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Methane Biofiltration Processes: A Summary of Biotic and Abiotic Factors 甲烷生物过滤过程:生物和非生物因素概述
Pub Date : 2024-02-21 DOI: 10.3390/methane3010008
Fatemeh Ahmadi, Tatiana Bodraya, Maximilian Lackner
The ongoing yearly rise in worldwide methane (CH4) emissions is mostly due to human activities. Nevertheless, since over half of these emissions are scattered and have a concentration of less than 3% (v/v), traditional physical–chemical methods are not very effective in reducing them. In this context, biotechnologies like biofiltration using methane-consuming bacteria, also known as methanotrophs, offer a cost-efficient and practical approach to addressing diffuse CH4 emissions. The present review describes recent findings in biofiltration processes as one of the earliest biotechnologies for treating polluted air. Specifically, impacts of biotic (such as cooperation between methanotrophs and non-methanotrophic bacteria and fungi) and abiotic factors (such as temperature, salinity, and moisture) that influence CH4 biofiltration were compiled. Understanding the processes of methanogenesis and methanotrophy holds significant importance in the development of innovative agricultural practices and industrial procedures that contribute to a more favourable equilibrium of greenhouse gases. The integration of advanced genetic analyses can enable holistic approaches for unravelling the potential of biological systems for methane mitigation. This study pioneers a holistic approach to unravelling the biopotential of methanotrophs, offering unprecedented avenues for biotechnological applications.
全球甲烷(CH4)排放量逐年上升的主要原因是人类活动。然而,由于一半以上的甲烷排放是分散的,浓度低于 3%(v/v),传统的物理化学方法对减少甲烷排放并不十分有效。在这种情况下,利用甲烷消耗细菌(也称为甲烷营养菌)进行生物过滤等生物技术为解决扩散性甲烷排放问题提供了一种具有成本效益且实用的方法。本综述介绍了作为处理污染空气的最早生物技术之一的生物过滤过程的最新研究成果。具体而言,汇编了影响甲烷生物过滤的生物因素(如甲烷营养体与非甲烷营养体细菌和真菌之间的合作)和非生物因素(如温度、盐度和湿度)的影响。了解甲烷生成和甲烷营养过程对于开发有助于实现更有利的温室气体平衡的创新农业实践和工业程序具有重要意义。结合先进的遗传分析,可以采用整体方法来揭示生物系统在甲烷减排方面的潜力。这项研究开创了一种全面的方法来揭示甲烷营养体的生物潜力,为生物技术应用提供了前所未有的途径。
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引用次数: 0
Towards a Mechanistic Understanding of the Slagging Propensities of Petroleum Coke: Lessons Learned from Its Co-Combustion with Natural Gas in Oxygen-Enriched Atmospheres 从机理上理解石油焦的成渣倾向性:从石油焦与天然气在富氧环境中共燃中汲取的经验教训
Pub Date : 2024-01-24 DOI: 10.3390/methane3010005
Nghia Duc Tin Nguyen, G. Krishnamoorthy
A Computational Fluid Dynamic study was carried out to match the measured outer ash deposition rates associated with the combustion of petroleum coke (PC)–natural gas in AIR and O2/CO2 (70/30 vol%, OXY70). The fly ash PSD associated with high-fixed-carbon, non-porous fuel was estimated using a shrinking sphere burnout model and employed in conjunction with particle kinetic energy (PKE), particle viscosity (µP), and a critical Weber-number-based capture criterion. Deposition rate predictions were sensitive to the fly ash composition employed for estimating µP due to the significant enrichment of Fe in the deposits. Predictions were insensitive to the specific µP model formulation employed or whether the V2O5 in the ash was assumed to play the role of a glass former or a glass modifier. OXY70 scenario impaction rates were significantly lower than the measured deposition rates when the fly ash PSD associated with the AIR scenario was employed in the calculations. This necessitated an ad hoc modification of the OXY70 fly ash PSD to a coarser range to match the measurements and attributing it to agglomeration resulting from longer residence times and higher temperatures. This shift in PSD was in line with AIR and OXY70 fly ash PSD measurements reported previously.
为了与石油焦(PC)-天然气在空气和氧气/二氧化碳(70/30 vol%,OXY70)中燃烧时测得的外灰沉积率相匹配,我们进行了一项计算流体动力学研究。与高固定碳、无孔燃料相关的飞灰 PSD 是使用收缩球燃烧模型估算的,并与粒子动能 (PKE)、粒子粘度 (µP) 和基于临界韦伯数的捕获标准结合使用。由于沉积物中铁的显著富集,沉积速率预测对用于估算 µP 的粉煤灰成分很敏感。预测结果对所采用的特定 µP 模型公式或假定灰烬中的 V2O5 起玻璃成形剂或玻璃改性剂的作用不敏感。如果在计算中采用与 AIR 情景相关的粉煤灰 PSD,则 OXY70 情景下的撞击率明显低于测得的沉积率。这就需要临时修改 OXY70 粉煤灰 PSD,使其在更粗的范围内,以符合测量结果,并将其归因于较长的停留时间和较高的温度导致的团聚。PSD 的这种变化与之前报告的 AIR 和 OXY70 粉煤灰 PSD 测量结果一致。
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引用次数: 0
High-Pressure Hydrogenation: A Path to Efficient Methane Production from CO2 高压氢化:从二氧化碳高效生产甲烷的途径
Pub Date : 2024-01-15 DOI: 10.3390/methane3010004
M. L. Gothe, Adolfo L. Figueredo, Laís R. Borges, Ruben Ramos, A. F. Peixoto, P. Vidinha
Methane has a rather relevant role in the “Power-to-Gas” concept, which is central in the current paradigm of climate change and renewable energies. Methane, the main component of natural gas, can be produced by catalytic hydrogenation reactions, particularly of CO2. A very effective catalyst in this reaction, hydrotalcite-derived nickel nanoparticles supported on alumina, Ni/Al2O3-HTC, can be employed in a high-pressure flow reactor to convert CO2 and H2 into CH4 at 100% selectivity and 84% conversion, whereas at atmospheric pressure, methane can be obtained with up to 90% selectivity. The high-pressure aspect also allows fast-paced production—over 5 m3·h−1·kgcat−1 of CH4 can be generated.
甲烷在 "电力转化为天然气 "的概念中扮演着相当重要的角色,而这一概念在当前的气候变化和可再生能源范式中处于核心地位。甲烷是天然气的主要成分,可以通过催化加氢反应生产,特别是二氧化碳的加氢反应。该反应中一种非常有效的催化剂--以氧化铝为载体的氢铝酸盐衍生镍纳米颗粒(Ni/Al2O3-HTC),可用于高压流动反应器,将 CO2 和 H2 转化为 CH4,选择性为 100%,转化率为 84%,而在常压下,甲烷的选择性可达 90%。高压还可实现快速生产--可产生超过 5 m3-h-1-kgcat-1 的 CH4。
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引用次数: 0
A Review on Dry Anaerobic Digestion: Existing Technologies, Performance Factors, Challenges, and Recommendations 干法厌氧消化综述:现有技术、性能因素、挑战和建议
Pub Date : 2024-01-15 DOI: 10.3390/methane3010003
Umer Hayyat, M. U. Khan, Muhammad Sultan, Umair Zahid, S. A. Bhat, Mohammad Muzamil
With the increase in the growing rate of municipal solid waste throughout the world and due to the high moisture and organic components of the organic fraction of municipal solid waste, dry anaerobic digestion has become the future direction to cope with this waste while reducing the impact on the environment, including climate change. Dry anaerobic digestion has become a promising technology that converts the organic fraction of municipal solid waste into combustible biogases, which can be used as an alternative energy source. However, the technology faces several challenges that must be addressed to enhance its performance and adoption. This paper provides a comprehensive analysis of the current technologies used for dry anaerobic digestion in OFMSW and delves into the various factors that influence the performance of these technologies. This review paper also identifies and discusses the challenges faced in optimizing and scaling up these technologies, such as feedstock pretreatment requirements, characteristics of inoculum, and other crucial parameters.
随着全世界城市固体废物增长率的提高,由于城市固体废物中有机部分的水分和有机成分较高,干式厌氧消化已成为处理这些废物的未来方向,同时减少对环境的影响,包括气候变化。干式厌氧消化技术将城市固体废弃物中的有机成分转化为可燃生物气体,可用作替代能源,是一项前景广阔的技术。然而,该技术面临着一些挑战,必须加以解决,以提高其性能和采用率。本文全面分析了目前用于城市固体废物干法厌氧消化的技术,并深入探讨了影响这些技术性能的各种因素。本文还确定并讨论了在优化和推广这些技术时所面临的挑战,如原料预处理要求、接种物特性和其他关键参数。
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引用次数: 0
Dry Reforming of Methane over Li-Doped Ni/TiO2 Catalysts: Effect of Support Basicity 掺锂 Ni/TiO2 催化剂对甲烷的干法转化:支撑碱度的影响
Pub Date : 2023-12-15 DOI: 10.3390/methane2040031
Vicente Pérez-Madrigal, E. Ríos-Valdovinos, E. Rojas-García, Miguel A. Valenzuela, F. Pola-Albores
In this research, we investigate the impact of Li doping on a TiO2 support, synthesized through the sol-gel method, with a focus on varying the aging time. Our objective is to elucidate how aging duration and doping influence the surface basicity, thereby mitigating carbon formation and amplifying the catalytic efficacy of Ni-loaded catalysts (15 wt.%). Essential characterization techniques encompass X-ray diffraction, H2-TPR, FE-SEM, N2-physisorption, DLS, FTIR, and Raman spectroscopies. Our findings reveal that extended aging periods promote the development of a basic character, attributable to oxygen defects within TiO2. This inherent trait bears significant implications for catalyst performance, stability, and carbon formation during the reaction. Remarkably, the catalyst with the highest catalytic activity and stability boasts an 85% relative basicity, a property also induced by incorporating lithium into the TiO2 support.
在本研究中,我们研究了锂掺杂对通过溶胶-凝胶法合成的 TiO2 载体的影响,重点是改变老化时间。我们的目标是阐明老化时间和掺杂如何影响表面碱性,从而减少碳的形成并提高镍负载催化剂(15 wt.%)的催化效率。基本表征技术包括 X 射线衍射、H2-TPR、FE-SEM、N2-物理吸附、DLS、傅立叶变换红外光谱和拉曼光谱。我们的研究结果表明,由于二氧化钛中的氧缺陷,延长老化期会促进碱性特征的发展。这种固有特性对催化剂的性能、稳定性和反应过程中的碳形成具有重要影响。值得注意的是,催化活性和稳定性最高的催化剂具有 85% 的相对碱性,这一特性也是通过在 TiO2 载体中加入锂而产生的。
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引用次数: 0
Using Ground- and Drone-Based Surface Emission Monitoring (SEM) Data to Locate and Infer Landfill Methane Emissions 使用基于地面和无人机的地表排放监测 (SEM) 数据定位和推断垃圾填埋场甲烷排放量
Pub Date : 2023-12-11 DOI: 10.3390/methane2040030
T. Abichou, Nizar Bel Hadj Ali, Sakina Amankwah, Roger Green, Eric S. Howarth
Ground- and drone-based surface emission monitoring (SEM) campaigns were performed at two municipal solid waste landfills, during the same week as mobile tracer correlation method (TCM) testing was used to measure the total methane emissions from the same landfills. The G-SEM and the D-SEM data, along with wind data, were used as input into an inverse modeling approach combined with an optimization-based methane emission estimation method (implemented in a tool called SEM2Flux). This approach involves the use of backward dispersion modeling to estimate the whole-site methane emissions from a given landfill and the identification of locations and emission rates of major leaks. SEM2Flux is designed to exploit the measured surface methane concentration concurrently with wind data and tackle two problems: (1) inferring the estimates of methane rates from individual landfills, and (2) identifying the likely locations of the main emission sources. SEM2Flux results were also compared with emission estimates obtained using TCM. In Landfill B, the average TCM-measured methane emissions was 1178 Kg/h, with a standard deviation of 271 Kg/h. In Landfill C, the average TCM-measured emission rate was 601 Kg/h, with a standard deviation of 292 Kg/h. For both landfills, the D-SEM data yielded statistically similar estimates of methane emissions as the TCM-measured emissions. On the other hand, the G-SEM data yielded comparable estimates of emissions to TCM-measured emissions only for Landfill C, where the D-SEM and G-SEM data were statistically not different. The results of this study showcase the ability of this method using surface concentrations to provide a rapid and simple estimation of fugitive methane emissions from landfills. Such an approach can also be used to assess the effectiveness of different remedial actions in reducing fugitive methane emissions from a given landfill.
在使用移动示踪相关法(TCM)测试测量同一垃圾填埋场甲烷排放总量的同一周内,在两个城市固体废物填埋场开展了地面和无人机表面排放监测(SEM)活动。G-SEM 和 D-SEM 数据以及风力数据被用作反向建模方法的输入,该方法结合了基于优化的甲烷排放估算方法(在名为 SEM2Flux 的工具中实施)。这种方法包括使用反向扩散模型来估算特定垃圾填埋场的全场甲烷排放量,并确定主要泄漏点的位置和排放率。SEM2Flux 的设计目的是利用测量到的地表甲烷浓度和风力数据,解决两个问题:(1)推断各个垃圾填埋场的甲烷排放率估计值;(2)确定主要排放源的可能位置。SEM2Flux 的结果还与使用 TCM 得出的排放估计值进行了比较。在 B 垃圾填埋场,TCM 测量的甲烷平均排放量为 1178 千克/小时,标准偏差为 271 千克/小时。在垃圾填埋场 C 中,经 TCM 测量的平均甲烷排放量为 601 千克/小时,标准偏差为 292 千克/小时。对于这两个垃圾填埋场,D-SEM 数据得出的甲烷排放量估计值与 TCM 测量的排放量在统计上相似。另一方面,只有在 C 垃圾填埋场,G-SEM 数据得出的排放量估计值与 TCM 测量的排放量相当,D-SEM 和 G-SEM 数据在统计上没有差异。这项研究的结果表明,使用表面浓度的方法能够快速、简单地估算垃圾填埋场的甲烷逃逸排放量。这种方法还可用于评估不同补救措施在减少特定垃圾填埋场甲烷逃逸性排放方面的效果。
{"title":"Using Ground- and Drone-Based Surface Emission Monitoring (SEM) Data to Locate and Infer Landfill Methane Emissions","authors":"T. Abichou, Nizar Bel Hadj Ali, Sakina Amankwah, Roger Green, Eric S. Howarth","doi":"10.3390/methane2040030","DOIUrl":"https://doi.org/10.3390/methane2040030","url":null,"abstract":"Ground- and drone-based surface emission monitoring (SEM) campaigns were performed at two municipal solid waste landfills, during the same week as mobile tracer correlation method (TCM) testing was used to measure the total methane emissions from the same landfills. The G-SEM and the D-SEM data, along with wind data, were used as input into an inverse modeling approach combined with an optimization-based methane emission estimation method (implemented in a tool called SEM2Flux). This approach involves the use of backward dispersion modeling to estimate the whole-site methane emissions from a given landfill and the identification of locations and emission rates of major leaks. SEM2Flux is designed to exploit the measured surface methane concentration concurrently with wind data and tackle two problems: (1) inferring the estimates of methane rates from individual landfills, and (2) identifying the likely locations of the main emission sources. SEM2Flux results were also compared with emission estimates obtained using TCM. In Landfill B, the average TCM-measured methane emissions was 1178 Kg/h, with a standard deviation of 271 Kg/h. In Landfill C, the average TCM-measured emission rate was 601 Kg/h, with a standard deviation of 292 Kg/h. For both landfills, the D-SEM data yielded statistically similar estimates of methane emissions as the TCM-measured emissions. On the other hand, the G-SEM data yielded comparable estimates of emissions to TCM-measured emissions only for Landfill C, where the D-SEM and G-SEM data were statistically not different. The results of this study showcase the ability of this method using surface concentrations to provide a rapid and simple estimation of fugitive methane emissions from landfills. Such an approach can also be used to assess the effectiveness of different remedial actions in reducing fugitive methane emissions from a given landfill.","PeriodicalId":74177,"journal":{"name":"Methane","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2023-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139010278","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Anaerobic Co-Digestion of Vinasse and Pentose Liquor and the Role of Micronutrients in Methane Production within Sugarcane Biorefineries 甘蔗渣和戊糖液的厌氧协同消化以及微量营养元素在甘蔗生物炼油厂甲烷生产中的作用
Pub Date : 2023-12-08 DOI: 10.3390/methane2040029
Gabriela P. Freitas, Brenno Vinicius M. Lima, M. P. C. Volpi, Renata P. Rodriguez, Bruna S. Moraes
Anaerobic digestion (AD) of residues from integrated first- and second-generation ethanol (1G2G) biorefineries is a sustainable method for energy recovery through biogas production. This study evaluated the co-digestion of 1G vinasse, 2G vinasse and pentose liquor (from the pretreatment of sugarcane bagasse for 2G ethanol production) compared to individual digestions using biochemical methane potential (BMP) assays. The results showed some “key” micronutrients from the substrates that affected methane (CH4) production, while their balance provided by co-digestion achieved high digestibility (95%). High iron (Fe) and nickel (Ni) concentrations, in addition to furfural (0.33 g L−1) in pentose liquor seemed to decrease its CH4 production potential. Despite these adverse effects observed in mono-digestion, co-digestion was beneficial for this substrate, increasing digestibility (52%) and BMP (118%). The highest BMP was observed in vinasse 2G (631 ± 6 NmL CH4 gTVS−1), with no significant difference compared to the adjusted modified Gompertz model (624 ± 10 NmL CH4 gTVS−1). The co-digestion system also presented the highest specific CH4 production rate (20 ± 1 NmL CH4 gTVS−1day−1) and shortened the lag phase by 19% compared to the AD of isolated 1G vinasse with the second lowest BMP value (494 ± 11 NmL CH4 gTVS−1).
对来自第一代和第二代乙醇(1G2G)综合生物炼油厂的残渣进行厌氧消化(AD)是一种通过生产沼气回收能源的可持续方法。这项研究利用生化甲烷潜能(BMP)测定法,评估了 1G 甘蔗渣、2G 甘蔗渣和戊糖液(甘蔗渣预处理后用于 2G 乙醇生产)共同消化与单独消化的比较。结果表明,基质中的一些 "关键 "微量营养元素会影响甲烷(CH4)的产生,而共同消化所提供的微量营养元素平衡则实现了高消化率(95%)。除糠醛(0.33 g L-1)外,戊糖液体中铁(Fe)和镍(Ni)的高浓度似乎降低了其产生 CH4 的潜力。尽管在单一消化过程中观察到了这些不利影响,但共同消化对这种基质是有益的,可提高消化率(52%)和生物放大系数(118%)。蔗渣 2G 的生物放大系数最高(631 ± 6 NmL CH4 gTVS-1),与调整后的改良贡珀兹模型(624 ± 10 NmL CH4 gTVS-1)相比没有显著差异。与 BMP 值第二低(494 ± 11 NmL CH4 gTVS-1)的分离 1G 甘蔗渣厌氧消化相比,协同消化系统的特定 CH4 生成率最高(20 ± 1 NmL CH4 gTVS-1-day-1),滞后期缩短了 19%。
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引用次数: 0
Density Functional Theory Insight into Chemical Vapor Infiltration 密度泛函理论洞察化学蒸汽渗透
Pub Date : 2023-11-09 DOI: 10.3390/methane2040028
Eric A. Walker, Joseph J. Marziale, James Chen
Chemical Vapor Infiltration (CVI) has proven remarkably successful in producing strong and lightweight ceramic matrix composite materials. This technology has matured to regular industrial use. However, two fundamental problems remain, and those are the formation of pores and depositing of weaker material than silicon carbide (SiC), namely, Si. Definitive knowledge of the molecular mechanism would catalyze an advance in the chemical precursors used in CVI. In this work, the CVI reaction is modeled using density functional theory (DFT) calculations. The DFT calculations here use the Bayesian Error Estimation Functional with van der Waals correction (BEEF-vdW). The main findings begin with C deposition determining the rate of solid SiC growth due to Si being far more reactive. Therefore, increasing the C content of the precursor is a logical CVI strategy. Methane (CH4) is more reactive than ethane (C2H6) and ethylene (C2H2) and would be effective as an additive to the chemical precursor. Increasing the deposition rate of C has the benefit of decreasing pure Si deposits. Si melts at 1410 °C and CMCs are used in high-temperature settings beyond this melting point, including in aeroengines and nuclear fuel cladding.
化学蒸汽渗透(CVI)技术在生产高强度和轻质陶瓷基复合材料方面取得了显著的成功。这项技术已经成熟,可以用于常规工业用途。然而,仍然存在两个基本问题,即孔隙的形成和比碳化硅(SiC)更弱的材料(即Si)的沉积。分子机制的明确知识将催化CVI中使用的化学前体的进步。在这项工作中,使用密度泛函理论(DFT)计算模拟了CVI反应。这里的DFT计算使用带有范德华校正的贝叶斯误差估计函数(cow - vdw)。主要的发现开始于C沉积决定了固体SiC的生长速率,因为Si的反应性更强。因此,增加前体的C含量是一种合乎逻辑的CVI策略。甲烷(CH4)比乙烷(C2H6)和乙烯(C2H2)的反应性更强,可以作为化学前体的添加剂。提高C的沉积速率有利于减少纯Si的沉积。硅熔体在1410°C, cmc用于超过该熔点的高温环境,包括航空发动机和核燃料包壳。
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引用次数: 0
Methane Removal from Air: Challenges and Opportunities 从空气中去除甲烷:挑战与机遇
Pub Date : 2023-11-01 DOI: 10.3390/methane2040027
Jin Wang, Qinghua Peter He
Driven by increasing greenhouse gas (GHG) concentrations in the atmosphere, extreme weather events have become more frequent and their impacts on human lives have become more severe. Therefore, the need for short-term GHG mitigations is urgent. Recently, methane has been recognized as an important mitigation target due to its high global warming potential (GWP). However, methane’s low concentration in the atmosphere and stable molecular structure make its removal from the air highly challenging. This review first discusses the fundamental aspects of the challenges in atmospheric methane removal and then briefly reviews the existing research strategies following the mechanisms of natural methane sinks. Although still in its infancy, recent research on methane removal from the air holds great potential for slowing down global warming. At the same time, it is important to carefully examine the energy consumption of these methane removal strategies and whether they will be able to achieve net GHG reduction. In addition, due to the scale of methane removal from the air, any potential solution’s environmental impacts must be carefully evaluated before it can be implemented in practice.
在大气中温室气体(GHG)浓度增加的驱动下,极端天气事件变得越来越频繁,对人类生活的影响也越来越严重。因此,迫切需要短期缓解温室气体。近年来,由于甲烷具有较高的全球变暖潜能值(GWP),已被公认为重要的减排目标。然而,甲烷在大气中的低浓度和稳定的分子结构使其从空气中去除极具挑战性。本文首先讨论了大气甲烷去除面临的基本挑战,然后简要回顾了现有的研究策略,并遵循天然甲烷汇的机制。尽管仍处于起步阶段,但最近关于从空气中去除甲烷的研究对减缓全球变暖具有巨大的潜力。与此同时,重要的是要仔细检查这些甲烷去除策略的能源消耗以及它们是否能够实现温室气体净减排。此外,由于从空气中去除甲烷的规模,任何潜在解决方案的环境影响都必须在实际实施之前仔细评估。
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引用次数: 1
Autothermal Reforming of Methane: A Thermodynamic Study on the Use of Air and Pure Oxygen as Oxidizing Agents in Isothermal and Adiabatic Systems 甲烷的自热重整:在等温和绝热系统中使用空气和纯氧作为氧化剂的热力学研究
Pub Date : 2023-10-08 DOI: 10.3390/methane2040026
Matheus Henrique Silva Cavalcante, Ícaro Augusto Maccari Zelioli, Emílio Émerson Xavier Guimarães Filho, Julles Mitoura dos Santos Júnior, Annamaria Dória Souza Vidotti, Antonio Carlos Daltro de Freitas, Reginaldo Guirardello
In this paper, we analyze the autothermal reforming (ATR) of methane through Gibbs energy minimization and entropy maximization methods to analyze isothermic and adiabatic systems, respectively. The software GAMS® 23.9 and the CONOPT3 solver were used to conduct the simulations and thermodynamic analyses in order to determine the equilibrium compositions and equilibrium temperatures of this system. Simulations were performed covering different pressures in the range of 1 to 10 atm, temperatures between 873 and 1073 K, steam/methane ratio was varied in the range of 1.0/1.0 and 2.0/1.0 and oxygen/methane ratios in the feed stream, in the range of 0.5/1.0 to 2.0/1.0. The effect of using pure oxygen or air as oxidizer agent to perform the reaction was also studied. The simulations were carried out in order to maintain the same molar proportions of oxygen as in the simulated cases considering pure oxygen in the reactor feed. The results showed that the formation of hydrogen and synthesis gas increased with temperature, average composition of 71.9% and 56.0% using air and O2, respectively. These results are observed at low molar oxygen ratios (O2/CH4 = 0.5) in the feed. Higher pressures reduced the production of hydrogen and synthesis gas produced during ATR of methane. In general, reductions on the order of 19.7% using O2 and 14.0% using air were observed. It was also verified that the process has autothermicity in all conditions tested and the use of air in relation to pure oxygen favored the compounds of interest, mainly in conditions of higher pressure (10 atm). The mean reductions with increasing temperature in the percentage increase of H2 and syngas using air under 1.5 and 10 atm, at the different O2/CH4 ratios, were 5.3%, 13.8% and 16.5%, respectively. In the same order, these values with the increase of oxygen were 3.6%, 6.4% and 9.1%. The better conditions for the reaction include high temperatures, low pressures and low O2/CH4 ratios, a region in which there is no swelling in terms of the oxygen source used. In addition, with the introduction of air, the final temperature of the system was reduced by 5%, which can help to reduce the negative impacts of high temperatures in reactors during ATR reactions.
本文采用Gibbs能量最小化法和熵最大化法对甲烷自热重整(ATR)进行了分析,分别分析了等温和绝热系统。使用GAMS®23.9软件和CONOPT3求解器进行模拟和热力学分析,以确定该体系的平衡组成和平衡温度。模拟的压力范围为1 ~ 10atm,温度范围为873 ~ 1073 K,蒸汽/甲烷比范围为1.0/1.0和2.0/1.0,进料流中的氧/甲烷比范围为0.5/1.0至2.0/1.0。研究了用纯氧或空气作氧化剂进行反应的效果。在考虑反应器进料中纯氧的情况下,为了保持与模拟情况相同的氧摩尔比,进行了模拟。结果表明,随着温度的升高,氢气和合成气的生成量增加,空气和O2的平均组成分别为71.9%和56.0%。这些结果是在低摩尔氧比(O2/CH4 = 0.5)的饲料中观察到的。较高的压力降低了甲烷ATR过程中产生的氢气和合成气的产量。总的来说,使用氧气可以减少19.7%,使用空气可以减少14.0%。还验证了该工艺在所有测试条件下都具有自热性,并且与纯氧相比,空气的使用有利于感兴趣的化合物,主要是在较高压力(10 atm)的条件下。在不同O2/CH4比下,1.5和10 atm空气中H2和合成气的增加百分比随温度的升高平均下降幅度分别为5.3%、13.8%和16.5%。随氧气添加量的增加,这些值依次为3.6%、6.4%和9.1%。较好的反应条件包括高温、低压和较低的O2/CH4比,在这个区域内,所用的氧气源不会膨胀。此外,随着空气的引入,系统的最终温度降低了5%,这有助于减少ATR反应过程中反应器内高温的负面影响。
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引用次数: 0
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Methane
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