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In-depth exploration of NH3-SCR over metal-based zeolite catalyst improvement research at low-temperature: Catalytic activity, sulfur/phosphorus resistance and hydrothermal stability 深入探索NH3-SCR金属基沸石催化剂在低温下的改进研究:催化活性、耐硫/磷性和水热稳定性
IF 7.7 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2026-06-01 Epub Date: 2026-02-13 DOI: 10.1016/j.fuproc.2026.108412
Zhiqing Zhang , Zicheng He , Yanshuai Ye , Yuguo Wang , Chuan Liu , Yan Tan , Zibin Yin , Mingzhang Pan
Ammonia selective catalytic reduction (NH3-SCR) is the mainstream technology for controlling nitrogen oxide (NOx) emissions. However, the widespread application of zeolite catalysts faces multiple challenges: susceptibility to sulfur/phosphoru (S/P)-poisoning, narrow reaction temperature windows, and poor hydrothermal stability. This paper systematically reviews recent advances in metal zeolite catalysts, focusing on their low-temperature reaction mechanisms. Analysis addresses the aforementioned issues from two dimensions: (1) For Fe- and Cu-based monometallic catalysts, this study investigates the influence of active sites, framework Al, metal species migration, and acidity modification strategies on catalyst performance. (2) For composite metal catalysts, this study elucidates intermetallic electron transfer and synergistic effects within different frameworks, emphasizing the refinement of low-temperature reaction mechanisms and performance. It also supplements key techniques such as X-ray absorption spectroscopy (XAS), X-ray diffraction (XRD), and brunauer emmett teller (BET) for SCR applications. The aim is to provide a theoretical foundation and research pathway for developing novel, highly efficient NH3-SCR catalysts, while proposing future research directions.
氨选择性催化还原(NH3-SCR)是控制氮氧化物(NOx)排放的主流技术。然而,沸石催化剂的广泛应用面临着多重挑战:易受硫磷(S/P)中毒、反应温度窗窄、水热稳定性差。本文系统地综述了金属沸石催化剂的研究进展,重点介绍了其低温反应机理。分析从两个方面解决了上述问题:(1)对于铁基和铜基单金属催化剂,本研究考察了活性位点、框架Al、金属物种迁移和酸性改性策略对催化剂性能的影响。(2)对于复合金属催化剂,本研究阐明了金属间电子转移和不同框架下的协同效应,强调了低温反应机理和性能的细化。它还补充了用于SCR应用的关键技术,如x射线吸收光谱(XAS)、x射线衍射(XRD)和brunauer emmett teller (BET)。旨在为开发新型高效NH3-SCR催化剂提供理论基础和研究途径,同时提出未来的研究方向。
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引用次数: 0
Prospective life cycle sustainability assessment and benchmarking of hydrogen from solid oxide electrolysis coupled with concentrated solar power 固体氧化物电解结合聚光太阳能发电制氢的前瞻性生命周期可持续性评估与基准测试
IF 7.7 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2026-06-01 Epub Date: 2026-02-13 DOI: 10.1016/j.fuproc.2026.108417
Mario Martín-Gamboa , Felipe Campos-Carriedo , Santiago Abelleira , Pedro L. Cruz , Christina Wulf , Javier Dufour , Diego Iribarren
Achieving sustainable hydrogen systems requires balancing environmental, economic and social aspects. In this regard, research on the life-cycle sustainability of emerging pathways such as solid oxide electrolysis (SOE) coupled with concentrated solar power (CSP) remains limited. This study presents a prospective life cycle sustainability assessment (LCSA) of hydrogen production via SOE coupled with CSP, benchmarked against hydrogen from steam methane reforming (SMR) as a conventional counterpart. By following the latest guidelines for LCSA of hydrogen-related systems developed within the SH2E project, this study applies consistent methodological choices across sustainability dimensions (e.g. functional unit definition), while transparently addressing model asymmetries. Results highlight notable differences in hotspots across dimensions and indicators. The CSP section dominates environmental impacts due to high material demand, while economic hotspots additionally include electrolysers and operational wages. Social impacts are primarily linked to the high relative share of worker hours in the Spanish hydrogen production facility itself, with added supply chain risks associated with chromium extraction in Kazakhstan and natural gas sourcing from Algeria. Even though conventional hydrogen from SMR outperforms hydrogen from SOE in four out of seven sustainability indicators, the latter offers promising results in terms of lower carbon footprint, reduced fair salary risk, and enhanced prospects for economic growth. Overall, these findings highlight the potential of SOE to contribute to a sustainable hydrogen economy, while they also stress areas (e.g. cost competitiveness, resource efficiency, and supply chain risk management) where sustainable-by-design research is essential to mitigate burden-shifting across impact categories and sustainability dimensions.
实现可持续的氢系统需要平衡环境、经济和社会方面。在这方面,对新兴途径如固体氧化物电解(SOE)与聚光太阳能(CSP)耦合的生命周期可持续性的研究仍然有限。本研究提出了通过SOE结合CSP制氢的前瞻性生命周期可持续性评估(LCSA),以蒸汽甲烷重整(SMR)制氢为基准。通过遵循SH2E项目中开发的氢相关系统的最新LCSA指南,本研究在可持续性维度(例如功能单元定义)上采用一致的方法选择,同时透明地解决模型不对称问题。结果显示,不同维度和指标的热点存在显著差异。由于高材料需求,CSP部分在环境影响方面占主导地位,而经济热点还包括电解槽和操作工资。社会影响主要与西班牙制氢设施本身的工人工时相对较高有关,此外还与哈萨克斯坦的铬提取和阿尔及利亚的天然气采购相关的供应链风险增加有关。尽管传统的SMR制氢在7项可持续性指标中的4项表现优于国有企业制氢,但后者在降低碳足迹、降低公平薪酬风险和增强经济增长前景方面表现良好。总体而言,这些研究结果强调了国有企业为可持续氢经济做出贡献的潜力,同时也强调了一些领域(例如成本竞争力、资源效率和供应链风险管理),在这些领域,可持续设计研究对于减轻影响类别和可持续性维度之间的负担转移至关重要。
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引用次数: 0
Fluidized bed combustion characteristics of high-ash coal char under O2/H2O and O2/CO2/H2O environments O2/H2O和O2/CO2/H2O环境下高灰分煤焦的流化床燃烧特性
IF 7.7 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2026-06-01 Epub Date: 2026-02-12 DOI: 10.1016/j.fuproc.2026.108415
Sachin K.S. , David Pallarès , Bo Leckner , Pratikash Panda , R.V. Ravikrishna
<div><div>The combustion characteristics of a batch of in-situ prepared high-ash coal char have been investigated under different fluidized bed operating conditions (i.e. O<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> concentration, balance gas, bed temperature, particle size) in an optically accessible fluidized bed. A fast Universal Exhaust Gas Oxygen (UEGO) sensor measured the oxygen partial pressure at the exhaust to determine the reaction rate and burnout time of char particles, which demonstrates a novel application of this type of sensor in high H<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>O (wet) environments. A pre-calibrated two-colour pyrometry technique was employed to measure the temperature of char particles. The effect of the oxyfuel atmosphere on the burnout time of char particles was found to be prominent at higher bed temperatures, lower O<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> concentrations, and larger particle sizes. The sensitivity of combustion behaviour to variations in the combustion environment was higher for larger particle size. Results show that the burnout time was the lowest in O<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>/H<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>O for both 1.2 mm and 3 mm particle sizes. This was attributed to the higher diffusivity of O<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> in H<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>O and the H<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>O gasification reaction. The addition of H<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>O to O<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>/CO<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> environment enhanced the diffusivity of O<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>, making it comparable to that in N<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>. In 10% O<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>/45% CO<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>/45% H<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>O environment, competitive interactions among O<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>, CO<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> and H<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>O were more pronounced for smaller particles. The reactivity of char in 10% O<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>/90% H<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>O at higher bed temperat
研究了一批原位制备的高灰分煤焦在不同的流化床操作条件(O2浓度、平衡气体、床温、粒度)下在光学可及流化床中的燃烧特性。快速通用废气氧(UEGO)传感器测量排气时的氧分压,以确定炭颗粒的反应速率和燃尽时间,这证明了这种传感器在高水(湿)环境中的新应用。采用预先标定的双色热法测定炭颗粒的温度。在较高的床层温度、较低的氧浓度和较大的颗粒尺寸下,含氧气氛对炭颗粒燃尽时间的影响最为显著。颗粒尺寸越大,燃烧行为对燃烧环境变化的敏感性越高。结果表明:在O2/H2O中,1.2 mm和3 mm粒径的烧蚀时间最短;这是由于O2在水中的高扩散率和水的气化反应。在O2/CO2环境中加入H2O增强了O2的扩散率,使其与N2中的扩散率相当。在10% O2/45% CO2/45% H2O环境中,O2、CO2和H2O之间的竞争性相互作用对于较小的颗粒更为明显。在较高床层温度下,焦炭在10% O2/90% H2O环境中的反应性与在20% O2/80% N2环境中的反应性相当,这使得氧气蒸汽燃烧有可能向氧气燃料燃烧发展。
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A fast Universal Exhaust Gas Oxygen (UEGO) sensor measured the oxygen partial pressure at the exhaust to determine the reaction rate and burnout time of char particles, which demonstrates a novel application of this type of sensor in high H&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;O (wet) environments. A pre-calibrated two-colour pyrometry technique was employed to measure the temperature of char particles. The effect of the oxyfuel atmosphere on the burnout time of char particles was found to be prominent at higher bed temperatures, lower O&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt; concentrations, and larger particle sizes. The sensitivity of combustion behaviour to variations in the combustion environment was higher for larger particle size. Results show that the burnout time was the lowest in O&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;/H&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;O for both 1.2 mm and 3 mm particle sizes. This was attributed to the higher diffusivity of O&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt; in H&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;O and the H&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;O gasification reaction. The addition of H&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;O to O&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;/CO&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt; environment enhanced the diffusivity of O&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;, making it comparable to that in N&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;. In 10% O&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;/45% CO&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;/45% H&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;O environment, competitive interactions among O&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;, CO&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt; and H&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;O were more pronounced for smaller particles. The reactivity of char in 10% O&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;/90% H&lt;span&gt;&lt;math&gt;&lt;msub&gt;&lt;mrow&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mn&gt;2&lt;/mn&gt;&lt;/mrow&gt;&lt;/msub&gt;&lt;/math&gt;&lt;/span&gt;O at higher bed temperat","PeriodicalId":326,"journal":{"name":"Fuel Processing Technology","volume":"284 ","pages":"Article 108415"},"PeriodicalIF":7.7,"publicationDate":"2026-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146154165","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
A density functional theory study of CH4 oxidation over LaMnO3 oxygen carrier during chemical looping combustion 化学环燃烧过程中LaMnO3氧载体上CH4氧化的密度泛函理论研究
IF 7.7 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2026-06-01 Epub Date: 2026-02-13 DOI: 10.1016/j.fuproc.2026.108418
Zhongze Bai , Kai H. Luo
LaMnO3-based oxygen carriers (OCs) are considered a promising class of materials for chemical looping combustion (CLC); however, elucidating their detailed microscopic reaction mechanisms remains challenging. In this study, density functional theory (DFT) calculations were employed to investigate the reaction mechanisms of CH4 combustion on the LaMnO3(010) surface. The results reveal that CH4 weakly adsorbs with negligible charge transfer, whereas CHx species (x = 0–3) exhibit strong chemisorption, which strengthens as hydrogen atoms are removed. The CH → C + H step is identified as the rate-limiting step during CH4 dehydrogenation, featuring an energy barrier of 2.233 eV. For CO2 formation, the adsorbed carbon atom (C*) reacts first with O1 (the first lattice oxygen atom) to form CO*, which then reacts with O2 (the second lattice oxygen atom) to produce CO2*, followed by desorption, with an overall energy barrier of 1.693 eV. H2O formation occurs via surface hydrogen reacting with lattice O1, forming H2O* at the Ov1 (the vacancy formed by O1 removal) site prior to desorption, with an energy barrier of 1.465 eV. Overall, CH4 dehydrogenation governs the reaction kinetics, while surface oxygen is critical for enabling complete oxidation to CO2 and H2O. This study provides fundamental insights into CH4 oxidation on LaMnO3(010), which may guide the design of novel OCs in the future.
lamno3基氧载体(OCs)被认为是一类很有前途的化学环燃烧(CLC)材料。然而,阐明它们详细的微观反应机制仍然具有挑战性。本研究采用密度泛函理论(DFT)计算方法研究了CH4在LaMnO3(010)表面燃烧的反应机理。结果表明,CH4的吸附较弱,电荷转移可以忽略不计,而CHx (x = 0-3)则表现出较强的化学吸附,并且随着氢原子的去除而增强。在CH4脱氢过程中,CH→C + H步骤被确定为限速步骤,其能垒为2.233 eV。对于CO2的生成,被吸附的碳原子(C*)首先与O1(第一个晶格氧原子)反应生成CO*,然后与O2(第二个晶格氧原子)反应生成CO2*,然后进行解吸,总能垒为1.693 eV。H2O的生成是通过表面氢与晶格O1反应,在解吸前在Ov1 (O1去除形成的空位)位置形成H2O*,能垒为1.465 eV。总的来说,CH4脱氢控制了反应动力学,而表面氧对于完全氧化成CO2和H2O至关重要。该研究为CH4在LaMnO3(010)上的氧化提供了基本的见解,这可能指导未来新型OCs的设计。
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引用次数: 0
HydroStor-PMX: A multi-phase hybrid system for high-density hydrogen storage via pressure-modulated MXene frameworks HydroStor-PMX:一种通过压力调制MXene框架实现高密度储氢的多相混合系统
IF 7.7 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2026-05-01 Epub Date: 2026-02-06 DOI: 10.1016/j.fuproc.2026.108409
Rabia Qammar , Muhammad Bilal Yaseen , Rana Zain Ul Abidin , Sadashiv Chaturvedi
The study proposes a new kind of multi-phase hybrid energy-storage device, namely HydroStor-PMX, in which pressure-modulated MXene structures are combined with a pressure-based machine learning optimization algorithm to create a pressure-induced hydrogen storage process with unprecedented results. The new method provides a combination of two-dimensional MXene materials (Ti3C2Tx,V2CTx,Mo2CTx) with dynamic pressure modulation methodologies that allow optimization of interlayer distances and binding energies occurring in real time. In depth density functional theory calculations indicate the optimum binding energies of hydrogen bonded as 28.5 to 49.7 kJ/mol H2 which can be stored in reversible form under ambient temperature and pressure. Ensemble models of machine learning allow obtaining excellent predictive performance. Experimental confirmation of breakthrough performance can be seen with hydrogen storage capacities as high as 8.5 wt% at moderate pressure (50 bar) and room temperature (25C), and which is 150% better than static MXene systems with rapid kinetics (8.9 min to 90% capacity). It is quite stable as long term cyclability testing shows that less than 5% of its capacity lost during the same charge-discharge cycles of 5000.
该研究提出了一种新型多相混合储能装置HydroStor-PMX,该装置将压力调制的MXene结构与基于压力的机器学习优化算法相结合,创建了压力诱导的储氢过程,并取得了前所未有的效果。新方法将二维MXene材料(Ti3C2Tx,V2CTx,Mo2CTx)与动态压力调制方法相结合,可以实时优化层间距离和结合能。深度密度功能理论计算表明,氢键的最佳结合能为28.5 ~ 49.7 kJ/mol H2,可在常温常压下以可逆形式储存。机器学习的集成模型可以获得出色的预测性能。实验证实,在中压(50 bar)和室温(25C)下,储氢容量高达8.5 wt%,比具有快速动力学(8.9 min至90%容量)的静态MXene系统好150%。长期可循环性测试表明,在相同的5000次充放电循环中,其容量损失不到5%,因此非常稳定。
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引用次数: 0
High-quality biochar from the catalytic pyrolysis of Brachychiton seeds: Optimization and characterization 长柄石种子催化热解制备高品质生物炭:优化与表征
IF 7.7 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2026-05-01 Epub Date: 2026-02-02 DOI: 10.1016/j.fuproc.2026.108410
Anass Choukoud , Hammadi El Farissi , Lokmane Abdelouahed , Abdesselam Tahani , Abdelmonaem Talhaoui
This study aims to describe the effect of pyrolysis conditions (temperature, particle size, and type of catalyst) on the production of biochar from Brachychiton seeds. Pyrolysis experiments were conducted at between 300 °C–550 °C with particle sizes from <315 μm to 800–1600 μm and catalysts including Al₂O₃, CaO, H3BO3, ZrO(NO3)2, V₂O₅, ZnO, Fe₂O₃, and TiO₂. The results showed that the temperature range from maximum biochar yield was 400 °C and smaller particle (smaller than <315 μm) showed higher biochar yield.Char yield was significantly improved by Al2O3 even at low temperatures while higher catalyst concentration led to an increased yield till 2% catalyst. Biochar had alkaline pH values, varying from 7.81 to 9.80, making them suitable as soil ameliorants. Electrical conductivity ranged from 308 μS.cm−1 to 1650 μS.cm−1 with the effect of temp and catalyst type measured, demonstrating ranges of ion concentrations available for agricultural application. ATR-IR analysis also revealed a decrease in the concentration of functional groups such as OH, CH and CO, signifying a conversion of the original biomass to more aromatic species with increasing temperature. Scanning electron microscopy (SEM), X-ray diffraction (XRD) and elemental analyses indicate a remarkable change in the surface morphology as well as the composition of biochars, such as increased pore volume, the formation of numerous mineral phases and the successful incorporation of catalysts. Notably, TiO₂, H₃BO₃ and Fe₂O₃ are effective in enhancing their calorific value, which reaches 49.464 MJ.kg-1. The results highlight the importance of biochar pyrolysis conditions for improving their properties for energy, environmental and agricultural use.
本研究旨在描述热解条件(温度、粒度和催化剂类型)对短柄石种子生产生物炭的影响。热解实验在300°C - 550°C之间进行,粒度为<;315 μm至800-1600 μm,催化剂包括Al₂O₃,CaO, H3BO3, ZrO(NO3)2, V₂O₅,ZnO, Fe₂O₃和TiO₂。结果表明:在400℃的温度范围内,颗粒越小(小于315 μm),生物炭产率越高;Al2O3在低温条件下也能显著提高炭的产率,催化剂浓度越高,产率越高,达到2%。生物炭具有7.81 ~ 9.80的碱性pH值,适合作为土壤改良剂。电导率为308 μS。cm−1 ~ 1650 μS。Cm−1与温度和催化剂类型的影响测量,显示可用于农业应用的离子浓度范围。ATR-IR分析还显示,OH、CH和CO等官能团的浓度下降,表明随着温度的升高,原始生物量向更多芳香物种转化。扫描电镜(SEM)、x射线衍射(XRD)和元素分析表明,生物炭的表面形貌和组成发生了显著变化,如孔隙体积增加、大量矿物相的形成以及催化剂的成功掺入。特别是,TiO₂、H₃BO₃、Fe₂O₃的热值达到49.464 MJ.kg-1,有效地提高了热值。研究结果强调了生物炭热解条件对改善其能源、环境和农业利用性能的重要性。
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引用次数: 0
Techno-economic analysis of waste-to-SAF pathways with carbon capture and storage and green hydrogen integrations 碳捕获和储存以及绿色氢集成的废物到saf途径的技术经济分析
IF 7.7 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2026-05-01 Epub Date: 2026-02-07 DOI: 10.1016/j.fuproc.2026.108416
Mohammad A. Rasheed, Massimiliano Materazzi
De-fossilising the aviation sector is essential for global climate goals, with sustainable aviation fuels (SAF) identified as a key low-emission solution. Municipal solid waste (MSW), when converted to refuse-derived fuel (RDF), offers an abundant, largely biogenic feedstock for SAF production while diverting waste from landfills. This research study analyses the production of SAF from RDF gasification via bioenergy with carbon capture and storage (BECCS) and power biomass to liquid (PBtL) concepts with Fischer-Tropsch (FT) and Methanol-to-Jet (MTJ) fuel syntheses as production pathways. The processes are modelled within Aspen Plus and single process units are validated against industrial plant data. In the BECCS route, 95% of carbon dioxide (CO₂) is captured post-syngas conditioning and permanently sequestered, enabling potential negative emissions and carbon credits. The PBtL route integrates green hydrogen from water electrolysis for syngas conditioning, with the electrolytic oxygen supporting gasification and reforming. Results show that integrating green H₂ boosts SAF yield but increases energy demand. The MTJ-H2 pathway demonstrated the lowest levelized cost of production of £7.7/kg SAF, although this is still higher than conventional jet fuel and thus not competitive within the current market. As such, policy frameworks and economic incentives remain essential to achieve large-scale deployment of SAF.
航空业去化石化对实现全球气候目标至关重要,可持续航空燃料(SAF)被确定为关键的低排放解决方案。城市固体废物(MSW)在转化为垃圾衍生燃料(RDF)时,为SAF生产提供了丰富的生物原料,同时转移了垃圾填埋场的废物。本研究分析了以碳捕获和储存(BECCS)为基础的生物能源从RDF气化生产SAF,以及以费托(FT)和甲醇制喷气(MTJ)燃料合成为生产途径的动力生物质制液体(PBtL)概念。在Aspen Plus中对流程进行建模,并根据工业工厂数据验证单个流程单元。在BECCS路线中,95%的二氧化碳(CO₂)在合成气调节后被捕获并永久封存,从而实现潜在的负排放和碳信用。PBtL路线整合了用于合成气调节的水电解绿色氢,以及支持气化和重整的电解氧。结果表明,整合绿色H₂提高了SAF产量,但增加了能源需求。MTJ-H2途径的最低生产成本为7.7英镑/千克SAF,尽管这仍然高于传统航空燃料,因此在当前市场上没有竞争力。因此,政策框架和经济激励对于实现SAF的大规模部署仍然至关重要。
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引用次数: 0
Combined steam and CO2 reforming of ethanol over Ni–Cu/ZrO2 catalyst: Experimental and statistical optimization for sustainable syngas and hydrogen production Ni-Cu /ZrO2催化剂上乙醇蒸汽和CO2联合重整:可持续合成气和制氢的实验和统计优化
IF 7.7 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2026-05-01 Epub Date: 2026-02-03 DOI: 10.1016/j.fuproc.2026.108408
Hossein Hassanzadeh , Reza Abedini , Amir Mosayebi
The combined steam and CO2 reforming of ethanol (CSCRE) is a promising route for sustainable syngas and hydrogen production, enabling simultaneous utilization of renewable ethanol and CO2. In this study, a bimetallic Ni–Cu/ZrO2 catalyst was synthesized and evaluated for the CSCRE reaction through an integrated approach combining catalyst characterization, long-term stability testing, and statistical process optimization. Structural and redox characterization (XRD, BET, H2-TPR, TEM, Raman, and TGA) revealed that Cu incorporation enhances Ni dispersion, improves reducibility, and suppresses sintering and carbon deposition. Response surface methodology (RSM) was employed to investigate the effects of temperature, CO2/H2O ratio, and (CO2 + H2O)/ethanol ratio on ethanol and CO2 conversions, syngas yields, and H2/CO ratio. Reaction temperature was identified as the dominant parameter influencing conversions and product yields, while the CO2/H2O ratio effectively tuned syngas composition. Under the optimized conditions (900 °C, CO2/H2O = 2, (CO2 + H2O)/ethanol = 2), the Ni–Cu/ZrO2 catalyst exhibited high ethanol and CO2 conversions (>90%) and maintained stable activity for approximately 950 min, followed by only moderate deactivation during prolonged operation. The stability tests demonstrated that Ni–Cu/ZrO2 consistently outperforming monometallic Ni/ZrO2 under the different operating conditions. These results highlight the importance of both catalyst design and operating condition optimization in achieving high performance and sustained stability in CSCRE processes.
乙醇蒸汽和二氧化碳联合重整(CSCRE)是一条有前途的可持续合成气和氢气生产途径,可以同时利用可再生乙醇和二氧化碳。本研究合成了一种双金属Ni-Cu /ZrO2催化剂,并通过催化剂表征、长期稳定性测试和统计过程优化相结合的综合方法对CSCRE反应进行了评价。结构和氧化还原表征(XRD, BET, H2-TPR, TEM, Raman和TGA)表明,Cu的加入增强了Ni的分散性,提高了还原性,抑制了烧结和碳沉积。采用响应面法(RSM)考察了温度、CO2/H2O比和(CO2 + H2O)/乙醇比对乙醇和CO2转化率、合成气产率和H2/CO比的影响。反应温度是影响转化率和产率的主要参数,而CO2/H2O比有效地调节了合成气的组成。在优化条件(900℃,CO2/H2O = 2, (CO2 + H2O)/乙醇= 2)下,Ni-Cu /ZrO2催化剂表现出较高的乙醇和CO2转化率(>90%),并保持约950 min的稳定活性,随后在长时间运行中只有适度失活。稳定性测试表明,在不同的操作条件下,Ni - cu /ZrO2的性能始终优于单一金属Ni/ZrO2。这些结果强调了催化剂设计和操作条件优化对于实现CSCRE过程的高性能和持续稳定性的重要性。
{"title":"Combined steam and CO2 reforming of ethanol over Ni–Cu/ZrO2 catalyst: Experimental and statistical optimization for sustainable syngas and hydrogen production","authors":"Hossein Hassanzadeh ,&nbsp;Reza Abedini ,&nbsp;Amir Mosayebi","doi":"10.1016/j.fuproc.2026.108408","DOIUrl":"10.1016/j.fuproc.2026.108408","url":null,"abstract":"<div><div>The combined steam and CO<sub>2</sub> reforming of ethanol (CSCRE) is a promising route for sustainable syngas and hydrogen production, enabling simultaneous utilization of renewable ethanol and CO<sub>2</sub>. In this study, a bimetallic Ni–Cu/ZrO<sub>2</sub> catalyst was synthesized and evaluated for the CSCRE reaction through an integrated approach combining catalyst characterization, long-term stability testing, and statistical process optimization. Structural and redox characterization (XRD, BET, H<sub>2</sub>-TPR, TEM, Raman, and TGA) revealed that Cu incorporation enhances Ni dispersion, improves reducibility, and suppresses sintering and carbon deposition. Response surface methodology (RSM) was employed to investigate the effects of temperature, CO<sub>2</sub>/H<sub>2</sub>O ratio, and (CO<sub>2</sub> + H<sub>2</sub>O)/ethanol ratio on ethanol and CO<sub>2</sub> conversions, syngas yields, and H<sub>2</sub>/CO ratio. Reaction temperature was identified as the dominant parameter influencing conversions and product yields, while the CO<sub>2</sub>/H<sub>2</sub>O ratio effectively tuned syngas composition. Under the optimized conditions (900 °C, CO<sub>2</sub>/H<sub>2</sub>O = 2, (CO<sub>2</sub> + H<sub>2</sub>O)/ethanol = 2), the Ni–Cu/ZrO<sub>2</sub> catalyst exhibited high ethanol and CO<sub>2</sub> conversions (&gt;90%) and maintained stable activity for approximately 950 min, followed by only moderate deactivation during prolonged operation. The stability tests demonstrated that Ni–Cu/ZrO<sub>2</sub> consistently outperforming monometallic Ni/ZrO<sub>2</sub> under the different operating conditions. These results highlight the importance of both catalyst design and operating condition optimization in achieving high performance and sustained stability in CSCRE processes.</div></div>","PeriodicalId":326,"journal":{"name":"Fuel Processing Technology","volume":"283 ","pages":"Article 108408"},"PeriodicalIF":7.7,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146186128","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Evolution of the hydrothermal aging mechanism in Ni/CeO2 catalysts for N2O decomposition based on surface effect 基于表面效应的Ni/CeO2分解N2O催化剂水热老化机理演化
IF 7.7 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2026-05-01 Epub Date: 2026-02-02 DOI: 10.1016/j.fuproc.2026.108407
Hongyu Zhao , Pan Wang , Lili Lei , Zonglin Li , Xuteng Zhao , He Lin
The utilization of Ni/CeO2 catalysts for direct catalytic decomposition of N2O represents a promising technological pathway to mitigate N2O emissions from ammonia-fueled combustion. This study investigated the influence of Ni doping on the N2O decomposition process over both fresh and hydrothermal aging CeO2 catalysts through simulated gas test bench. By combining comprehensive physicochemical characterization with DFT calculations, the hydrothermal aging mechanism underlying the deterioration of catalytic activity and physicochemical properties in Ni/CeO2 catalysts was elucidated. The findings revealed that hydrothermal aging was accompanied by crystallite growth and textural deterioration. Further, hydrothermal aging altered the crystal structure of Ni/CeO2 via edge/corner truncation, resulting in a decreased Ce3+/Ce4+ ratio, an increased OII/OI ratio, and consequently, a reduction in the comprehensive combustion index (S) and combustion stability index (Rw) for N2O decomposition. Ni doping was found to modify the catalytic activity of CeO2 by regulating the adsorption energies of N2O and H2O molecules on low-Miller-index surfaces. The Gibbs free energy changes induced by H2O adsorption on these low-index surfaces (153.6 °C → 430.2 °C → 531.4 °C) were identified as the primary cause for the directional surface migration of CeO2, which ultimately led to the degradation of the catalytic activity of Ni/CeO2 catalysts.
利用Ni/CeO2催化剂直接催化分解N2O是减少氨燃料燃烧中N2O排放的一种有前途的技术途径。通过模拟气体实验台,研究了Ni掺杂对新鲜和水热老化CeO2催化剂上N2O分解过程的影响。通过综合理化表征与DFT计算相结合,阐明了Ni/CeO2催化剂催化活性和理化性能下降的水热老化机理。结果表明,热液老化过程伴随着晶粒的生长和结构的恶化。此外,水热时效通过边角截断改变了Ni/CeO2的晶体结构,导致Ce3+/Ce4+比值降低,OII/OI比值升高,从而降低了N2O分解的综合燃烧指数S和燃烧稳定性指数Rw。发现Ni掺杂通过调节N2O和H2O分子在低米勒指数表面的吸附能来修饰CeO2的催化活性。在这些低指数表面(153.6°C→430.2°C→531.4°C)上,H2O吸附引起的吉布斯自由能变化是CeO2定向表面迁移的主要原因,最终导致Ni/CeO2催化剂的催化活性下降。
{"title":"Evolution of the hydrothermal aging mechanism in Ni/CeO2 catalysts for N2O decomposition based on surface effect","authors":"Hongyu Zhao ,&nbsp;Pan Wang ,&nbsp;Lili Lei ,&nbsp;Zonglin Li ,&nbsp;Xuteng Zhao ,&nbsp;He Lin","doi":"10.1016/j.fuproc.2026.108407","DOIUrl":"10.1016/j.fuproc.2026.108407","url":null,"abstract":"<div><div>The utilization of Ni/CeO<sub>2</sub> catalysts for direct catalytic decomposition of N<sub>2</sub>O represents a promising technological pathway to mitigate N<sub>2</sub>O emissions from ammonia-fueled combustion. This study investigated the influence of Ni doping on the N<sub>2</sub>O decomposition process over both fresh and hydrothermal aging CeO<sub>2</sub> catalysts through simulated gas test bench. By combining comprehensive physicochemical characterization with DFT calculations, the hydrothermal aging mechanism underlying the deterioration of catalytic activity and physicochemical properties in Ni/CeO<sub>2</sub> catalysts was elucidated. The findings revealed that hydrothermal aging was accompanied by crystallite growth and textural deterioration. Further, hydrothermal aging altered the crystal structure of Ni/CeO<sub>2</sub> via edge/corner truncation, resulting in a decreased Ce<sup>3+</sup>/Ce<sup>4+</sup> ratio, an increased O<sub>II</sub>/O<sub>I</sub> ratio, and consequently, a reduction in the comprehensive combustion index (<em>S</em>) and combustion stability index (<em>R</em><sub>w</sub>) for N<sub>2</sub>O decomposition. Ni doping was found to modify the catalytic activity of CeO<sub>2</sub> by regulating the adsorption energies of N<sub>2</sub>O and H<sub>2</sub>O molecules on low-Miller-index surfaces. The Gibbs free energy changes induced by H<sub>2</sub>O adsorption on these low-index surfaces (153.6 °C → 430.2 °C → 531.4 °C) were identified as the primary cause for the directional surface migration of CeO<sub>2</sub>, which ultimately led to the degradation of the catalytic activity of Ni/CeO<sub>2</sub> catalysts.</div></div>","PeriodicalId":326,"journal":{"name":"Fuel Processing Technology","volume":"283 ","pages":"Article 108407"},"PeriodicalIF":7.7,"publicationDate":"2026-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146186137","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Effect of flue gas recirculation on the formation of unburned hydrocarbons in oxy-fuel and air flames in a semi-industrial scale burner 烟气再循环对半工业规模燃烧器中含氧燃料和空气火焰中未燃烃形成的影响
IF 7.7 2区 工程技术 Q1 CHEMISTRY, APPLIED Pub Date : 2026-05-01 Epub Date: 2026-02-06 DOI: 10.1016/j.fuproc.2026.108413
D. König, D. Hülsbruch, J. Ströhle, B. Epple
Oxy-fuel combustion is a promising technology for reducing CO2 emissions in the energy sector. In this process, nitrogen from air is replaced with CO2, to ensure the purity of CO2 in the flue gas, altering the properties of the oxidizer. For industrial applications, different methods of supplying CO2 for the combustion are possible, typically categorized into different recirculation pathways: These include recirculation pathways with higher moisture and minority species content as well as a recirculation of cleaned flue gas after the scrubbing stages of the plant. These approaches differ primarily in oxidizer temperature, the amount of H2O present in the oxidizer stream and the occurrence of minority species. However, the presence of H2O in the combustion environment influences the gasification mechanisms within the flame, similar to the effects of CO2. This paper compares the formation and presence of unburned hydrocarbons between a conventional air flame and two oxy-fuel combustion cases, one using a mixture of synthetic CO2 and O2 and the other incorporating flue gas recirculation. Analyzing these intermediate species in the different flames, features a significant insight into the combustion chemistry and can be used as validation data for a detailed Computational Fluid Dynamics (CFD) and kinetic modeling of this process. This comparison for the same flame leads to increased knowledge about the differences between synthetic oxy-fuel combustion and flue gas recirculation and is a novelty in the field of semi-industrial oxy-fuel combustion. For the experiments, milled walnut shells are used as fuel. Comparing air and oxy-fuel combustion, the oxy-fuel flames shows significantly higher unburned hydrocarbons in the flame. However, the results indicate that differences in unburned hydrocarbon formation between the two oxy-fuel cases become apparent only at greater distances from the burner inlet, which is attributed to higher oxidizer inlet temperatures, adiabatic flame temperature, and increased H2O content in the oxy-fuel case with flue gas recirculation. This leads to increased hydrocarbons present in the end of the synthetic oxy-fuel case.
在能源领域,全氧燃烧是一种很有前途的减少二氧化碳排放的技术。在这个过程中,空气中的氮被二氧化碳取代,以确保烟气中二氧化碳的纯度,改变氧化剂的性质。对于工业应用,可以采用不同的方法为燃烧提供二氧化碳,通常分为不同的再循环途径:这些再循环途径包括具有较高水分和少数物种含量的再循环途径,以及在工厂洗涤阶段之后的清洁烟气再循环。这些方法的主要区别在于氧化剂温度、氧化剂流中存在的水的量和少数物种的出现。然而,燃烧环境中H2O的存在会影响火焰内的气化机制,类似于CO2的影响。本文比较了传统空气火焰和两种含氧燃料燃烧情况下未燃烧碳氢化合物的形成和存在,其中一种使用合成CO2和O2的混合物,另一种使用烟气再循环。分析不同火焰中的这些中间物质,对燃烧化学有重要的了解,可以用作详细的计算流体动力学(CFD)和该过程的动力学建模的验证数据。这种对同一火焰的比较增加了对合成全氧燃料燃烧和烟气再循环之间差异的认识,并且在半工业全氧燃料燃烧领域是一种新颖的方法。在实验中,磨碎的核桃壳被用作燃料。与空气燃烧和全氧燃烧相比,全氧燃烧火焰中未燃烧的碳氢化合物含量明显较高。然而,结果表明,两种含氧燃料情况下未燃烃形成的差异仅在距离燃烧器入口较远的地方才会变得明显,这是由于在含氧燃料情况下,烟气再循环时氧化剂入口温度、绝热火焰温度和H2O含量较高。这导致在合成含氧燃料的情况下,末端存在更多的碳氢化合物。
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引用次数: 0
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Fuel Processing Technology
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