Journal of The Energy Institute最新文献_第6页

Experimental investigation on emission characteristics of laminar premixed CH4-NH3 jet impinging flames across a wide range of conditions 层流预混CH4-NH3射流大范围冲击火焰发射特性的实验研究

IF 6.2 2区工程技术 Q2 ENERGY & FUELS

Journal of The Energy Institute

Pub Date : 2025-11-24 DOI: 10.1016/j.joei.2025.102392

Zhilong Wei, Guanglong Huang, Guangyu Zeng, Haisheng Zhen

This study investigates the CO and NO emission characteristics of laminar premixed CH₄-NH₃ jet impinging flames under various conditions. Effects of equivalence ratio (φ), ammonia fraction in the fuel blends (η_NH3) and Reynolds number (Re) on pollutant formation are analyzed comprehensively under different impingement conditions. Results show that CO emissions generally increase with φ due to oxidizer deficiency, with their variations mainly controlled by wall-cooling effects on CO oxidation in lean flames. In contrast, NO emissions exhibit a V-shaped dependence on φ, with higher levels in fuel-rich flames. Additional air entrainment at fuel-rich conditions promotes NH₃ oxidation and suppresses DeNOx reactions, leading to the elevated NO levels. Meanwhile, strong wall cooling at small nozzle-to-wall distance (H) favors the HNO pathway, further increasing NO emissions near the wall. When increasing η_NH3, CO emissions decrease steadily owing to reduced carbon input. However, the extent of reduction depends on the impingement condition, showing a moderate decrease at large H and a more pronounced decline at small H. NO emissions initially rise with η_NH3 up to about 60 %, driven by enhanced NH/NH₂ radical formation and thermal-NO production, and then decrease at higher η_NH3 as reduced reactivity slows NH₃ oxidation and strengthens DeNOx reactions. Besides, CO emissions decrease with increasing Re at small H because stronger impingement suppresses premixed combustion and CO generation, while they increase at large H due to enhanced CO formation resulting from the coupling effects of the reduced wall cooling, extended post-flame zones and limited ambient oxidizer. NO emissions rise monotonically with Re, driven by higher flame temperatures, enhanced NH₃ consumption and inhibited NO destruction. Overall, flame impingement dominates the overall CO/NO emission levels, while φ, η_NH3 and Re modulate detailed emission behaviors through coupled effects of wall cooling and air entrainment.

研究了不同条件下层流预混CH4-NH3射流撞击火焰的CO和NO排放特性。综合分析了不同撞击条件下当量比（φ）、燃料混合物中氨分数（ηNH3）和雷诺数（Re）对污染物形成的影响。结果表明：由于氧化剂缺乏，CO排放量普遍随φ增加而增加，其变化主要受稀薄火焰中CO氧化的壁冷效应控制；相比之下，NO排放量与φ呈v型关系，在燃料丰富的火焰中排放量更高。在燃料丰富的条件下，额外的空气夹带促进NH3氧化并抑制DeNOx反应，导致NO水平升高。同时，在喷嘴与壁面距离(H)较小的情况下，强壁面冷却有利于HNO途径，进一步增加了壁面附近的NO排放。当ηNH3增加时，由于碳输入减少，CO排放量稳定下降。然而，减少的程度取决于撞击条件，在大H时，减少幅度适中，在小H时下降更为明显，当ηNH3达到60%左右时，由于nhh /NH2自由基形成和热NO生成的增强，NO排放量开始上升，然后在高ηNH3时，由于反应性降低减缓了NH3氧化并加强了DeNOx反应，NO排放量下降。此外，在小H下，CO排放量随着Re的增加而减少，这是因为更强的撞击抑制了预混燃烧和CO的生成，而在大H下，CO排放量增加，这是由于壁面冷却减少、火焰后区域延长和环境氧化剂限制的耦合作用导致CO生成增强。由于火焰温度升高、NH3消耗增加和NO破坏受到抑制，NO排放量随Re单调上升。总体而言，火焰撞击主导了CO/NO的总体排放水平，而φ、ηNH3和Re通过壁面冷却和夹带空气的耦合作用调节了详细的排放行为。

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引用次数: 0

Chemiluminescence-based control for low-emission combustion in a rich-lean staged burner 富贫分级燃烧器低排放燃烧的化学发光控制

IF 6.2 2区工程技术 Q2 ENERGY & FUELS

Journal of The Energy Institute

Pub Date : 2025-11-24 DOI: 10.1016/j.joei.2025.102397

Weiqi Luo , Wenjun Ding , Jianguo Du , Yu Wang

Staged burners have been widely used in industry to reduce NO_x emissions. However, the overall effectiveness depends on its operation conditions. Traditional monitoring methods of NO_x and CO emissions, such as gas analyzers, are too slow and impractical for real-time optimization. This study investigates flame chemiluminescence as a practical, non-intrusive indicator for combustion control. A staged-burner experimental platform was developed allowing independent control of fuel and air supply. Pollutant concentrations (CO, NO_x) and flame radiative emission spectra (OH*, CH*, C₂*) were measured under varied excess air ratios. Results reveal that CH*/OH* ratios decrease linearly, while C₂*/CH* and C₂*/OH* exhibit unimodal behaviors with increasing air ratio. These spectral signatures strongly correlate with emission levels, enabling indirect yet reliable indicators for low-emission operation. Spatially resolved measurements with ICCD imaging further validate optimal detection zones and filter bandwidth effects, ensuring applicability with cost-effective sensors. Overall, this work demonstrates the feasibility of chemiluminescence-guided closed-loop control, offering a pathway toward cleaner and more efficient industry burners.

分级燃烧器已广泛应用于工业中，以减少氮氧化物的排放。然而，整体效果取决于其运行条件。传统的NOx和CO排放监测方法，如气体分析仪，速度太慢，无法实现实时优化。本研究将火焰化学发光作为一种实用的、非侵入性的燃烧控制指标。研制了可独立控制燃料和空气供给的分级燃烧器实验平台。测量了不同过量空气比下污染物浓度（CO, NOx）和火焰辐射发射光谱（OH*, CH*, C2*）。结果表明，随着空气比的增加，CH*/OH*的比值呈线性下降，而C2*/CH*和C2*/OH*表现为单峰态。这些光谱特征与发射水平密切相关，为低发射操作提供了间接但可靠的指标。ICCD成像的空间分辨率测量进一步验证了最佳检测区域和滤波器带宽效果，确保了具有成本效益的传感器的适用性。总的来说，这项工作证明了化学发光引导闭环控制的可行性，为更清洁、更高效的工业燃烧器提供了一条途径。

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引用次数: 0

Research on performance improvement of ammonia engine based on optimization of active pre-chamber hydrogen injection strategy 基于主动预室喷氢策略优化的氨发动机性能提升研究

IF 6.2 2区工程技术 Q2 ENERGY & FUELS

Journal of The Energy Institute

Pub Date : 2025-11-19 DOI: 10.1016/j.joei.2025.102383

Liming Wang , Fangxi Xie , Linghai Han , Yanfeng Gong , Hanshi Qu , Zhe Zhao , Xiangyang Wang

Ammonia is a zero-carbon fuel with broad application prospects, yet it faces challenges such as difficulty in ignition and slow flame propagation speed. Active pre-chamber hydrogen jet ignition represents a highly promising technical approach to overcoming the combustion challenges of ammonia. In this experiment, the effects of pre-chamber hydrogen injection parameters on engine combustion, fuel economy, and emission characteristics were investigated. The results indicate that a hydrogen energy ratio (HER) around 6.6 % yields the most concentrated combustion, significantly increases the peak heat release rate, and shortens the combustion duration. The brake thermal efficiency (BTE) shows a non-monotonic relationship with HER, achieving its maximum value at HER = 6.6 %, which is 3.62 % higher than at HER = 1.8 %. Regarding emissions, increasing HER reduces unburned NH₃ but increases NO_x emissions. Excessively advanced or retarded hydrogen injection timing (HIT) delays the combustion phasing, reduces the indicated mean effective pressure (IMEP), and increases NH₃ emissions. Combustion performance are optimal when HIT is between 75°CA BTDC and 100°CA BTDC. In comparison, HIP exhibits a minor influence on engine performance, with 1 MPa yielding superior performance in IMEP and BTE while maintaining the coefficient of variation of IMEP (COV_IMEP) below 2.3 %. This work establishes optimized injection parameter ranges for active pre-chamber ammonia engines, providing critical insights for scaling up hydrogen-enhanced ammonia combustion systems.

氨是一种具有广泛应用前景的零碳燃料，但它也面临着点火困难、火焰传播速度慢等挑战。主动预室氢喷射点火是克服氨燃烧挑战的一种非常有前途的技术方法。本试验研究了预室喷氢参数对发动机燃烧、燃油经济性和排放特性的影响。结果表明，当氢能比（HER）为6.6%左右时，燃烧最集中，峰值放热率显著提高，燃烧持续时间缩短。制动热效率（BTE）与HER呈非单调关系，在HER = 6.6%时达到最大值，比HER = 1.8%时高出3.62%。在排放方面，增加HER减少了未燃烧的NH3，但增加了NOx排放。过度提前或延迟的氢喷射时间（HIT）会延迟燃烧阶段，降低指示的平均有效压力（IMEP），并增加NH3排放。燃烧性能在75°CA下止点到100°CA下止点之间最佳。相比之下，低压力对发动机性能的影响较小，当压力为1 MPa时，发动机在IMEP和BTE方面表现优异，同时IMEP的变异系数（COVIMEP）保持在2.3%以下。这项工作为主动预室氨发动机建立了优化的喷射参数范围，为扩大氢增强氨燃烧系统提供了重要见解。

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引用次数: 0

Morphology-engineered Y2O3 nanostructures for boosting the RWGS reaction performance over Cu-based catalysts 形态工程Y2O3纳米结构在cu基催化剂上提高RWGS反应性能

IF 6.2 2区工程技术 Q2 ENERGY & FUELS

Journal of The Energy Institute

Pub Date : 2025-11-11 DOI: 10.1016/j.joei.2025.102381

Peng Zhang , Guang-Hui Liu , Yao-Shun Wen , Yu-Hong Kang , Yang-Fan Yin , Sheng Li , Zhi-Xin Li , Zhi-Hao Ma

Morphology engineering plays a pivotal role in boosting catalytic performance over heterogeneous catalysis. However, although Y₂O₃ (a rare earth oxide) has been found to possess various morphologies, including nanoplate (NP), nanosphere (NS) and nanorod (NR), the lack of understanding of its catalytic mechanism still limits its further application. Herein, catalytic mechanism of Y₂O₃ morphologies in reverse water-gas shift (RWGS) reaction over Cu-based catalysts was systematically investigated. Although Y₂O₃ morphologies don't affect CO selectivity, it has a significant impact on CO₂ conversion and stability. Systematic characterization reveals that Y₂O₃ morphologies not only can optimize the CO₂ adsorption capacity and Cu nanoparticles size to enhance catalytic activity, but also can regulate the metal-support interaction to improve catalytic stability. The order of activity and stability of the Cu/Y₂O₃ catalysts from high to low is: Cu/_NPY₂O₃ > Cu/_NRY₂O₃ > Cu/_NSY₂O₃. This work clarifies the morphological-performance relationship in rare earth oxide-Y₂O₃, providing a new approach for the design of high-performance Cu-based catalysts for RWGS reaction and promoting the application of morphology engineering in heterogeneous catalysis.

形态学工程在提高多相催化性能方面起着关键作用。然而，尽管Y2O3（一种稀土氧化物）已经被发现具有多种形态，包括纳米板（NP）、纳米球（NS）和纳米棒（NR），但对其催化机理的缺乏了解仍然限制了它的进一步应用。本文系统研究了Y2O3形态在cu基催化剂上催化水气反变换反应的机理。虽然Y2O3的形貌不影响CO的选择性，但对CO2的转化率和稳定性有显著影响。系统表征表明，Y2O3形态不仅可以优化CO2吸附能力和Cu纳米颗粒尺寸，提高催化活性，还可以调节金属-载体相互作用，提高催化稳定性。Cu/Y2O3催化剂的活性和稳定性由高到低的顺序为：Cu/NPY2O3 >； Cu/NRY2O3 > Cu/NSY2O3。本研究阐明了稀土氧化物- y2o3的形态-性能关系，为设计高性能cu基RWGS反应催化剂提供了新途径，促进了形态工程在多相催化中的应用。

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引用次数: 0

Ozone-enhanced extinction limits of ammonia counterflow diffusion flames: Detections by chemical explosive mode analysis 臭氧增强氨逆流扩散火焰的消光极限：化学爆炸模式分析检测

IF 6.2 2区工程技术 Q2 ENERGY & FUELS

Journal of The Energy Institute

Pub Date : 2025-11-11 DOI: 10.1016/j.joei.2025.102382

Jiuyi Zhang , Yinhu Kang , Haoran Wang , Wenxuan Zhou , Xiaomei Huang , Xiaofeng Lu , Jiayi Chang , Wenjin Lai

This article studies the promotion effect as well as the underlying physics of ozone (O₃) addition on the ammonia (NH₃) flammability. By the aid of chemical explosive mode analysis (CEMA) and diffusion index (DI), this study systematically elucidates the mechanisms through which O₃ extends the extinction limits of NH₃ counterflow diffusion flames. It shows that at the O₃ substitution ratio θ = 0.4 (X_O3 = 8.54 %), the extinction strain rate increases by 15.68-folds, and the maximum temperature is elevated by 16.9 % compared to the pure-air condition. O atoms produced via the O₃ decomposition in the low-temperature zone trigger the subsequent exothermic chain-branching reactions, substantially elevating radical pool concentrations and augmenting reactivity across both the low- and high-temperature regions. The extension of flammability limit upon O₃ addition is primarily due to the ozone chemistry, while the oxygen-enrichment effect is relatively less important. Moreover, CEMA diagnostics indicate that heat and N₂ diffusions play distinct roles in the low-temperature ignition chemistry, which determines the local combustion mode transition from extinction (EXTC) to diffusion-assisted ignition (DIFF), a process fundamentally-significant to the extension of extinction limit. Diffusion and chemistry in the secondary heat release zone are rather insensitive to strain rate, exerting minimal influence on extinction. In contrast, the primary reaction zone exhibits a distinct modal sequence (exhaust→DIFF→EXTC) with increasing strain rate. Extinction eventually happens when the EXTC branch encroaches into the primary heat release peak, arising from flame inhibition induced by NH₃ diffusion (DI(NH₃)<0, α < −1), which surpasses the augmentation effect by heat conduction. In summary, O₃ enhances the NH₃ flammability by reshaping the low-temperature reaction pathways and intensity and altering the local combustion modes. The findings would be fundamentally meaningful to the development of efficient and reliable ammonia-fueled combustion systems in practical scenarios.

本文研究了臭氧（O3）的加入对氨（NH3）可燃性的促进作用及其潜在的物理性质。借助化学爆炸模式分析（CEMA）和扩散指数（DI），系统阐述了O3扩展NH3逆流扩散火焰消灭极限的机理。结果表明，当O3取代比θ = 0.4 （XO3 = 8.54 %）时，消光应变率提高了15.68倍，最高温度比纯空气条件下提高了16.9%。低温区O3分解产生的O原子引发了随后的放热链支反应，大大提高了自由基池浓度，增强了低温区和高温区的反应活性。O3加入后可燃性极限的扩大主要是由于臭氧化学作用，而富氧作用相对不太重要。此外，CEMA诊断表明，高温和氮气扩散在低温点火化学过程中起着明显的作用，这决定了局部燃烧模式从熄灭（EXTC）到扩散辅助点火（DIFF）的转变，这一过程对熄灭极限的扩展具有根本意义。二次放热区的扩散和化学对应变速率不敏感，对消光的影响最小。随着应变速率的增加，主反应区呈现出明显的排气→DIFF→EXTC的模态序列。NH3扩散（DI(NH3)<0, α <−1）引起的火焰抑制作用超过了热传导的增强作用，当EXTC分支侵入主放热峰时最终发生熄灭。综上所述，O3通过重塑低温反应路径和强度以及改变局部燃烧模式来增强NH3的可燃性。这一发现对于开发高效可靠的氨燃料燃烧系统具有重要意义。

{"title":"Ozone-enhanced extinction limits of ammonia counterflow diffusion flames: Detections by chemical explosive mode analysis","authors":"Jiuyi Zhang , Yinhu Kang , Haoran Wang , Wenxuan Zhou , Xiaomei Huang , Xiaofeng Lu , Jiayi Chang , Wenjin Lai","doi":"10.1016/j.joei.2025.102382","DOIUrl":"10.1016/j.joei.2025.102382","url":null,"abstract":"<div><div>This article studies the promotion effect as well as the underlying physics of ozone (O3) addition on the ammonia (NH3) flammability. By the aid of chemical explosive mode analysis (CEMA) and diffusion index (DI), this study systematically elucidates the mechanisms through which O3 extends the extinction limits of NH3 counterflow diffusion flames. It shows that at the O3 substitution ratio θ = 0.4 (XO3 = 8.54 %), the extinction strain rate increases by 15.68-folds, and the maximum temperature is elevated by 16.9 % compared to the pure-air condition. O atoms produced via the O3 decomposition in the low-temperature zone trigger the subsequent exothermic chain-branching reactions, substantially elevating radical pool concentrations and augmenting reactivity across both the low- and high-temperature regions. The extension of flammability limit upon O3 addition is primarily due to the ozone chemistry, while the oxygen-enrichment effect is relatively less important. Moreover, CEMA diagnostics indicate that heat and N2 diffusions play distinct roles in the low-temperature ignition chemistry, which determines the local combustion mode transition from extinction (EXTC) to diffusion-assisted ignition (DIFF), a process fundamentally-significant to the extension of extinction limit. Diffusion and chemistry in the secondary heat release zone are rather insensitive to strain rate, exerting minimal influence on extinction. In contrast, the primary reaction zone exhibits a distinct modal sequence (exhaust→DIFF→EXTC) with increasing strain rate. Extinction eventually happens when the EXTC branch encroaches into the primary heat release peak, arising from flame inhibition induced by NH3 diffusion (DI(NH3)<0, α < −1), which surpasses the augmentation effect by heat conduction. In summary, O3 enhances the NH3 flammability by reshaping the low-temperature reaction pathways and intensity and altering the local combustion modes. The findings would be fundamentally meaningful to the development of efficient and reliable ammonia-fueled combustion systems in practical scenarios.</div></div>","PeriodicalId":17287,"journal":{"name":"Journal of The Energy Institute","volume":"124 ","pages":"Article 102382"},"PeriodicalIF":6.2,"publicationDate":"2025-11-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145517264","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

Using waste to treat waste: elemental mercury removal from flue gas by coal gasification slag 利用废物处理废物：利用煤气化渣去除烟气中的单质汞

IF 6.2 2区工程技术 Q2 ENERGY & FUELS

Journal of The Energy Institute

Pub Date : 2025-11-10 DOI: 10.1016/j.joei.2025.102364

Yili Zhang , Xin Su , Hao Guo , Rihong Xiao , Xuebin Wang , Junying Zhang

Coal gasification slag (GS), a solid waste from the coal chemical industry, holds promise as an efficient and environmentally friendly adsorbent. This study selected four typical gasification slag samples and conducted mercury removal experiments at different reaction temperatures. The results showed that sample refined carbon (RC) was suitable for low-temperature mercury removal, achieving an efficiency of 90.91 %, while sample fine slag (FS) was more effective at high temperatures, with a removal efficiency of 83.64 %. Subsequently, we investigated the mercury removal performance of the different types of gasifier slag samples in the presence of SO₂, NO, HCl, and H₂S. The results indicated that sample FS exhibited better resistance to flue gas components. Regarding the adsorption mechanism, the mercury adsorption by RC was attributed to the action of surface-adsorbed hydroxyl groups, whereas the mercury adsorption by FS was due to chemical adsorption by oxygen. The low leaching toxicity further confirms the safety of GS. This study provided valuable guidance for the application of gasification slag in mercury removal processes.

煤气化渣（GS）是煤化工工业产生的一种固体废弃物，是一种高效、环保的吸附剂。本研究选取了四种典型的气化渣样品，在不同的反应温度下进行了除汞实验。结果表明：样品精炭（RC）适用于低温除汞，其除汞效率为90.91%；样品细渣（FS）适用于高温除汞，其除汞效率为83.64%。随后，我们研究了不同类型的气化炉渣样品在SO2、NO、HCl和H2S存在下的除汞性能。结果表明，FS样品对烟气组分具有较好的抗性。在吸附机理上，RC对汞的吸附是由于表面羟基的作用，FS对汞的吸附是由于氧的化学吸附。低浸出毒性进一步证实了GS的安全性。该研究为气化渣在除汞工艺中的应用提供了有价值的指导。

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引用次数: 0

Boosting hydrogen production in biomass pyrolysis via Pr - doped Ni/ZrO2 catalysts Pr掺杂Ni/ZrO2催化剂促进生物质热解制氢

IF 6.2 2区工程技术 Q2 ENERGY & FUELS

Journal of The Energy Institute

Pub Date : 2025-11-08 DOI: 10.1016/j.joei.2025.102370

Xiawen Yu, Zhenxing Bu, Quantian Li, Jianfen Li

This study aims to develop an efficient hydrogen production route by enhancing nickel-based catalysts for biomass pyrolysis toward syngas. To this end, a series of Pr-modified ZrO₂-supported nickel catalysts were synthesized and compared with unmodified Ni/ZrO₂ counterparts. The catalysts were systematically characterized to elucidate morphological and compositional changes induced by Pr doping. Evaluation of catalytic performance revealed a 29 % increase in hydrogen yield for the Pr-doped catalysts relative to the undoped system. Under optimized conditions—including a pyrolysis temperature of 900 °C, pyrolysis time of 30 min, calcination temperature of 500 °C, Ni loading of 5 wt%, and a Zr/Pr molar ratio of 8:2—the Pr-doped Ni/ZrO₂ catalyst achieved a maximum H₂ yield of 0.7359 L/g and exhibited remarkable catalytic stability. The enhancement in performance is mainly ascribed to the role of Pr doping, which not only stabilizes the ZrO₂ support but also modulates the acid–base properties of the catalyst, thereby improving Ni dispersion and reinforcing the antioxidant capacity of the system. These combined effects contribute to highly efficient hydrogen production during biomass pyrolysis.

本研究旨在通过强化镍基催化剂，开发生物质热解制合成气的高效制氢路线。为此，合成了一系列pr改性ZrO2负载镍催化剂，并与未改性的Ni/ZrO2催化剂进行了比较。对催化剂进行了系统表征，以阐明Pr掺杂引起的形貌和组成变化。催化性能的评估表明，与未掺杂的体系相比，掺pr的催化剂的氢产率提高了29%。在热解温度为900℃、热解时间为30 min、煅烧温度为500℃、Ni负载为5 wt%、Zr/Pr摩尔比为8:2的优化条件下，掺Pr的Ni/ZrO2催化剂H2产率最高可达0.7359 L/g，且具有良好的催化稳定性。性能的增强主要是由于Pr掺杂的作用，它不仅稳定了ZrO2载体，而且调节了催化剂的酸碱性质，从而改善了Ni的分散性，增强了体系的抗氧化能力。这些综合效应有助于在生物质热解过程中高效产氢。

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引用次数: 0

Experimental study and kinetic analysis of the role of H2O on CO-NH3 Co-oxidation in a plug flow reactor 塞流反应器中H2O对CO-NH3共氧化作用的实验研究及动力学分析

IF 6.2 2区工程技术 Q2 ENERGY & FUELS

Journal of The Energy Institute

Pub Date : 2025-11-07 DOI: 10.1016/j.joei.2025.102369

Kun Li, Leming Cheng, Qifeng Yu, Weiguo Zhang

Co-firing of NH₃ with coal became an interesting topic due to the issues of carbon dioxide emissions. The reactivity variations of NH₃ with CO, as well as the formation of NO and N₂O under H₂O-free and H₂O-containing condition is one of the important aspects during the coal and NH₃ co-firing process. In this work, experimental and kinetic studies were conducted on the co-oxidation of CO and NH₃ in a plug flow reactor to investigate these characteristics. Influencing parameters including temperature, initial CO and H₂O concentration were examined. Results indicates that the onset temperature of NH₃ decreases and the formation of NO and N₂O increases with increasing initial CO concertation under H₂O-free conditions. The presence of NH₃ inhibits CO conversion due to their competition for OH. Under H₂O-containing conditions, H₂O reduces the onset temperature of the CO-NH₃ co-oxidation and promotes CO burnout under both fuel-lean and fuel-rich conditions. Meanwhile, H₂O inhibits NO formation while N₂O generation was enhanced. This is attributed to increased OH level through the reactions H₂O + O = 2OH and H₂O + H = OH + H₂, along with reduced concentrations of O and H radicals. These changes enhance CO reactivity in the early stages and alters NO formation pathway. The decrease in O radical suppresses the NH₂ → HNO → NO pathway, while the increase in OH radical promotes NH₂ to NH conversion. It enhances the NH₂ → NH → NO and NH₂ → NH → HNO → NO pathways. Additionally, the increased NH radical concentration favors the NH₂ → NH → N₂O pathway, which contributes to increased N₂O yields.

由于二氧化碳排放的问题，NH3与煤共烧成为一个有趣的话题。无水和含水条件下NH3与CO的反应性变化以及NO和N2O的生成是煤与NH3共烧过程的重要方面之一。在这项工作中，通过实验和动力学研究在塞流反应器中CO和NH3共氧化来研究这些特性。考察了温度、CO初始浓度和H2O初始浓度等参数的影响。结果表明：在无h2o条件下，随着初始CO浓度的增加，NH3的起始温度降低，NO和N2O的生成增加；NH3的存在抑制了CO的转化，因为它们竞争OH。在含水条件下，H2O降低了CO- nh3共氧化的起始温度，促进了贫燃料和富燃料条件下CO的燃尽。同时，H2O抑制NO的生成，促进N2O的生成。这是由于H2O + O = 2OH和H2O + H = OH + H2反应增加了OH水平，同时O和H自由基浓度降低。这些变化在早期阶段增强了CO的反应性，改变了NO的形成途径。O自由基的减少抑制NH2→HNO→NO途径，而OH自由基的增加促进NH2到NH的转化。增强NH2→NH→NO和NH2→NH→HNO→NO通路。此外，NH自由基浓度的增加有利于NH2→NH→N2O途径，这有助于提高N2O产率。

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引用次数: 0

Development of a copper doped iron-based oxygen carrier for hydrogen production via mid-temperature chemical looping 中温化学环法制氢用铜掺杂铁基氧载体的研制

IF 6.2 2区工程技术 Q2 ENERGY & FUELS

Journal of The Energy Institute

Pub Date : 2025-11-07 DOI: 10.1016/j.joei.2025.102361

Yu Fang , Jiquan Luo , Zhulian Li , Junnan Zhan , Kai Liu , Qibin Liu

Chemical looping reforming (CLR) offers a promising approach for low-carbon hydrogen production by integrating fuel conversion with inherent CO₂ separation. In this study, iron-based oxygen carriers doped with nickel and copper were synthesized to improve reactivity and cyclic stability. Structural characterization via X-ray diffractometer (XRD) and energy-dispersive X-ray spectrometer (SEM/EDS) confirmed the formation of active phases including NiFe₂O₄ and CuFe₂O₄, which have homogeneous elemental dispersion and nanostructured morphologies. Temperature programmed reduction experiments in TGA revealed that Ni doping enhances reaction rates, while copper doping lowers the reduction temperature. Among the synthesized carriers, 1 wt%Cu–20NiFe exhibited the best overall performance in terms of methane conversion (82.45 %), hydrogen yield (74.40 mL/g_OC), and carbon monoxide yield (22.04 mL/g_OC) at 600 °C. Steam-assisted CLR experiments show that water significantly improved H₂ production, and appropriate steam flow could maximize hydrogen yield while suppressing carbon deposition. Long-term redox cycling (200 cycles) verified the structural integrity and oxygen transfer stability of 1 wt%Cu–20NiFe. X-ray photoelectron spectroscopy (XPS) analyses across different reaction stages confirmed the cyclic migration of lattice oxygen and complete regeneration of the oxygen carrier. This work demonstrates that micro-doped Cu in Ni–Fe-based oxygen carriers effectively enhances CLR hydrogen production, providing a foundation for further scale-up and integration in chemical looping hydrogen systems.

化学环重整（CLR）将燃料转化与固有的二氧化碳分离相结合，为低碳制氢提供了一种很有前途的方法。本研究合成了掺杂镍和铜的铁基氧载体，以提高反应性和循环稳定性。通过x射线衍射仪（XRD）和能量色散x射线能谱仪（SEM/EDS）的结构表征，证实了NiFe2O4和CuFe2O4等活性相的形成，具有均匀的元素色散和纳米结构形态。温度程序还原实验表明，Ni的加入提高了反应速率，而铜的加入降低了反应温度。在600℃时，1 wt% Cu-20NiFe在甲烷转化率（82.45%）、氢气产率（74.40 mL/gOC）和一氧化碳产率（22.04 mL/gOC）方面表现最佳。蒸汽辅助CLR实验表明，水可以显著提高H2产量，适当的蒸汽流量可以最大限度地提高氢气产量，同时抑制碳沉积。长期氧化还原循环（200次）验证了1 wt% Cu-20NiFe的结构完整性和氧传递稳定性。不同反应阶段的x射线光电子能谱（XPS）分析证实了晶格氧的循环迁移和氧载体的完全再生。本研究表明，在ni - fe基氧载体中微掺杂Cu有效地提高了CLR制氢量，为进一步扩大和集成化学环氢系统提供了基础。

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引用次数: 0

Upgrading of bio-oil from torrefied wheat straw over Fe-Ni modified HZSM-5@MCM-41: Influence of pyrolysis temperature and catalyst-feedstock ratio Fe-Ni改性HZSM-5@MCM-41改性麦秸生物油的提质研究：热解温度和催化剂进料比的影响

IF 6.2 2区工程技术 Q2 ENERGY & FUELS

Journal of The Energy Institute

Pub Date : 2025-11-07 DOI: 10.1016/j.joei.2025.102366

Ziwen Zhao, Hong Tian, Zhengye Chen, Zhangjun Huang, Shan Cheng, Siying Liu

This study employed torrefied wheat straw (260 °C) as feedstock to synthesize a bifunctional metal-modified composite zeolite catalyst through alkali treatment (NaOH), dual metal loading (Fe and Ni), and hierarchical MCM-41 construction. Catalytically assisted pyrolysis behaviour was investigated using a tube furnace and Py-GC/MS system, evaluating the effects of pyrolysis temperature and catalyst/feedstock mixing ratio on product distribution and bio-oil composition. Results indicate that at a catalyst/feedstock ratio of 3:2, bio-oil yield peaked at 28.41 % at 500 °C, concurrently achieving a maximum monocyclic aromatic content of 66.36 %. Elevating pyrolysis temperature promoted aromatic formation while significantly suppressing oxygenated compounds; notably, phenolic components decreased by 13.94 % at 500 °C, indicating the 1Ni1FeHR@M catalyst's potent deoxygenation capability. Further optimization of the catalyst/feedstock blending ratio revealed that a 3:2 ratio yielded the highest combined bio-oil and monocyclic aromatic hydrocarbon production (18.62 %), confirming this catalytic strategy effectively shifts the product distribution towards higher-value hydrocarbon fuels.

本研究以碳化麦秸（260°C）为原料，经碱处理（NaOH）、双金属负载（Fe和Ni）、MCM-41分层结构合成双功能金属改性复合沸石催化剂。采用管式炉和Py-GC/MS系统研究了催化辅助热解行为，评估了热解温度和催化剂/原料混合比例对产物分布和生物油组成的影响。结果表明，在催化剂与原料比为3:2的条件下，生物油收率在500℃时达到28.41%，同时单环芳烃含量达到66.36%。提高热解温度促进芳香族的形成，同时显著抑制含氧化合物的形成；值得注意的是，在500°C时，酚类成分减少了13.94%，表明1Ni1FeHR@M催化剂具有强大的脱氧能力。进一步优化催化剂/原料混合比例发现，3:2的比例可产生最高的生物油和单环芳烃产量（18.62%），证实该催化策略有效地将产品分布转向高价值的碳氢燃料。

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