Article
Chemistry, Applied
B. Rabindran Jermy, Abdulkadir Tanimu, M. Abdulbari Siddiqui, Ziyauddin S. Qureshi, Abdullah Aitani, Aaron Akah, Qi Xu, Mansour AlHerz
Summary: The study demonstrates the conversion of crude oil to basic chemicals using a template-free green synthesis of ZSM-5(40) zeolite. Hierarchical porous structures with high surface areas were achieved using halloysite and bolus alpha as silica and alumina precursors. The addition of a soft template resulted in a zeolite with lower surface area. The synthesized zeolites were impregnated with 2wt%Mn and tested for catalytic cracking of crude oil, achieving high yields of light olefins and aromatics.
FUEL PROCESSING TECHNOLOGY
(2023)
Article
Energy & Fuels
Di Zhang, Peijie Zong, Jiaoyang Wang, Hongwei Gao, Jinzhuang Guo, Jingxian Wang, Yuxin Wang, Yuanyu Tian, Yingyun Qiao
Summary: This study investigated the catalytic dehydrogenation cracking of CTO using Py-GC/MS and a fluidized bed reactor, and analyzed the cracking characteristics, kinetics, and product release rules using TG-FTIR. The results showed that the bifunctional catalyst 1Ca/ZSM-5 significantly increased the production of light olefins by adjusting the basicity/acidity.
Article
Engineering, Chemical
Qi Xu, Aaron C. Akah, Mansour AlHerz, Abdullah Aitani, Ziyauddin S. Qureshi, M. Abdul Bari Siddiqui, Nabeel Abo-Ghander
Summary: This study presents new experimental results on the direct conversion of crude oil to chemicals via steam-enhanced catalytic cracking. The experimental results were organized using a kinetics model and showed that the steam cracking reaction of heavy oil fractions had an order of 2.0, while the reaction of light oil fractions had an order of 1.0. The estimated activation energies for the steam cracking reactions ranged between 20 and 200 kJ/mol. The study also found that an equal yield of propylene and ethylene was observed between 650 and 670 degrees C, indicating a transition from catalytic cracking to thermal cracking at higher temperatures.
CANADIAN JOURNAL OF CHEMICAL ENGINEERING
(2023)
Article
Chemistry, Analytical
Ziyauddin S. Qureshi, M. Abdullbari Siddiqui, Abdulkadir Tanimu, Abdullah Aitani, Aaron C. Akah, Qi Xu, Mansour AlHerz
Summary: In this study, a novel core-shell structured ZSM-5 zeolite was used for the direct conversion of crude oil to basic chemicals. The thickness of the mesoporous silica-alumina shell and its alumina content were controlled by adjusting the ratios of TEOS/zeolite and TEOS/aluminum sulfate. The optimized mesoporous silica-alumina composite showed improved cracking potential and selectivity towards light olefins.
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
(2022)
Article
Chemistry, Applied
Xinyu He, Yajie Tian, Congzhen Qiao, Zhenheng Diao, Guozhu Liu
Summary: A core-shell PtZn catalyst was prepared for catalytic cracking of n-pentane, achieving high yields of ethylene and propylene. The catalyst consisted of nanosheet silicalite-1 and microporous ZSM-5, facilitating the generation of light olefins through a proposed dehydrogenation-cracking pathway.
MICROPOROUS AND MESOPOROUS MATERIALS
(2023)
Article
Chemistry, Analytical
Noah Niwamanya, Jinhong Zhang, Andrew Barigye, Chunxiao Gao, Daniel Takyi Sekyere, Haoyang Sun, Yaozheng Chen, Lilian Orest Msale, Yuanyu Tian
Summary: Direct catalytic cracking of heavy crude oil is a cost-effective method for producing raw materials for the petrochemical industry. This study investigated the effects of calcium aluminate base catalysts and ZSM-5 acid zeolites on heavy crude oil conversion using the Py-GC/MS technique. The results showed that ZSM-5 with a Si/Al ratio of 40 had the highest selectivity for light olefins and BTX, while calcium aluminate (CaAl-3) had the highest selectivity for C2-C4 olefins and BTX. The Mix model of acid-base coupled catalytic pyrolysis demonstrated the best performance in terms of hydrogen transfer reactions and yield of light olefins.
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
(2023)
Article
Chemistry, Analytical
Emad N. Al-Shafei, Mohammed Z. Albahar, Mohammad F. Aljishi, Abdullah Aitani, Ali N. Aljishi, Ali S. Alnasir, Anaam H. Al-ShaikhAli, Ahmed Alasseel
Summary: The influence of ZSM-5 zeolite crystal size on the selectivity to light olefin during the catalytic cracking of heavy AGO was investigated. Nano ZSM-5 crystals with short pores showed enhanced cracking activity and selectivity to light olefins, while micro ZSM-5 crystals with long pores favored the production of naphtha, kerosene and LPG. The P/E ratio was affected by the type of feed, cracking temperature, steam presence, and catalyst crystal size.
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
(2023)
Article
Chemistry, Inorganic & Nuclear
Esmat Koohsaryan, Mansoor Anbia, Kourosh Tabar Heydar
Summary: In this study, highly crystalline hierarchical FAU zeolite was prepared and activated by MoO3 for oxidative desulfurization of fuel oils. Various characterization techniques were employed to identify the structural properties of the catalyst and the mechanism of the ODS process. The results showed that Meso-Mo-FAU with 19 wt.% molybdenum exhibited high catalytic activity at 70 degrees C, and the spent catalyst had a robust heterogeneous nature.
JOURNAL OF SOLID STATE CHEMISTRY
(2022)
Article
Energy & Fuels
Qingjing Niu, Lisha Wei, Ruifeng Hou, Ling Zhang, Kun Hao, Caixia Hu, Xiaodong Wen, Hongwei Xiang, Zhichao Tao, Yong Yang, Yongwang Li
Summary: 3D zeolite with 10-membered ring channels has the advantage of increasing light olefins in catalytic cracking reactions. IM-5, ZSM-5, and ZSM-11 zeolites were synthesized hydrothermally to achieve similar texture properties and SiO2/Al2O3 ratios. The acid content and strength were IM-5 > ZSM-5 > ZSM-11. IM-5 zeolite showed a synergistic effect between Bronsted and Lewis acids. However, it had unexpectedly low TOF in n-heptane cracking. The selectivity of light olefins was IM-5 > ZSM-11 > ZSM-5, with IM-5 zeolite having a particular advantage in ethylene production.
Article
Chemistry, Multidisciplinary
Galal A. Nasser, M. H. M. Ahmed, Mochamad A. Firdaus, Mohammed A. Sanhoob, Idris A. Bakare, E. N. Al-Shafei, M. Z. Al-Bahar, A. N. Al-Jishi, Z. H. Yamani, Ki-Hyouk Choi, Oki Muraza
Summary: Nano BEA zeolite catalysts were synthesized and modified by desilication and Co ion-exchange, altering the acidity of the catalysts. The conversion and yield of light olefins increased with higher reaction temperatures in the range of 400 to 600 degrees Celsius.
Article
Chemistry, Multidisciplinary
Mengya Xia, Qiaoxian Tong, Huai Sun, Yingxin Sun, Sheng Han, Qianggen Li
Summary: The reaction mechanisms of methanol to propene on a phosphorus-modified acidic FAU zeolite were studied using a two-layer ONIOM method. The potential energy surface analysis showed that the rate-determining steps differ for each pathway. The addition of phosphorus atoms to the zeolite decreases the energy barriers of the rate-determining steps. The electron migration direction and nature of the transition states were revealed by DCD, LOL, and RDG plots. The presence of van der Waals and weak covalent interactions were found in the transition state structures.
NEW JOURNAL OF CHEMISTRY
(2023)
Article
Chemistry, Applied
Yong Wang, Toshiyuki Yokoi, Takashi Tatsumi
Summary: Compared to conventional steam cracking, catalytic cracking of naphtha and methanol-to-olefins (MTO) over zeolite catalysts have been proven as the most successful processes for producing light olefins. In this review, the impacts of topology, acidity, and particle size of zeolites on the catalytic performance of naphtha cracking and MTO reactions, especially the light olefins selectivity and lifetime are systematically discussed. The goal is to provide a deeper understanding of the structure-property-performance relationship of various zeolite catalysts and facilitate the design of more excellent zeolite catalysts for these two processes.
MICROPOROUS AND MESOPOROUS MATERIALS
(2023)
Article
Energy & Fuels
Nguyen Le-Phuc, Tri Van Tran, Tuan Trung Phan, Phuong Thuy Ngo, Thuy Ngoc Luong
Summary: This study investigates the direct cracking of Bach Ho crude oil using different catalysts, and finds that the modified FCC catalyst (HT-FCC) exhibits high activity and can achieve high yields of light olefins and gasoline at a low catalyst-to-oil ratio. The addition of ZSM-5 catalyst helps to enhance the conversion of gasoline to light olefins.
PETROLEUM SCIENCE AND TECHNOLOGY
(2023)
Article
Chemistry, Physical
Son Dong, Houqian Li, Iris K. Bloede, Abdullah J. Al Abdulghani, Edgard A. Lebron-Rodriguez, George W. Huber, Ive Hermans
Summary: The catalytic conversion of model compounds for plastic pyrolysis oil (1-octene, octadiene, octane, and toluene) over ZSM-5 in a fixed-bed reactor was investigated mechanistically. The conversion of 1-octene resulted in the production of benzene, toluene, xylene, coke, and hydrogen through a series of cracking, oligomerization, cyclization, and hydrogen transfer reactions. Octadiene mainly contributed to reactor fouling through thermal coking, while octane and toluene were converted through cracking reactions and disproportionation, dealkylation, and coking reactions, respectively. The use of mesoporous ZSM-5 maintained product selectivity for 70 hours in time-on-stream experiments.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Engineering, Environmental
Xinyu He, Yajie Tian, Congzhen Qiao, Guozhu Liu
Summary: Nanocrystalline ZSM-5 aggregates catalysts with preserved micropores and newly generated intercrystalline mesopores enhance the conversion rate and selectivity of light olefins.
CHEMICAL ENGINEERING JOURNAL
(2023)
Review
Chemistry, Physical
Shekhar R. Kulkarni, Vijay K. Velisoju, Fernanda Tavares, Alla Dikhtiarenko, Jorge Gascon, Pedro Castano
Summary: Silicon carbide (SiC) has excellent thermal stability and conductivity, making it suitable for catalysis. This review tracks the development of SiC and evaluates its applications in catalysis.
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING
(2023)
Article
Engineering, Chemical
Rongrong He, Shenzhen Cong, Donglai Peng, Yatao Zhang, Meixia Shan, Junyong Zhu, Jing Wang, Jorge Gascon
Summary: In this study, the modification of MOF filler via dopamine polymerization greatly improved the interfacial compatibility between polymer and MOF, resulting in membranes with outstanding separation performance and long-term stability.
Article
Chemistry, Applied
Kun Liu, Mustafa Caglayan, Alla Dikhtiarenko, Xin Zhang, Orxan Sayidov, Edy Abou-Hamad, Jorge Gascon, Abhishek Dutta Chowdhury
Summary: To comply with stricter carbon emissions requirements, it is necessary to reduce the socioeconomic dependence on natural gas. However, avoiding natural gas from the future energy mix is challenging. Lignocellulosic biomass-derived biomethane provides a potential solution, and this study explores the technical feasibility and challenges of methane dehydroaromatization over hierarchical zeolite ZSM-5. The study also finds that the catalyst deactivation is influenced by inter- and intra-particle diffusion properties.
Article
Chemistry, Physical
Jose J. Delgado-Marin, Alejandra Rendon-Patino, Vijay Kumar Velisoju, Gadde Sathish Kumar, Naydu Zambrano, Magnus Rueping, Jorge Gascon, Pedro Castano, Javier Narciso, Enrique V. Ramos-Fernandez
Summary: We demonstrate that ZIFs used as catalysts for CO2 insertion suffer from irreversible degradation by leaching, leading to decreased stability and catalytic activity. Additional treatments are necessary to improve their stability.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Il Son Khan, Luis Garzon-Tovar, Toni Grell, Genrikh Shterk, Jose Cerrillo, Tuiana Shoinkhorova, Juan C. Navarro, Faisal Alahmadi, Angel Sousa, Anastasiya Bavykina, Daria Poloneeva, Mustafa Caglayan, Stephanie Terruzzi, Javier Ruiz-Martinez, Nikolay Kosinov, Valentina Colombo, Jorge Gascon
Summary: The use of metal-organic frameworks (MOFs) as precursors for heterogeneous catalysts has attracted much attention. Steaming during the controlled decomposition of MOFs leads to the formation of smaller, well-dispersed metal nanoparticles, resulting in more efficient catalysts. This study demonstrates the benefits of steam addition, including improved phase composition control and catalyst activity, for CO2 hydrogenation.
Article
Chemistry, Multidisciplinary
Zaoming Wang, Aydin Ozcan, Gavin. A. Craig, Frederik Haase, Takuma Aoyama, Daria Poloneeva, Keiji Horio, Masakazu Higuchi, Ming-Shui Yao, Cara. M. Doherty, Guillaume Maurin, Kenji Urayama, Anastasiya Bavykina, Satoshi Horike, Jorge Gascon, Rocio Semino, Shuhei Furukawa
Summary: A new concept of pore-networked gels is demonstrated by trapping the solvent phase with molecular networks to achieve accessible microporosity. These gels show enhanced CO2 capacities and improved mechanical properties and low volatility, making them potentially useful in gas adsorption and separation.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Review
Chemistry, Physical
Leidy Figueroa-Quintero, David Villalgordo-Hernandez, Jose J. Delgado-Marin, Javier Narciso, Vijay Kumar Velisoju, Pedro Castano, Jorge Gascon, Enrique V. Ramos-Fernandez
Summary: Metal-organic frameworks (MOFs) are porous hybrid materials with potential applications in catalysis, adsorption, drug delivery, mixed matrix membranes, and stabilization of porous liquids. While there has been considerable focus on functionalizing the inner surface of MOF crystals, methods to selectively functionalize the outer crystal surface are less developed. This article provides an overview of different types of post-synthetic modifications and their applications in various fields.
Article
Materials Science, Multidisciplinary
Nikita Kolobov, Abdelali Zaki, Katarzyna Swirk, Partha Maity, Luis Garzon-Tovar, Giasemi K. Angeli, Alla Dikhtiarenko, G. Delahay, Pantelis N. Trikalitis, Abdul-Hamid Emwas, Amandine Cadiau, Omar F. Mohammed, Christopher H. Hendon, Karim Adil, Jorge Gascon
Summary: Despite efforts to develop efficient Ti-based metal-organic framework (MOF) photocatalysts, MIL-125-NH2 remains the benchmark, and few design principles have been offered to improve photocatalytic performance. Linker functionalization in Ti MOFs has been shown to enhance photocatalysis under visible light by closing the electronic band gap and improving charge carrier lifetimes. The role of node nuclearity and topology on photocatalytic activity in known Ti-based MOFs is still unclear. Here, we report a new MOF, ICGM-1, with a 3D-connected framework featuring 1D Ti-O rods. Photocatalytic hydrogen evolution experiments reveal a significant difference in activity, solely attributed to node geometry. Time-resolved spectroscopy and DFT calculations explain these differences in terms of electronic and geometric properties, paving the way for the development of Ti-MOF photocatalysts.
ACS MATERIALS LETTERS
(2023)
Article
Chemistry, Multidisciplinary
Rushana Khairova, Sarah Komaty, Alla Dikhtiarenko, Jose Luis Cerrillo, Sudheesh Kumar Veeranmaril, Selvedin Telalovic, Antonio Aguilar Tapia, Jean-Louis Hazemann, Javier Ruiz-Martinez, Jorge Gascon
Summary: Metal encapsulation in zeolitic materials through one-pot hydrothermal synthesis is an attractive technique to prepare zeolites with high metal dispersion. Metallosiloxanes are used as an alternative metal precursor, leading to quantitative metal loading and high dispersion. Fe-MFI zeolites synthesized using this method exhibit high catalytic activity in NH3-mediated selective catalytic reduction (SCR) of NOx.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Umair H. Bhatti, Masood S. Alivand, Francesco Barzagli, Meher Geetika Sanku, Jorge Gascon, Kathryn A. Mumford
Summary: Catalyst-facilitated amine regeneration provides an energy-efficient and economically feasible CO2 capture process. Glucose-derived carbon sphere nanocatalysts with isethionic acid functionalization were developed to optimize the CO2 desorption rate of CO2-loaded monoethanolamine solutions. The synthesized catalysts accelerated the CO2 desorption rate by up to 108% and reduced the heat duty by approximately 10.8% compared to traditional uncatalyzed regeneration. These catalysts can be separated easily, stable in cyclic uses, and suitable for industrial-scale applications. Regenerating solvents with catalysts at 86°C allows the use of low-grade industrial waste heat, enabling efficient CO2 capture facilities to be installed at various industrial sites for achieving net zero emissions by 2050.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Multidisciplinary Sciences
Patricia Mayer, Adrian Ramirez, Giuseppe Pezzella, Benedikt Winter, S. Mani Sarathy, Jorge Gascon, Andre Bardow
Summary: A techno-economic analysis and lifecycle assessment were conducted to compare the economics and environmental impacts of blue and green ammonia production. It was found that methane leakage can exacerbate the climate change impacts of blue ammonia in short time horizons, emphasizing the importance of low natural gas leakage for the sustainability of blue ammonia. Technological advances have the potential to further reduce the environmental impacts of photovoltaics-based green ammonia.
Article
Chemistry, Physical
Mustafa Caglayan, Abdallah Nassereddine, Stefan-Adrian F. Nastase, Antonio Aguilar-Tapia, Alla Dikhtiarenko, Sang-Ho Chung, Genrikh Shterk, Tuiana Shoinkhorova, Jean-Louis Hazemann, Javier Ruiz-Martinez, Luigi Cavallo, Samy Ould-Chikh, Jorge Gascon
Summary: Tungsten is a promising metal with higher thermal stability for replacing molybdenum in methane dehydroaromatization (MDA) catalysis. However, the MDA activity of W-ZSM-5 catalysts is lower than their Mo counterpart. In order to understand the differences in catalytic activity, thorough investigations are conducted on the dispersion and distribution of W sites on the zeolite.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Review
Engineering, Chemical
Faisal Alahmadi, Anastasiya Bavykina, Natalia Morlanes, Robert Schucker, Jorge Gascon
Summary: This review provides an overview of the challenges faced by the oxidative coupling of methane (OCM) and explores the use of a distributed feed policy and mixed-ionic-electronic-conducting (MIEC) membranes to enhance OCM performance. The review also discusses the chemical and mechanical stability of MIEC membranes for OCM applications.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Chemistry, Multidisciplinary
Qingpeng Cheng, Xueli Yao, Lifeng Ou, Zhenpeng Hu, Lirong Zheng, Guanxing Li, Natalia Morlanes, Jose Luis Cerrillo, Pedro Castano, Xingang Li, Jorge Gascon, Yu Han
Summary: Researchers achieved high incorporation of nickel (Ni) catalysts into the framework of ZSM-5 zeolite using a ligand-protected synthesis method. The incorporated Ni species formed metal-oxygen pairs, promoting the dissociation of C-H bonds in methane. The catalyst exhibited higher activity and stability, inhibiting coke formation through the CHx oxidation pathway.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Rushana Khairova, Sarah Komaty, Alla Dikhtiarenko, Jose Luis Cerrillo, Sudheesh Kumar Veeranmaril, Selvedin Telalovic, Antonio Aguilar Tapia, Jean-Louis Hazemann, Javier Ruiz-Martinez, Jorge Gascon
Summary: Encapsulating metal in zeolitic materials through one-pot hydrothermal synthesis is an attractive technique to prepare zeolites with high metal dispersion. This study introduces the use of metallosiloxanes as an alternative metal precursor and demonstrates their effectiveness in achieving quantitative metal loading and high dispersion. Fe-MFI zeolites obtained through this method exhibit high catalytic activity and good tolerance in the NH3-mediated SCR of NOx.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)