IF 7.5 1区工程技术 Q2 ENERGY & FUELS

Fuel

Pub Date : 2025-12-15 DOI: 10.1016/j.fuel.2025.138018

Feng Chen , Pan Deng , Jing-Ping Zhao , Zhi-Yang Ren , Tianlong Liu , Xiao-Bo Feng , Jing-Pei Cao

The design and synthesis of directly shaped zeolites via one-step hydrothermal method are attractive for industrial applications. However, realizing zeolites with millimeter level and sufficient mechanical strength remains a formidable challenge. Herein, the mechanically robust FER, MOR, and FER/MOR composite zeolite monoliths about 2 mm spherical monoliths were synthesized by one-setp without bindeless. These millimeter-sized spherical monoliths, assembled from nanosheets and nanorods, combine superior acidity and mass transfer efficiency. The differences in pore structure and acid site distribution between monolithic and conventional binder-based zeolites is elucidate. Over these millimeter-sized spherical monoliths, the DME catalytic performance is surpasses commercial shaped catalysts by 2–3 times. Moreover, regeneration under a low-oxygen atmosphere stabilizes the framework Al and ensures outstanding structural integrity and catalytic durability under cyclic operation. In addition, the influence of pyridine poison the acid site of shanped MOR zeolite is expounded. By finely adjusted the pyridine poison procedure over the MOR millimeter-sized MOR zeolite, the catalyst life can be significantly improved. Our findings provide novel and valuable insights for the design of industrial catalysts in syngas/CO₂ to ethanol technology.

一步水热法直接成型沸石的设计和合成具有较好的工业应用前景。然而，实现毫米级的沸石和足够的机械强度仍然是一个艰巨的挑战。本文采用一步无粘结法制备了机械性能稳定的FER、MOR和FER/MOR复合沸石单体，孔径约为2mm。这些毫米大小的球形单体，由纳米片和纳米棒组装而成，结合了优越的酸度和传质效率。阐明了整体型和常规粘结剂型沸石在孔结构和酸位分布上的差异。在这些毫米大小的球形单体上，二甲醚的催化性能比商业形状的催化剂高出2-3倍。此外，在低氧气氛下的再生稳定了框架Al，并确保了循环操作下出色的结构完整性和催化耐久性。此外，还阐述了吡啶中毒对异形MOR沸石酸位的影响。在毫米级MOR分子筛上精细调整吡啶中毒过程，可显著提高催化剂寿命。我们的研究结果为合成气/二氧化碳制乙醇工业催化剂的设计提供了新的和有价值的见解。

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引用次数: 0

Enhancing the efficiency of methylcyclohexane dehydrogenation of Pt/Al2O3 catalyst doped by Ga and Ce adding: Unraveling the role of oxygen vacancy 添加Ga和Ce提高Pt/Al2O3催化剂甲基环己烷脱氢效率：揭示氧空位的作用

IF 7.5 1区工程技术 Q2 ENERGY & FUELS

Fuel

Pub Date : 2025-12-15 DOI: 10.1016/j.fuel.2025.137981

Chen-Xu Chen , Jing-Pei Cao , Nai-Yu Yao , Wen Tang , Wei Jiang , Chuang Zhang , Xiao-Yan Zhao , Xiao-Yu Qiao , Tungalagtamir Bold

Improving the catalytic efficiency and catalyst life of Pt/Al₂O₃ catalyst for methylcyclohexane dehydrogenation is of great significance for the study of organic liquid hydrogen storage. In this work, the promotion effects of Ga and Ce on the substantial improvement of catalytic stability and activity over the Pt/Al₂O₃ during the methylcyclohexane dehydrogenation were investigated. The catalyst with optimizing Ga and Ce loading (1.5 wt%) exhibits ∼99.76 % selectivity and H₂ evolution rate of 2102 mol/g_Pt/min at 300 °C. In 100 h long-time reaction, the conversion of methylcyclohexane remains around 75 % with no significant decrease. The characterization results show that introducing proper amount of Ga and Ce helps Ga³⁺ cations incorporate into the lattice structure of CeO₂ that increase concentration of oxygen vacancies and CeO₂ reducibility in the catalyst, which boost the capability of methylcyclohexane dehydrogenation and tolerance for coke formation. Thus, the excellent stability and activity are achieved over the GaCe-modified catalyst. This study may share new light on the rational construction of highly efficient Pt-based catalysts for methylcyclohexane dehydrogenation.

提高Pt/Al2O3催化剂对甲基环己烷脱氢的催化效率和催化剂寿命，对有机液氢储氢的研究具有重要意义。本文研究了Ga和Ce对Pt/Al2O3在甲基环己烷脱氢过程中催化稳定性和活性的显著提高的促进作用。优化后的Ga和Ce负载（1.5 wt%）的催化剂在300℃下具有~ 99.76%的选择性和2102 mol/gPt/min的析氢速率。在100 h的长时间反应中，甲基环己烷的转化率保持在75%左右，没有明显下降。表征结果表明，适量的Ga和Ce的加入有助于Ga3+离子进入CeO2的晶格结构，提高了催化剂中氧空位的浓度和CeO2的还原性，提高了甲基环己烷脱氢能力和耐结焦能力。因此，gace改性催化剂具有优异的稳定性和活性。本研究为合理构建高效的pt基甲基环己烷脱氢催化剂提供了新的思路。

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引用次数: 0

Experimental study on methane reforming coupled with thermochemical water splitting using kilogram scale oxygen carriers for co-production of hydrogen and syngas 千克氧载体甲烷重整与热化学水裂解联产氢合成气的实验研究

IF 7.5 1区工程技术 Q2 ENERGY & FUELS

Fuel

Pub Date : 2025-12-15 DOI: 10.1016/j.fuel.2025.138016

Rongjing Wang , Xiaolong Xu , Guangxuan Chen , Yunkun Zhao , Yibo Guo , Shuting Min , Tingting Xu , Xun Wang

This study systematically evaluated the reactivity of four iron-based oxygen carriers (OCs) in a pilot-scale methane reforming coupled with thermochemical water-splitting system for hydrogen and syngas co-production. The oxygen carriers were synthesized with a kilogram-scale mechanical method. Two high-entropy OCs, (Ni_0.2Co_0.2Mg_0.2Cu_0.2Ca_0.2)Fe₂O₄ (HEO1) and (Ni_0.2Co_0.2Mg_0.2Cr_0.2Mn_0.2)Fe₂O₄ (HEO2), showed good cycling stability during a 50-hour test. HEO1 showed a higher oxygen transfer capacity (OTC) of 24.6 % and better carbon-resistance performance. It reached the highest hydrogen yield of 10.40 mmol/g-OC and a hydrogen purity of 98.75 %. HEO2 showed slight carbon deposition during methane reforming in the fuel reactor (FR), which led to a lower hydrogen purity of 93.37 % and a hydrogen yield of 9.52 mmol/g-OC. The composite OC 0.3NiFe₂O₄/0.7SrFe₁₂O₁₉ (Sr-Ni-Fe-O) showed a high hydrogen purity of 98.60 % but a lower hydrogen yield of 6.90 mmol/g-OC. This was attributed to its low lattice oxygen activity, which hindered deep reduction during the FR stage. Ca₂Ni_0.75Fe_1.25O₅ (Ca-Ni-Fe-O) tended to produce carbon deposition in the FR and was more suitable for syngas production. It reached the highest syngas yield of 1.97 L/L_CH4 because of its low lattice oxygen activity and low OTC. Overall, HEO1 showed superior cyclic stability and sintering resistance, providing a strong foundation for the scalable application of high-entropy oxides in thermochemical hydrogen production.

本研究系统地评价了四种铁基氧载体（OCs）在甲烷重整-热化学水裂解联产氢气和合成气中试系统中的反应性。采用公斤级机械法合成氧载体。两种高熵oc (Ni0.2Co0.2Mg0.2Cu0.2Ca0.2)Fe2O4 （HEO1）和（Ni0.2Co0.2Mg0.2Cr0.2Mn0.2）Fe2O4 （HEO2）在50小时的测试中表现出良好的循环稳定性。HEO1具有较高的氧传递容量（OTC）（24.6%）和较好的抗碳性能。产氢率最高，为10.40 mmol/g-OC，氢纯度为98.75%。在燃料反应器（FR）甲烷重整过程中，HEO2表现出轻微的积碳现象，导致氢纯度较低，为93.37%，产氢率为9.52 mmol/g-OC。复合OC 0.3NiFe2O4/0.7SrFe12O19 （Sr-Ni-Fe-O）的氢纯度高达98.60%，但产氢率较低，仅为6.90 mmol/g-OC。这是由于其晶格氧活性低，阻碍了FR阶段的深度还原。Ca2Ni0.75Fe1.25O5 （Ca-Ni-Fe-O）倾向于在FR中产生积碳，更适合合成气生产。由于其晶格氧活性低，OTC低，合成气产率最高，为1.97 L/LCH4。总体而言，HEO1表现出优异的循环稳定性和抗烧结性能，为高熵氧化物在热化学制氢中的大规模应用提供了坚实的基础。

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引用次数: 0

Doping Ru on Ni2P with phosphorus vacancies for overall seawater electrolysis 带磷空位的Ni2P上掺杂Ru用于海水电解

IF 7.5 1区工程技术 Q2 ENERGY & FUELS

Fuel

Pub Date : 2025-12-15 DOI: 10.1016/j.fuel.2025.137985

Xueling Wei , Youjun Huang , Qiguan Wang , Taotao Ai , Xiangyu Zou , Wenhu Li , Sumin Wang , Weiwei Bao , Jie Han

Direct seawater electrolysis represents a promising technology for large-scale green hydrogen production. In this study, a ruthenium-doped nickel phosphide with phosphorus vacancies (Ru/Ni₂P_v/NF) was successfully synthesized through galvanic replacement reaction integrated with plasma-assisted phosphidation and vacancy engineering. The Ru/Ni₂P_v/NF demonstrates exceptional oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) performance in seawater splitting. The electrolyzer coupled with Ru/Ni₂P_v/NF achieves an industrial current density of 1 A cm⁻² at 2.0 V under 1 M KOH mixed seawater. The integration of theoretical calculations and experimental analyses reveals that the synergistic interaction between phosphorus vacancies and Ru effectively modulates the electronic structure of the electrocatalyst, thereby facilitating the formation of active NiOOH species and a protective PO₄^3- anion layer. This study proposes a simple yet effective strategy for the rapid incorporation of dopants and defects to enhance electrocatalytic performance.

海水直接电解是一种很有前途的大规模绿色制氢技术。本研究通过电取代反应结合等离子体辅助磷化和空位工程，成功合成了含磷空位的钌掺杂磷化镍（Ru/Ni2Pv/NF）。Ru/Ni2Pv/NF在海水裂解中表现出优异的析氧反应（OER）和析氢反应（HER）性能。电解槽与Ru/Ni2Pv/NF耦合，在1 M KOH混合海水中，在2.0 V下可获得1 A cm−2的工业电流密度。理论计算和实验分析相结合表明，磷空位和Ru之间的协同作用有效地调节了电催化剂的电子结构，从而促进了活性NiOOH物质和PO43-阴离子保护层的形成。本研究提出了一种简单而有效的快速掺入掺杂剂和缺陷以提高电催化性能的策略。

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引用次数: 0

Valorization of catalytically improved combustion stability for low-concentration methane in a gradient pore-density porous media burner 在梯度孔密度多孔介质燃烧器中催化提高低浓度甲烷燃烧稳定性

IF 7.5 1区工程技术 Q2 ENERGY & FUELS

Fuel

Pub Date : 2025-12-15 DOI: 10.1016/j.fuel.2025.137979

Yunqi Cao , Haonan Rong , Li Yang , Yifan Ding , Fang Liu , Cheng Zhai

Low calorific value and fluctuation of low-concentration methane (LCM) from coal mines pose awkward challenges for stable combustion and utilization. A gradient catalytic porous media (PM) burner by loading Fe₂O₃ on the surface of Al₂O₃ foam ceramics was designed to validate the enhanced combustion stability. The cold startup and combustion characteristics were investigated with different equivalence ratio (φ) and inlet velocity (v), and the heat transfer and reaction mechanisms were revealed based on experimental results. The results indicated that porous media catalytic combustion achieved rapid preheating response (<150 s) in the cold-startup process. The flame variation from surface combustion to submerged combustion reflected the combustion integrity. Fe₂O₃/Al₂O₃ had robust mid-to-high temperature reactivity, achieving greater than 98 % CH₄ conversion and lower than 5 ppm NO_x emissions under all conditions. Flame stabilization occurred optimally at the interface of 20/30 PPI region under φ = 0.40 and v = 11 cm/s, leveraging thermal feedback and flame buffering effects of the gradient porous media structure. Long-term combustion testing verified the system’s stability with high combustion efficiency and low emissions. Mechanistic analysis revealed that oxygen vacancies facilitated efficient activation of CH bonds, FeOAl bonds could inhibit carbon deposition and improved mechanical strength, with the Vickers hardness decreased by less than 50 % compared to fresh catalyst. The synergy between the gradient structure and catalytic reaction improved the combustion stability of LCM, providing a viable solution for the utilization of coal mine methane.

煤矿低浓度甲烷的低热值和波动性给稳定燃烧和利用带来了棘手的挑战。设计了一种梯度催化多孔介质燃烧器，通过在Al2O3泡沫陶瓷表面加载Fe2O3来验证其增强的燃烧稳定性。研究了不同当量比（φ）和进口速度(v)下的冷启动和燃烧特性，并根据实验结果揭示了传热和反应机理。结果表明，多孔介质催化燃烧在冷启动过程中实现了快速的预热响应（<150 s）。火焰从表面燃烧到水下燃烧的变化反映了燃烧的完整性。Fe2O3/Al2O3具有强大的中高温反应活性，在所有条件下均可实现98%以上的CH4转化率和低于5 ppm的NOx排放量。在φ = 0.40和v = 11 cm/s条件下，利用梯度多孔介质结构的热反馈和火焰缓冲效应，在20/30 PPI区域的界面处火焰稳定效果最佳。长期燃烧试验验证了系统的稳定性，燃烧效率高，排放低。机理分析表明，氧空位促进了CH键的有效活化，FeOAl键抑制了碳沉积，提高了机械强度，与新鲜催化剂相比，维氏硬度降低不到50%。梯度结构与催化反应的协同作用提高了LCM的燃烧稳定性，为煤矿瓦斯的利用提供了可行的解决方案。

{"title":"Valorization of catalytically improved combustion stability for low-concentration methane in a gradient pore-density porous media burner","authors":"Yunqi Cao , Haonan Rong , Li Yang , Yifan Ding , Fang Liu , Cheng Zhai","doi":"10.1016/j.fuel.2025.137979","DOIUrl":"10.1016/j.fuel.2025.137979","url":null,"abstract":"<div><div>Low calorific value and fluctuation of low-concentration methane (LCM) from coal mines pose awkward challenges for stable combustion and utilization. A gradient catalytic porous media (PM) burner by loading Fe<sub>2</sub>O<sub>3</sub> on the surface of Al<sub>2</sub>O<sub>3</sub> foam ceramics was designed to validate the enhanced combustion stability. The cold startup and combustion characteristics were investigated with different equivalence ratio (<em>φ</em>) and inlet velocity (<em>v</em>), and the heat transfer and reaction mechanisms were revealed based on experimental results. The results indicated that porous media catalytic combustion achieved rapid preheating response (<150 s) in the cold-startup process. The flame variation from surface combustion to submerged combustion reflected the combustion integrity. Fe<sub>2</sub>O<sub>3</sub>/Al<sub>2</sub>O<sub>3</sub> had robust mid-to-high temperature reactivity, achieving greater than 98 % CH<sub>4</sub> conversion and lower than 5 ppm NO<sub>x</sub> emissions under all conditions. Flame stabilization occurred optimally at the interface of 20/30 PPI region under <em>φ</em> = 0.40 and <em>v</em> = 11 cm/s, leveraging thermal feedback and flame buffering effects of the gradient porous media structure. Long-term combustion testing verified the system’s stability with high combustion efficiency and low emissions. Mechanistic analysis revealed that oxygen vacancies facilitated efficient activation of C<img>H bonds, Fe<img>O<img>Al bonds could inhibit carbon deposition and improved mechanical strength, with the Vickers hardness decreased by less than 50 % compared to fresh catalyst. The synergy between the gradient structure and catalytic reaction improved the combustion stability of LCM, providing a viable solution for the utilization of coal mine methane.</div></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":"411 ","pages":"Article 137979"},"PeriodicalIF":7.5,"publicationDate":"2025-12-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145750038","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

Pilot-scale optimization of a physical–chemical biogas upgrading system based on a high alkalinity absorbent at ambient pressure and temperature 常压常温高碱度吸附剂理化沼气升级系统的中试优化

IF 7.5 1区工程技术 Q2 ENERGY & FUELS

Fuel

Pub Date : 2025-12-15 DOI: 10.1016/j.fuel.2025.138010

Edwin G. Hoyos , Saeed Rasekhi , Rogelio Mazaeda , Raúl Muñoz

The optimization of an innovative process consisting of chemical absorption–desorption at ambient pressure and temperature with EDTA-Fe/carbonate solutions devoted to biogas upgrading was conducted. The influence of parameters such as the initial pH (9–10), inorganic carbon concentration (IC) (4000–8000 mg/L), biogas flowrate (BF) (30–90 L/d), air flowrate (AF) (300–1500 L/d), L/G ratio (0.7–3) and EDTA-Fe concentration (Fe) (0–30 mM) on biomethane composition was evaluated. In addition, the effect of carbon-coated iron nanoparticles on CO₂ absorption performance was investigated. The L/G ratio governed the O₂ concentration in the biomethane. Interestingly, the addition of EDTA-Fe was not necessary for the complete removal of H₂S from the biogas. BF, AF and IC exerted a significant influence on the biomethane CO₂ concentration (BF > AF > IC), while the initial pH induced no effect. On the other hand, the supplementation of iron nanoparticles did not significantly influence on the CO₂ absorption performance. The optimal conditions in a 7 L absorption-7 L desorption system were: BF = 90 L/d, AF = 1500 L/d, L/G = 0.7, IC = 8000 mg C/L, initial pH = 9.5 and Fe = 0 mM. Under these operational conditions, the biomethane obtained was free of H₂S and average concentrations of CO₂, O₂, N₂ and CH₄ of 1.7 ± 0.1 %, 0.7 ± 0.1 %, 2.7 ± 0.5 % and 94.9 ± 0.6 %, respectively, were recorded for 3 weeks of continuous operation. This biomethane complied with the European standard EN 16273 on the biomethane use for injection into natural gas networks.

以EDTA-Fe/碳酸盐溶液为原料，对常压常温化学吸附-解吸工艺进行了优化。考察了初始pH（9 ~ 10）、无机碳浓度（IC）（4000 ~ 8000 mg/L）、沼气流量（BF）（30 ~ 90 L/d）、空气流量（AF）（300 ~ 1500 L/d）、L/G比（0.7 ~ 3）、EDTA-Fe浓度（Fe）（0 ~ 30 mM）等参数对生物甲烷组成的影响。此外，还研究了碳包覆铁纳米颗粒对CO2吸收性能的影响。L/G比值决定了生物甲烷中O2的浓度。有趣的是，EDTA-Fe的加入并不是完全去除沼气中H2S的必要条件。BF、AF和IC对生物甲烷CO2浓度（BF > AF >； IC）有显著影响，而初始pH对生物甲烷CO2浓度没有影响。另一方面，铁纳米颗粒的添加对CO2吸收性能没有显著影响。最优条件7 L absorption-7 L解吸系统:男朋友= 90 L / d,房颤= 1500 L / d, L / G = 0.7, IC C / L = 8000毫克,初始pH = 9.5和铁= 0毫米。在这些操作条件下,获得免费硫化氢和甲烷,平均浓度的二氧化碳,氧气,氮气和CH4 1.7±0.1%,0.7±0.1%,2.7±0.5%和94.9±0.6%,分别记录3周的连续操作。这种生物甲烷符合欧洲标准EN 16273关于生物甲烷用于注入天然气网络。

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引用次数: 0

Near-Zero NH3/N2O emissions enabled in two-stroke ammonia-diesel dual-direct-injection engines: an experimental study via synergistic diesel multiple injection strategy 二冲程氨柴油双直喷发动机实现近零NH3/N2O排放：一项基于柴油多重协同喷射策略的实验研究

IF 7.5 1区工程技术 Q2 ENERGY & FUELS

Fuel

Pub Date : 2025-12-15 DOI: 10.1016/j.fuel.2025.137926

Weize Chen , Jingchen Cui , Zhenxian Zhang , Qingyang Wang , Pengbo Dong , Xiangyu Meng , Jiangping Tian , Hua Tian , Wuqiang Long , Shiying Liu

Ammonia stands as a pivotal carbon-free energy vector with the potential to decarbonize hard-to-abate sectors like heavy industry and maritime transport. However, its widespread adoption in internal combustion engines is critically challenged by the dual emissions of unburned NH₃, a toxic gas, and N₂O, a potent greenhouse gas. This study demonstrates a novel diesel multiple injection strategy (first injection and second injection), based on the Jet Controlled Compression Ignition (JCCI) concept, to achieve near-zero emissions in a two-stroke ammonia-diesel engine. The results elucidate that the first injection creates a high-temperature reaction zone and elevates the in-cylinder thermal state, which is essential for robustly igniting the subsequent liquid ammonia spray. The timing and mass of this first injection, coupled with an optimised injection interval, are critical for stabilizing the flame and forming a pervasive high-temperature environment. This environment is key to minimizing incomplete combustion products. Compared to a conventional single-injection strategy, the optimised multi-injection approach enhanced the dominance of diffusion combustion, leading to a marginal improvement in indicated thermal efficiency while achieving drastic emission reductions: unburned NH₃ and N₂O were reduced by 90 % (to 62 ppm) and 83 % (to 7 ppm), respectively. This work provides a practical and effective combustion management strategy, transforming a fundamental combustion concept (JCCI) into a viable solution for enabling clean ammonia combustion. It thus presents a significant step towards the application of ammonia as a sustainable fuel for high-power energy systems and contributes directly to the goals of the green energy transition.

氨是一种关键的无碳能源，有可能使重工业和海运等难以减排的行业脱碳。然而，它在内燃机中的广泛应用受到了未燃烧的NH3（一种有毒气体）和N2O（一种强效温室气体）双重排放的严峻挑战。该研究展示了一种基于喷气控制压缩点火（JCCI）概念的新型柴油多重喷射策略（一次喷射和二次喷射），可在二冲程氨柴油发动机上实现近零排放。结果表明，第一次喷射产生了一个高温反应区，提高了缸内热状态，这对于随后的液氨喷雾的稳定点燃至关重要。第一次喷射的时机和质量，再加上优化的喷射间隔，对于稳定火焰和形成普遍的高温环境至关重要。这种环境是减少不完全燃烧产物的关键。与传统的单次喷射策略相比，优化后的多次喷射方法增强了扩散燃烧的优势，在显著减少排放的同时，还能略微提高热效率：未燃烧的NH3和N2O分别减少了90%（至62 ppm）和83%（至7 ppm）。这项工作提供了一种实用有效的燃烧管理策略，将基本燃烧概念（JCCI）转化为实现清洁氨燃烧的可行解决方案。因此，它向将氨作为大功率能源系统的可持续燃料的应用迈出了重要的一步，并直接有助于实现绿色能源转型的目标。

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引用次数: 0

Metal-modified Na-X zeolite/carbon composites derived from coal gasification fine slag for enhanced catalytic pyrolysis of biomass 煤气化细渣金属改性Na-X沸石/碳复合材料增强生物质催化热解性能

IF 7.5 1区工程技术 Q2 ENERGY & FUELS

Fuel

Pub Date : 2025-12-15 DOI: 10.1016/j.fuel.2025.138044

Xiaodong You , Zhenjie Sun , Chen Yang , Songtao Wu , Zhenming Li , Jialong Chen , Mingjie Xiong , Guanshuai Zhang , Yuan Liu , Yunpu Wang , Chunlei Gao , Feiqiang Guo

To address the dual challenges of coal gasification fine slag (CGFS) disposal and the demand for efficient catalysts for bio-oil upgrading, this study aimed to synthesize metal-modified Na-X zeolite/carbon composites from CGFS and evaluate their performance in biomass catalytic pyrolysis. The composites were prepared via acid leaching, alkali fusion, and hydrothermal crystallization, followed by impregnation with different metals (Ni, Co, Fe, Ca). Characterization revealed that metal modification dramatically reconstructed the acid properties, eliminating weak/medium sites while generating abundant strong Lewis acid sites, with the total strong acid amount increasing from 0.289 mmol/g (parent support) to 0.563 mmol/g (GZ-Co). In the catalytic fast pyrolysis of pine wood at 600 °C, metal modification significantly enhanced deoxygenation. Notably, the optimal GZ-Ni catalyst increased the gas yield from 37.23 wt% (non-catalytic) to 53.16 wt%, while the relative hydrocarbon content in bio-oil rose substantially from 15 % to 38 %. The strong Lewis acidity introduced by the metals was identified as the key factor promoting decarbonylation, decarboxylation, and aromatization reactions. Although reversible deactivation occurred due to coking, regeneration effectively restored catalytic activity. This work provides not only a sustainable “waste-to-catalyst” strategy for CGFS valorization but also elucidates the critical role of tailored strong Lewis acidity in designing efficient catalysts for bio-oil upgrading.

为了解决煤气化细渣处理和生物油升级对高效催化剂需求的双重挑战，本研究以细渣为原料合成了金属改性Na-X沸石/碳复合材料，并对其在生物质催化热解中的性能进行了评价。复合材料经酸浸、碱熔、水热结晶、不同金属（Ni、Co、Fe、Ca）浸渍制备。表征结果表明，金属改性显著地重建了酸性质，消除了弱/中位，产生了丰富的强Lewis酸位点，总强酸量从0.289 mmol/g（亲本支持）增加到0.563 mmol/g （gc - co）。在600℃下松木催化快速热解中，金属改性显著增强了脱氧。值得注意的是，最佳的GZ-Ni催化剂将气产率从37.23 wt%（非催化）提高到53.16 wt%，而生物油中的相对烃含量从15%大幅提高到38%。金属引入的强刘易斯酸是促进脱碳、脱羧和芳构化反应的关键因素。虽然由于焦化发生了可逆失活，但再生有效地恢复了催化活性。这项工作不仅为CGFS的增值提供了可持续的“废物转化为催化剂”策略，而且阐明了定制强刘易斯酸度在设计高效生物油升级催化剂中的关键作用。

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引用次数: 0

Artificial photosynthetic interfaces for enhanced photocatalytic hydrogen generation 用于增强光催化制氢的人工光合界面

IF 7.5 1区工程技术 Q2 ENERGY & FUELS

Fuel

Pub Date : 2025-12-15 DOI: 10.1016/j.fuel.2025.138009

Suleyman I. Allakhverdiev

The growing demand for low-carbon energy carriers has renewed interest in photocatalytic hydrogen production as a viable solar-to-fuel route. Natural photosynthesis offers an elegant blueprint for coupling light harvesting, charge separation and catalysis, but its direct exploitation for hydrogen evolution is limited by low efficiency and restricted control over the underlying interfaces. Semi-artificial and artificial photosynthetic platforms address these limitations by combining biological or bio-inspired catalysts with engineered inorganic light harvesters and support architectures. This review focuses on artificial photosynthetic interfaces for photocatalytic hydrogen production, using semi-artificial systems as a conceptual and experimental bridge. We first outline the continuum from natural to semi-artificial and fully artificial photosynthesis, highlighting how the degree and nature of interface control evolve across these platforms. We then analyse semi-artificial architectures to extract design principles for soft bio–inorganic interfaces that wire inorganic photocatalysts to microbial cells, sub-cellular compartments and isolated enzymes. Building on these insights, we discuss artificial photosynthetic systems in terms of their key interfacial motifs, including semiconductor–semiconductor and semiconductor–metal junctions, cocatalyst-semiconductor contacts and solid–liquid boundaries that govern charge separation, redox selectivity and mass transport. Finally, we identify cross-cutting challenges related to reproducibility, operational durability, scalability and the use of earth-abundant components. By framing recent progress through the lens of interface engineering, this review provides a unified basis for the rational design of next-generation hydrogen-producing photosystems.

对低碳能源载体的需求不断增长，重新激发了人们对光催化制氢作为一种可行的太阳能制氢途径的兴趣。自然光合作用为耦合光收集、电荷分离和催化提供了一个优雅的蓝图，但其对氢的直接开发受到低效率和对底层界面控制的限制。通过将生物或仿生催化剂与工程无机光收集器和支持架构相结合，半人工和人工光合平台解决了这些限制。本文综述了用于光催化制氢的人工光合界面，以半人工系统为概念和实验桥梁。我们首先概述了从自然到半人工和完全人工光合作用的连续体，强调了界面控制的程度和性质如何在这些平台上演变。然后，我们分析了半人工结构，以提取软生物无机界面的设计原则，这些界面将无机光催化剂连接到微生物细胞、亚细胞区室和分离酶。在这些见解的基础上，我们讨论了人工光合系统的关键界面基序，包括半导体-半导体和半导体-金属结，共催化剂-半导体接触和控制电荷分离，氧化还原选择性和质量传输的固液边界。最后，我们确定了与可重复性、操作耐久性、可扩展性和地球丰富组件的使用相关的跨领域挑战。本文从界面工程的角度综述了近年来的研究进展，为下一代产氢光系统的合理设计提供了统一的依据。

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引用次数: 0

Performance prediction and multi-objective optimization of a CH4-fueled SOFC power/cooling system using ANN–GA: thermodynamic, economic, and environmental evaluation 基于ANN-GA的ch4燃料SOFC电源/冷却系统性能预测和多目标优化：热力学、经济和环境评价

IF 7.5 1区工程技术 Q2 ENERGY & FUELS

Fuel

Pub Date : 2025-12-15 DOI: 10.1016/j.fuel.2025.137971

Amir Abdolhosseinnejad , Sajad Rezazadeh , H. Rostamnejad Takleh , Milad Razbin

While solid oxide fuel cells (SOFCs) offer strong performance, the selection of appropriate subsystems for waste-heat recovery and the reliable prediction of overall system behavior remain insufficiently addressed in the literature. Therefore, a novel CH₄-fueled, SOFC-based hybrid power and cooling system, integrating an organic flash cycle and an ejector refrigeration unit to simultaneously generate electricity and dual-level cooling, is proposed. The configuration harnesses high-grade exhaust energy from the SOFC without relying on mechanical compressors, thereby improving energy recovery and operational efficiency. A comprehensive framework combining thermodynamic, economic, and environmental analyses is applied to evaluate system performance. Artificial neural networks trained on response surface methodology data are employed to predict system outputs, while genetic algorithms are used to optimize key design parameters under multi-objective scenarios. The main objectives are to maximize thermal efficiency, minimize levelized cost of system (

L C O S

), and reduce emitted rate of CO₂. Numerical results show that thermal efficiency improves to 83.1 % and exergy efficiency reaches 44.9 %. The

L C O S

decreases by more than 15 %, while emitted rate of CO₂ is reduced by 11.4 %. Exergy analysis reveals that the SOFC and thermoelectric generator are the dominant sources of irreversibility. From an economic perspective, optimization enhances net present value by 39.5 % and shortens the payback period from 7.48 to 6.39 years.

虽然固体氧化物燃料电池（sofc）提供了强大的性能，但在文献中仍然没有充分解决为废热回收选择适当的子系统和对整个系统行为的可靠预测。因此，提出了一种新型的以甲烷为燃料，基于sofc的混合动力和冷却系统，该系统集成了有机闪蒸循环和喷射器制冷装置，可以同时发电和双级冷却。该配置利用SOFC的高级废气能量，而不依赖于机械压缩机，从而提高了能量回收和运行效率。一个综合的框架结合热力学，经济和环境分析应用于评估系统的性能。采用响应面方法训练的人工神经网络预测系统输出，采用遗传算法优化多目标场景下的关键设计参数。主要目标是最大限度地提高热效率，最小化系统的平准化成本（LCOS），并减少二氧化碳的排放率。数值计算结果表明，热效率提高到83.1%，火用效率达到44.9%。LCOS降低了15%以上，CO2排放量降低了11.4%。火用分析表明，SOFC和热电发电机是不可逆性的主要来源。从经济角度来看，优化后的净现值提高了39.5%，投资回收期从7.48年缩短到6.39年。

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