FuelPub Date : 2025-03-10DOI: 10.1016/j.fuel.2025.134999
Jian Li , Heping Yang , Mengfei Wang , Xiaowei Bai , Zhenghua Dai , Yunpeng Zhao , Jianzhong Yin
{"title":"Revealing the role of CuMgAlOx catalyst components in cellulose depolymerization and alcohol formation","authors":"Jian Li , Heping Yang , Mengfei Wang , Xiaowei Bai , Zhenghua Dai , Yunpeng Zhao , Jianzhong Yin","doi":"10.1016/j.fuel.2025.134999","DOIUrl":"10.1016/j.fuel.2025.134999","url":null,"abstract":"<div><div>Low-carbon alcohols are clean and renewable energy sources with applications in fuel and chemical industries. This study investigates CuMgAlOx catalysts for cellulose methanolysis under hydrogen-free conditions, focusing on their catalytic mechanisms and kinetic behavior. Catalyst characterization revealed synergistic roles of Cu, Mg, and Al in enhancing acidity, surface area, and dispersion. Cu is essential for methanol reforming and hydrogenolysis, while Mg optimizes the nanostructure by reducing Cu crystallite size from 10.1 nm (CuO) to 8.0 nm and increasing medium-strength acidity (314.9 μmol/g). Al uniquely facilitates acid-base duality, significantly enhancing methoxy ether alcohol (MOA) selectivity to 31.1 % through etherification (k<sub>9</sub> = 6.0 h<sup>−1</sup>). The Structure-Oriented Lumping (SOL) kinetic model, with strong predictive accuracy (R<sup>2</sup> > 0.996), illustrates that CuMgAlOx accelerates cellulose depolymerization and hydrodeoxygenation, yielding unprecedented alcohol selectivity (94.3 %) and yield (58.0C%) under hydrogen-free conditions. The study establishes a comprehensive framework for the design of multi-metal catalysts in biomass valorization and advances sustainable alcohol production technologies.</div></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":"393 ","pages":"Article 134999"},"PeriodicalIF":6.7,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143592238","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}
FuelPub Date : 2025-03-09DOI: 10.1016/j.fuel.2025.134993
Yadong Xiao , Guangzhu Feng , Ghazala Mustafa , Murtaza Hasan
{"title":"Improved electrocatalytic performance of TiS2 by nanohybrid with MoC nanosheets towards overall water-splitting for green hydrogen","authors":"Yadong Xiao , Guangzhu Feng , Ghazala Mustafa , Murtaza Hasan","doi":"10.1016/j.fuel.2025.134993","DOIUrl":"10.1016/j.fuel.2025.134993","url":null,"abstract":"<div><div>The depletion of conventional resources has enhanced researchers’ interest in searching for renewable energy sources. Due to the zero-emission of by-products, there is a strong demand for H<sub>2</sub> production by typical water electrolysis. In this study, we demonstrated that a composite strategy of dual transition metal functional (MoC-TiS<sub>2</sub>) was prepared for the first time as a bifunctional electrocatalyst via a hydrothermal route and used in three and two electrolyser setups. Using analytical tools like XRD, SEM/EDX, and XPS, phase purity, morphology, and valances of synthesized electrocatalysts are characterized. Combined with pure MoC and TiS<sub>2</sub> samples, microspheres with numerous sheets-like MoC-TiS<sub>2</sub> exhibited superior overall water splitting performance at OER overpotential of 130 mV and HER overpotential of 84 mV, along with small Tafel slopes (82 mVdec<sup>-1</sup>@OER & 45 mVdec<sup>-1</sup>@HER). The EIS study suggests that the small resistive values of MoC-TiS<sub>2</sub> endow high conductivity with improved electrochemical performance. The interaction induces a charge shift from Ti<sup>3+</sup>/Ti<sup>4+</sup> to Mo<sup>2+</sup>/Mo<sup>6+</sup> across cationic-anionic bonds regulated by the number of hetero-interfaces between MoC and TiS<sub>2</sub> and oxygen vacancies. Serving as a robust bifunctional electrode in a two-electrode configuration for an alkaline water electrolyzer, the MoC-TiS<sub>2</sub> attained benchmark current density by a cell voltage of 1.44 V and maintains its stable performance for at least 185 h. The present study presents a novel bifunctional efficient/durable electrocatalysts for practical water electrolysis application.</div></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":"393 ","pages":"Article 134993"},"PeriodicalIF":6.7,"publicationDate":"2025-03-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576407","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}
FuelPub Date : 2025-03-09DOI: 10.1016/j.fuel.2025.134996
Masoud Safari Yazd, Ali Haghtalab, Farzaneh Arabpour Roghabadi
{"title":"Screening the footprints of water in the Fischer Tropsch synthesis over a Ru promoted Co-based catalyst supported by ceria, “a mechanistic insight”","authors":"Masoud Safari Yazd, Ali Haghtalab, Farzaneh Arabpour Roghabadi","doi":"10.1016/j.fuel.2025.134996","DOIUrl":"10.1016/j.fuel.2025.134996","url":null,"abstract":"<div><div>The pursuit of greener alternatives to combat air pollution has intensified, with Fischer-Tropsch synthesis (FTS) considered a promising solution for converting syngas into clean fuels. However, the presence of water, a by-product of FTS, poses challenges to catalyst performance. This study investigates the impact of water on a Co-based catalyst through a combination of molecular dynamics simulations, FTS performance tests, and experimental characterizations. Experimental data reveal that water vapor significantly enhances CO conversion and reduces methane selectivity, particularly at low pressures. The findings suggest that water, while inhibiting the mass transfer of FTS reactants and products, plays a crucial role in enhancing the adsorption and desorption of key molecules on the catalyst surface. The study proposes a mechanistic approach to elucidate the role of water in FTS, highlighting its influence on intermediate reactions and the water–gas shift reaction (WGSR). Specifically, it investigates the interaction between CO and water, highlighting how water facilitates CO dissociation and enhances CO reactivity. MD simulations are employed to calculate the minimum energy pathway (MEP) for all elementary subsequent steps over the catalyst, shedding light on the energetically favorable pathways in the presence of water. The study identifies distinct reaction routes facilitated by water, including WGSR pathways and H<sub>2</sub>O-assisted CO dissociation pathways, each contributing to the overall FTS mechanism. Through computational analysis, the study reveals that water plays a crucial role in promoting CO dissociation and chain growth, ultimately impacting the selectivity and productivity of the FTS process. Eventually, a comprehensive kinetic model incorporating water effects accurately predicts experimental results, confirming the significant role of water in altering reaction pathways and selectivity.</div></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":"393 ","pages":"Article 134996"},"PeriodicalIF":6.7,"publicationDate":"2025-03-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576789","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}
FuelPub Date : 2025-03-09DOI: 10.1016/j.fuel.2025.134923
Yan-Hong Chen , Qiang Zhang , Dong-Min Han , Xiao-bo Chen , Chao-He Yang
{"title":"Facile synthesis of mesoporous MFI crystals with multilamellar morphology and its application in catalytic cracking of 1-hexene","authors":"Yan-Hong Chen , Qiang Zhang , Dong-Min Han , Xiao-bo Chen , Chao-He Yang","doi":"10.1016/j.fuel.2025.134923","DOIUrl":"10.1016/j.fuel.2025.134923","url":null,"abstract":"<div><div>Turning crystal morphology and size of zeolite materials is crucial for promoting their diffusion and catalytic properties. Herein, MFI hierarchical lamellar zeolites with tunable SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> ratios were synthesized under hydrothermal conditions through the self-assembly of commercially available simple surfactant and inorganic zeolite precursor. Through detailed investigation of the crystallization process using various characterization techniques, a reliable formation mechanism of hierarchical lamellar ZSM-5 zeolite was proposed. Cetyltrimethylammonium bromide (CTAB) acted both as a structure-directing agent and a mesoporogen, responsible for creating such structure. Hierarchical lamellar ZSM-5 can be successfully obtained by regulating the SiO<sub>2</sub>/Al<sub>2</sub>O<sub>3</sub> ratios and crystallization temperature. In the 1-hexene cracking process, the hierarchical lamellar ZSM-5 zeolite exhibited significantly enhanced propylene selectivity and stability compared to conventional microporous ZSM-5. The enhanced textural and diffusion properties can effectively suppress the hydrogen transfer reaction, which plays a crucial role in determining the selectivity of C<sub>3</sub>-C<sub>5</sub> olefins. These findings provide a facile and rational synthesis route to reduce diffusion resistance and enhance the catalytic performance of zeolite.</div></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":"393 ","pages":"Article 134923"},"PeriodicalIF":6.7,"publicationDate":"2025-03-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576735","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}
FuelPub Date : 2025-03-09DOI: 10.1016/j.fuel.2025.134983
Nafiseh Elmi Fard , Alireza Sarkar , Nader Hasanzadeh
{"title":"Potential detrimental effects of bacterial activity on bitumen","authors":"Nafiseh Elmi Fard , Alireza Sarkar , Nader Hasanzadeh","doi":"10.1016/j.fuel.2025.134983","DOIUrl":"10.1016/j.fuel.2025.134983","url":null,"abstract":"<div><div>This study was conducted to validate the hypothesis that one of the detrimental influences on bituminous pavements is the negative impact of specific bacterial species. To achieve this objective, the bacteria present within bituminous mixtures were isolated, followed by an examination of their phenotypic attributes and their capacity to degrade bitumen. Among 24 bacterial isolates, five predominant isolates exhibiting characteristic phenotypic features and significant destructive potential were identified through polymerase chain reaction (PCR) and named <em>Stutzerimonas</em> sp., <em>Brevundimonas aurantiaca, Bacillus</em> sp., <em>Stutzerimonas stutzeri</em>, and <em>Pseudomonas aeruginosa</em>. The destructive impacts of these target bacteria on the properties of bitumen were assessed employing various methodologies including scanning electron microscopy (SEM), fourier transform infrared spectroscopy (FTIR), contact angle (CA), gel permeation chromatography (GPC), and differential scanning calorimetry (DSC). The results showed that the bacteria caused aging and reduced adhesion by changing the surface texture, increasing C=O and S=O functional groups, and decreasing hydrophobicity. They also cause a change in the molecular structure of bitumen, a decrease in molecular weight dispersion, and an increase in heat capacity, which indicate the negative effects of bitumen aging. In fact, bacteria in bituminous environments can cause bacterial aging of bitumen and cause various damages in the environment in the end.</div></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":"393 ","pages":"Article 134983"},"PeriodicalIF":6.7,"publicationDate":"2025-03-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577391","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}
{"title":"Material characterization and engineering performance evaluation of phosphogypsum as a high-performance filler for bituminous pavements","authors":"Xiong Xu , Guohao Xu , Xiaomei Huang , GM Badiul Alam , Xuyong Chen , Anand Sreeram","doi":"10.1016/j.fuel.2025.134977","DOIUrl":"10.1016/j.fuel.2025.134977","url":null,"abstract":"<div><div>The effective recycling of waste materials as alternatives to traditional mineral fillers in asphalt mixtures has both economic and environmental benefits. Phosphogypsum (PG), as one of the industrial solid wastes is a promising alternative to be used in asphalt mixture. However, in terms of the physical nature of PG, its high-absorption and moisture-expansion cause significant deterioration in engineering properties, particularly moisture-induced damage. To address these concerns, this study considered adopting polymeric diphenylmethane diisocyanate (PMDI) to activate asphalt binder with the introduction of active isocyanate (–NCO) groups, to chemically capture and stabilize the treated PG (TPG) fillers in the mixture. Based on this, the moisture-induced properties and other engineering performances of TPG-containing asphalt mixture (PGAM) with various PMDI contents were evaluated through a series of mechanical tests, and the chemical interaction mechanism between PG and PMDI in asphalt mixture was further simulated and analysed by X-ray diffraction (XRD), infrared spectroscopy (FTIR), thermogravimetry–differential thermogravimetry (TG-DTG), X-ray photoelectron spectroscopy (XPS), and scanning electron microscopy (SEM) tests. The results indicated that PMDI can effectively improve the moisture-induced performance of PGAM, in addition to enhancing the high- and low-temperature stability and reducing rutting and cracking risks. The thermal and microstructural analyses confirmed PMDI in asphalt binder helps consume water released from TPG fillers through promoting the formation of surface coatings, while also enhancing chemical bonding with –OH groups on mineral aggregates. Overall, the recycling approach developed in this study provides an effective solution for improving the engineering performance of PG in asphalt pavement applications.</div></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":"393 ","pages":"Article 134977"},"PeriodicalIF":6.7,"publicationDate":"2025-03-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576787","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
FuelPub Date : 2025-03-09DOI: 10.1016/j.fuel.2025.134995
Meihua Fu , Huaiyuan Tang , Jida Wang , Defa Hou , Fulin Yang , Yi Lu , Can Liu , Xu Lin , Zhifeng Zheng , Yunwu Zheng
{"title":"Unraveling the catalytic pyrolysis of oleic acid to produce biodiesel-range hydrocarbon fuel with Ni-loaded Ce-Zr mesoporous catalysts by tuning the crystal face structure","authors":"Meihua Fu , Huaiyuan Tang , Jida Wang , Defa Hou , Fulin Yang , Yi Lu , Can Liu , Xu Lin , Zhifeng Zheng , Yunwu Zheng","doi":"10.1016/j.fuel.2025.134995","DOIUrl":"10.1016/j.fuel.2025.134995","url":null,"abstract":"<div><div>This study investigated the catalytic upgrading of oleic acid in the presence of Ni-Ce-Zr catalysts to evaluate its potential for the synthesis of hydrocarbon fuels. For this purpose, a series of Ce-Zr and Ni-Ce-Zr catalysts were synthesized via different methods (mechanical mixing (Mix), ball milling (BM), incipient impregnation (ImP), and coprecipitation (CoP)) and systematically characterized via various techniques to elucidate their structure–property relationships. Then, the effects of the synthesis methods on the product yield, hydrocarbon distribution, possible reaction pathways and catalytic deactivation mechanism were carefully determined. Detailed characterization and control experiments revealed that the catalytic activities of various Ni-Ce-Zr catalysts were in the following order: ImP-Ni > CoP-Ni > Mix-Ni > BM-Ni. ImP-Ni exhibited superior catalytic deoxygenation capacity and obtained a 100 % conversion rate, 86.22 % HCs yield with 82.43 % green diesel selectivity due to good dispersion of Ni and Ce species, abundant metal-to-acid sites, abundant oxygen vacancies and defects, high concentrations of Ni<sup>0</sup> and the interaction of Ni<sup>0</sup>/Ni<sup>2+</sup> and Ce<sup>3+</sup>/Ce<sup>4+</sup> redox pairs. Additionally, the samples exhibited outstanding reusability and coke resistance after the fourth cycle (HCs remained above 90 %, mass loss of 1.73 %). Ni addition notably enhanced hydrodeoxygenation activity toward diesel-range fuels compared with support catalysts with higher decarbonylation/decarboxylation selectivity. Furthermore, Ni was the main hydrodeoxygenation reactive site because it created more Lewis acid sites and provided active hydrogen atoms via the dissociation of H<sub>2</sub>. Ce functions as a decarbonylation/decarboxylation reactive site with abundant oxygen vacancies to adsorb and activate <img>COO*. This approach provides a straightforward and effective method for designing catalysts that are structurally tailored to the production of green diesel-range fuels via the waste-to-resource strategy.</div></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":"393 ","pages":"Article 134995"},"PeriodicalIF":6.7,"publicationDate":"2025-03-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577437","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}
FuelPub Date : 2025-03-09DOI: 10.1016/j.fuel.2025.134903
Singaram Somasundaram, Tara Congo, Karen M. Steel
{"title":"Biocoke: Carrying capacity of coking coals for sugarcane bagasse char in terms of viscoelastic behaviour during co-carbonization","authors":"Singaram Somasundaram, Tara Congo, Karen M. Steel","doi":"10.1016/j.fuel.2025.134903","DOIUrl":"10.1016/j.fuel.2025.134903","url":null,"abstract":"<div><div>Sugarcane bagasse was pyrolyzed to various temperatures and blended with three coking coals comprising two medium volatile bituminous (MVC 1 and MVC 2) and one high volatile bituminous (HVC 1) to assess carrying capacities and mechanisms behind fluidity loss during co-carbonization.</div><div>MVC 2 showed no fluidity loss when blended with 10 wt% char pyrolyzed to 600 °C and 800 °C. However, with higher char additions (20 and 25 wt%), fluidity loss progressively worsened due to reduced amount of coal-derived liquid filling voids, causing volatiles to exhaust the system more easily. Complete fluidity loss occurred at 30 wt% char addition. Conversely, for MVC 1, despite having similar properties to MVC 2 in terms of rank and volatile matter, a 10 wt% 800 °C char addition caused fluidity loss. MVC 2 swells to a greater extent than MVC 1 and it is hypothesized that char addition disrupts the bubble growth phase, promotes bubble coalescence, and exacerbates volatile release. Further, it is hypothesized that higher swelling coals, such as MVC 2, can better incorporate char, negating its effects on bubble growth and thereby retaining liquid.</div><div>For HVC 1, the addition of 5 wt% 800 °C char caused substantial fluidity loss which is attributed to the limited swelling behaviour of the coal alone, with bubble coalescence dominating over bubble growth early in the softening phase. The premature loss of volatiles caused by the addition of the char inhibits fluidity development and renders the blend unable to carry biochar. These results suggest that a coking blend’s carrying capacity for char may depend on its swelling behaviour, with greater swelling being advantageous.</div></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":"393 ","pages":"Article 134903"},"PeriodicalIF":6.7,"publicationDate":"2025-03-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577440","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
FuelPub Date : 2025-03-09DOI: 10.1016/j.fuel.2025.134925
Zhongrui Gai , Peng Li , Yuanhui Shen , Ruqi Zhang , Zihan Wan , Mingkai Liu , Sanli Tang , Ying Pan , Hongguang Jin
{"title":"Systematic evaluation of a high-performance solar-driven hybrid system for cost-effective methanol and hydrogen co-production via chemical looping methane reforming","authors":"Zhongrui Gai , Peng Li , Yuanhui Shen , Ruqi Zhang , Zihan Wan , Mingkai Liu , Sanli Tang , Ying Pan , Hongguang Jin","doi":"10.1016/j.fuel.2025.134925","DOIUrl":"10.1016/j.fuel.2025.134925","url":null,"abstract":"<div><div>During the transition from traditional commercial methanol synthesis to zero-carbon solar methanol production, an optimal strategy that bridges industry practices with future prospects is required to ensure both efficient and low-carbon methanol production. In this study, a solar-driven chemical looping reforming-based hybrid system is proposed for coproduction of methanol and hydrogen, an experimentally validated mid-temperature chemical looping reforming process is introduced to produce optimal syngas and high-purity hydrogen. The thermodynamic, economic and environmental evaluations are carried out, and mechanisms for improved performance are uncovered. The results show that the hybrid system showcases overall energy and exergy efficiencies of 64.6 % and 71.3 %, respectively, with over 5 % rise in efficiencies and a 300 °C reforming temperature drop compared to steam methane reforming-based system. Exergy destructions are reduced by 34.3 % in fuel conversion and 47.1 % in heat exchange. The levelized cost of methanol is cut by 23.8 % and lowered to 300 $ t<sup>−1</sup>, with over 60 % of the cost offset by value-added H<sub>2</sub> byproduct. CO<sub>2</sub> emission is reduced by 65 % at a lower carbon cost through effective vent gas utilization. This research is expected to offer an eco-friendly, efficient, and economical solution for utilizing solar energy in large-scale methanol production.</div></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":"393 ","pages":"Article 134925"},"PeriodicalIF":6.7,"publicationDate":"2025-03-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143577431","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}
FuelPub Date : 2025-03-09DOI: 10.1016/j.fuel.2025.135002
Huaming Wang , Zan Huang , Xiao Chen, Jiuqiang Ma, Ya Wang, Changhai Liang
{"title":"A synergistic catalyst system comprising PtPdCoNiCu/C High-Entropy alloy and H4SiW12O40 for Low-Temperature hydrogenolysis of C–O bonds in Coal-Derived compounds","authors":"Huaming Wang , Zan Huang , Xiao Chen, Jiuqiang Ma, Ya Wang, Changhai Liang","doi":"10.1016/j.fuel.2025.135002","DOIUrl":"10.1016/j.fuel.2025.135002","url":null,"abstract":"<div><div>The development of directed hydrogenolysis of coal under mild conditions to yield aromatic compounds signifies a pioneering approach for the non-energy utilization of coal, effectively augmenting the added value of coal-derived products. In this work, a synergistic catalyst system composed of PtPdCoNiCu/C high-entropy alloy (HEA) and H<sub>4</sub>SiW<sub>12</sub>O<sub>40</sub> has been formulated for the catalytic hydrogenolysis of C–O bonds in coal-derived compounds and low-rank coal. Due to the high-entropy effect, the PtPdCoNiCu/C catalyst exhibits markedly enhanced catalytic activity in comparison to its monometallic counterparts. The conversion of benzyl phenyl ether achieves an impressive 99.8 %, with yields of toluene (99.8 %) and phenol (99.2 %) at 50 °C and 0.1 MPa H<sub>2</sub> for 2 h. The apparent activation energy (Ea) for this synergistic catalyst system is merely 31.6 kJ/mol, significantly lower than that of the PtPdCoNiCu/C catalyst alone (86.4 kJ/mol), suggesting that hydrogen spillover facilitates the surface hydrogenolysis of C–O bonds. Furthermore, for the hydrogenolysis of benzyl ether and phenoxy ethylbenzene, the synergistic catalyst system demonstrates remarkable efficiency, with Ea values of 58.6 kJ/mol and 100.0 kJ/mol, respectively. The products formed are aromatic compounds, devoid of any over-hydrogenated derivatives. Notably, the cleavage barrier of the aryl C–O bonds is profoundly influenced by the energy associated with the C–O bonds. Additionally, the synergistic catalyst system comprising PtPdCoNiCu/C and H<sub>4</sub>SiW<sub>12</sub>O<sub>40</sub> represents a promising catalyst for the hydrogenolysis of Naomaohu coal under mild conditions. This study will establish a foundation for the directed pyrolysis of coal under mild conditions to generate high-end fine chemicals, providing a novel pathway for the clean, low-carbon, and high-value utilization of coal resources.</div></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":"393 ","pages":"Article 135002"},"PeriodicalIF":6.7,"publicationDate":"2025-03-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576874","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}