, but the buoyancy instability gradually decreased as the percentage of hydrogen addition increased. The addition of diluent gas reduces the spreading speed of the stretching flame and reduces the stretching rate in the initial stage of flame development. The laminar flame propagation velocity calculated by the experiment in this paper is consistent with the laminar flow velocity of the hydrogen/methane premixed gas calculated by GRI Mech 3.0. Considering the explosion parameters such as flammability limit, laminar combustion rate and deflagration index, when hydrogen is added to 70%, it is the turning point of hydrogen/methane premixed fuel.     

沁水盆地赵庄矿3号煤层地面煤层气抽采低产原因分析

在对沁水盆地赵庄矿煤层气开发地质、煤层气生产井资料深入研究的基础上，分析、总结了区内煤层气直井低产原因，并据此提出了区内地面抽采后续开发方向。研究认为:3号煤层气含量偏低、含气饱和度低、临储比低，致使排采阶段气含量可降幅度低，是其低产的宏观表征；3号煤储层不匹配孔级，较差连通性，即微、小孔为主，中孔次之，大孔不发育，微裂隙连通性差，致使扩散缓慢、影响储层改造和抽采效果，是其低产的微观表征；3号煤层远高于顶底板塑性及相近的水平应力，进一步造成改造缝长受限，泄流面积不足。因此，建议区内后续地面抽采方式应以增大泄流面积开发方式为主。     

四台矿均压硐室的优化与研究

四台矿属于近距离容易自燃煤层开采,综采工作面采用均压通风系统。在进风顺槽中布置的本巷均压硐室,风机吸风口距离均压风门近,吸风风流经过带式输送机,往往会造成均压风门漏风严重,均压硐室周围温度较高、煤尘较大。据此四台矿优化均压硐室布置方式,采用独立均压硐室代替先前的本巷均压硐室。对优化前后的数据进行研究分析,得出独立均压硐室的应用在减少风门漏风量,降低温度,抑制煤尘方面均有很大改善,实践证明了采用独立均压硐室的可行性及优点。     

Thermal management and catalytic combustion stability characteristics of premixed methane/air in heat recirculation meso‐combustors

In order to illuminate heat recirculation effect on catalytic combustion stability and further improve energy conversion efficiency in meso‐combustor, the catalytic combustion characteristics of the combustor with/without preheating channels are numerically studied at steady conditions. It is found that methane conversion rate and combustion efficiency increases by 2% to 3% and approximately 9% in the heat recirculation meso‐combustor, indicating that heat recirculation effect facilitates more complete combustion of methane and medium components. Preheating channels show positive effects on improving combustion stability in the heat recirculation meso‐combustor. On one hand, preheating channels facilitate heat recirculation effect, and heat recirculation rate exceeds 10% for all cases and reaches 31.8% with an inlet velocity of 0.5 m/s, leading to significant increment of methane‐specific enthalpy at the preheating channel outlet. On the other hand, Rh(s)/O(s) ratios of catalytic surface and catalytic surface temperature in main reaction zone are enlarged by the preheating channels, facilitating methane adsorption at catalytic surface. Specially, most of fuels are consumed in a shorter distance with higher methane conversion speed, which brings benefits to promote combustion efficiency and may be helpful to inhibit the combustion instability in heat recirculation meso‐combustors.     

Catalytic combustion of methane over a highly active and stable NiO/CeO2 catalyst

In the last decades, many reports dealing with technology for the catalytic combustion of methane (CH₄) have been published. Recently, attention has increasingly focused on the synthesis and catalytic activity of nickel oxides. In this paper, a NiO/CeO₂ catalyst with high catalytic performance in methane combustion was synthesized via a facile impregnation method, and its catalytic activity, stability, and water-resistance during CH₄ combustion were investigated. X-ray diffraction, low-temperature N₂ adsorption, thermogravimetric analysis, Fourier transform infrared spectroscopy, hydrogen temperature programmed reduction, methane temperature programmed surface reaction, Raman spectroscopy, electron paramagnetic resonance, and transmission electron microscope characterization of the catalyst were conducted to determine the origin of its high catalytic activity and stability in detail. The incorporation of NiO was found to enhance the concentration of oxygen vacancies, as well as the activity and amount of surface oxygen. As a result, the mobility of bulk oxygen in CeO₂ was increased. The presence of CeO₂ prevented the aggregation of NiO, enhanced reduction by NiO, and provided more oxygen species for the combustion of CH₄. The results of a kinetics study indicated that the reaction order was about 1.07 for CH₄ and about 0.10 for O₂ over the NiO/CeO₂ catalyst.     

三塘湖盆地中—下侏罗统煤层甲烷风化带划分

以三塘湖盆地中、低煤阶煤层含气量和主要气体成分为基础,结合盆地构造、沉积及水文地质特征,对汉水泉凹陷和条湖凹陷煤层甲烷风化带进行了划分,并对库木苏凹陷、马朗凹陷、淖毛湖凹陷和苏鲁克凹陷煤层甲烷风化带进行了预测。结果表明,三塘湖盆地甲烷风化带深度为400~1000 m.由于受东北冲断隆起带的影响,三塘湖盆地北部甲烷风化带浅于南部。沉积方面,盆地东部淖毛湖凹陷、马朗凹陷和条湖凹陷深湖—半深湖和辫状河三角洲成煤环境优于盆地西部汉水泉凹陷和库木苏凹陷扇三角洲成煤环境,盆地东部甲烷风化带普遍浅于西部;水文地质方面,条湖凹陷和马朗凹陷中开启性局部滞留水文地质单元形成的甲烷风化带浅于其他凹陷封闭性弱径流水文地质单元的甲烷风化带。初步预测马朗凹陷北部为下一步煤层气勘探开发的优势区块,条湖凹陷北部为下一步煤系气勘探开发的优势区块。     

Reactivity,Selectivity, and Stability of Zeolite-Based Catalysts for Methane Dehydroaromatization

Non-oxidative dehydroaromatization is arguably the most promising process for the direct upgrading of cheap and abundant methane to liquid hydrocarbons. This reaction has not been commercialized yet because of the suboptimal activity and swift deactivation of benchmark Mo-zeolite catalysts. This progress report represents an elaboration on the recent developments in understanding of zeolite-based catalytic materials for high-temperature non-oxidative dehydroaromatization of methane. It is specifically focused on recent studies, relevant to the materials chemistry and elucidating i) the structure of active species in working catalysts; ii) the complex molecular pathways underlying the mechanism of selective conversion of methane to benzene; iii) structure, evolution and role of coke species; and iv) process intensification strategies to improve the deactivation resistance and overall performance of the catalysts. Finally, unsolved challenges in this field of research are outlined and an outlook is provided on promising directions toward improving the activity, stability, and selectivity of methane dehydroaromatization catalysts.     

酸改性CoPd/TiO2催化CH4-CO2直接合成C2含氧化合物

采用酸处理方法对CoPd/TiO₂催化剂进行改性，并将酸改性催化剂用于温和条件下CH₄-CO₂梯阶转化直接合成C₂含氧化合物（乙酸和乙醇）的反应。在150～300℃考察了浸酸方式和不同种类酸处理对催化剂活性和选择性的影响。采用X射线衍射（XRD）、X射线光电子能谱（XPS）、NH₃程序升温脱附（NH₃-TPD）和N₂吸附对催化剂进行了表征。结果表明，酸改性明显提高了CoPd/TiO₂上C₂含氧化合物的生成速率和选择性。浸酸方式对催化剂性能和结构有显著影响，先用酸浸渍载体然后再浸渍活性金属所得催化剂具有更高的活性。在H₃PO₄、HNO₃和HCl中，H₃PO₄浸渍的催化剂活性最佳，在150℃时C₂含氧化合物（乙酸和乙醇）的生成速率为3365 μg/(g·h)，选择性达到91%。