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Combustion of NH3/DME and NH3/DME/NO mixtures NH3/DME 和 NH3/DME/NO 混合物的燃烧
IF 6.7 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-04 DOI: 10.1016/j.fuel.2024.133253
The objective of this work is to study the oxidation of ammonia and dimethyl ether mixtures (NH3/DME) both in the absence and the presence of monoxide of nitrogen (NO). For this purpose, laboratory experiments have been conducted in a quartz flow reactor setup in the 875–1425 K temperature range at atmospheric pressure, modifying the oxygen excess ratio (λ), and the NH3/DME mixture ratio with and without NO. The experimental results have been simulated with a literature-based kinetic mechanism. The results show that the presence of DME and an oxygen excess ratio affect the conversion of NH3, shifting its oxidation to lower temperatures, which decrease as the DME concentration in the mixture and λ increase. Interactions between ammonia and DME seem to be important under the studied conditions, presumably involving the formation and thermal decomposition of methyl nitrite (CH3ONO). These interactions affect the oxidation of ammonia at low temperatures, consume and produce NO, which would determine the final NO emission. When there is NO in the NH3/DME mixtures, NO is reduced up to 60 %, also favouring the oxidation of ammonia, but with an almost imperceptible effect of NO in the case of DME. The addition of different concentrations of DME also affects the oxidation behaviour of ammonia in NH3/DME/NO mixtures. In general, the conversion of both NH3 and DME is highly determined by the concentration of OH radicals, although thermal decomposition is also relevant for DME.
这项工作的目的是研究氨和二甲醚混合物(NH3/DME)在没有一氧化氮(NO)和有一氧化氮(NO)的情况下的氧化过程。为此,我们在石英流动反应器中进行了实验室实验,温度范围为 875-1425 K,压力为大气压,改变了氧气过剩率 (λ),以及有氮氧化物和无氮氧化物时的 NH3/DME 混合物比率。实验结果通过基于文献的动力学机制进行了模拟。结果表明,二甲醚的存在和氧过量比会影响 NH3 的转化,使其氧化温度降低,而随着混合物中二甲醚浓度和 λ 的增加,温度也会降低。在研究条件下,氨和二甲醚之间的相互作用似乎很重要,可能涉及亚硝酸甲酯(CH3ONO)的形成和热分解。这些相互作用会影响氨在低温下的氧化,消耗并产生 NO,从而决定最终的 NO 排放量。当 NH3/DME 混合物中含有 NO 时,NO 的减少量可达 60%,这也有利于氨的氧化,但在 DME 的情况下,NO 的影响几乎无法察觉。添加不同浓度的二甲醚也会影响 NH3/DME/NO 混合物中氨的氧化行为。一般来说,NH3 和二甲醚的转化在很大程度上取决于 OH 自由基的浓度,尽管热分解也与二甲醚有关。
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引用次数: 0
Robust mussel-inspired LBL carbon nanotube-based superhydrophobic polyurethane sponge for efficient oil–water separation utilizing photothermal effect 受贻贝启发的基于 LBL 碳纳米管的超疏水聚氨酯海绵,可利用光热效应实现高效油水分离
IF 6.7 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-04 DOI: 10.1016/j.fuel.2024.133353
Superhydrophobic materials possessing efficient and rapid oil–water separation capabilities, as well as robustness, have emerged as the epicenter of global attention. Conventional three-dimensional adsorbent materials often succumb to impaired performance under extreme environmental conditions, rendering it arduous to ensure the efficacy of oil–water separation, and confining the application scenarios. In this study, polyurethane sponges (PUs) co-modified with stearic acid (SA), polydimethylsiloxane (PDMS), and multi-walled carbon nanotubes (MWCNTs), designated as SA-PDMS/MWCNTs@PU (SPMPU), were successfully synthesized via layer-by-layer (LBL) self-assembly and liquid-phase deposition. The SPMPU sponge exhibits an overall separation efficiency of not less than 90 %. It boasts a stable adsorption capacity, formidable mechanical properties, and commendable reusability. SPMPU sponges maintain unparalleled stability in extreme environments, such as strong acids and alkalis, and in the photothermal effect experiment, the SPMPU sponge can attain a temperature of 101.5 °C within 2 min, with rapid reaction kinetics, high efficiency, and unwavering stability. Through the photothermal effect-assisted oil–water separation, a reliable solution is furnished for the current oil–water separation endeavors. The SPMPU sponge preparation is uncomplicated, economical, and yields stable performance, holding significant potential for application in marine oil spills and industrial oil–water separation scenarios.
具有高效、快速油水分离能力和坚固性的超疏水材料已成为全球关注的焦点。传统的三维吸附材料往往在极端环境条件下性能受损,难以保证油水分离的效果,应用场景也受到限制。本研究通过逐层自组装和液相沉积法成功合成了硬脂酸(SA)、聚二甲基硅氧烷(PDMS)和多壁碳纳米管(MWCNTs)共修饰的聚氨酯海绵(PUs),命名为 SA-PDMS/MWCNTs@PU (SPMPU)。SPMPU 海绵的总体分离效率不低于 90%。它具有稳定的吸附能力、强大的机械性能和值得称赞的可重复使用性。SPMPU 海绵在强酸和强碱等极端环境中保持着无与伦比的稳定性,在光热效应实验中,SPMPU 海绵可在 2 分钟内达到 101.5 ℃ 的温度,反应动力学快,效率高,稳定性好。通过光热效应辅助油水分离,为当前的油水分离工作提供了可靠的解决方案。SPMPU 海绵的制备方法简单、经济、性能稳定,在海洋溢油和工业油水分离领域具有巨大的应用潜力。
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引用次数: 0
Microwave-induced alterations in the structure of coals at different metamorphic stages 不同变质阶段微波引起的煤炭结构变化
IF 6.7 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-04 DOI: 10.1016/j.fuel.2024.133326
Despite the global trend toward decarbonization, coal continues to play a significant role in energy production, as current renewable energy sources cannot fully meet the increasing global energy demand. The main objective of decarbonization is to reduce greenhouse gas emissions, especially carbon dioxide. Enhancing coal usage efficiency can help decrease these emissions. Electromagnetic activation of bituminous coal is already employed for dehydration, ash removal, desulfurization, and improving the grinding process of raw coal. This research aims to study the specifics of coal electromagnetic activation using microwave radiation and its effects on the physical and chemical processes occurring in coals at different metamorphic stages. The results suggest that this electromagnetic treatment leads to the destruction of hydroxyl groups and the formation of free hydrogen. Coals at higher metamorphic stages heat up faster due to their higher structural density. Coals at lower metamorphic stages take longer to heat up and require more processing time to be effective, while lower power levels are necessary to avoid mechanical breakdown. Activation time and coal particle size are significant factors; their optimal combination provides the maximum effect. These findings contribute to optimizing microwave treatment parameters for different coal types, potentially enhancing coal utilization efficiency and reducing environmental impact.
尽管全球都在朝着去碳化的方向发展,但由于目前的可再生能源无法完全满足日益增长的全球能源需求,煤炭仍在能源生产中发挥着重要作用。去碳化的主要目标是减少温室气体排放,尤其是二氧化碳。提高煤炭使用效率有助于减少这些排放。烟煤的电磁活化已被用于脱水、除灰、脱硫和改善原煤的研磨工艺。本研究旨在研究利用微波辐射进行煤炭电磁活化的具体方法及其对不同变质阶段煤炭中发生的物理和化学过程的影响。结果表明,这种电磁处理会导致羟基的破坏和游离氢的形成。变质阶段较高的煤炭由于结构密度较高,因此升温较快。变质阶段较低的煤加热时间较长,需要更多的处理时间才能有效,同时需要较低的功率水平以避免机械破坏。活化时间和煤的粒度是重要因素;它们的最佳组合能产生最大效果。这些发现有助于优化不同煤种的微波处理参数,从而提高煤炭利用效率并减少对环境的影响。
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引用次数: 0
CO2 absorption with polyethyleneimine solution intensified by a rotating packed bed with liquid detention 用液体截留旋转填料床加强聚乙烯亚胺溶液对二氧化碳的吸收
IF 6.7 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-03 DOI: 10.1016/j.fuel.2024.133318
This study explored the absorption of CO2 by the polyethyleneimine (PEI) solution in a rotating packed bed (RPB). In order to boost the CO2 absorption effect, the liquid detention phenomenon in the RPB was utilized to overcome the short residence time of liquid. The effects of different operating parameters on CO2 absorption efficiency (η) and gas-phase volumetric mass transfer coefficient (KGav) in the RPB were investigated. The experimental results indicated that the RPB can greatly intensify the absorption of CO2. η and KGav increased from 3.3 % and 0.041 kmol·m−3·h−1·kPa−1 to 76.0 % and 1.634 kmol·m−3·h−1·kPa−1, respectively, as the rotational speed of the RPB rose from zero to 700 rpm with 250 mL detained liquid. It was also found that the liquid detention phenomenon can significantly elevate η and KGav as a result of extended liquid residence time and increased liquid holdup in the RPB. When the detained liquid volume increased from zero to 250 mL, η and KGav increased by 55.6 % and 113.1 %, respetively. In addition, it was observed that CO2 load in the rich PEI solution increased from 9.650 to 11.189 molCO2/kg PEI while η remained around 85 % after five cycles of absorption–desorption, suggesting an excellent cyclic stability of PEI. This work contributes to the development of viable CO2 capture technologies by intensifying the CO2 absorption process in the RPB with an efficient absorbent.
本研究探讨了旋转填料床(RPB)中聚乙烯亚胺(PEI)溶液对二氧化碳的吸收。为了提高二氧化碳的吸收效果,利用了液体在 RPB 中的滞留现象来克服液体停留时间短的问题。研究了不同操作参数对 RPB 中二氧化碳吸收效率(η)和气相体积传质系数(KGav)的影响。实验结果表明,当 RPB 的转速从 0 rpm 升至 700 rpm 时,η 和 KGav 分别从 3.3 % 和 0.041 kmol-m-3-h-1-kPa-1 增加到 76.0 % 和 1.634 kmol-m-3-h-1-kPa-1。研究还发现,由于延长了液体在 RPB 中的停留时间和增加了液体滞留,液体滞留现象会显著提高 η 和 KGav。当滞留液体量从零增加到 250 毫升时,η 和 KGav 分别增加了 55.6% 和 113.1%。此外,还观察到富 PEI 溶液中的二氧化碳负荷从 9.650 molCO2/kg PEI 增加到 11.189 molCO2/kg PEI,而经过五个吸收-解吸循环后,η 仍保持在 85% 左右,这表明 PEI 具有极佳的循环稳定性。这项研究利用一种高效吸收剂强化了 RPB 中的二氧化碳吸收过程,为开发可行的二氧化碳捕集技术做出了贡献。
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引用次数: 0
Biochars from waste as an additive material in anaerobic co-digestion: Characterization and application in batch and semi-continuous systems 从废物中提取生物炭作为厌氧联合消化的添加材料:间歇式和半连续式系统中的表征和应用
IF 6.7 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-03 DOI: 10.1016/j.fuel.2024.133342
The conversion of organic waste into energy through anaerobic digestion (AD) is a profitable and environmentally friendly strategy. Enhancing the process is crucial for optimizing and maximizing biogas and methane production. To achieve this, various strategies can be employed, such as anaerobic co-digestion (co-AD) and the use of biochar. Biochar aids in process stability, provides buffering capacity, mitigates inhibitory toxins, immobilizes microorganisms, facilitates microbial colonization, and accelerates electron transfer between microorganisms. This study aimed to produce biochar from different wastes and pyrolysis temperatures and to investigate its use as an additive material in the co-AD of fruit and vegetable waste (FVW) and laying chicken manure (LCM) in batch and semi-continuous systems. Thermogravimetric analysis (TGA) and differential scanning calorimetry were performed to determine the pyrolysis temperature for biochar production, defining temperatures of 450 and 550 °C. A biochemical methane potential (BMP) test was conducted in 120 mL reactors (working volume) with the addition of 10 g/L of biochar from FVW, LCM, and wood pruning waste (WPW). WPW450 biochar showed the highest fixed carbon content, rough surface, and deep porous structure, factors that contributed to a 28 % increase in methane production compared to the control. Semi-continuous tests were conducted in 50 L reactors (working volume) using a reduced dosage (1 g/L) of WPW450 biochar, providing process stability and better biogas quality, resulting in a 31 % increase in methane production. The reduction in biochar dosage did not negatively impact the semi-continuous system, which showed a 74 % higher methane yield compared to the batch system. The results of this study highlight the importance of biochar addition to increase methane production in the co-AD of FVW and LCM at different scales, as well as the study of different biomasses and temperatures for biochar production.
通过厌氧消化(AD)将有机废物转化为能源是一项既有利可图又环保的战略。改进工艺对于优化和最大限度地提高沼气和甲烷产量至关重要。为此,可以采用多种策略,如厌氧协同消化(co-AD)和使用生物炭。生物炭有助于提高工艺稳定性、提供缓冲能力、减轻抑制性毒素、固定微生物、促进微生物定植以及加速微生物之间的电子传递。本研究旨在利用不同的废物和热解温度生产生物炭,并研究生物炭在间歇式和半连续式系统中作为果蔬废物(FVW)和蛋鸡粪(LCM)共同厌氧消化的添加材料的用途。通过热重分析(TGA)和差示扫描量热法确定生物炭生产的热解温度,确定温度为 450 和 550 °C。在 120 毫升反应器(工作容积)中加入 10 克/升来自 FVW、LCM 和木材修剪废料(WPW)的生物炭后,进行了生化甲烷潜能(BMP)测试。WPW450 生物炭显示出最高的固定碳含量、粗糙的表面和深孔隙结构,与对照组相比,这些因素使甲烷产量增加了 28%。在 50 升反应器(工作容积)中进行了半连续试验,减少了 WPW450 生物炭的用量(1 克/升),提高了工艺稳定性和沼气质量,使甲烷产量增加了 31%。生物炭用量的减少并未对半连续式系统产生负面影响,该系统的甲烷产量比间歇式系统高出 74%。这项研究的结果突显了在不同规模的 FVW 和 LCM 共同厌氧发酵中添加生物炭以提高甲烷产量的重要性,以及对不同生物质和生物炭生产温度进行研究的重要性。
{"title":"Biochars from waste as an additive material in anaerobic co-digestion: Characterization and application in batch and semi-continuous systems","authors":"","doi":"10.1016/j.fuel.2024.133342","DOIUrl":"10.1016/j.fuel.2024.133342","url":null,"abstract":"<div><div>The conversion of organic waste into energy through anaerobic digestion (AD) is a profitable and environmentally friendly strategy. Enhancing the process is crucial for optimizing and maximizing biogas and methane production. To achieve this, various strategies can be employed, such as anaerobic co-digestion (co-AD) and the use of biochar. Biochar aids in process stability, provides buffering capacity, mitigates inhibitory toxins, immobilizes microorganisms, facilitates microbial colonization, and accelerates electron transfer between microorganisms. This study aimed to produce biochar from different wastes and pyrolysis temperatures and to investigate its use as an additive material in the co-AD of fruit and vegetable waste (FVW) and laying chicken manure (LCM) in batch and semi-continuous systems. Thermogravimetric analysis (TGA) and differential scanning calorimetry were performed to determine the pyrolysis temperature for biochar production, defining temperatures of 450 and 550 °C. A biochemical methane potential (BMP) test was conducted in 120 mL reactors (working volume) with the addition of 10 g/L of biochar from FVW, LCM, and wood pruning waste (WPW). WPW450 biochar showed the highest fixed carbon content, rough surface, and deep porous structure, factors that contributed to a 28 % increase in methane production compared to the control. Semi-continuous tests were conducted in 50 L reactors (working volume) using a reduced dosage (1 g/L) of WPW450 biochar, providing process stability and better biogas quality, resulting in a 31 % increase in methane production. The reduction in biochar dosage did not negatively impact the semi-continuous system, which showed a 74 % higher methane yield compared to the batch system. The results of this study highlight the importance of biochar addition to increase methane production in the co-AD of FVW and LCM at different scales, as well as the study of different biomasses and temperatures for biochar production.</div></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":null,"pages":null},"PeriodicalIF":6.7,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142420016","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Beyond gas supersaturation: Dissecting the secondary formation of methane hydrate 超越气体过饱和:剖析甲烷水合物的二次形成
IF 6.7 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-02 DOI: 10.1016/j.fuel.2024.133310
Rapid secondary formation of gas hydrate is a critical issue in gas transportation and at the same time has foreseeable potential in future gas storage. Despite the devoted research in the past decade, the intrinsic mechanism of the secondary formation of gas hydrate, is still an on-going subject of debate. Because the secondary formation of gas hydrate is commonly observed under conditions with extraordinarily high content of gas, gas supersaturation is hypothesized as one crucial mechanism. To dissect the gas supersaturation hypothesis, Molecular Dynamics simulations were conducted systematically with hydrate secondary formation in solutions with various gas concentrations covering supersaturation conditions. The effects of key parameters influencing the secondary formation of hydrate, including system temperature and local methane concentration, were explored. The results revealed for the first time a U-shape-like trend in the induction time of hydrate formation with the increase of gas concentration, pinpointing an optimal gas content with the given environmental temperature and pressure. Importantly, the findings highlighted the needed revision of the current gas supersaturation hypothesis in both methane hydrate mitigation and application. This work not only advanced the current understanding of the secondary formation of methane hydrate but also contributed to the fundamental knowledge essential for future gas storage by gas hydrates.
天然气水合物的快速二次形成是天然气运输中的一个关键问题,同时在未来的天然气储存中也具有可预见的潜力。尽管过去十年间人们对其进行了深入研究,但天然气水合物二次形成的内在机理仍是一个争论不休的问题。由于气体水合物的二次形成通常是在气体含量极高的条件下观察到的,因此气体过饱和被假定为一种关键机制。为了剖析气体过饱和假说,我们在不同气体浓度的溶液中,在过饱和条件下,对水合物的二次形成进行了系统的分子动力学模拟。研究探讨了影响水合物二次形成的关键参数的影响,包括系统温度和局部甲烷浓度。结果首次发现,随着气体浓度的增加,水合物形成的诱导时间呈 U 型趋势,从而确定了特定环境温度和压力下的最佳气体含量。重要的是,研究结果强调了在甲烷水合物缓解和应用方面对当前气体过饱和假说进行必要修正的必要性。这项工作不仅推进了当前对甲烷水合物二次形成的理解,还为未来利用天然气水合物储存天然气提供了必要的基础知识。
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引用次数: 0
Controlled synthesis of the M doped (M = Fe, Cu, Zn, Mn)-Co4S3/Ni3S2 catalyst with high electrocatalytic performance for hydrogen evolution reaction in seawater and urea 掺杂 M(M = Fe、Cu、Zn、Mn)-Co4S3/Ni3S2 催化剂的可控合成及其在海水和尿素中氢进化反应的高电催化性能
IF 6.7 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-02 DOI: 10.1016/j.fuel.2024.133314
Electrolysis of seawater is a promising method for producing hydrogen, but sluggish reaction kinetics and electrolyte containing corrosive ions limit its development. In this work, a series of M doped (M = Fe, Cu, Zn, Mn)-Co4S3/Ni3S2 catalyst has been prepared on Ni foam by hydrothermal method with excellent seawater and urea splitting performance. The unique 3D porous structure provides a large number of active sites for the catalyst, which has strong catalytic activity. Fe-Co4S3/Ni3S2 electrode showed excellent hydrogen evolution reaction (HER) catalytic activity in 1 M KOH + seawater and 1 M KOH + 0.5 M urea, driving a current density of 10 mA cm−2 at a low overpotential of 81 and 66 mV. In addition, Fe-Co4S3/Ni3S2 electrode also shows strong stability in 15 h stability test. The results show that although the impurity ions in seawater affect the activity of catalyst, the corrosion resistance of catalyst also improves the catalytic activity and stability. Density functional theory calculations show that this Fe-Co4S material exhibits the optimal Gibbs free energy of hydrogen, the introduction of this Ni3S2 material enhances the electrical conductivity of the material, and the synergistic catalysis of the two materials promotes the optimal hydrogen production performance of the Fe-Co4S3/Ni3S2 material. This work provides a novel understanding for the research of catalysts used in the electrolysis of seawater and urea.
电解海水是一种很有前途的制氢方法,但反应动力学缓慢和电解液含有腐蚀性离子限制了其发展。本研究采用水热法在泡沫镍上制备了一系列掺杂 M(M = Fe、Cu、Zn、Mn)-Co4S3/Ni3S2 催化剂,具有优异的海水和尿素拆分性能。独特的三维多孔结构为催化剂提供了大量的活性位点,具有很强的催化活性。在 1 M KOH + 海水和 1 M KOH + 0.5 M 尿素中,Fe-Co4S3/Ni3S2 电极表现出优异的氢进化反应催化活性,在 81 和 66 mV 的低过电位下可驱动 10 mA cm-2 的电流密度。此外,Fe-Co4S3/Ni3S2 电极在 15 小时稳定性测试中也表现出很强的稳定性。结果表明,虽然海水中的杂质离子会影响催化剂的活性,但催化剂的耐腐蚀性也提高了催化活性和稳定性。密度泛函理论计算表明,Fe-Co4S 材料具有最佳的氢气吉布斯自由能,Ni3S2 材料的引入增强了材料的导电性,两种材料的协同催化促进了 Fe-Co4S3/Ni3S2 材料的最佳制氢性能。这项工作为研究用于电解海水和尿素的催化剂提供了新的认识。
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引用次数: 0
Multiple active sites of CuO/CeO2 catalysts toward enhanced hydrogenolysis of hardwood lignin into phenolic monomers CuO/CeO2 催化剂的多个活性位点可增强硬木木质素氢解为酚类单体的能力
IF 6.7 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-02 DOI: 10.1016/j.fuel.2024.133301
Reductive catalytic deconstruction (RCD) is a promising strategy for achieving high-value added utilization of lignocellulose. Herein, we report a CuO/CeO2 catalyst with multiple active sites for effective RCD lignocellulose into phenolic compounds, affording monomer yields up to 41.9 wt%. Notably, this fabricated catalyst achieves rapidly hydrogenolysis of hardwood lignin with yields of 32.7 wt% within 1 h. The enhanced catalytic reactivity is obtained by the efficient C–O bond scission, which is confirmed by the nuclear magnetic resonance spectra and examination of lignin model compound reactions. Moreover, the resultant CuO/CeO2 catalyst reveals relatively stability under a H2 atmosphere duo to the strong interactions between nanorods CeO2 and Cu. The effects of key parameters, such as time, temperature and solvent, were investigated by monomeric yields. This work provides new insights into lignin first strategy and paves the way for the rational design of non-precious metal catalysts with multiple-active sites.
还原催化解构(RCD)是实现木质纤维素高附加值利用的一种前景广阔的策略。在此,我们报告了一种具有多个活性位点的 CuO/CeO2 催化剂,可有效地将木质纤维素还原催化分解成酚类化合物,单体产率高达 41.9 wt%。值得注意的是,这种催化剂能在 1 小时内实现硬木木质素的快速氢解,产率达 32.7 wt%。催化反应活性的增强得益于高效的 C-O 键裂解,这一点已通过核磁共振谱和木质素模型化合物反应的检测得到证实。此外,由于纳米棒 CeO2 和 Cu 之间的强相互作用,生成的 CuO/CeO2 催化剂在 H2 大气中显示出相对的稳定性。通过单体产量研究了时间、温度和溶剂等关键参数的影响。这项工作为木质素第一策略提供了新的见解,并为合理设计具有多活性位点的非贵金属催化剂铺平了道路。
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引用次数: 0
Designing organic structure-directing agent for cost-effective production of multipore MSE zeolite 设计有机结构引导剂,以经济高效的方式生产多孔 MSE 沸石
IF 6.7 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-02 DOI: 10.1016/j.fuel.2024.133274
Multipore MSE zeolite possesses three-dimensional (3D) pore-network constructed of interconnected 10- and 12- membered rings (MRs), i.e., between its broadly used cousins, medium-pore MFI and large-pore Beta, and has exhibited promising catalytic performances in catalytic cracking reactions. One major bottleneck for the commercial deployment of MSE zeolite is the prohibitive production cost due to the use of expensive organic structure directing agent (OSDA). We report here a designed inexpensive OSDA, dispiro[piperidine-1,2′-(1′,2′,3′,5′,6′,7′-hexahydrobenzo [1,2-c: 4, 5-c′] dipyrrolium)-6′,1″-piperidine, that can better stabilize the framework and is specific to the generation of MSE in the presence of K+. The OSDA is occluded in the supercage and 12-MR straight channel, while the K+ occupies the 625442 cage, affording high crystallinity and strong acidity. The dealuminated zeolite shows improved light olefin (in particular, propylene) selectivity and catalyst lifetime in catalytic cracking of typical naphtha pool molecule n-heptane. The recipe is a step forward for the specific, low-cost generation of the MSE zeolite and may inspire more investigations on its catalytic applications.
多孔 MSE 沸石具有三维(3D)孔网,由相互连接的 10 个和 12 个成员环(MR)构成,介于中孔 MFI 和大孔 Beta 之间,在催化裂解反应中表现出良好的催化性能。MSE 沸石商业化应用的一个主要瓶颈是由于使用昂贵的有机结构引导剂(OSDA)而导致生产成本过高。我们在此报告了一种设计廉价的 OSDA,二螺[哌啶-1,2′-(1′,2′,3′,5′,6′,7′-六氢苯并[1,2-c:4,5-c′]二吡咯烷)-6′,1″-哌啶,它能更好地稳定框架,并能在 K+ 存在下生成特定的 MSE。OSDA 被封闭在超笼子和 12-MR 直通道中,而 K+ 则占据 625442 笼子,因此具有高结晶性和强酸性。在催化裂解典型石脑油池分子正庚烷时,脱铝沸石显示出更好的轻烯烃(尤其是丙烯)选择性和催化剂寿命。该配方在特定、低成本生成 MSE 沸石方面向前迈出了一步,并可能激发对其催化应用的更多研究。
{"title":"Designing organic structure-directing agent for cost-effective production of multipore MSE zeolite","authors":"","doi":"10.1016/j.fuel.2024.133274","DOIUrl":"10.1016/j.fuel.2024.133274","url":null,"abstract":"<div><div>Multipore <strong>MSE</strong> zeolite possesses three-dimensional (3D) pore-network constructed of interconnected 10- and 12- membered rings (MRs), i.e., between its broadly used cousins, medium-pore MFI and large-pore Beta, and has exhibited promising catalytic performances in catalytic cracking reactions. One major bottleneck for the commercial deployment of <strong>MSE</strong> zeolite is the prohibitive production cost due to the use of expensive organic structure directing agent (OSDA). We report here a designed inexpensive OSDA, dispiro[piperidine-1,2′-(1′,2′,3′,5′,6′,7′-hexahydrobenzo [1,2-c: 4, 5-c′] dipyrrolium)-6′,1″-piperidine, that can better stabilize the framework and is specific to the generation of <strong>MSE</strong> in the presence of K<sup>+</sup>. The OSDA is occluded in the supercage and 12-MR straight channel, while the K<sup>+</sup> occupies the 6<sup>2</sup>5<sup>4</sup>4<sup>2</sup> cage, affording high crystallinity and strong acidity. The dealuminated zeolite shows improved light olefin (in particular, propylene) selectivity and catalyst lifetime in catalytic cracking of typical naphtha pool molecule <em>n</em>-heptane. The recipe is a step forward for the specific, low-cost generation of the MSE zeolite and may inspire more investigations on its catalytic applications.</div></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":null,"pages":null},"PeriodicalIF":6.7,"publicationDate":"2024-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142419929","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Quercus ballot as an innovative feedstock for biodiesel production using ZnO nanocatalyst 使用 ZnO 纳米催化剂将柞树选票作为生产生物柴油的创新原料
IF 6.7 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2024-10-02 DOI: 10.1016/j.fuel.2024.133307
Selecting non-edible plant seed oil remains the best choice for biodiesel production using an effective nanocatalyst. In this study, the ZnO was prepared as a nanocatalyst using an aqueous extract from the Alhaji marorum plant. Nano ZnO has shown high catalytic activity, is cost-effective, environmentally friendly and converts triglycerides into fatty acid methyl esters. The results indicate that ZnO nanocatalyst exhibit a high specific surface area (146.82 m2 g-1), large pore volume (0.35 cm3 g-1), and an average crystallite size of 42.3 nm. The FESEM analysis shows that the particle size of ZnO lies in the range of 30–50 nm with a rod shape and densely packed morphology. The biodiesel is produced using a transesterification process from novel non-edible Quercus ballot plant seeds. The resulting biodiesel has a 98.06 % yield under a methanol/oil ratio of 6:1 with 0.5 wt% ZnO nanocatalyst at 65 °C for 80 min. It is established that the methanol-to-oil ratio and the catalyst concentration significantly affect the transesterification reaction. The biodiesel produced is characterized by GC–MS to determine its exact composition and FTIR is used to confirm functional groups and is evaluated according to ASTM D6751.
选择非食用植物种子油仍然是使用有效的纳米催化剂生产生物柴油的最佳选择。本研究使用 Alhaji marorum 植物的水提取物制备了纳米氧化锌催化剂。纳米氧化锌具有催化活性高、成本效益高、环境友好等特点,可将甘油三酯转化为脂肪酸甲酯。研究结果表明,纳米氧化锌催化剂具有高比表面积(146.82 m2 g-1)、大孔径(0.35 cm3 g-1)和 42.3 nm 的平均结晶尺寸。FESEM 分析表明,氧化锌的粒径在 30-50 纳米之间,呈棒状,形态密集。生物柴油是利用新型非食用柞树种子的酯交换过程生产的。在甲醇/油比例为 6:1 的条件下,使用 0.5 wt% 的 ZnO 纳米催化剂,在 65 °C 下反应 80 分钟,生物柴油的产量为 98.06%。结果表明,甲醇与油的比例和催化剂浓度对酯交换反应有显著影响。生成的生物柴油通过气相色谱-质谱仪(GC-MS)进行表征,以确定其确切成分,傅立叶变换红外光谱(FTIR)用于确认官能团,并根据 ASTM D6751 进行评估。
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