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Pd nanocatalyst supported on amine-functionalized mesoporous graphitic carbon nitride for formic acid hydrogen generator in the polymer electrolyte membrane fuel cell system 用于聚合物电解质膜燃料电池系统中甲酸制氢器的、支撑在胺功能介孔氮化石墨碳上的钯纳米催化剂
IF 7.2 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2024-09-24 DOI: 10.1016/j.fuproc.2024.108133
Tae Hoon Lee , Seong Mo Yun , Min Jae Kim , Gibeom Kim , Eun Sang Jung , Taek Hyun Oh
Pd nanocatalyst supported on amine-functionalized mesoporous graphitic carbon nitride (Pd/NH2-mpg-C3N4) was investigated for dehydrogenation of formic acid. The catalyst was analyzed and tested to investigate the effect of amine functionalization on hydrogen generation from formic acid. Pd nanocatalyst was dispersed uniformly on NH2-mpg-C3N4 without agglomeration. The turnover frequency value of Pd/NH2-mpg-C3N4 was 1870 h−1, which was higher than that of Pd/mpg-C3N4 because of the amine functionalization. The Pd/NH2-mpg-C3N4 was also tested to investigate the effect of various reaction conditions (formic acid concentration, sodium formate concentration, and reaction temperature) on hydrogen generation from formic acid. Formic acid concentration negatively affected the catalytic activity, whereas sodium formate concentration positively affected it. Reaction temperature significantly affected the catalytic activity. The apparent activation energy of the Pd/NH2-mpg-C3N4 catalyst was 60.7 kJ mol−1, and a hydrogen generator with the catalyst exhibited high conversion efficiency at an elevated temperature. Consequently, a hydrogen generator with Pd/NH2-mpg-C3N4 is suitable for polymer electrolyte membrane fuel cell systems.
研究了以胺功能化介孔氮化石墨(Pd/NH2-mpg-C3N4)为载体的钯纳米催化剂在甲酸脱氢过程中的应用。对催化剂进行了分析和测试,以研究胺官能化对甲酸制氢的影响。钯纳米催化剂均匀地分散在 NH2-mpg-C3N4 上,没有团聚现象。由于胺官能化,Pd/NH2-mpg-C3N4 的翻转频率值为 1870 h-1,高于 Pd/mpg-C3N4 的翻转频率值。此外,还对 Pd/NH2-mpg-C3N4 进行了测试,以研究各种反应条件(甲酸浓度、甲酸钠浓度和反应温度)对甲酸制氢的影响。甲酸浓度对催化活性有负面影响,而甲酸钠浓度对催化活性有正面影响。反应温度对催化活性有明显影响。Pd/NH2-mpg-C3N4 催化剂的表观活化能为 60.7 kJ mol-1,使用该催化剂的制氢装置在高温下具有较高的转化效率。因此,使用 Pd/NH2-mpg-C3N4 的氢气发生器适用于聚合物电解质膜燃料电池系统。
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引用次数: 0
An experimental investigation of the impacts of titanium dioxide (TiO2) and ethanol on performance and emission characteristics on diesel engines run with castor Biodiesel ethanol blended fuel 二氧化钛(TiO2)和乙醇对使用蓖麻生物柴油乙醇混合燃料的柴油发动机性能和排放特性影响的实验研究
IF 7.2 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2024-09-21 DOI: 10.1016/j.fuproc.2024.108137
Dinku Seyoum Zeleke, Addisu Kassahun Tefera
Investigating the impact of ethanol and TiO2 on the performance and emission characteristics of diesel engines running on a blend of ethanol and castor biodiesel is the primary goal of this study. The nanoparticles of ethanol, biodiesel, and TiO2 diesel fuel were combined at several concentrations. Diesel, B10, B20, B30, B10E10T, B20E10T, B30E10T, B10E20T, B20E20T, and B30E20T were among the various fuels that were investigated. The physiochemical properties of all the sample fuels were assessed, including density, pour point, cloud point, fire point, flash point, and kinematic viscosity. Following this, other engine performance indicators, such as torque, power, and fuel-consumption, were examined. Studies were also carried out on the properties of emissions, including CO, CO2, HC, and NO. Peak braking power and engine torque were found for each fuel under investigation at around 2750 and 2500 rpm, respectively. The addition reduced the brake-specific fuel consumption for B10E20T by 7.41 % while increasing the braking engine's torque and power by 8.64 and 3.86 %, respectively, in compared to blends without the TiO2 additions. When compared to diesel, the exhaust emission data without the addition of TiO2 revealed a decrease in CO and HC emissions but an increase in CO2 and NO emissions. On the other hand, using ethanol blend reduced NO emissions. According to the overall findings, diesel engine performance, combustion characteristics, and exhaust gas emissions were enhanced averagely by 7.43 % when a certain ratio of ethanol, biodiesel, and TiO2 additives (B10E20 + 50 ppm) was used.
本研究的主要目的是调查乙醇和二氧化钛对使用乙醇和蓖麻生物柴油混合燃料的柴油发动机的性能和排放特性的影响。乙醇、生物柴油和 TiO2 柴油的纳米颗粒以多种浓度混合。研究的燃料包括柴油、B10、B20、B30、B10E10T、B20E10T、B30E10T、B10E20T、B20E20T 和 B30E20T。对所有样本燃料的理化特性进行了评估,包括密度、倾点、浊点、燃点、闪点和运动粘度。随后,还考察了其他发动机性能指标,如扭矩、功率和耗油量。此外,还对 CO、CO2、HC 和 NO 等排放物的特性进行了研究。研究发现,每种燃料的峰值制动功率和发动机扭矩分别约为 2750 rpm 和 2500 rpm。与不添加二氧化钛的混合燃料相比,添加二氧化钛使 B10E20T 的制动油耗降低了 7.41%,同时使制动发动机的扭矩和功率分别提高了 8.64% 和 3.86%。与柴油相比,未添加二氧化钛的废气排放数据显示 CO 和 HC 排放有所减少,但 CO2 和 NO 排放有所增加。另一方面,使用乙醇混合物则减少了氮氧化物的排放。根据总体研究结果,当使用一定比例的乙醇、生物柴油和二氧化钛添加剂(B10E20 + 50 ppm)时,柴油发动机的性能、燃烧特性和废气排放平均提高了 7.43%。
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引用次数: 0
Investigation of NO reduction mechanism of nitrogen-impregnated biomass across wide temperature range 氮浸渍生物质在宽温度范围内的氮氧化物还原机制研究
IF 7.2 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2024-09-20 DOI: 10.1016/j.fuproc.2024.108132
Jing Wang , Yingying Qu , Xinyu Jiang , Frédéric Marias , Fei Wang , Yuanyuan Zhang
Traditional denitrification methods for coal-fired power boilers face challenges like reduced flue gas temperature at low loads, decreased efficiency of existing denitrification devices, and increased ammonia consumption. Biomass, a renewable energy source, has proven effective for denitrification in medium to high-temperature ranges. To improve denitrification efficiency at low loads, this study focuses on optimizing re-burning denitrification of biomass by nitrogen-impregnated of corncob at room temperature. Investigating the effects of nitrogen impregnation and washing on biomass re-burning denitrification reactivity within 550–950 °C, the study finds that denitrification efficiency improvement is not caused only by surface-covered urea or washing. Nitrogen impregnation enhances biomass pyrolysis, releasing more CO, HCN, and NH3 products, thereby enhancing NO reduction during denitrification. Additionally, nitrogen impregnation boosts nitrogen-containing functional groups such N-6 on biomass char surfaces during the re-burning process, improving denitrification efficiency. The maximum denitrification efficiency of the nitrogen impregnated sample reached 97.52 % at 950 °C, while it reached 76.51 % at 650 °C when the coated urea was washed. Furthermore, chlorine and alkali metal contents in biomass notably decrease after nitrogen-impregnation and washing, optimizing biomass combustion conditions for furnace protection. This study offers theoretical insights for promoting and applying biomass denitrification techniques.
燃煤发电锅炉的传统脱硝方法面临着低负荷时烟气温度降低、现有脱硝装置效率降低以及氨消耗量增加等挑战。生物质作为一种可再生能源,已被证明可在中高温范围内有效脱硝。为了提高低负荷下的脱硝效率,本研究重点关注优化室温下玉米芯浸氮对生物质的再燃烧脱硝。通过研究氮浸渍和洗涤对 550-950 ℃ 范围内生物质再燃脱硝反应活性的影响,研究发现脱硝效率的提高并不仅仅是由表面覆盖尿素或洗涤引起的。氮浸渍可促进生物质热解,释放出更多的 CO、HCN 和 NH3 产物,从而提高脱硝过程中的 NO 还原能力。此外,氮浸渍还能在再燃烧过程中提高生物质炭表面的含氮官能团(如 N-6),从而提高脱硝效率。氮浸渍样品在 950 ℃ 时的最大脱硝效率达到 97.52%,而在 650 ℃ 洗涤涂层尿素时的脱硝效率为 76.51%。此外,经过氮浸渍和洗涤后,生物质中的氯和碱金属含量明显降低,从而优化了生物质燃烧条件以保护炉子。这项研究为推广和应用生物质脱硝技术提供了理论依据。
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引用次数: 0
Investigation of the mechanism behind the surge in nitrogen dioxide emissions in engines transitioning from pure diesel operation to methanol/diesel dual-fuel operation 研究从纯柴油发动机过渡到甲醇/柴油双燃料发动机时二氧化氮排放量激增的机理
IF 7.2 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2024-09-19 DOI: 10.1016/j.fuproc.2024.108131
Qiao Huang , Ruomiao Yang , Junheng Liu , Tianfang Xie , Jinlong Liu
In diesel engines, nitrogen monoxide (NO) is the predominant component of nitrogen oxides (NOx) emissions. However, when transitioning to methanol/diesel dual-fuel operation, even with a small percentage of methanol replacing diesel energy (e.g. 10 %), the concentration of nitrogen dioxide (NO2) increases significantly, becoming comparable to that of NO. This study employs multi-dimensional computational fluid dynamics (CFD) modeling to reproduce this NO2/NOx surge ratio phenomenon and investigates the underlying mechanism driving the surge in NO2 emissions, an area insufficiently explored in existing literature. By comparing CFD simulations with and without the NO+HO2↔NO2 + OH reaction in the chemical mechanism, the results reveal that the surge in NO2 concentration disappears when this reaction is invalidated, while engine efficiency, combustion phasing, and overall NOx emissions remain largely unchanged. This indicates that the NO+HO2↔NO2 + OH reaction is the primary contributor to the sudden increase in the NO2/NOx ratio. Further analysis during the main combustion stage shows that the diesel spray splits into two distinct regions after impinging on the bowl boundary, with one region deep within the bowl and the other near the squish region. During the late oxidation stage, the diffusion flame directed towards the deep bowl area remains a high-temperature zone with a high concentration of NO, whereas the flame near the squish region evolves into a low-temperature zone due to effective mixing with the low-temperature methanol/air mixture. In these low-temperature regions, almost all NO formed during the main combustion stage is converted to NO2 during the late oxidation stage, leading to the observed NO2/NOx ratio surge. Methanol oxidation contributes HO2 radicals, which facilitate the NO-to-NO2 conversion. Consequently, the low-temperature oxidation of methanol outside the high-temperature region does not lead to thermal ignition but is instead responsible for the rare occurrence of the NO2 surge.
在柴油发动机中,一氧化氮(NO)是氮氧化物(NOx)排放的主要成分。然而,当过渡到甲醇/柴油双燃料运行时,即使甲醇替代柴油的比例很小(例如 10%),二氧化氮(NO2)的浓度也会显著增加,与氮氧化物的浓度相当。本研究采用多维计算流体动力学(CFD)建模来再现这种 NO2/NOx 比率激增现象,并研究驱动 NO2 排放量激增的内在机制,现有文献在这一领域的研究还不够深入。通过比较在化学机制中包含和不包含 NO+HO2↔NO2 + OH 反应的 CFD 模拟,结果显示,当该反应无效时,NO2 浓度激增现象消失,而发动机效率、燃烧阶段和整体 NOx 排放量基本保持不变。这表明 NO+HO2↔NO2 + OH 反应是导致 NO2/NOx 比率突然增加的主要原因。对主燃烧阶段的进一步分析表明,柴油喷射在撞击燃烧碗边界后会分裂成两个不同的区域,一个区域位于燃烧碗深处,另一个则靠近压扁区域。在后期氧化阶段,朝向碗状深处的扩散火焰仍然是一个高温区,氮氧化物浓度较高,而靠近压扁区的火焰则由于与低温甲醇/空气混合物的有效混合而演变成一个低温区。在这些低温区,主要燃烧阶段形成的几乎所有 NO 都会在后期氧化阶段转化为 NO2,从而导致观察到的 NO2/NOx 比率激增。甲醇氧化会产生 HO2 自由基,从而促进 NO 向 NO2 的转化。因此,甲醇在高温区以外的低温氧化不会导致热点火,而是导致了罕见的 NO2 激增。
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引用次数: 0
Highly efficient Co-added Ni/CeO2 catalyst for co-production of hydrogen and carbon nanotubes by methane decomposition 通过甲烷分解协同生产氢气和碳纳米管的高效共添加 Ni/CeO2 催化剂
IF 7.2 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2024-09-13 DOI: 10.1016/j.fuproc.2024.108130
Jae-Rang Youn , Min-Jae Kim , Ki Cheol Kim , Mincheol Kim , Taesung Jung , Kang-Seok Go , Sang Goo Jeon , Woohyun Kim

The catalytic decomposition of methane (CDM) is a hydrogen and nanostructured carbon production process with minimal CO2 emission. Among the transition metal-based catalysts (e.g. Ni, Fe, Co, etc.), Ni-based catalysts are most widely studied due to the higher catalytic activity in decomposing methane. However, the limited lifespan of the catalyst makes it unsuitable for practical applications. Effective methane decomposition catalysts should be designed to optimize both reaction efficiency and catalyst lifetime. A Ni/CeO2 catalyst, developed in previous studies, Co was added to promote low-temperature (< 700 °C) activity manipulating the redox property of Co. Among the prepared catalysts with varying Ni:Co ratio, the methane conversion rate of the Ni8Co2/CeO2 catalyst was approximately twice that of the Ni10/CeO2 catalyst, confirming its excellent low-temperature activity. The reaction rate of Ni8Co2/CeO2 catalyst was 4.38 mmol/min∙gcat at 600 °C with WHSV of 36 L/gcat∙h. In terms of characteristics of carbon products, Raman spectroscopy analysis revealed that the carbon grown on the catalyst surface exhibited high crystallinity, with D-G band ratio (ID/IG) of 1.01. The fresh and used catalyst samples were characterized by TEM, XPS, XAS, and other methods to analyze the parameters affecting catalytic activity.

催化分解甲烷(CDM)是一种氢气和纳米碳生产工艺,二氧化碳排放量极低。在过渡金属基催化剂(如 Ni、Fe、Co 等)中,Ni 基催化剂由于在分解甲烷方面具有较高的催化活性而得到最广泛的研究。然而,催化剂的有限寿命使其不适合实际应用。设计有效的甲烷分解催化剂时,应同时优化反应效率和催化剂寿命。在所制备的不同 Ni:Co 比例的催化剂中,Ni8Co2/CeO2 催化剂的甲烷转化率约为 Ni10/CeO2 催化剂的两倍,证实了其出色的低温活性。Ni8Co2/CeO2 催化剂在 600 °C 时的反应速率为 4.38 mmol/min∙gcat,WHSV 为 36 L/gcat∙h。从碳产物的特征来看,拉曼光谱分析表明催化剂表面生长的碳具有较高的结晶度,D-G 带比(ID/IG)为 1.01。利用 TEM、XPS、XAS 等方法对新催化剂样品和使用过的催化剂样品进行了表征,以分析影响催化活性的参数。
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引用次数: 0
A simultaneous depolymerization and hydrodeoxygenation process to produce lignin-based jet fuel in continuous flow reactor 在连续流反应器中生产木质素喷气燃料的同时解聚和加氢脱氧工艺
IF 7.2 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2024-09-02 DOI: 10.1016/j.fuproc.2024.108129
Adarsh Kumar , David C. Bell , Zhibin Yang , Joshua Heyne , Daniel M. Santosa , Huamin Wang , Peng Zuo , Chongmin Wang , Ashutosh Mittal , Darryl P. Klein , Michael J. Manto , Xiaowen Chen , Bin Yang

Economical production of lignin-based jet fuel (LJF) can improve the sustainability of sustainable aviation fuels (SAFs) as well as can reduce the overall greenhouse gas emissions. However, the challenge lies in converting technical lignin polymer from biorefinery directly to jet fuel in a continuous operation. In this work, we demonstrate a simultaneous depolymerization and hydrodeoxygenation (SDHDO) process to produce lignin-based jet fuel from the alkali corn stover lignin (ACSL) using engineered Ru-HY-60-MI catalyst in a continuous flow reactor, for the first time. The maximum carbon yield of LJF of 17.9 wt% was obtained, and it comprised of 60.2 wt% monocycloalkanes, and 21.6 wt% polycycloalkanes. Catalyst characterization of Ru-HY-60-MI suggested there was no significant change in HY zeolite structure and its crystallinity after catalyst engineering. Catalyst characterizations performed post the SDHDO experiments indicate presence of carbon and K content in the catalyst. K content presence in the spent catalyst was due to K+ ion was exchanged between lignin solution and HY-60 while carbon presence validated the SDHDO chemistry on the catalyst surface. Tier α fuel property testing indicates that LJF production using SDHDO chemistry can produce SAF with high compatibility, good sealing properties, low emissions, and high energy density for aircraft.

经济地生产木质素基喷气燃料(LJF)可提高可持续航空燃料(SAF)的可持续性,并减少整体温室气体排放。然而,将生物炼制中的技术木质素聚合物直接连续转化为喷气燃料是一项挑战。在这项工作中,我们首次展示了一种同时解聚和加氢脱氧(SDHDO)工艺,该工艺使用工程化 Ru-HY-60-MI 催化剂在连续流反应器中从碱玉米秸秆木质素(ACSL)中生产木质素基喷气燃料。LJF 的最大碳产量为 17.9 wt%,其中包括 60.2 wt% 的单环烷烃和 21.6 wt% 的多环烷烃。Ru-HY-60-MI 的催化剂表征表明,催化剂工程后,HY 沸石的结构及其结晶度没有发生显著变化。在 SDHDO 实验后进行的催化剂表征表明,催化剂中存在碳和 K 含量。废催化剂中的 K 含量是由于 K+ 离子在木质素溶液和 HY-60 之间进行了交换,而碳的存在则验证了催化剂表面的 SDHDO 化学反应。Tier α 燃料性能测试表明,使用 SDHDO 化学方法生产 LJF 可以为飞机生产出兼容性高、密封性好、低排放和高能量密度的 SAF。
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引用次数: 0
Crystal structure of asphaltene under mechanical stress of ball milling 球磨机械应力下沥青烯的晶体结构
IF 7.2 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2024-08-27 DOI: 10.1016/j.fuproc.2024.108119
Fahad Al-Ajmi, Jun Li

This work aims to investigate the structural behaviour of asphaltene under mechanical stress using ball milling. Asphaltene samples were collected and separated from Kuwait export crude using n-heptane and subsequently ball milled for up to 24 h. X-ray diffraction was used to provide an insight into asphaltene macrostructure properties, which subsequently utilised to determine crystallite parameters. The results showed that the mechanical stress has a great influence on these structural parameters, with an increase of the aromatic sheet's inter-layer distance from 3.6 Å to 3.9 Å. While the height of stacked aromatic sheets per cluster and the number of stacked aromatic sheets per cluster decreased from 24.6 Å to 9.3 Å and 8 to 3.2, respectively. A significant increment in the aromaticity value was also observed after the ball milling experimentations, indicating mechanical stress induces cyclisation and aromatisation. The XRD profiles of the higher milling time samples reveals a high background intensity. This suggests a formation and/or increasing the proportion of highly disordered materials. In addition, the effects magnitude on asphaltene crystal parameters between the mechanical stress against heat stress was compared. The results showed core structural parameters are more sensitive to mechanical stress over heat stress.

这项研究旨在利用球磨法研究沥青质在机械应力作用下的结构行为。从科威特出口原油中收集并用正庚烷分离出沥青质样品,然后进行长达 24 小时的球磨。利用 X 射线衍射法深入了解沥青质的宏观结构特性,然后利用这些特性确定晶粒参数。结果表明,机械应力对这些结构参数有很大影响,芳香片的层间距离从 3.6 Å 增加到 3.9 Å,而每个簇的叠层芳香片高度和每个簇的叠层芳香片数量则分别从 24.6 Å 和 8 Å 下降到 9.3 Å 和 3.2 Å。在球磨实验后,还观察到芳香度值明显增加,这表明机械应力诱导了环化和芳香化。研磨时间较长的样品的 XRD 图谱显示出较高的背景强度。这表明高度无序材料的形成和/或比例增加。此外,还比较了机械应力和热应力对沥青晶体参数的影响程度。结果表明,核心结构参数对机械应力比对热应力更敏感。
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引用次数: 0
Multi-stage pretreatment of hydrothermal liquefaction biocrude oil as a precursor for sustainable aviation fuel production 将水热液化生物原油的多级预处理作为可持续航空燃料生产的前驱体
IF 7.2 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2024-08-26 DOI: 10.1016/j.fuproc.2024.108118
Sabrina Summers , Siyu Yang , Zixin Wang , Buchun Si , Harshal Kawale , Yuanhui Zhang

A major challenge for upgrading hydrothermal liquefaction biocrude into sustainable aviation fuel is the presence of inorganic material. Unlike commercial crude oil or biofuel from energy crops, excessive amounts of contaminants such as salt, water, and ash in biocrude oil from hydrothermal liquefaction can cause catalyst deactivation during hydroprocessing, decreased distillation efficiency, and equipment fouling from alkali deposits. Therefore, efficient removal of these impurities in HTL biocrude oil is essential. This work investigated a novel 3-stage pretreatment process, removing water, salt, and ash without chemicals, to produce a HTL biocrude oil precursor suitable for hydroprocessing. The influence of water to oil (W:O) ratio, temperature, and time on desalting efficiency was determined. After pretreatment, 81% of salt was removed, reducing total salt content to <0.1%. Improvements in elemental composition and physicochemical fuel properties were observed in biocrude oils from two feedstocks, with up to 39.8% decrease in oxygen content, 55% decrease in sulfur content, 22.2% decrease in nitrogen content, 9.86% increase in higher heating value, 73.4% decrease in total acid number, 99.9% decrease in viscosity, and 17.0% decrease in density. Compared with a single-step distillation as pretreatment, 3-stage pretreatment resulted in increased salt and heteroatom removal, improved heating value, and lower acidity. The precursor quality was viable for subsequential hydrotreating and other downstream refinery processes.

将热液液化生物原油升级为可持续航空燃料所面临的一个主要挑战是无机材料的存在。与商业原油或能源作物生物燃料不同,水热液化生物原油中过量的盐、水和灰分等杂质会导致加氢处理过程中催化剂失活、蒸馏效率降低以及碱沉积物造成设备堵塞。因此,有效去除高温热液化生物原油中的这些杂质至关重要。这项工作研究了一种新型的三阶段预处理工艺,在不使用化学品的情况下去除水、盐和灰分,从而生产出适合加氢处理的 HTL 生物原油前体。研究确定了水油比(W:O)、温度和时间对脱盐效率的影响。预处理后,81% 的盐分被去除,总含盐量降至 0.1%。从两种原料中提取的生物原油的元素组成和燃料理化性质得到了改善,氧含量降低了 39.8%,硫含量降低了 55%,氮含量降低了 22.2%,高热值提高了 9.86%,总酸值降低了 73.4%,粘度降低了 99.9%,密度降低了 17.0%。与单步蒸馏预处理相比,三步预处理增加了盐和杂原子的去除率,提高了热值,降低了酸度。前驱体质量可用于后续加氢处理和其他下游炼油工艺。
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引用次数: 0
Influence mechanism of emulsion collector on the flotation effect of coal gasification fine slag 乳化液捕收剂对煤气化细渣浮选效果的影响机理
IF 7.2 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2024-08-22 DOI: 10.1016/j.fuproc.2024.108120
Panpan Fan , Wenwen Dai , Xiaoting Fan , Lianping Dong , Jiancheng Wang , Weiren Bao , Liping Chang , Minqiang Fan

Coal gasification slag (CGS) presents significant challenge to the green and low-carbon development of the coal gasification industry due to its limited utilization restriction. In this study, cationic surfactant DTAB was used with kerosene to formulate an emulsion collector. The flotation results showed that, the increase in collector dosage could significantly improve the combustible recovery. At an optimal collector dosage of 10 kg/t, an increased DTAB ratio could significantly diminish the ash content of flotation concentrates and improve flotation precision. Through flotation dynamics experiments and fitting of the Fuerstenau upgrading curve, it confirmed that the entrainment of fine-grained particles with high ash content is the primary contributor to high ash content in flotation concentrates. Combined with FTIR spectroscopy, XPS and other analysis method, it validated that the surfactant effectively reduced the dispersed particle size of the agent, the increased contact angle of RC surface also improved hydrophobicity and improved particles hydrophobic agglomeration strength. Molecular dynamics simulation further illuminated that the surfactant covered part of the hydrophilic sites on the residue carbon (RC) surface and influenced the electrostatic interaction. The research results have important theoretical significance for perfecting the flotation theory of CGFS.

煤气化炉渣(CGS)因其有限的利用限制,对煤气化行业的绿色低碳发展提出了重大挑战。本研究采用阳离子表面活性剂 DTAB 与煤油配制成乳液捕收剂。浮选结果表明,增加捕收剂用量可显著提高可燃物回收率。在最佳捕收剂用量为 10 kg/t 时,增加 DTAB 的配比可显著降低浮选精矿的灰分含量,提高浮选精度。通过浮选动力学实验和福尔斯滕瑙提升曲线拟合,证实高灰分细粒的夹带是造成浮选精矿高灰分的主要原因。结合傅立叶变换红外光谱、XPS 等分析方法,验证了表面活性剂有效降低了药剂的分散粒度,RC 表面接触角的增大也改善了疏水性,提高了颗粒的疏水团聚强度。分子动力学模拟进一步表明,表面活性剂覆盖了残炭(RC)表面的部分亲水位点,并影响了静电作用。该研究成果对完善 CGFS 的浮选理论具有重要的理论意义。
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引用次数: 0
Highly effective Pt-Pd/ZSM-22 catalysts prepared by the room temperature electron reduction method for the n-hexadecane hydroisomerization 室温电子还原法制备的正十六烷加氢异构化高效 Pt-Pd/ZSM-22 催化剂
IF 7.2 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2024-08-14 DOI: 10.1016/j.fuproc.2024.108117
Huiyan Li , Kaihang Sun , Shuxiang Xiong , Wei Wang , Wei Wu

The development of highly effective bifunctional catalysts for n-hexadecane hydroisomerization is still essential to produce second-generation biodiesel. Herein, a Pt-Pd/ZSM-22-G (abbreviated as Pt-Pd/Z22-G) bimetallic catalyst was prepared by employing a room temperature electron reduction (RTER) method with glow discharge as the electron source. As a contrast, a series of Pt/Z22-H, Pd/Z22-H and Pt-Pd/Z22-H catalysts were prepared by the conventional hydrogen reduction method. The Pt-Pd/Z22-G catalyst reveals more exposed metal sites, larger CMe/CH+ values and an enhanced distribution of Pt-Pd(111) facets compared with the Pt/Z22-H, Pd/Z22-H and Pt-Pd/Z22-H catalysts. These modifications are originated from the stronger electron interactions and the smaller metal nanoparticles because of the effects of highly energetic reducing electrons. The n-hexadecane hydroisomerization results show that the iso-hexadecane yield over the Pt-Pd/Z22-G catalyst is 82.9%, which is the highest among four investigated catalysts in this work. This phenomenon occurs because more exposed Pt-Pd(111) facets and larger CMe/CH+ ratios are beneficial for the adsorption and hydrogenation of iso-alkene intermediates at metal sites to increase the iso-alkanes yield based on density functional theory (DFT) calculations. Furthermore, the iso-alkanes yield over the Pt-Pd/Z22-G catalyst also keeps steady after long-term tests for 120 h because of the limited metal aggregation and carbon deposition.

开发高效的正十六烷加氢异构化双功能催化剂对于生产第二代生物柴油仍然至关重要。本文采用室温电子还原(RTER)法,以辉光放电为电子源,制备了一种 Pt-Pd/ZSM-22-G(简称 Pt-Pd/Z22-G)双金属催化剂。相比之下,传统的氢还原法制备了一系列 Pt/Z22-H、Pd/Z22-H 和 Pt-Pd/Z22-H 催化剂。与 Pt/Z22-H、Pd/Z22-H 和 Pt-Pd/Z22-H 催化剂相比,Pt-Pd/Z22-G 催化剂暴露的金属位点更多,CMe/CH+ 值更大,Pt-Pd(111) 面分布更广。这些变化源于高能还原电子作用下更强的电子相互作用和更小的金属纳米颗粒。正十六烷加氢异构化结果表明,Pt-Pd/Z22-G 催化剂的异构十六烷产率为 82.9%,是本次研究的四种催化剂中产率最高的。出现这种现象的原因是,根据密度泛函理论(DFT)计算,更多的 Pt-Pd(111)面暴露和更大的 CMe/CH+ 比有利于异构烯中间体在金属位点的吸附和氢化,从而提高异构烷烃的产率。此外,由于金属聚集和碳沉积有限,Pt-Pd/Z22-G 催化剂上的异构烷烃产率在经过 120 小时的长期测试后也保持稳定。
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Fuel Processing Technology
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