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Catalytic pyrolysis of plastic to produce aromatic hydrocarbons over the Zn modified ZSM-5 catalysts Zn改性ZSM-5催化剂催化塑料热解生成芳烃的研究
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-28 DOI: 10.1016/j.joei.2026.102462
Daoxuan Sun , Weidong Nie , Shue Tian , Dong Han , Laizhi Sun , Lei Chen , Shuangxia Yang , Tianjin Li , Zhiguo Dong , Baofeng Zhao , Meirong Xu , Xinping Xie , Hongyu Si , Dongliang Hua
The catalytic pyrolysis of high-density polyethylene (HDPE) over the Zn modified ZSM-5 zeolite catalysts was systematically examined to improve the yield of aromatic hydrocarbons. The Zn/ZSM-5 catalysts with different zinc loadings were synthesized by the incipient wetness impregnation method and thoroughly characterized by the BET, XRD, NH3-TPD, SEM, and TG techniques. The influences of the Zn content, the reaction temperature, and the catalyst-to-feedstock mass ratio on the distribution of products and the selectivity of aromatics were investigated. The results indicated that under the optimized conditions of 5 % Zn loading, the reaction temperature of 450 °C, and the catalyst-to-feedstock mass ratio of 2/1, the selectivity of monocyclic aromatic hydrocarbons (MAHs) reached 85.65 %, while the selectivity of benzene, toluene, ethylbenzene, and xylene (BTEX) was as high as 62.06 %. The 5 % Zn/ZSM-5 catalyst also exhibited the excellent structural stability and retained about 85 % selectivity of MAHs after 10 successive cycles. The characterization analyses confirmed that the incorporation of Zn metal altered the pore environment and the acidity profile of the ZSM-5, thereby enhancing the dehydrogenation and aromatization of the pyrolytic intermediates. A reaction mechanism of the catalytic pyrolysis of HDPE over the Zn/ZSM-5 was proposed, suggesting that the generation of the aromatic hydrocarbons was promoted through the hydrogen-transfer, oligomerization, and cyclization pathways. These findings demonstrated that the Zn/ZSM-5 catalysts provide a promising strategy for the selective conversion of plastic waste into the value-added aromatic hydrocarbons.
系统研究了Zn改性ZSM-5沸石催化剂对高密度聚乙烯(HDPE)的催化热解,以提高芳香烃的收率。采用初湿浸渍法制备了不同锌载量的Zn/ZSM-5催化剂,并用BET、XRD、NH3-TPD、SEM和TG等技术对其进行了表征。考察了锌含量、反应温度、催化剂与原料质量比对产物分布和芳烃选择性的影响。结果表明,在Zn负载5%、反应温度450℃、催化剂与原料质量比为2/1的优化条件下,单环芳烃(MAHs)的选择性达到85.65%,苯、甲苯、乙苯和二甲苯(BTEX)的选择性高达62.06%。5% Zn/ZSM-5催化剂在连续循环10次后仍保持85%的mah选择性,具有良好的结构稳定性。表征分析证实,锌金属的掺入改变了ZSM-5的孔隙环境和酸度分布,从而促进了热解中间体的脱氢和芳构化。提出了HDPE在Zn/ZSM-5催化剂上催化热解的反应机理,表明HDPE通过氢转移、低聚和环化等途径促进了芳烃的生成。这些发现表明,Zn/ZSM-5催化剂为塑料垃圾选择性转化为高附加值芳烃提供了一种很有前途的策略。
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引用次数: 0
A combined experimental and simulation study on toluene cracking: synergistic strategy of Ni loading, alkali treatment, and atmosphere activation on HZSM-5 zeolite HZSM-5沸石甲苯裂化实验与模拟相结合:Ni负载、碱处理和气氛活化协同策略
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-28 DOI: 10.1016/j.joei.2026.102467
Qinlong Hu, Haoyang Lou, Zhuqing Niu, Jiankai Zhang, Xinjia Wang, Hui Jin, Zhongming Bu, Guoneng Li, Yuanjun Tang, Chao Ye
This study systematically explores nickel-based HZSM-5 zeolite activated by NaOH treatment in different atmospheres (air and CO2), revealing the intricate synergistic mechanisms between structure, acidity, and metal active sites during the catalytic cracking of toluene. The research found that the pore structure and acid site distribution of the catalyst can be directionally tuned through the choice of atmosphere: air activation primarily expands mesopores and optimizes mass transfer, while CO2 activation finely tunes the acid sites, significantly enhancing the weak and medium-strength acid sites, thereby constructing a rich reactive interface for the adsorption and initial activation of toluene. In the reaction pathway, a significant synergistic effect between the metal and the support was observed: nickel species were reduced to highly dispersed nanoparticles, serving as the core sites for activating C-H and C-C bonds, which cooperated with the acidic centers of the zeolite to promote the cleavage of toluene molecules and the opening of the benzene ring, ultimately converting them into small molecule synthesis gas. Under conditions of 7% nickel loading and CO2 activation, the maximum toluene conversion rate reached 78.92%. The flow-mass transfer-reaction coupling model constructed using COMSOL successfully replicated the experimental trends (simulation efficiency 79%) and clarified that temperature and feed flow rate are key operational parameters affecting the cracking behavior. From the perspectives of "structure-acidity synergy" and "metal-support interaction," this study deepens the understanding of the micro-mechanism of toluene catalytic cracking, providing a theoretical basis for the rational design of catalysts and process optimization.
本研究系统研究了不同气氛(空气和CO2)下NaOH处理后的镍基HZSM-5沸石,揭示了甲苯催化裂化过程中结构、酸度和金属活性位点之间复杂的协同机制。研究发现,催化剂的孔结构和酸位分布可以通过气氛的选择进行定向调节:空气活化主要是扩大介孔和优化传质,而CO2活化则对酸位进行精细调节,显著增强弱、中强酸位,从而为甲苯的吸附和初始活化构建了丰富的反应界面。在反应途径中,观察到金属与载体之间存在显著的协同作用:镍被还原为高度分散的纳米颗粒,作为活化C-H和C-C键的核心位点,与沸石的酸性中心协同作用,促进甲苯分子的裂解和苯环的打开,最终转化为小分子合成气体。在含镍量为7%、CO2活化的条件下,甲苯转化率最高可达78.92%。利用COMSOL建立的流动-传质-反应耦合模型成功地复制了实验趋势(模拟效率79%),并阐明了温度和进料流量是影响裂解行为的关键操作参数。本研究从“结构-酸度协同”和“金属-载体相互作用”的角度,加深了对甲苯催化裂化微观机理的认识,为催化剂的合理设计和工艺优化提供了理论依据。
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引用次数: 0
Enhanced CO2 methanation over SiO2-supported catalysts with embedded and surface Ni sites 在嵌入和表面Ni位点的sio2负载催化剂上增强CO2甲烷化
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-27 DOI: 10.1016/j.joei.2026.102466
Duc-Thang Tran , Nguyen-Phuong Nguyen , Thanh-Linh H. Duong , Anh Minh-Nhat Lai , Quang-Long Nguyen , Minh-Tuan Nguyen-Dinh , Tri Nguyen , Hoang-Duy P. Nguyen , Thuy-Phuong T. Pham
Mitigation of CO2 emissions has become a global challenge, and its catalytic conversion to CH4 represents a promising route for carbon utilization as well as renewable fuel production. In this work, a series of Ni/SiO2 catalysts were synthesized via wet impregnation, a modified sol-gel process, and a combined sol-gel/post-impregnation approach to balance embedded and surface Ni species for efficient CO2 methanation. The as-prepared, reduced and spent catalysts were characterized by XRD, N2 physisorption, TEM, H2-TPR, CO2-TPD, H2-TPD and TPO to correlate structural properties with catalytic performance. The Ni-embedded SiO2 catalyst (20Ni-SiO2) exhibited higher BET surface area, uniform mesoporosity, better dispersion and stronger MSI compared to the impregnated 20Ni/SiO2, highlighting the importance of sol-gel incorporation in texture control. Interestingly, CO2-TPD revealed greater CO2 adsorption ability for impregnated Ni species, whereas H2-TPD indicated superior hydrogen dissociation activity for embedded Ni species. Consequently, due to the synergistic contribution of embedded and surface Ni species, the post-impregnated 10Ni/(20Ni-SiO2) catalyst achieved 81.6 % CO2 conversion and 99.5 % CH4 selectivity at 350 °C, outperforming conventional impregnated and sol-gel catalysts. Stability tests and TPO profiles confirm that the 10Ni/(20Ni-SiO2) catalyst maintains efficient performance over 100 h, with only a 5 % decrease in CO2 conversion, negligible change in CH4 selectivity, and excellent resistance to coke formation.
减缓二氧化碳排放已成为一项全球性挑战,其催化转化为CH4是碳利用和可再生燃料生产的一条有希望的途径。本文通过湿浸渍法、溶胶-凝胶法和溶胶-凝胶/浸渍后相结合的方法合成了一系列Ni/SiO2催化剂,以平衡嵌入和表面Ni,实现高效的CO2甲烷化。采用XRD、N2物理吸附、TEM、H2-TPR、CO2-TPD、H2-TPD和TPO等手段对制备、还原和废催化剂进行了表征,以确定催化剂的结构性能与催化性能之间的关系。与浸渍的20Ni/SiO2相比,ni包埋SiO2催化剂(20Ni-SiO2)表现出更高的BET比表面积、均匀的介孔、更好的分散性和更强的MSI,凸显了溶胶-凝胶掺入在织构控制中的重要性。有趣的是,CO2- tpd对浸渍的Ni具有更强的CO2吸附能力,而H2-TPD对浸渍的Ni具有更强的氢解离活性。因此,由于包埋镍和表面镍的协同作用,浸渍后的10Ni/(20Ni-SiO2)催化剂在350°C时的CO2转化率为81.6%,CH4选择性为99.5%,优于传统的浸渍和溶胶-凝胶催化剂。稳定性测试和TPO曲线证实,10Ni/(20Ni-SiO2)催化剂在100 h内保持高效性能,CO2转化率仅下降5%,CH4选择性变化可以忽略不计,并且具有优异的抗焦性。
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引用次数: 0
Catalytic cracking of biomass gasification tar integrated with carbon fixation over steel slag-based catalyst 钢渣基催化剂催化裂解生物质气化焦油及固碳
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-17 DOI: 10.1016/j.joei.2026.102455
Hanrui Ma , Guangzhe Zhang , Hongkai Di , Tao Zhang , Yuxin Li , Jingsi Yang , Ruihong Zhao , Jiangze Han , Kunjie Li
This study addresses the dual challenges of tar yield control and CO2 emissions in biomass gasification by developing a composite catalyst derived from converter steel slag. Through KOH activation and Ni impregnation, the optimized 10Ni-A-SS catalyst achieved 87.1 % tar cracking efficiency, increasing hydrogen yield from 232.2 to 576.3 mL/g biomass while retaining a CO2 adsorption capacity of 120.0 mg/(g cat). Characterization results indicated that KOH activation significantly increased the catalyst's specific surface area, with NiO impregnation providing additional active sites. Mechanistic analysis revealed that the catalyst suppressed tar polymerization and polycondensation reactions, redirecting reaction pathways toward phenols and light aromatics, thereby substantially reducing polycyclic aromatic hydrocarbon formation. This work demonstrates an effective strategy for valorizing industrial steel slag waste while enabling cleaner, hydrogen-rich syngas production from biomass gasification, offering both environmental and economic benefits.
本研究通过开发从转炉钢渣中提取的复合催化剂,解决了生物质气化中焦油产率控制和二氧化碳排放的双重挑战。通过KOH活化和Ni浸渍,优化后的10Ni-A-SS催化剂的焦油裂解效率为87.1%,产氢量从232.2 mL/g生物质提高到576.3 mL/g生物质,同时保持了120.0 mg/(g cat)的CO2吸附量。表征结果表明,KOH活化显著提高了催化剂的比表面积,而NiO浸渍则提供了额外的活性位点。机理分析表明,该催化剂抑制了焦油聚合缩聚反应,使反应途径转向酚类和轻芳烃,从而大大减少了多环芳烃的生成。这项工作证明了一种有效的策略,可以使工业钢渣废物增值,同时使生物质气化产生更清洁、富氢的合成气,提供环境和经济效益。
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引用次数: 0
Reactivity and stability optimization of oxygen carriers in chemical looping systems 化学环系中氧载体的反应性及稳定性优化
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-17 DOI: 10.1016/j.joei.2026.102456
Huijia Liang , Jie Yang , Juan Hou , Changye Han , Lizhuo Peng , Junjie Shi , Liping Ma
Chemical looping technology (CLT) produces flue gas enriched with carbon dioxide, which can then be captured, utilized, or stored. The oxygen carrier (OC) plays a central role in the chemical looping process, but its low activity and short lifespan hinder its industrial application. The existing review literature on CLT primarily focuses on the application of specific OCs and their developmental trends, but lacks a comprehensive summary of OC activity and cycle life. To address the gaps in existing literature, this paper explores the activity and recycling lifespan of OCs in relation to their defects. Furthermore, strategies to improve OC reactivity are discussed, beginning with the selection of active species aided by Ellingham diagrams. The advantages of non-metallic and solid waste-based OCs in chemical looping reactions are compared, along with a summary of strategies to enhance their activity. To prolong the service life of OCs, this paper outlines the primary mechanisms of carrier failure, which are primarily attributed to the combined effects of wear and stress. For different types of stress, targeted solutions are proposed: a supported carrier approach for chemical stress, a core-shell structure for mechanical stress, and elemental doping for thermal stress. Finally, the paper explores the application prospects of solid waste-based OCs and their development towards achieving a tripartite stress equilibrium, thus opening new avenues for the practical application of OCs. These studies contribute to advancing the efficient utilization of chemical looping systems in environmental protection and sustainable energy supply.
化学环技术(CLT)产生富含二氧化碳的烟气,然后可以捕获、利用或储存。氧载体(OC)在化学环过程中起着核心作用,但其活性低、寿命短,阻碍了其工业应用。现有关于CLT的综述文献主要集中于特定OC的应用及其发展趋势,缺乏对OC活性和循环寿命的全面总结。为了解决现有文献中的空白,本文探讨了与OCs缺陷相关的OCs的活性和回收寿命。此外,本文还讨论了提高OC反应性的策略,首先是利用Ellingham图进行活性物质的选择。比较了非金属和固体废物基OCs在化学环反应中的优点,并总结了提高其活性的策略。为了延长OCs的使用寿命,本文概述了载体失效的主要机制,主要是由于磨损和应力的共同作用。针对不同类型的应力,提出了有针对性的解决方案:支持载体方法用于化学应力,核壳结构用于机械应力,元素掺杂用于热应力。最后,探讨了固体废物基复合材料的应用前景及其在实现三方应力平衡方面的发展,从而为复合材料的实际应用开辟了新的途径。这些研究有助于促进化学环系统在环境保护和可持续能源供应中的有效利用。
{"title":"Reactivity and stability optimization of oxygen carriers in chemical looping systems","authors":"Huijia Liang ,&nbsp;Jie Yang ,&nbsp;Juan Hou ,&nbsp;Changye Han ,&nbsp;Lizhuo Peng ,&nbsp;Junjie Shi ,&nbsp;Liping Ma","doi":"10.1016/j.joei.2026.102456","DOIUrl":"10.1016/j.joei.2026.102456","url":null,"abstract":"<div><div>Chemical looping technology (CLT) produces flue gas enriched with carbon dioxide, which can then be captured, utilized, or stored. The oxygen carrier (OC) plays a central role in the chemical looping process, but its low activity and short lifespan hinder its industrial application. The existing review literature on CLT primarily focuses on the application of specific OCs and their developmental trends, but lacks a comprehensive summary of OC activity and cycle life. To address the gaps in existing literature, this paper explores the activity and recycling lifespan of OCs in relation to their defects. Furthermore, strategies to improve OC reactivity are discussed, beginning with the selection of active species aided by Ellingham diagrams. The advantages of non-metallic and solid waste-based OCs in chemical looping reactions are compared, along with a summary of strategies to enhance their activity. To prolong the service life of OCs, this paper outlines the primary mechanisms of carrier failure, which are primarily attributed to the combined effects of wear and stress. For different types of stress, targeted solutions are proposed: a supported carrier approach for chemical stress, a core-shell structure for mechanical stress, and elemental doping for thermal stress. Finally, the paper explores the application prospects of solid waste-based OCs and their development towards achieving a tripartite stress equilibrium, thus opening new avenues for the practical application of OCs. These studies contribute to advancing the efficient utilization of chemical looping systems in environmental protection and sustainable energy supply.</div></div>","PeriodicalId":17287,"journal":{"name":"Journal of The Energy Institute","volume":"125 ","pages":"Article 102456"},"PeriodicalIF":6.2,"publicationDate":"2026-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146034580","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
Experimental study and process analysis on Co-production of hydrogen-rich gas and carbon nanotubes via catalytic pyrolysis of solid wastes 固体废物催化热解产富氢气体与碳纳米管的实验研究及工艺分析
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-17 DOI: 10.1016/j.joei.2026.102454
Zhongfa Hu , Bixiu Lv , Wenjing Ma , Bin Liu , Xuebin Wang , Yili Zhang , Zia ur Rahman , Renhui Ruan
<div><div>The decomposition of polyethylene into hydrogen and carbon nanotubes by pyrolysis not only enables the proper disposal of large amounts of waste plastic but also achieves the targeted production of hydrogen and high-value carbon nanotubes, thus it is widely applied in industry. In this paper, typical solid wastes, such as polyethylene (PE) and sawdust, were used as raw materials, and continuous pyrolysis-catalysis experiments were conducted on a two-stage pilot system (rotary kiln for pyrolysis and fixed-bed for catalysis).To overcome the limitations of traditional fixed-bed reactors in organic waste treatment, this study develops a continuous pyrolysis-catalytic co-production process for the simultaneous generation of high-value hydrogen gas and carbon nanotube (CNTs), aiming for system energy self-sufficiency. The core research encompasses experimental validation under specific conditions and simulation analysis of three process routes based on experimental results. Successful experimental validation was achieved under continuous operation at a feeding rate of 1 g min<sup>−1</sup>, pyrolysis temperature of 500 °C, catalytic temperature of 750 °C, and using a coal gangue-based nickel catalyst (loading 10 %) for processing polyethylene (PE) and wood chips; significant PE conversion yielded a hydrogen concentration (H<sub>2</sub>) in the gas product as high as 64.6 vol%, with a production rate reaching 27.4 mmol g<sup>−1</sup> while substantial coking occurred on the catalyst surface achieving a yield of 32.5 wt%. Characterization of the PE-derived coke indicated that it primarily consisted of CNTs with hollow tubular structures confirmed by TEM images and high graphitization degree and good crystallinity indicated by Raman spectroscopy (<em>I</em><sub>D</sub>/<em>I</em><sub>G</sub> = 0.75) and TPO results where graphite carbon accounted for 38.8 wt%. Based on experimental data, three process routes were established using Aspen Plus software all utilizing partial pyrolysis oil/gas combustion to supply energy for the system balance but differing in the handling of pyrolyzed coke; simulation optimization showed that route I (coke combustion) performed best under optimal conditions (raw material moisture content 20 %, oil/gas ratio 25 %, gasification stage O<sub>2</sub>/feedstock = 0.25, H<sub>2</sub>O/feedstock = 0.5) achieving a hydrogen yield of 1102.6 Nm<sup>3</sup>·t<sup>−1</sup> and a CNTs yield of 43.9 kg t<sup>−1</sup> whereas route II (coke gasification) had slightly lower target product yields compared to route I and route III (coke collection) collected pyrolyzed coke as solid products (biochar) without thermal treatment resulting in the lowest carbon emissions but also the lowest target product yields. Comprehensive analysis indicates that adopting a continuous pyrolysis-catalytic unit combined with the design of utilizing pyrolyzed coke for energy supply efficiently converts organic solid waste into high-value hydrogen and CNTs
通过热解将聚乙烯分解为氢气和碳纳米管,不仅可以合理处理大量废塑料,而且可以有针对性地生产氢气和高价值的碳纳米管,因此在工业上得到了广泛的应用。本文以聚乙烯(PE)、木屑等典型固体废弃物为原料,在两段式中试系统(热解为回转窑,催化为固定床)上进行了连续热解催化实验。为了克服传统固定床反应器在有机废物处理中的局限性,本研究开发了一种连续热解-催化联产工艺,同时生成高值氢气和碳纳米管(CNTs),旨在实现系统能源自给。核心研究包括特定条件下的实验验证和基于实验结果的三种工艺路线的仿真分析。在加料速度为1 g min−1、热解温度为500℃、催化温度为750℃、煤矸石基镍催化剂(负载10%)处理聚乙烯(PE)和木屑的连续运行条件下,实验验证成功;显著的PE转化率使产物中的氢浓度(H2)高达64.6 vol%,产率达到27.4 mmol g−1,而催化剂表面发生了大量焦化,产率达到32.5 wt%。对pe衍生焦炭的表征表明,其主要由具有空心管状结构的CNTs组成,TEM图像证实了其结构,拉曼光谱结果表明石墨化程度高,结晶度好(ID/IG = 0.75), TPO结果表明石墨碳占38.8 wt%。基于实验数据,利用Aspen Plus软件建立了3条工艺路线,均采用部分热解油气燃烧为系统平衡提供能量,但对焦炭的处理方式不同;模拟优化结果表明,在原料含水率20%、油气比25%、气化阶段O2/原料= 0.25的最优条件下,路线1(焦炭燃烧)效果最佳。H2O/原料= 0.5),氢气产率为1102.6 Nm3·t−1,碳纳米管产率为43.9 kg t−1,而路线II(焦炭气化)的目标产物产率略低于路线I和路线III(焦炭收集),未经热处理将热解焦炭作为固体产物(生物炭)收集,导致碳排放最低,但目标产物产率也最低。综合分析表明,采用连续热解催化装置结合焦炭供能设计,能有效地将有机固体废弃物转化为高价值的氢和碳纳米管,同时实现系统能量的自我维护,为工业应用提供了一个很有前景的方案。
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引用次数: 0
Pyrolysis process intensification of mixed medical waste using grinding beads and hematite in an indirectly heated rotary kiln 利用磨珠和赤铁矿在间接加热回转窑中强化混合医疗废物的热解过程
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-14 DOI: 10.1016/j.joei.2026.102453
Zhipeng Zhou , Shuo Ma , Kexun Wang , Hongting Ma
This study investigates the efficacy of grinding beads as a heat transfer intensifier and hematite catalyst for the pyrolysis of mixed medical waste (MMW) in an indirectly heated rotary kiln. The focus was on elucidating the impact of these additives on intra-bed heat-mass transfer and the product distribution. Thermogravimetric and kinetic analyses revealed the fundamental pyrolysis characteristics and interaction effects during the co-pyrolysis of cellulose-based MW and polypropylene(PP), notably the inhibition of PP degradation. Subsequent rotary kiln experiments demonstrated that the addition of silicon carbide(SiC) beads at an additive-to-feedstock mass ratio of 0.6 increased the wall-to-bed heat transfer coefficient by approximately 24 %, from 174.5 to 217.0 W/(m2·K), and reduced the radial temperature gradients. Tar yield increased from 35.38 % to 38.71 %. Powdered hematite (Fe2O3) acted as a catalyst, altering selectivity towards gas production and enhancing the hydrogen yield by over 62.13 %. This study concludes that the deliberate selection of additives provides a highly effective strategy for process intensification: high-thermal-conductivity beads (SiC) mitigate heat transfer limitations, whereas catalytic media (Fe2O3) actively steer the product distribution.
研究了磨珠作为传热强化剂和赤铁矿催化剂在间接加热回转窑中热解混合医疗废弃物的效果。重点阐明了这些添加剂对床内热质传递和产物分布的影响。热重分析和动力学分析揭示了纤维素基MW与聚丙烯(PP)共热解的基本热解特征和相互作用效应,特别是对PP降解的抑制作用。随后的回转窑实验表明,添加掺料质量比为0.6的碳化硅(SiC)微球,使壁床传热系数从174.5 W/(m2·K)提高到217.0 W/(m2·K),提高了约24%,并减小了径向温度梯度。焦油收率由35.38%提高到38.71%。粉末赤铁矿(Fe2O3)作为催化剂,改变了产气的选择性,使产氢率提高了62.13%以上。本研究的结论是,添加剂的精心选择为过程强化提供了一种非常有效的策略:高导热珠子(SiC)减轻了传热限制,而催化介质(Fe2O3)积极地引导产品分布。
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引用次数: 0
Comparative study of the effects of reactor system and catalysts on glycerol valorisation via aqueous-phase reforming 反应器体系和催化剂对水相重整甘油增值影响的比较研究
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-10 DOI: 10.1016/j.joei.2026.102447
Carine T. Alves , Francisco Maldonado-Martín , Alejandro Lete , Seyed Emad Hashemnezhad , Lucía García , Jude A. Onwudili
The conversion of glycerol through aqueous phase reforming (APR) presents an important opportunity for sustainable chemical and fuel production. This study explores the APR of glycerol using three catalysts (nickel supported on alumina (NiAl), copper supported on alumina (CuAl), and bimetallic nickel-iron supported on alumina (NiAlFe)), synthesized via the coprecipitation method. The APR experiments were conducted in both batch and fixed-bed reactors. In the batch reactor, a 75 mL Parr reactor was utilised, operating at 238 °C and 5 bar initial nitrogen pressure with 20 mL of a 5 wt% glycerol solution and 0.3 g of catalyst (catalyst/glycerol mass ratio = 0.3). The fixed-bed reactor was made of a stainless steel tube loaded with 2 g of catalyst, operating at 238 °C and 37 bar, with a continuous feed of 5 wt% glycerol solution, equivalent to catalyst/glycerol mass ratio of 0.33. NiAl produced the highest conversion of glycerol to gases and the highest yield of hydrogen (230 mg H2/mol C fed). However, among the tested catalysts, NiAlFe demonstrated superior performance, achieving a carbon yield to total products (liquid and gases) of approximately 80 % in the batch reactor as well as a relatively high hydrogen yield (141 mg H2/mol C fed). These results underscore the promising potential of the NiAlFe catalyst for efficient glycerol conversion in APR processes, paving the way for advancements in sustainable fuel and chemical production.
通过水相重整(APR)转化甘油为可持续的化学品和燃料生产提供了重要的机会。本研究采用共沉淀法合成了三种催化剂(氧化铝负载镍(NiAl)、氧化铝负载铜(CuAl)和氧化铝负载镍铁双金属(NiAlFe)),探讨了甘油的APR。在间歇式反应器和固定床反应器中进行了APR实验。在间歇式反应器中,使用75 mL Parr反应器,在238℃和5 bar初始氮压下运行,20 mL 5 wt%的甘油溶液和0.3 g催化剂(催化剂/甘油质量比= 0.3)。固定床反应器由一根不锈钢管制成,负载2g催化剂,在238℃和37 bar下工作,连续进料5 wt%的甘油溶液,相当于催化剂/甘油质量比为0.33。NiAl产生最高的甘油气体转化率和最高的氢气产量(230 mg H2/mol C)。然而,在测试的催化剂中,NiAlFe表现出优异的性能,在间歇反应器中实现了总产物(液体和气体)的碳收率约为80%,以及相对较高的氢气收率(141 mg H2/mol C)。这些结果强调了NiAlFe催化剂在APR过程中有效转化甘油的潜力,为可持续燃料和化学品生产的进步铺平了道路。
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引用次数: 0
Mechanistic investigation of H2/CO ratio on laminar flame characteristics of NH3/syngas blends H2/CO比对NH3/合成气共混物层流火焰特性的影响机理研究
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-09 DOI: 10.1016/j.joei.2026.102452
Fahui Wang , Yan Guo , Dan Zhang , Huolong Chen , Zihan Liu , Jun Zhao
Ammonia (NH3) blended with syngas offers a promising strategy for enhancing its combustion performance. However, the practical application of such fuel blends is frequently constrained by variations in the H2/CO ratio. This study combines an integrated experimental and numerical approach, incorporating both global and local sensitivity analyses, to elucidate how the H2/CO ratio affects the laminar burning velocity (SL) and flame instability of NH3/H2/CO blends. The results reveal that variations in SL are predominantly governed by chemical kinetic effects, which weaken as the equivalence ratio (Ф) increases. This behavior is affected by the competition among CO oxidation reactions, H radical consumption pathways, and third-body (H2O) termination reactions, in which both H and OH radicals play critical roles. Regarding the variation in flame instability with the H2/CO ratio, it is primarily governed by thermal diffusive instability and flame thickness effects. As the Ф changes, thermal diffusive dominates under fuel-lean conditions, whereas both thermal diffusive and the thermal expansion ratio collectively dominate flame instability under fuel-rich conditions. When considering the combined effects of pressure and temperature, it is observed that an increased H2/CO ratio markedly enhances the pressure dependence of NH3/H2/CO flames, whereas its influence on temperature dependence remains relatively limited. These findings provide a theoretical basis for the application of NH3-based fuels in combustion systems.
氨(NH3)与合成气混合是提高合成气燃烧性能的一种很有前途的策略。然而,这种燃料混合物的实际应用经常受到H2/CO比变化的限制。本研究结合综合实验和数值方法,结合全局和局部敏感性分析,阐明H2/CO比如何影响NH3/H2/CO混合物的层流燃烧速度(SL)和火焰不稳定性。结果表明,SL的变化主要由化学动力学效应控制,随着等效比(Ф)的增大,化学动力学效应减弱。这种行为受到CO氧化反应、H自由基消耗途径和第三体(H2O)终止反应之间竞争的影响,其中H和OH自由基都起着关键作用。火焰不稳定性随H2/CO比的变化主要受热扩散不稳定性和火焰厚度的影响。随着Ф的变化,在贫燃料条件下,热扩散占主导地位,而在富燃料条件下,热扩散和热膨胀比共同主导火焰不稳定性。当考虑压力和温度的综合影响时,H2/CO比值的增加显著增强了NH3/H2/CO火焰的压力依赖性,而其对温度依赖性的影响相对有限。这些研究结果为nh3基燃料在燃烧系统中的应用提供了理论依据。
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引用次数: 0
Sustainable thermocatalytic conversion of CO2 to fuels and chemicals via reverse water-gas shift reactions for carbon neutrality 可持续的热催化将二氧化碳转化为燃料和化学品,通过逆向水气转换反应实现碳中和
IF 6.2 2区 工程技术 Q2 ENERGY & FUELS Pub Date : 2026-01-08 DOI: 10.1016/j.joei.2026.102449
Ijaz Hussain , Gazali Tanimu , Niladri Maity , Khalid Alhooshani , Saheed Ganiyu , Abdullah Aitani , Mohammad Alalouni , Mohammad Aljishi , Emad N. Al-Shafei
The pressing urge to address climate change and reduce atmospheric CO2 levels has driven significant research into CO2 conversion technologies. Among these, the reverse water-gas shift (RWGS) reaction presents a promising pathway for transforming CO2 into CO, which can subsequently be utilized in syngas conversion processes to generate valuable chemicals and fuels. However, the RWGS reaction faces challenges related to its moderate endothermic nature and competition with the highly exothermic CO2 methanation reaction at low temperatures. Enhancing low-temperature reaction efficiency and CO selectivity remains a critical focus in catalyst development. This review paper explores novel developments in diverse catalyst materials and presents practical insights into thermocatalytic pathways for the RWGS reaction. Emerging strategies for improving CO2 conversion efficiency, CO selectivity, and energy utilization are explored. Additionally, reactor designs, operational parameters, and their integration with other processes are analyzed to enhance overall process performance. A techno-economic assessment is presented, highlighting the feasibility and potential impacts of these advancements, along with recommendations for future research directions. This work underscores the importance of interdisciplinary collaboration to overcome existing challenges and realize the full potential of RWGS technologies for sustainable CO2 utilization.
应对气候变化和降低大气二氧化碳水平的迫切需求推动了对二氧化碳转化技术的重大研究。其中,逆向水气转换(RWGS)反应是将CO2转化为CO的一个有希望的途径,随后可用于合成气转化过程,以产生有价值的化学品和燃料。然而,RWGS反应面临着中等吸热性质和与低温高放热CO2甲烷化反应竞争的挑战。提高低温反应效率和CO选择性仍然是催化剂发展的一个关键问题。本文综述了各种催化剂材料的最新进展,并对RWGS反应的热催化途径提出了实际的见解。探讨了提高CO2转化效率、CO选择性和能源利用的新策略。此外,还分析了反应器设计、操作参数及其与其他工艺的集成,以提高整体工艺性能。提出了技术经济评估,强调了这些进步的可行性和潜在影响,并对未来的研究方向提出了建议。这项工作强调了跨学科合作的重要性,以克服现有的挑战,实现RWGS技术在可持续利用二氧化碳方面的全部潜力。
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引用次数: 0
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