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
Chemistry, Analytical
Xinyu He, Yajie Tian, Congzhen Qiao, Guozhu Liu
Summary: In this study, the acid properties of ZSM-5 zeolite catalysts were modified through secondary addition of aluminum. The modified catalysts showed significantly enhanced performance in cracking of n-pentane, leading to increased yield and improved catalytic stability.
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
(2022)
Article
Chemistry, Applied
Shiying Li, Huanhuan Yang, Sen Wang, Mei Dong, Jianguo Wang, Weibin Fan
Summary: Hierarchical macro/microporous ZSM-5 zeolite synthesized from silica spheres showed improved catalytic performance in methanol to olefins reaction due to enhanced diffusion, reduced coke deposition, and increased production of propene and butene through alkene cycle contribution.
MICROPOROUS AND MESOPOROUS MATERIALS
(2022)
Article
Engineering, Environmental
Shangfeng Li, Hao Yan, Yibin Liu, Xiaobo Chen, Xin Zhou, Xiang Feng, Chaohe Yang
Summary: Metal doped ZSM-5 catalysts have been extensively studied for their unique catalytic activity in C-H bond activation. In this work, we used density functional theory calculations and microkinetic analysis to explore the catalytic activity of 12 transition metal single-atom-doped ZSM-5 zeolite catalysts in the catalytic cracking of naphtha. Our results show a strong electronic interaction between the metal atom and ZSM-5 skeleton, leading to a stable structure that enhances hydrocarbon adsorption and promotes C-H bond activation and carbenium ion cracking. Carbon and hydrogen binding energy were identified as descriptors for catalytic activity.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Shufang Zhao, Kyung Duk Kim, Lizhuo Wang, Ryong Ryoo, Jun Huang
Summary: A high-efficiency method for synthesizing hierarchical ZSM-5 zeolites with micropore and multistage mesopores using water-soluble carbon dots of various size distributions has been proposed. The obtained catalysts showed excellent catalytic performance and stability, attributed to improved reactant and product diffusion, anti-coking stability, suitable acidity, and increased accessibility of acid sites facilitated by multistage mesopores.
ADVANCED MATERIALS INTERFACES
(2021)
Article
Chemistry, Physical
Kang Chen, Xueqiu Wu, Jiyu Zhao, Hongjuan Zhao, Anhui Li, Qiang Zhang, Tian Xia, Peng Liu, Bo Meng, Weiyu Song, Xiaochun Zhu, Honghai Liu, Xionghou Gao, Chunming Xu, Baojian Shen
Summary: The distribution of aluminum and magnesium in [Al, Mg]-ZSM-5 zeolites significantly affects their catalytic performance, and the hydrothermal synthesis method can effectively regulate the location of framework aluminum. The introduction of magnesium by this method inhibits the hydride transfer process, thereby increasing the yields of propylene in catalytic cracking reactions.
JOURNAL OF CATALYSIS
(2022)
Article
Energy & Fuels
Joao Manuel Rego Silva, Aruzza Mabel de Morais Araujo, Joao Paulo da Costa Evangelista, Djalma Ribeiro da Silva, Amanda Duarte Gondim, Antonio Souza de Araujo
Summary: The sunflower oil pyrolysis process was evaluated using TGA-FTIR technology with microporous (H-ZSM-5) and mesoporous (Al-MCM-41) catalysts. The catalysts were characterized and shown to have good structural organization. The reaction kinetics were determined using isoconversional methods, and the apparent activation energies for different conversion rates were calculated.
Article
Engineering, Chemical
Zihan Zhou, Xingwen Wang, Rui Yu, Rongli Jiang, Yu Gao, Xueshuai Chen, Huilin Hou
Summary: In this paper, b-axis oriented ZSM-5 zeolite was synthesized by a solvent-free method using ammonia as a growth regulator. The zeolites were characterized using modern detection techniques such as XRD, SEM, BET, and NH3-TPD. The results showed that ammonia not only promoted the crystallization of ZSM-5 zeolite but also directed the synthesis of b-axis oriented ZSM-5 zeolite, which enhanced the selectivity of light olefins. The synthesis process of b-axis oriented ZSM-5 zeolite eliminated the need for mixing and aging in aqueous solution, reducing sewage discharge and autogenic pressure generation. This environmentally friendly approach could guide the green preparation of industrial ZSM-5 zeolites.
ADVANCED POWDER TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Gaixiu Yang, Juntao Yang, Dalong Huang, Weihong Zhou, Lingmei Yang, Pengmei Lv, Weiming Yi, Yongming Sun, Beibei Yan
Summary: The hierarchical zeolites doped with different amounts of Ga element were successfully synthesized via an isometric impregnation method. The addition of Ga increased Brønsted-Lewis (B + L) acids, leading to improved benzene, toluene, and xylene (BTX) selectivity and anti-coking properties. The 2%Ga-ZSM-5/SBA-15 zeolite composite showed the best BTX catalytic selectivity, with a BTX yield of 25.52%, demonstrating its potential for practical applications in BTX production and petrochemical industries.
NEW JOURNAL OF CHEMISTRY
(2021)
Article
Engineering, Environmental
Wissem Ben Soltan, Jianbiao Peng, Zhiguo Cao, Zheng Fu, Haijin Liu
Summary: The synthesis of bimetal catalyst Fe-Mn/H-ZSM-5 with high adsorption and low-temperature catalytic characteristics for the decomposition of VOCs was conducted. The zeolite-supported bimetal catalyst exhibited excellent catalytic-oxidation capacity for toluene at low temperatures and high stability. The mechanism of toluene oxidation over the catalyst was proposed and elucidated. This study is of great importance for the design of highly efficient catalysts for the removal of VOCs.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Applied
Y. Zhang, B. Louis
Summary: A modified ZSM-5 zeolite with high external surface area (ESA) and mild acidity was efficiently synthesized using a biochar obtained from algae as a hard template. The modified zeolite exhibited an ESA of 171 m2/g, compared to 121 m2/g for pristine ZSM-5. It also showed improved catalytic lifetime in the methanol-to-hydrocarbons (MTH) reaction, with a methanol conversion >95% for 16 hours, compared to only 10 hours for H-ZSM-5.
MICROPOROUS AND MESOPOROUS MATERIALS
(2023)
Article
Chemistry, Inorganic & Nuclear
Zihan Zhou, Rongli Jiang, Xueshuai Chen, Xingwen Wang, Huilin Hou
Summary: This paper successfully synthesized a hierarchical lamellar H-ZSM-5 zeolite with excellent catalytic performance for methanol to olefin conversion, using urea and PEG2000 as synthesis materials, providing an energy-efficient and eco-friendly synthesis strategy.
JOURNAL OF SOLID STATE CHEMISTRY
(2021)
Article
Chemistry, Applied
Hagos Birhane Asfha, Ashenafi Hailu Berta, Nayoung Kang, Danim Yun, Jaedeuk Park, Yong-Ki Park, Kiwoong Kim
Summary: In this study, a reaction mechanism of light straight run naphtha cracking over micro-spherical catalyst containing HZSM-5 was systematically investigated. The results showed that light paraffins and olefins were the primary products, and oligomerization and β-scission cracking dominated the secondary reactions. Experiments on single hydrocarbon feeds indicated that BTX formation proceeded via the formation of cycloalkanes and cyclo-olefinic intermediates. Temperature and space time influenced the product selectivity, with propylene selectivity increasing at lower temperatures and ethylene selectivity increasing at higher temperatures.
Article
Chemistry, Physical
Chenggong Song, Xu Hou, Hao Zhou, Huimin Qiao, Li Yin, Jing Huang, Enxian Yuan, Tingting Cui
Summary: Plastic waste management and disposal has become a significant environmental concern. This study focuses on the use of catalysts, specifically introducing mesopores into HZSM-5 zeolites, to enhance catalytic activity and decrease the degradation temperature of plastic waste. The results demonstrate that mesopore volume has a positive impact on degradation efficiency.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Neda Kalantari, Maged F. Bekheet, Parastoo Delir Kheyrollahi Nezhad, Jan O. Back, Ali Farzi, Simon Penner, Nagihan Delibas, Sabine Schwarz, Johannes Bernardi, Dariush Salari, Aligholi Niaei
Summary: In this study, chromium and boron were introduced into the hierarchical structure of ZSM-5 to enhance the catalysts' performance in the methanol-to-propylene process. The crystal structure and orientation of the synthesized zeolites were analyzed, revealing that the introduction of chromium and boron resulted in changes in the crystallinity and symmetry of the zeolites. The impregnated chromium-ZSM-5 catalyst showed superior performance in the production of light olefins, while the introduction of boron further improved the propylene selectivity and ratio.
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
(2022)
Article
Chemistry, Applied
Cristina Martinez, Alejandro Vidal-Moya, Bilge Yilmaz, C. P. Kelkar, Avelino Corma
Summary: Fluidized Catalytic cracking (FCC) is a main conversion process in refineries, using Y zeolite as the main source of activity and selectivity. A new Y zeolite catalyst, Phinesse(TM), based on partial substitution of RE by P, has been developed and shown to have similar performance to the conventional RE stabilized counterpart. The hydrothermal stability of different USYs with different dealumination degrees, containing P or La alone or a combination of both stabilizing elements, was compared. The results provide insights into the benefits of P-La stabilization observed in the commercial PhinesseTM catalyst.
Review
Chemistry, Multidisciplinary
Lichen Liu, Avelino Corma
Summary: This review discusses the structure, synthesis, and catalytic applications of heterogeneous bimetallic catalysts, including binuclear sites, nanoclusters, and nanoparticles. Recent progress in the field of bimetallic catalysts is highlighted, along with the future research directions and prospects in both fundamental and practical aspects of heterogeneous catalysis.
Article
Chemistry, Multidisciplinary
Estefan Tiburcio, Yongkun Zheng, Cristina Bilanin, Juan Carlos Hernandez-Garrido, Alejandro Vidal-Moya, Judit Oliver-Meseguer, Nuria Martin, Marta Mon, Jesus Fernando-Soria, Donatella Armentano, Antonio Leyva-Perez, Emilio Pardo
Summary: This study reports the characterization of a combination of well-defined Fe3+ isolated single-metal atoms and Ag2 subnanometer metal clusters within a metal-organic framework. The resulting material exhibits superior catalytic activity for the direct conversion of styrene to phenylacetylene.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Pau Ferri, Chengeng Li, Daniel Schwalbe-Koda, Mingrou Xie, Manuel Moliner, Rafael Gomez-Bombarelli, Mercedes Boronat, Avelino Corma
Summary: Approaching the level of molecular recognition of enzymes with solid catalysts is a challenging goal, achieved in this work for the competing transalkylation and disproportionation of diethylbenzene catalyzed by acid zeolites. The key diaryl intermediates for the two competing reactions only differ in the number of ethyl substituents in the aromatic rings, and therefore finding a selective zeolite able to recognize this subtle difference requires an accurate balance of the stabilization of reaction intermediates and transition states inside the zeolite microporous voids.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Risheng Bai, Guangyuan He, Lin Li, Tianjun Zhang, Junyan Li, Xingxing Wang, Xiumei Wang, Yongcun Zou, Donghai Mei, Avelino Corma, Jihong Yu
Summary: In this work, a carbonization-reduction method was used to create palladium carbide subnanometric species within pure silicate MFI zeolite. The developed catalyst showed superior performance in the selective hydrogenation of alkynes.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Francisco Gonell, Miriam Rodenes, Santiago Martin, Mercedes Boronat, Ivan Sorribes, Avelino Corma
Summary: Developing precious-metal-free electrocatalysts for the hydrogen evolution reaction (HER) is crucial. Amorphous molybdenum sulfide-based materials provide highly active HER electrocatalysts by introducing active sites at both the edge positions and the typically inactive basal planes. The bottom-up synthesis using molecular complexes with Mo3S4 and Mo3S7 cluster cores enhances the HER activity and allows the modification of the derived materials with atomic-scale precision.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Miriam Rodenes, Frederic Dhaeyere, Santiago Martin, Patricia Concepcion, Avelino Corma, Ivan Sorribes
Summary: A defect-engineered molybdenum sulfide catalyst is used to establish straightforward synthetic processes using alcohols. Developing tandem catalytic strategies based on readily available, stable, and renewable feedstocks is crucial for sustainable chemical industries. The catalyst, defect-engineered basal planes of a molybdenum sulfide nanomaterial ({Mo3S4}( n )), enables one-pot single-step synthesis and facilitates various coupling reactions involving alcohol dehydrogenation and hydrogen activation processes.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Reisel Millan, Estefania Bello-Jurado, Manuel Moliner, Mercedes Boronat, Rafael Gomez-Bombarelli
Summary: This study reports a machine learning method to accurately simulate the mobility of Cu ions in Cu-exchanged zeolites, revealing that aluminum pairing accelerates local hopping dynamics and increased NH3 concentration enhances long-range diffusion of Cu ions. Furthermore, the probability of finding metal complexes in the same cage increases with higher Cu and Al content.
ACS CENTRAL SCIENCE
(2023)
Article
Materials Science, Multidisciplinary
Ander Diego-Lopez, Oscar Cabezuelo, Alejandro Vidal-Moya, M. Luisa Marin, Francisco Bosca
Summary: A new optimized photocatalyst with SiO2 as a supporting substrate and a shell of WO3 nanoparticles decorated with Fe3O4 nanocrystals has been developed for wastewater remediation at neutral pH. Its photocatalytic activity was evaluated on the photodegradation of methylene blue (MB) and diclofenac (DCF), and the generation of .OH was proven to be responsible for the oxidation processes. The synergistic effect between Fe3O4 and WO3 in the presence of light and H2O2 enhances the generation of .OH.
APPLIED MATERIALS TODAY
(2023)
Editorial Material
Chemistry, Physical
Mercedes Boronat
Summary: This article investigates the impact of zeolite framework topology on catalyst performance and proposes new strategies for improved material design.
Review
Chemistry, Multidisciplinary
Lichen Liu, Avelino Corma
Summary: Heterogeneous bimetallic catalysts are widely used in industrial processes, but understanding the active sites in these catalysts at the atomic and molecular level is challenging due to their structural complexity. Comparing the structural features and catalytic performances of different bimetallic entities can aid in developing a unified understanding of the structure-reactivity relationships and improving current bimetallic catalysts. This review discusses the geometric and electronic structures of three representative types of bimetallic catalysts, as well as the synthesis methods, characterization techniques, and catalytic applications of these catalysts.
Article
Chemistry, Physical
Risheng Bai, Yue Song, Ge Tian, Fei Wang, Avelino Corma, Jihong Yu
Summary: The synthesis of highly efficient nano-sized Ti-rich TS-1 zeolites with controllable titanium species is crucial in zeolite catalytic reactions. A new method was developed using tetrabutyl orthotitanate tetramer as the titanium source, which slowed down the zeolite crystallization process and prevented the formation of anatase species. The Ti-rich TS-1 zeolite prepared with this method exhibited enriched active titanium species, enlarged external surface area, and superior catalytic performance in oxidative desulfurization reactions.
GREEN ENERGY & ENVIRONMENT
(2023)
Review
Chemistry, Multidisciplinary
Alexandra Velty, Avelino Corma
Summary: For many years, capturing, storing or sequestering CO2 from emission sources has been an effective method for reducing atmospheric CO2. The chemical conversion of CO2 into valuable chemicals has gained much attention due to CO2's abundance and renewable nature. Catalysts, particularly zeolite and ordered mesoporous materials, play a critical role in the conversion of CO2. By studying the reactions involving these catalysts, this review aims to explore the potential opportunities for using them to convert CO2 into essential chemicals and fuels.
CHEMICAL SOCIETY REVIEWS
(2023)
Article
Chemistry, Physical
Joaquin Martinez-Ortigosa, Reisel Millan, Jorge Simancas, Manuel Hernandez-Rodriguez, J. Alejandro Vidal-Moya, Jose L. Jorda, Charlotte Martineau-Corcos, Vincent Sarou-Kanian, Mercedes Boronat, Teresa Blasco, Fernando Rey
Summary: This study investigates the synthesis of all-silica RTH zeolites using triisopropyl(methyl)phosphonium as the organic SDA. The results show the formation of two distinct crystalline phases under different synthesis conditions, with fluoride bonding to different silicon sites. It demonstrates the possibility of controlling the placement of fluoride in RTH zeolites through synthesis conditions.
JOURNAL OF MATERIALS CHEMISTRY A
(2024)