Catalysis TodayPub Date : 2025-07-01DOI: 10.1016/j.cattod.2025.115443
Irene Barba-Nieto , Marcos Fernández-García , Jorge Moncada , Guilherme Felipe Lenz , Juan D. Jimenez , Sooyeon Hwang , Akhil Tayal , Sanjaya D. Senanayake , Anna Kubacka , José A. Rodriguez
{"title":"Activity and selectivity for CO2 methanation of clusters and nanoplates of ruthenium dispersed on ceria: In-situ studies with XAFS and DRIFTS","authors":"Irene Barba-Nieto , Marcos Fernández-García , Jorge Moncada , Guilherme Felipe Lenz , Juan D. Jimenez , Sooyeon Hwang , Akhil Tayal , Sanjaya D. Senanayake , Anna Kubacka , José A. Rodriguez","doi":"10.1016/j.cattod.2025.115443","DOIUrl":"10.1016/j.cattod.2025.115443","url":null,"abstract":"<div><div>The performance of Ru/CeO<sub>2</sub> catalysts under CO<sub>2</sub> hydrogenation conditions was studied using in situ X-ray absorption fine structure (XAFS) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) to understand the structural evolution and chemical nature of each component under reaction conditions. The catalysts were prepared using a reverse microemulsion method that maximized the dispersion of RuO<sub>x</sub> particles on ceria. A RuO<sub>x</sub> → Ru transformation was observed upon exposure of the RuO<sub>x</sub>/CeO<sub>2</sub> systems to H<sub>2</sub> at 250 °C. For a sample with 5 % molar Ru, two-dimensional clusters (2–4 atoms) of Ru formed on top of the ceria support. An increase in the loading of ruthenium to 20 % molar led to the formation of nanoplates of the metal 2–3 at. layers thick. Both Ru structures were highly dispersed on ceria. They were oxidized after exposure to CO<sub>2</sub> at 250 °C. However, under CO<sub>2</sub>/H<sub>2</sub> mixture, they remained in a metallic state as two-dimensional clusters and nanoplates. In situ DRIFTS studies, the 5 % and 20 % Ru/CeO<sub>2</sub> catalysts showed distinct reaction intermediates when exposed to CO<sub>2</sub> or CO<sub>2</sub>/H<sub>2</sub> (1/4) reaction mixtures. Normalized to the Ru molar percentage, the 5 % Ru/CeO<sub>2</sub> system was the most active catalyst exhibiting a selectivity of ∼ 60 % CH<sub>4</sub> and 40 % CO at 250 °C. On the other hand, under the same reaction conditions, the 20 % Ru/CeO<sub>2</sub> system was less active but had a CH<sub>4</sub> selectivity close to 80 %. These results highlight the importance of the structure of the metallic Ru particles as a factor that determines the catalytic performance.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"459 ","pages":"Article 115443"},"PeriodicalIF":5.2,"publicationDate":"2025-07-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144548858","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Catalysis TodayPub Date : 2025-06-26DOI: 10.1016/j.cattod.2025.115440
Arturo Sanz-Marco , Jose L. Hueso , Víctor Sebastian , Francisco Balas , Jesus Santamaria
{"title":"Continuous photothermal gas-phase CO2 hydrogenation over highly dispersed Ru-Ni on TiO2","authors":"Arturo Sanz-Marco , Jose L. Hueso , Víctor Sebastian , Francisco Balas , Jesus Santamaria","doi":"10.1016/j.cattod.2025.115440","DOIUrl":"10.1016/j.cattod.2025.115440","url":null,"abstract":"<div><div>Photocatalytic and photothermal carbon dioxide (CO<sub>2</sub>) hydrogenation are investigated as key strategies for CO<sub>2</sub> depletion by transformation into valuable products. Ni and Ru are well known Sabatier's reaction catalysts. In the present work we study their activity as Ni, Ru and bimetallic nanoparticles over the surface of titanium dioxide (TiO<sub>2</sub>) in the photocatalytic reduction of CO<sub>2</sub>, following a process of photo-assisted deposition that yield highly dispersed nanoparticles with sizes under 2 nm. Outstanding production of solar fuels was observed from Ni and Ru 2-nm nanoparticles deposited onto P25 TiO<sub>2</sub>. The photocatalytic activity tests under light irradiation from low-energy LEDs at different wavelengths, from UV-A at 365 nm to infrared at 940 nm at 523 K, rendered up to 6 % CO<sub>2</sub> conversion under continuous feed, with CO and CH<sub>4</sub> productivities above 5 mmol/g<sub>cat</sub>·h.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"459 ","pages":"Article 115440"},"PeriodicalIF":5.2,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144518907","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Catalysis TodayPub Date : 2025-06-26DOI: 10.1016/j.cattod.2025.115436
R. Palcheva , L. Kaluza , P. Shestakova , J. Moravcik , A. Lyutskanova , K. Soukup , Y. Kalvachev , G. Tyuliev , K. Jiratova
{"title":"C-C coupling of 1-butanol over Mg- and Li-doped L-zeolite","authors":"R. Palcheva , L. Kaluza , P. Shestakova , J. Moravcik , A. Lyutskanova , K. Soukup , Y. Kalvachev , G. Tyuliev , K. Jiratova","doi":"10.1016/j.cattod.2025.115436","DOIUrl":"10.1016/j.cattod.2025.115436","url":null,"abstract":"<div><div>In chemical technologies, the formation of carbon-carbon bonds has gained an increasing importance in recent years. In this work, we studied L-zeolite as a catalyst support for the gas-phase Guerbet coupling of 1-butanol at atmospheric pressure and 400 °C. Low-loaded monometallic (Mg and Li) catalysts were synthesized by incipient wetness impregnation and their physicochemical properties were characterized by N<sub>2</sub> and Ar adsorption-desorption isotherms, XRD, FT-IR, temperature-programmed desorption of NH<sub>3</sub> and CO<sub>2</sub>, <sup>29</sup>Si and <sup>27</sup>Al MAS NMR, and XPS. XRD and FTIR results showed no major change in the crystal structure of the doped zeolite. Impregnation of the zeolite by Mg and Li decreased the surface area and significantly reduced the micropore volume, but crystallinity was preserved. <sup>29</sup>Si MAS NMR indicated that desilication had occurred to some extent during catalyst impregnation, which led to the formation of mesopores. The Li/L catalyst showed more basic sites of intermediate strength due to surface Li-O pairs on the surface, which, together with mesoporosity, contribute to enhancing 1-butanol conversion by C-C coupling. The Li/L catalyst was more selective to C<sub>8</sub> oxygenate products than the reference aldol condensation catalyst.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"459 ","pages":"Article 115436"},"PeriodicalIF":5.2,"publicationDate":"2025-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144501968","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Catalysis TodayPub Date : 2025-06-25DOI: 10.1016/j.cattod.2025.115437
I. Yordanova , S. Todorova , K. Tenchev , E. Encheva , H. Kolev , A. Naydenov
{"title":"Application of clinoptilolite as carrier for VOCs removal by cobalt and manganese oxides","authors":"I. Yordanova , S. Todorova , K. Tenchev , E. Encheva , H. Kolev , A. Naydenov","doi":"10.1016/j.cattod.2025.115437","DOIUrl":"10.1016/j.cattod.2025.115437","url":null,"abstract":"<div><div>Bulgarian natural zeolite Clinoptilolite was used for catalyst carrier. To improve carrier properties modification by nitric acid and ion exchange through ammonium nitrate was performed. Catalytic active phase of cobalt and manganese was applied by wet impregnation method. Synthesised Co or Mn catalysts were characterized by means of AES-ICP, XRD, low-temperature N<sub>2</sub> adsorption, TPR, XPS, and HRTEM. The zeolite catalysts were tested in the reaction of total oxidation of n-hexane. All samples demonstrated good catalytic activity. Samples with low amount of the active phase (10 %) manifested a higher catalytic activity. This is due to uniform distribution of the active phase on the carrier surface, diminished crystallite size, and readily reducible Co oxide and Mn oxide phases.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"459 ","pages":"Article 115437"},"PeriodicalIF":5.2,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144501969","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Catalysis TodayPub Date : 2025-06-25DOI: 10.1016/j.cattod.2025.115438
Khalid Umer , Khuram Hasnain , Bonan Li , Hira Shahid , Xiao Fang , Xi Zhang , Baochun Ma , Yong Ding
{"title":"Synergistic charge transfer engineering in Mo368POM@Nb2CTx@MoS2 heterostructure for accelerated visible light-driven hydrogen evolution","authors":"Khalid Umer , Khuram Hasnain , Bonan Li , Hira Shahid , Xiao Fang , Xi Zhang , Baochun Ma , Yong Ding","doi":"10.1016/j.cattod.2025.115438","DOIUrl":"10.1016/j.cattod.2025.115438","url":null,"abstract":"<div><div>The transition to sustainable energy systems urgently demands high-performance photocatalysts capable of efficient solar-driven hydrogen production to combat fossil fuel dependency. Herein, a rationally designed ternary heterostructure, Mo<sub>368</sub>@Nb<sub>2</sub>CT<em><sub>x</sub></em>@MoS<sub>2</sub> is presented by incorporation of MoS<sub>2</sub>, Mo<sub>368</sub> polyoxometalate (POM) and Nb<sub>2</sub>CT<em><sub>x</sub></em> MXene. This breakthrough arises from the synergistic interplay of MoS<sub>2</sub> as a semiconductor host for light-harvesting, Mo<sub>368</sub> polyoxometalate (POM) as reduction co-catalyst, and Nb<sub>2</sub>CT<em><sub>x</sub></em> as an electron sink, which collectively establish a cascade charge-transfer network. The integration of Nb<sub>2</sub>CT<em><sub>x</sub></em> accelerates electron extraction and transport due to its metallic conductivity, while Mo<sub>368</sub> POM functions as reduction agent, dynamically trapping photogenerated carriers and suppressing recombination losses. The composite catalyst Mo<sub>368</sub>@Nb<sub>2</sub>CT<em><sub>x</sub></em>@MoS<sub>2</sub> achieves a hydrogen evolution rate of 1.6 mmol g⁻¹ h⁻<sup>1</sup> under visible-light irradiation with apparent quantum yield (AQY) of 6.4 %. By elucidating the complementary roles of MXene and POM in modulating carrier dynamics, this work establishes a unique design framework for heterostructure photocatalysts. The findings advance the frontier of solar fuel production, providing a scalable strategy to engineer multifunctional catalytic architectures, specifically engineered for high-efficiency solar-driven hydrogen evolution through rational material design.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"459 ","pages":"Article 115438"},"PeriodicalIF":5.2,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144501967","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Photocatalytic oxidation of 2,4-D by g-C3N4-CuFe2O4 catalyst: statistical modeling and optimization via Box–Behnken design","authors":"Ngo Thi Tuong Vy , Dang Nguyen Nha Khanh , Doan Thi Minh Phuong , Pham Tuan Nhi , Nguyen Thi Mong Lan , Nguyen Ngoc Nghia , Nguyen Thi Kim Phuong","doi":"10.1016/j.cattod.2025.115435","DOIUrl":"10.1016/j.cattod.2025.115435","url":null,"abstract":"<div><div>Response surface methodology (RSM) is an outstanding tool for optimizing pollutant photodegradation processes that involve many complex operational factors. This study aims to model and optimize the photodegradation parameters of 2,4-Dichlorophenoxyacetic acid (2,4-D) using a Z-scheme g-C<sub>3</sub>N<sub>4</sub>-CuFe<sub>2</sub>O<sub>4</sub> catalyst, with a Box–Behnken design (BBD) as the RSM statistical model. The effects of independent variables such as the g-C<sub>3</sub>N<sub>4</sub>-CuFe<sub>2</sub>O<sub>4</sub> catalyst with different loadings of g-C<sub>3</sub>N<sub>4</sub> (X<sub>1</sub>), reaction time (X<sub>2</sub>), initial 2,4-D concentration (X<sub>3</sub>), catalyst dosage (X<sub>4</sub>), and solution pH (X<sub>5</sub>) on 2,4-D photodegradation were studied. All independent variables tested during 2,4-D photodegradation were found to be statistically significant based on the ANOVA results. The results show that the amount of g-C<sub>3</sub>N<sub>4</sub> introduced into the CuFe<sub>2</sub>O<sub>4</sub> structure had the most significant influence among the variables on 2,4-D photodegradation. The photodegradation efficiency predicted by the BBD model was 98.21 % under optimal operating conditions, including a solution pH of 5.0 using 1000 mg/L of g-C<sub>3</sub>N<sub>4</sub>(2 %)-CuFe<sub>2</sub>O<sub>4</sub> at an initial 2,4-D concentration of 20 mg/L. The actual 2,4-D photodegradation efficiency was close to the predicted value (97.78 ± 0.80 %), suggesting that BBD can be effectively used to optimize 2,4-D photodegradation using a Z-scheme g-C<sub>3</sub>N<sub>4</sub>(2 %)-CuFe<sub>2</sub>O<sub>4</sub> catalyst under visible light. The enhanced photodegradation efficiency of 2,4-D is mainly due to the effective separation of photoinduced electron–hole pairs and the formation of highly active species (O<sub>2</sub><sup>•−</sup> and OH<sup>•</sup>) in the Z-scheme g-C<sub>3</sub>N<sub>4</sub>-CuFe<sub>2</sub>O<sub>4</sub> heterojunction system. Furthermore, g-C<sub>3</sub>N<sub>4</sub>(2 %)-CuFe<sub>2</sub>O<sub>4</sub> is durable and easily recycled and reused many times in succession, showing great application potential in the removal of toxic pollutants through the efficient use of solar energy.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"459 ","pages":"Article 115435"},"PeriodicalIF":5.2,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144489501","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Catalysis TodayPub Date : 2025-06-23DOI: 10.1016/j.cattod.2025.115428
Gyungmin Kim, Alex Liu, Jack Jarvis, Erika Bonatti, Zhaofei Li, Hua Song
{"title":"Machine learning assisted bio-oil deoxygenation under methane environment: The model compound study on guaiacol","authors":"Gyungmin Kim, Alex Liu, Jack Jarvis, Erika Bonatti, Zhaofei Li, Hua Song","doi":"10.1016/j.cattod.2025.115428","DOIUrl":"10.1016/j.cattod.2025.115428","url":null,"abstract":"<div><div>The novel approach of methane-assisted deoxygenation on bio-oil is highly promising based on our previous studies. In this study, guaiacol was chosen as the model compound to further screen the catalyst to achieve optimal performances aiming to realize hydrogen-free deoxygenation while enhancing the yield of valuable BTX (benzene, toluene, and xylene). A catalyst of multi-metals doped ZSM-5 was predicted using machine learning model and fabricated to meet the requirements. Additionally, the synergistic effect between the support material and the loading metals were taking into account during the rational design and fabrication process of the catalyst. ZSM-5 was chosen as the support material to achieve a proper acidity to trigger the conversion of guaiacol while maintaining excellent selectivity towards the target products: benzene, toluene, and xylene (BTX). Zn and Ga was co-coped to enhance the methane activation at low temperatures, while Ce was further introduced to prohibit the over coking. A batch mode reactor was applied in the reaction performance studies aiming to understand the conversion, coke yield, selectivity of desired products, etc. The optimized Zn-Ga-Ce/ZSM-5 catalyst showed a conversion of guaiacol with the liquid yield of 58 wt% and BTX selectivity of as high as 90 %. Comprehensive characterizations including NH<sub>3</sub>-TPD, DRIFTS, XRD, TEM, BET, and TGA were conducted to gain in-depth understanding on the physicochemical properties of the catalyst. The relationship between the reaction performance and physicochemical properties of the catalyst has been explored carefully. This study will shed light on the catalyst engineering for the methane-assisted conversions.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"459 ","pages":"Article 115428"},"PeriodicalIF":5.2,"publicationDate":"2025-06-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144470259","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Recent advances in sulfur-resistant DeNOx catalysts for stationary source emissions: A state-of-the-art review","authors":"Ziying Hong, Haodan Cheng, Yangming Xie, Dekai Liu, Han Sun, Haijun Chen","doi":"10.1016/j.cattod.2025.115434","DOIUrl":"10.1016/j.cattod.2025.115434","url":null,"abstract":"<div><div>Selective catalytic reduction (SCR) has become the mainstream technology for industrial flue gas purification, widely adopted at stationary sources due to its high nitrogen oxides (NO<sub>x</sub>) removal efficiency, environmental friendliness, and proven reliability. However, the presence of SO<sub>2</sub> in flue gas leads to catalyst poisoning and deactivation, posing a major challenge to the system's core components. Therefore, understanding sulfur-induced deactivation mechanisms and developing sulfur-resistant strategies are critical for optimizing SCR systems, with significant theoretical and practical implications. This review systematically examines recent advances in the understanding of sulfur poisoning mechanisms, sulfur-resistant design strategies, and regeneration technologies for SCR catalysts. Distinct deactivation mechanisms have been identified across various non-precious metal-based catalysts, such as V, Mn, Ce, Cu, and Fe. Subsequently, sulfur-resistance strategies — including element doping, bimetallic synergy, support optimization, morphological engineering, and operational parameter adjustment — are comprehensively discussed. Moreover, regeneration methods for sulfur-poisoned catalysts are systematically evaluated, considering both cost-effectiveness and environmental sustainability. Finally, the design strategies and future challenges for the development of sulfur-resistant deNO<sub>x</sub> catalysts are highlighted, aiming to guide their practical application in real-world flue gas purification systems.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"459 ","pages":"Article 115434"},"PeriodicalIF":5.2,"publicationDate":"2025-06-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144501966","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Catalysis TodayPub Date : 2025-06-20DOI: 10.1016/j.cattod.2025.115433
Yingrui Zhang , Su He , Zhu Yuan , Chunchun Li , Yuanting Qiao , Steven E.J. Bell , Ningbo Gao , Yikai Xu , Chunfei Wu
{"title":"Interfacial self-assembly of preformed colloidal nanocatalysts for pyrolysis upcycling of waste plastic","authors":"Yingrui Zhang , Su He , Zhu Yuan , Chunchun Li , Yuanting Qiao , Steven E.J. Bell , Ningbo Gao , Yikai Xu , Chunfei Wu","doi":"10.1016/j.cattod.2025.115433","DOIUrl":"10.1016/j.cattod.2025.115433","url":null,"abstract":"<div><div>Catalytic pyrolysis of waste plastics offers a sustainable approach to transform plastic waste into valuable carbon nanomaterials such as carbon nanotubes. Conventional methods for catalyst preparation provides limited control over catalyst morphology and loading. In addition, the powder catalysts remain entangled with the product carbonaceous materials and are difficult to separate. To mitigate these challenges, here, we present the first example of an interfacial self-assembly based approach for the construction of bulk catalysts with well-defined nanoscale morphologies for catalytic pyrolysis. The versatility of the self-assembly approach allowed us to deposit model Fe<sub>3</sub>O<sub>4</sub> catalyst nanoparticles onto various types of supporting materials (S304, Ni, Ti, and Cu) to systematically investigate their impact on catalytic efficiency. Our studied revealed that CNT formation is influenced significantly by substrate-introduced effects. Among the tested supports, S304 system offered the highest selectivity for CNT growth, giving a carbon yield with a value of 207 mg/g plastic. While Ni and Ti generated more carbon products but with lower CNT mass ratio. Importantly, the self-assembled catalyst system also enables facile separation of carbon products from the support, offering a practical advantage over conventional powder-based systems. More broadly, our approach provides a versatile platform for designing robust and efficient catalysts with potential applications beyond plastic upcycling.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"459 ","pages":"Article 115433"},"PeriodicalIF":5.2,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144365287","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Catalysis TodayPub Date : 2025-06-19DOI: 10.1016/j.cattod.2025.115429
Oğuzhan Akin, Qing He, Mohammadhossein Havaei, Fatma Defne Calik, Daniël Withoeck, Robin John Varghese, Parviz Yazdani, Paul Van Steenberge, Kevin M. Van Geem
{"title":"Enhanced production of BTX from PET-LDPE co-pyrolysis via Ga- and Zn-impregnated HZSM-5 catalysts","authors":"Oğuzhan Akin, Qing He, Mohammadhossein Havaei, Fatma Defne Calik, Daniël Withoeck, Robin John Varghese, Parviz Yazdani, Paul Van Steenberge, Kevin M. Van Geem","doi":"10.1016/j.cattod.2025.115429","DOIUrl":"10.1016/j.cattod.2025.115429","url":null,"abstract":"<div><div>The coexistence of polyethylene terephthalate (PET) and polyolefins in plastic waste poses a significant challenge for pyrolysis-based recycling, as PET decomposition generates oxygenates that reduce product quality. To address this, we developed a two-stage reactor system that catalytically upgrades vapors from PET–LDPE mixtures using Ga- and Zn-impregnated HZSM-5 catalysts. XPS analysis revealed that impregnation with Ga and Zn leads to the formation of GaO<sub>x</sub> and ZnOH<sup>+</sup> species, which introduce new Lewis acid sites. When these sites are located near Brønsted acid sites, synergistic interactions enhance both deoxygenation and aromatization, improving the catalytic performance of HZSM-5. At 600 °C, PET pyrolysis produces significant amounts of CO<sub>2</sub>, CO, and benzoic acid, resulting in oxygen-rich pyrolysis oil. While unmodified HZSM-5 achieves full deoxygenation, the resulting PyOil yield is modest, ranging from 24 to 34 wt%. In contrast, Ga- and Zn-modified catalysts increase PyOil yield to ∼50 wt% and improve mono-aromatic (BTX) selectivity to 80–89 % by shifting the acid site distribution toward weaker acidity, thereby favoring decarboxylation, decarbonylation, and aromatization. Notably, Zn-HZSM-5 maintained high BTX selectivity even with increasing PET content, outperforming Ga-HZSM-5, which exhibited higher polyaromatic hydrocarbon formation under similar conditions. These results demonstrate the potential of Ga- and Zn-modified HZSM-5 catalysts for the efficient conversion of mixed plastic waste into BTX-rich oils suitable for fuel and chemical applications.</div></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":"459 ","pages":"Article 115429"},"PeriodicalIF":5.2,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144338795","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}