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Low-temperature CO2 activation and methanation promoted by a hydroxyl-bearing Ni/complex-support catalyst 含羟基Ni/配合物载体催化剂促进低温CO2活化和甲烷化
IF 7.5 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-09 DOI: 10.1016/j.fuel.2026.138275
Baowang Lu , Jiahao Zhang , Jingyun Chen , Zhihua Han , Yuyu Liu , Yanyan Diao , Xingyun Li , Zepeng Wang , Zhou-jun Wang , Chaonan Cui
To gain a deeper understanding of the CO2 activation and methanation mechanism from a deeper perspective, a brand-new method was employed to track CO2 dissociation via DRIFT spectroscopy, instead of the traditional method of monitoring the methanation process with DRIFT spectroscopy. Herein, we designed complex-supports by incorporating CaO or CeO2 into SBA-15 to prepare Ni-based catalyst. These complexes significantly enhanced the catalytic activity of CO2 methanation, lowering the reaction temperature by approximately 60 °C. The CeO2 composite improved catalyst stability by suppressing polymeric carbon, while CaO exerted the opposite effect. Increasing the NiO amount in Ni/CeO2-SBA-15 had no significant impact on CH4 selectivity of ∼100 %, whereas it reduced CH4 selectivity in Ni/CaO-SBA-15 to below 100 %. Based on DRIFT observations, H2 dissociation species (Ni(H)) on Ni, spillover H species (Ni(H)s) and OH species (Ni(OH)s) were identified as three driving forces for CO2 dissociation. By compounding CaO or CeO2 into SBA-15, Ni(OH)s sites were found to significantly enhance the CO2 dissociation process, while no obvious enhancement was observed for Ni(H) and Ni(H)s sites. CO and formate were detected as intermediates in CO2 methanation, and the formation of CHx was promoted by the CaO or CeO2 composite. Combined with theoretical calculations, the role of surface OH groups in the CO2 hydrogenation mechanism was also investigated. The results demonstrated that the methanation process could be significantly accelerated by introducing the CeO2 composite. This fundamental understanding of the CO2 methanation mechanism will facilitate the design of highly efficient catalysts and promote their commercial application.
为了更深入地了解CO2的活化和甲烷化机理,采用了一种全新的方法,即利用DRIFT光谱来跟踪CO2的解离,取代了传统的利用DRIFT光谱监测甲烷化过程的方法。在此,我们通过在SBA-15中加入CaO或CeO2来设计络合载体来制备ni基催化剂。这些配合物显著提高了CO2甲烷化的催化活性,使反应温度降低了约60℃。CeO2复合材料通过抑制聚合碳来提高催化剂的稳定性,而CaO则起到相反的作用。增加Ni/CeO2-SBA-15中NiO的含量对CH4选择性没有显著影响,达到100%,而将Ni/CaO-SBA-15中的CH4选择性降低到100%以下。基于DRIFT观测,确定H2解离态(Ni(H))对Ni、溢出H态(Ni(H)s)和OH态(Ni(OH)s)是CO2解离的三个驱动力。在SBA-15中掺入CaO或CeO2后,发现Ni(OH)s位点明显增强了CO2的解离过程,而Ni(H)和Ni(H)s位点没有明显增强。CO和甲酸盐是CO2甲烷化的中间产物,CaO或CeO2复合材料促进了CHx的形成。结合理论计算,研究了表面羟基在CO2加氢过程中的作用。结果表明,CeO2复合材料的引入可显著加快甲烷化过程。这种对二氧化碳甲烷化机理的基本认识将有助于设计高效催化剂并促进其商业应用。
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引用次数: 0
Tailoring the physicochemical properties of alumina-metal-organic framework templated nickel nanocatalysts through basic promoter (Ce, La, Mg) incorporation for enhanced activity in methane tri-reforming 通过加入碱性促进剂(Ce, La, Mg)调整铝-金属-有机框架模板镍纳米催化剂的物理化学性质以增强甲烷三重整活性
IF 7.5 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-08 DOI: 10.1016/j.fuel.2026.138269
Arisha Sharma, Anjali Garg, Prakash Biswas
The effect of basic promoters on the alumina metal organic frameworks (MOF) templated nickel-based catalyst was examined for the tri-reforming of methane. The objective of this study was to enhance the CO2 conversion and to produce the synthesis gas with a H2/CO molar ratio of 1.5–2.5, which is a feedstock in the Fischer-Tropsch process for the synthesis of methanol and/or dimethyl ether. A series of MgO, CeO2, and La2O3 promoted 5 wt% Ni-alumina (Ni/AlM-53) derived from the MOF was synthesized via the solvothermal method, followed by the co-impregnation technique. The tri-reforming activity of the catalysts was evaluated in a tubular downflow packed bed reactor at atmospheric pressure in the temperature range of 600–800 °C. Results demonstrated that the CO2 conversion activity was significantly improved after the incorporation of an appropriate amount of basic promoter (2.5 % Ce, 1 % La, 1 % Mg) into the Ni-alumina MOF templated catalyst. The CO2 conversion increased from 37.5 % to ∼48 % with a simultaneous improvement of the H2/CO ratio from 3.2 to 2.5. This improvement of the catalytic activity was attributed to the generation of oxygen vacancies, formation of a stable spinel structure, enhanced metal dispersion, strong metal-support interaction, electron transfer, and the availability of more basic sites after the addition of a basic promoter into the Ni/AlM-53 catalyst. The strong metal-support interaction combined with the oxygen vacancies created a carbon-resistant atmosphere on the catalyst surface, which suppressed carbon deposition and metal sintering even after prolonged reaction duration of >100 h at a high reaction temperature of 800 °C.
研究了碱性促进剂对氧化铝金属有机骨架(MOF)模板镍基催化剂甲烷三重整反应的影响。本研究的目的是提高CO2的转化率,并生产H2/CO摩尔比为1.5-2.5的合成气,这是合成甲醇和/或二甲醚的费托法的原料。采用溶剂热法制备了MgO、CeO2和La2O3促进的5wt % Ni-氧化铝(Ni/AlM-53)。在常压下,在600 ~ 800℃的管状下流填料床反应器中对催化剂的三重整活性进行了评价。结果表明,在ni -氧化铝MOF模板催化剂中加入适量的碱性促进剂(2.5% Ce, 1% La, 1% Mg),可显著提高催化剂的CO2转化活性。CO2转化率从37.5%提高到48%,同时H2/CO比从3.2提高到2.5。这种催化活性的提高是由于在Ni/AlM-53催化剂中加入碱性促进剂后,氧空位的产生、稳定尖晶石结构的形成、金属分散性的增强、金属-载体相互作用的增强、电子转移以及更多碱性位点的可用性。在800℃的高温下,反应时间延长100 h后,强金属-载体相互作用和氧空位在催化剂表面形成了抗碳气氛,抑制了碳沉积和金属烧结。
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引用次数: 0
Tandem Rh-based structured reformer and Ni-YSZ SOFC for decentralized gasoline-to-power conversion 串联h型结构重整器和Ni-YSZ SOFC用于分散式汽油-电力转换
IF 7.5 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-08 DOI: 10.1016/j.fuel.2026.138249
N.V. Ruban , V.N. Rogozhnikov , D.A. Svintsitskiy , V.P. Pakharukova , P.V. Snytnikov , J.W. Thybaut , D.I. Potemkin
This work reports on the performance of a 0.24 wt% Rh/Ce0.75Zr0.25O2–δ–η-Al2O3/FeCrAl structured catalyst in the autothermal reforming of commercial gasoline with a research octane number of 92. Stable syngas production amounting to 70 Nl·h−1 containing of 33.8 vol% H2 and 9.8 vol% CO was demonstrated over 50 h of continuous operation. The origin of the high catalytic efficiency was elucidated by physicochemical characterization (XPS, STEM, XRD), which confirmed the role of Rh redox flexibility (Rh3+ ⇄ Rh⁰) and Ce4+ ⇄ Ce3+ cycling in suppressing carbon formation and maintaining active site dispersion. The compatibility of the produced syngas with Ni–YSZ solid oxide fuel cells was assessed, and a reformer–SOFC tandem concept was proposed to supply 50 W to telecommunication equipment, with operational parameters derived from the present reformer performance. Such a system highlights the potential of integrating catalytic reforming with SOFC conversion for decentralized power generation in remote applications where access to centralized infrastructure is limited.
本文报道了0.24 wt% Rh/Ce0.75Zr0.25O2 -δ -η-Al2O3 /FeCrAl结构催化剂在商品汽油自热重整中的性能,研究辛烷值为92。在50 h的连续运行中,稳定的合成气产量达到70 Nl·h−1,含33.8 vol%的H2和9.8 vol%的CO。高催化效率的来源由理化表征(XPS、STEM、XRD)阐明,证实了Rh氧化还原柔韧性(Rh3+当下Rh⁰)和Ce4+当下Ce3+循环在抑制碳形成和维持活性位点分散中的作用。评估了生产的合成气与Ni-YSZ固体氧化物燃料电池的相容性,并提出了转化炉- sofc串联概念,为电信设备提供50 W的功率,其运行参数来源于现有转化炉的性能。这种系统突出了将催化重整与SOFC转换相结合的潜力,可以在集中式基础设施有限的远程应用中进行分散发电。
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引用次数: 0
Effects of temperature on the modification and carbon sequestration of lignite via synergistic supercritical CO2 and microbial treatment 温度对超临界CO2与微生物协同处理褐煤改性及固碳的影响
IF 7.5 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-08 DOI: 10.1016/j.fuel.2025.138245
Daping xia , Hang Lv , Kuo Jian , Yan Liu , Bin Xu , Huizhen Chang , Liuqi Jia
Against the backdrop of global climate change, coal seam CO2 geological sequestration technology has garnered extensive attention due to its significant potential. To enhance the CO2 adsorption capacity of coal, the synergistic modification of lignite using supercritical CO2 (ScCO2) and microorganisms has emerged as a promising technical approach, in which temperature regulation plays a pivotal role. Through experimental studies conducted under different temperature conditions, the evolution of coal structure and variations in the liquid-phase environment were systematically analyzed. The experimental results indicate that 40 °C is the optimal temperature for the synergistic effects, at which the pore structure of coal is most notably developed, with the specific surface area and total pore volume increasing to 11.253 m2/g and 0.14589 cm3/g, respectively. Concurrently, the oxygen-containing functional groups on the coal surface increased notably, the degree of ordering of the microcrystalline structure was reduced, and the reactivity of the coal matrix was enhanced. Under this temperature condition, microbial metabolism was most active, which efficaciously neutralized the system’s acidity and promoted the formation of HCO3 and CO32–, thereby creating favorable conditions for the conversion of CO2 into stable carbonate minerals. In contrast, when the temperature was raised to 45 °C, microbial activity was inhibited, leading to a significant reduction in the modification effect. These findings confirm that temperature is a key parameter controlling the efficiency of synergistic carbon sequestration. Future research should further explore the coupling effects of temperature and pressure, as well as microbial metabolic mechanisms, to facilitate the practical application of this technology.
在全球气候变化的大背景下,煤层二氧化碳地质封存技术因其巨大的潜力而受到广泛关注。为了提高煤对CO2的吸附能力,利用超临界CO2 (ScCO2)和微生物对褐煤进行协同改性是一种很有前景的技术途径,其中温度调节起着关键作用。通过不同温度条件下的实验研究,系统分析了煤的结构演化和液相环境的变化。实验结果表明,40℃是协同作用的最佳温度,此时煤的孔隙结构发育最为明显,比表面积和总孔容分别增加到11.253 m2/g和0.14589 cm3/g。同时,煤表面含氧官能团明显增加,微晶结构的有序度降低,煤基体的反应性增强。在此温度条件下,微生物代谢最为活跃,有效中和了体系的酸性,促进了HCO3 -和CO32 -的生成,为CO2转化为稳定的碳酸盐矿物创造了有利条件。而当温度升高至45℃时,微生物活性受到抑制,改性效果明显降低。这些结果证实了温度是控制协同固碳效率的关键参数。未来的研究应进一步探索温度和压力的耦合效应,以及微生物代谢机制,以促进该技术的实际应用。
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引用次数: 0
The effect of CO2 and increased initial pressure on hydrothermal liquefaction for the production of high value fatty acids 二氧化碳和初始压力对水热液化生产高价值脂肪酸的影响
IF 7.5 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-08 DOI: 10.1016/j.fuel.2026.138317
D. Liakos , Maria Iosifidou , S. Vakalis
Hydrothermal liquefaction (HTL) of waste biomasses has been widely studied, yet the influence of the reaction atmosphere on carboxylation chemistry is often overlooked. In this study, HTL of anise (Pimpinella anisum L.) waste was performed at 310, 350 and 390 °C solely with air (no added pressure), under N2 with and without increased initial pressure, solely with CO2, and with combined N2/CO2 and increased pressure. The aim was to assess how total pressure and gas/ atmosphere composition affect product distribution and high‑value compound formation. Dissolved CO2 was found to acidify the aqueous phase and participate in carboxylation reactions that convert hydrolysis intermediates into volatile fatty acids (VFAs), as measured via a GC-BID in the form of fatty‑acid methyl esters (FAMEs). Chemical oxygen demand (COD) in the aqueous phase increased from 10,000 to 30000 mg/ L and was consistently higher under CO2. Hydrochar higher heating value peaked at approximately 35 MJ/ kg at 350 °C and declined at 390 °C. CO2‑rich runs exhibited an order‑of‑magnitude increase in VFA production, with acetic‑acid concentrations up to 2 g/ L. FAMEs formation increased with temperature; at 390 °C the combined N2/ CO2 system produced methyl hexanoate concentrations of approx. 13 g/ L and methyl octanoate 11.9 g/ L, more than threefold higher than in single‑gas or non‑pressurized runs. One‑way ANOVA revealed that pressure significantly influenced VFA and FAME yields at 310–350 °C but this effect diminished at 390 °C. These results highlight the importance of optimizing both gas atmosphere and pressure in HTL processes and demonstrate that reactive CO2 atmospheres can drive carboxylation pathways leading to higher yields of valuable fatty acids.
废弃生物质的水热液化(HTL)已被广泛研究,但反应气氛对羧化化学的影响往往被忽视。在本研究中,将大茴香(Pimpinella anisum L.)废弃物分别在310、350和390℃的条件下,在空气条件下(无加压),在初始压力增加和不增加的N2条件下,在CO2条件下,在N2/CO2联合加压条件下进行HTL。目的是评估总压力和气体/大气成分如何影响产品分布和高价值化合物的形成。溶解的CO2被发现使水相酸化,并参与羧基化反应,将水解中间体转化为挥发性脂肪酸(VFAs),通过GC-BID以脂肪酸甲酯(FAMEs)的形式测量。水相化学需氧量(COD)由10000 mg/ L增加到30000 mg/ L, CO2作用下COD持续升高。在350°C时,碳氢化合物的热值最高,约为35 MJ/ kg,在390°C时下降。富CO2组的VFA产量增加了一个数量级,乙酸浓度高达2 g/ L. FAMEs的形成随着温度的升高而增加;在390℃下,N2/ CO2组合体系产生的己酸甲酯浓度约为。13 g/ L和辛酸甲酯11.9 g/ L,比单气体或非加压运行高出三倍以上。单因素方差分析显示,压力在310-350°C时显著影响VFA和FAME产率,但在390°C时这种影响减弱。这些结果强调了在HTL过程中优化气体气氛和压力的重要性,并证明了活性CO2气氛可以驱动羧基化途径,从而提高有价值脂肪酸的产量。
{"title":"The effect of CO2 and increased initial pressure on hydrothermal liquefaction for the production of high value fatty acids","authors":"D. Liakos ,&nbsp;Maria Iosifidou ,&nbsp;S. Vakalis","doi":"10.1016/j.fuel.2026.138317","DOIUrl":"10.1016/j.fuel.2026.138317","url":null,"abstract":"<div><div>Hydrothermal liquefaction (HTL) of waste biomasses has been widely studied, yet the influence of the reaction atmosphere on carboxylation chemistry is often overlooked. In this study, HTL of anise (<em>Pimpinella anisum</em> L.) waste was performed at 310, 350 and 390 °C solely with air (no added pressure), under N<sub>2</sub> with and without increased initial pressure, solely with CO<sub>2</sub>, and with combined N<sub>2</sub>/CO<sub>2</sub> and increased pressure. The aim was to assess how total pressure and gas/ atmosphere composition affect product distribution and high‑value compound formation. Dissolved CO<sub>2</sub> was found to acidify the aqueous phase and participate in carboxylation reactions that convert hydrolysis intermediates into volatile fatty acids (VFAs), as measured via a GC-BID in the form of fatty‑acid methyl esters (FAMEs). Chemical oxygen demand (COD) in the aqueous phase increased from 10,000 to 30000 mg/ L and was consistently higher under CO<sub>2</sub>. Hydrochar higher heating value peaked at approximately 35 MJ/ kg at 350 °C and declined at 390 °C. CO<sub>2</sub>‑rich runs exhibited an order‑of‑magnitude increase in VFA production, with acetic‑acid concentrations up to 2 g/ L. FAMEs formation increased with temperature; at 390 °C the combined N<sub>2</sub>/ CO<sub>2</sub> system produced methyl hexanoate concentrations of approx. 13 g/ L and methyl octanoate 11.9 g/ L, more than threefold higher than in single‑gas or non‑pressurized runs. One‑way ANOVA revealed that pressure significantly influenced VFA and FAME yields at 310–350 °C but this effect diminished at 390 °C. These results highlight the importance of optimizing both gas atmosphere and pressure in HTL processes and demonstrate that reactive CO<sub>2</sub> atmospheres can drive carboxylation pathways leading to higher yields of valuable fatty acids.</div></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":"413 ","pages":"Article 138317"},"PeriodicalIF":7.5,"publicationDate":"2026-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145922615","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
Understanding the differences in ignition and combustion characteristics between raw coal and pyrolyzed char: A combined PLIF measurement and DFT calculation 了解原煤和热解焦之间点火和燃烧特性的差异:PLIF测量和DFT计算的结合
IF 7.5 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-08 DOI: 10.1016/j.fuel.2026.138268
Yawei Song , Sheng Su , Qifu Lin , Longwei Chen , Chengzhou Liu , Weiye Chen , Zhenyang Li , Yiman Jiang , Dianwu Wu , Hansheng Feng , Guangnan Luo , Jun Xiang
Fuel selection is critical for achieving stable low-load combustion and rapid load response in coal-fired power plants. As an important source of steam coal, understanding the combustion behavior of low-rank coal and its pyrolyzed char is essential for fuel optimization. The ignition behaviors, OH radical generation, and flame front evolution of the raw coal and chars pyrolyzed at four temperatures (500 °C, 600 °C, 700 °C and 800 °C) were investigated using OH-Planar laser-induced fluorescence (OH-PLIF). Density functional theory (DFT) calculations were conducted to clarify the interaction between polycyclic aromatic hydrocarbons (PAHs) and H radicals during volatile combustion. The results showed that raw coal had a significantly shorter ignition delay time (tign) than pyrolyzed chars, and increasing pyrolysis temperature led to longer tign. Similarly, raw coal also displayed a higher peak flame temperature due to the strong radiative heat transfer of sooty flames, while chars prepared at lower temperatures showed relatively higher peak temperatures among the char samples. Based on the results of OH radical intensity profile, the coal combustion process exhibited two-peaks pattern, corresponding to volatile flame duration stage and char combustion stage, whereas the pyrolyzed chars exhibited one-peak pattern. The OH intensity at ignition moment of raw coal was higher than that of other four pyrolyzed chars, consistent with its shorter tign. Whereas, the peak OH radical intensity of raw coal during two stages are almost lower than the peak OH intensity of pyrolyzed chars, among them the peak OH intensity during volatile flame duration stage was much lower than that of others observed. DFT calculations showed that H radicals promote PAHs formation by lowering reaction barriers, but their consumption by PAHs reduces OH production via H + O2 → OH + O. This explains the significantly weaker OH intensity observed during the volatile combustion of raw coal compared with that during char combustion stage and the combustion of pyrolyzed char.
燃料选择是燃煤电厂实现稳定低负荷燃烧和快速负荷响应的关键。作为重要的动力煤来源,了解低阶煤及其热解焦的燃烧行为对燃料优化至关重要。利用OH- planar激光诱导荧光(OH- plif)研究了在500℃、600℃、700℃和800℃四种温度下热解的原煤和焦炭的着火行为、OH自由基生成和火焰前缘演变。采用密度泛函理论(DFT)计算了挥发性燃烧过程中多环芳烃(PAHs)与H自由基的相互作用。结果表明,原煤的点火延迟时间(tin)明显短于热解后的焦炭,且热解温度的升高会导致tin的延长。同样,由于煤烟火焰的强辐射传热,原煤也表现出较高的火焰峰值温度,而在较低温度下制备的煤焦样品中峰值温度相对较高。OH自由基强度谱结果表明,煤的燃烧过程呈现双峰型,分别对应于挥发性火焰持续阶段和焦炭燃烧阶段,而热解后的焦炭则呈现单峰型。原煤在点火时刻的OH强度高于其他4种热解炭,这与其较短的长度相一致。而原煤在两个阶段的OH自由基峰值强度几乎低于热解炭的OH峰值强度,其中挥发性火焰持续阶段的OH峰值强度远低于其他阶段。DFT计算表明,H自由基通过降低反应势垒促进PAHs的生成,但PAHs对H自由基的消耗通过H + O2→OH + o减少OH的生成,这就解释了原煤挥发燃烧阶段OH强度明显弱于焦炭燃烧阶段和热解炭燃烧阶段的原因。
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引用次数: 0
Effects of different jet forms on the gas–solid flow behavior in a downer reactor 不同射流形式对下行反应器内气固流动行为的影响
IF 7.5 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-08 DOI: 10.1016/j.fuel.2026.138293
Zihan Yan , Huimin Yin , Lining Wu , Mengxin Wen , Zhihang Zheng , Xiuying Yao , Chunxi Lu
In this study, to explore the influence of nozzle jets on the gas–solid flow behavior in a downer reactor, different forms of jets are introduced in the fully developed section of the downer reactor. Numerical simulations are conducted to examine the effects of different jet forms (upward and downward-inclined jets) and jet angles on the gas–solid flow behavior. The Kutta-Joukowski theorem, which was originally developed in aerodynamics, is adopted in this study to analyze lateral forces in the gas–solid flow system. The results show that after the introduction of a jet, the radial particle velocity distribution in the downer reactor becomes more uniform. Compared to downward inclined jets, upward jets, which interact counter-currently with the particle flow, are more effective in increasing the particle concentration within the downer reactor. The solid holdup at the reactor center in the dense-phase region is 1 to 6.6 times higher in the presence of jets than in the absence of jets at the same gas flow rate. For both upward and downward jets, the 60° axial nozzle-wall angle shows the best center concentration enhancement effect. Additionally, the larger the axial nozzle-wall angle is, the easier it is for particles to recover to the uniform distribution.
在本研究中,为了探索喷嘴射流对下行反应器内气固流动行为的影响,在下行反应器的完全开发段引入了不同形式的射流。通过数值模拟研究了不同射流形式(向上和向下倾斜射流)和射流角度对气固流动特性的影响。本研究采用最初在空气动力学中发展起来的Kutta-Joukowski定理来分析气固流动系统中的侧向力。结果表明:射流引入后,降叶反应器内颗粒径向速度分布更加均匀;与向下倾斜射流相比,与颗粒流反向作用的向上射流在提高下行反应器内颗粒浓度方面更为有效。在相同的气体流速下,有射流存在时,反应器中心致密相区固体含率比无射流时高1 ~ 6.6倍。对于上下两种喷流,60°轴向喷嘴壁角的中心浓度增强效果最好。此外,轴向喷嘴-壁面角越大,颗粒越容易恢复均匀分布。
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引用次数: 0
Combined effects of pre-chamber nozzle diameter and fuel reactivity on jet ignition characteristics of ammonia-hydrogen blends 预室喷嘴直径和燃料反应性对氨氢混合物喷射着火特性的综合影响
IF 7.5 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-08 DOI: 10.1016/j.fuel.2026.138302
Jinguang Li, Lei Wang, Gequn Shu, Xingqian Mao, Haiqiao Wei, Jiaying Pan
Compared to active pre-chambers, passive pre-chambers offer significant advantages due to their simple structure and the elimination of major modifications to the cylinder head. The nozzle diameter is a key parameter affecting jet ignition characteristics, yet its effects under different reactive conditions, particularly in combination with fuel reactivity, remain insufficiently understood. This study investigates the influence of nozzle diameter on jet ignition characteristics of ammonia-hydrogen blends using a rapid compression machine equipped with a passive pre-chamber, allowing systematic variation of hydrogen blending ratios. Results indicate that excessively small nozzle diameters generate a strong throttling effect, suppressing pre-chamber ignition, whereas higher fuel reactivity enhances ignition. Conversely, high-speed jets promote intense shear interactions with the mixture, leading to significant heat loss and combustion instability in the main chamber. Large nozzle diameters result in lower jet kinetic energy and weaker turbulence, slowing flame propagation during the late combustion phase. For hydrogen blending ratios of 0–5 %, the 4 mm nozzle yields the fastest combustion rate, while optimal ignition performance occurs with the 3 mm and 2 mm nozzles at hydrogen blending ratios of 10 % and 20 %, respectively. Decreasing nozzle diameter or hydrogen content shifts ignition from flame-induced to jet-induced. The combined effects of fuel reactivity and nozzle diameter define four combustion regimes: misfire, unstable combustion, rapid combustion, and slow combustion. Additionally, ignition delay is found to be largely insensitive to jet velocity under high-reactivity conditions.
与主动预室相比,被动预室由于结构简单,无需对气缸盖进行重大修改,因此具有显著的优势。喷管直径是影响喷管点火特性的关键参数,但其在不同反应条件下的影响,特别是与燃料反应性的结合,目前还没有得到充分的了解。本研究利用配备被动预室的快速压缩机,研究喷嘴直径对氨氢共混物喷射点火特性的影响,允许系统地改变氢混合比。结果表明,过小的喷嘴直径会产生较强的节流效果,抑制预燃室点火,而较高的燃料反应性则会增强点火。相反,高速射流促进了与混合物的强烈剪切相互作用,导致主燃烧室显著的热损失和燃烧不稳定。喷嘴直径越大,射流动能越小,湍流越弱,燃烧后期火焰传播速度越慢。当掺氢比为0 - 5%时,4mm喷嘴的燃烧速度最快,而当掺氢比分别为10%和20%时,3mm和2mm喷嘴的点火性能最佳。减小喷嘴直径或氢含量会使点火从火焰诱导转变为喷射诱导。燃料反应性和喷嘴直径的综合影响决定了四种燃烧模式:失火、不稳定燃烧、快速燃烧和缓慢燃烧。此外,发现点火延迟在高反应性条件下对射流速度不敏感。
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引用次数: 0
An interfacially engineered Ni2P/Fe2P heterostructure grown on NiFe PBA/NF as a high-efficiency bifunctional electrocatalyst for overall water splitting 界面工程Ni2P/Fe2P异质结构在NiFe PBA/NF上生长,作为一种高效的双功能电催化剂,用于整体水分解
IF 7.5 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-08 DOI: 10.1016/j.fuel.2026.138306
Pan Qu , Zhenlu Zhao
The development of high-performance, long-lasting bifunctional electrocatalysts is crucial for overall water splitting to drive the advancement of sustainable energy technology. In this study, we developed a Ni2P/Fe2P heterostructure composite catalyst supported on a NiFe Prussian blue analog (PBA) framework, designated Ni2P/Fe2P@NiFe PBA/NF, through sequential hydrothermal and phosphidation syntheses. The robust three-dimensional network formed by the in situ growth of Ni2P/Fe2P@NiFe PBA/NF on nickel foam provides integrated conduction pathways. This composite structure may facilitate electron conduction among the NF, Ni2P/Fe2P, and NiFe PBA. The heterojunction between Ni2P and Fe2P effectively accelerated electron transport, thereby achieving stable and efficient catalytic performance. Consequently, electrochemical tests in 1 M KOH demonstrated outstanding bifunctional activity, with overpotentials as low as 239 ± 5 mV for the oxygen evolution reaction (OER) and 174 ± 12 mV for the hydrogen evolution reaction (HER) at a current density of 100 mA cm−2. The catalyst outperformed benchmark catalysts, such as RuO2 and Pt/C, at high current densities and maintained significant stability after 100 h of continuous operation. Moreover, a two-electrode electrolyzer assembled with Ni2P/Fe2P@NiFe PBA/NF as both the anode and cathode exhibited excellent overall water-splitting performance, achieving a low cell voltage of 1.49 V at 10 mA cm−2 along with remarkable stability exceeding 100 h.
高性能、长效双功能电催化剂的开发是推动可持续能源技术进步的关键。在本研究中,我们开发了Ni2P/Fe2P异质结构复合催化剂,负载在NiFe普鲁士蓝类似物(PBA)框架上,命名为Ni2P/Fe2P@NiFe PBA/NF。Ni2P/Fe2P@NiFe PBA/NF在泡沫镍上原位生长形成坚固的三维网络,提供了完整的传导途径。这种复合结构可以促进NF、Ni2P/Fe2P和NiFe - PBA之间的电子传导。Ni2P和Fe2P之间的异质结有效地加速了电子传递,从而实现了稳定高效的催化性能。因此,在1 M KOH条件下的电化学测试显示出出色的双功能活性,在电流密度为100 mA cm−2时,析氧反应(OER)的过电位低至239±5 mV,析氢反应(HER)的过电位低至174±12 mV。在高电流密度下,该催化剂的性能优于RuO2和Pt/C等基准催化剂,并在连续运行100小时后保持了显著的稳定性。此外,以Ni2P/Fe2P@NiFe PBA/NF作为阳极和阴极的双电极电解槽具有出色的整体水分解性能,在10 mA cm - 2下电池电压低至1.49 V,并且超过100 h的稳定性显著。
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引用次数: 0
Characterization of Fischer-Tropsch Diesel and Polyoxymethylene dimethyl ether x blends spray combustion using multiple optical diagnostics 使用多重光学诊断表征费托柴油和聚氧亚甲基二甲醚x混合物喷雾燃烧
IF 7.5 1区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-08 DOI: 10.1016/j.fuel.2026.138272
Min Xu, Xu Liu, Pengwei Wu, Huayang Sun, Zongqing Wang, Qian Wang
Synthetic fuels (E-fuels) present notable advantages for high-load compression ignition (CI) engines, including improved performance and decreased reliance on fossil fuels. Blends of Fischer-Tropsch (F-T) Diesel and Polyoxymethylene dimethyl ether x (PODEx) are expected to integrate well with existing infrastructure while supporting efficient, low-emission combustion. The current study aims to provide comprehensive spray combustion data for E-fuel blends, laying the foundation for “’Fuel-Engine” co-optimization. Optical diagnostics of spray combustion were conducted under CI engine-relevant conditions for F-T Diesel and two blends—75 % F-T Diesel + 25 % PODEx by volume (F-T75/P25) and 50 % F-T Diesel + 50 % PODEx by volume (F-T50/P50). Results from various optical techniques demonstrate enhanced ignition and reduced soot formation in the blends compared to F-T Diesel, underscoring their promise for CI applications. Notably, the spray combustion flames of F-T75/P25 and F-T Diesel displayed similar CH2O and OH structures, driven by diffusion flame chemistry that is alkane reaction-dominated. The flame structure of F-T50/P50, however, depended on the trade-off interaction between CH2O and OH. At low temperatures (750 K), an enrichment of CH2O suppresses downstream high-temperature combustion. While for high temperature condition above 800 K, the OH structure is restored, leading to a substantial reduction in flame lift-off length. Additionally, in F-T50/P50, CH2O and OH preferentially form HCO and CO rather than polycyclic aromatic hydrocarbons. Upon crossing the OH interface, HCO and CO will create a high-temperature layer downstream, likely linked to CO2 formation.
Novelty and Significance.
This study presents the first comprehensive optical investigation into the spray combustion characteristics of F-T diesel blended PODEx under compression ignition engine-relevant conditions, revealing the coupling between alkane and ether combustion chemistries.
The novelty of this work lies in the discovery of a temperature-dependent “trade-off” mechanism between CH2O and OH in E-fuel blends. Furthermore, we identify a distinct soot-free high-temperature reaction layer dominated by CO/HCO oxidation in high-ratio blends, providing a new understanding of how oxygenated blends alter the structure of diffusion flames. This research bridges the gap between macroscopic engine performance studies and fundamental chemical kinetics.
合成燃料(E-fuels)在高负荷压缩点火(CI)发动机中具有显著优势,包括提高性能和减少对化石燃料的依赖。费托柴油(F-T)和聚氧亚甲基二甲醚(PODEx)的混合物有望与现有基础设施很好地结合,同时支持高效、低排放的燃烧。本研究旨在为e -燃料混合燃料提供全面的喷雾燃烧数据,为“燃料-发动机”协同优化奠定基础。在CI发动机相关条件下,对F-T柴油和75% F-T柴油+ 25% PODEx (F-T75/P25)和50% F-T柴油+ 50% PODEx (F-T50/P50)两种混合物进行了喷雾燃烧的光学诊断。各种光学技术的结果表明,与F-T Diesel相比,混合燃料的点火能力增强,烟灰形成减少,这突显了它们在CI应用中的前景。值得注意的是,F-T75/P25和F-T Diesel的喷雾燃烧火焰表现出相似的CH2O和OH结构,由以烷烃反应为主的扩散火焰化学驱动。而F-T50/P50的火焰结构取决于CH2O和OH之间的权衡相互作用。在低温(750 K)下,CH2O的富集抑制了下游的高温燃烧。而在800k以上的高温条件下,OH结构恢复,导致火焰上升长度大幅减少。此外,在F-T50/P50中,CH2O和OH优先形成HCO和CO,而不是多环芳烃。在穿过OH界面后,HCO和CO将在下游形成一个高温层,这可能与二氧化碳的形成有关。新颖性和重要性。本研究首次对F-T柴油混合PODEx在压缩点火发动机相关条件下的喷雾燃烧特性进行了全面的光学研究,揭示了烷烃和醚燃烧化学物质之间的耦合。这项工作的新颖之处在于发现了电子燃料混合物中CH2O和OH之间依赖于温度的“权衡”机制。此外,我们确定了在高比例共混物中以CO/HCO氧化为主的明显无烟高温反应层,为氧化共混物如何改变扩散火焰的结构提供了新的理解。这项研究弥合了宏观发动机性能研究和基本化学动力学之间的差距。
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引用次数: 0
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