Article
Chemistry, Multidisciplinary
Manoj Ravi, Vitaly L. Sushkevich, Jeroen A. van Bokhoven
Summary: The Lewis acidic aluminum in zeolites can be transformed into octahedrally coordinated aluminum, which serves as the precursor of Lewis acid sites. These Lewis acid sites preferentially locate in the pore structure of mordenite, particularly in the side-pockets. By reverting the octahedrally coordinated aluminum back to a tetrahedral geometry, the corresponding Bronsted acid sites are restored, showing a reversible switch between Lewis and Bronsted acidity.
Article
Chemistry, Physical
Do Trung Hieu, Hendrik Kosslick, Muhammad Riaz, Axel Schulz, Armin Springer, Marcus Frank, Christian Jaeger, Nguyen Thi Minh Thu, Le Thanh Son
Summary: This study prepared acidic HCLIN catalysts by ion exchange and calcination using natural zeolite clinoptilolite as a starting material. The catalysts showed good catalytic performance in the etherification of glycerol.
Article
Chemistry, Applied
Bo Meng, Shenyong Ren, Xinyue Zhang, Kang Chen, Wenkai Wei, Qiaoxia Guo, Baojian Shen
Summary: This study aims to increase the density of strong Bronsted acid in Y zeolite by introducing Zr4+, which leads to improved catalytic cracking efficiency. The introduction of Zr4+ reduces the content of certain species in the zeolite and promotes the formation of abundant mesoporous structures.
MICROPOROUS AND MESOPOROUS MATERIALS
(2022)
Article
Chemistry, Applied
Mingyang Gao, Zhongmiao Gong, Xuefei Weng, Weixiang Shang, Yuchao Chai, Weili Dai, Guangjun Wu, Naijia Guan, Landong Li
Summary: Cationic Pd species encapsulated in MFI zeolite, Pd@MFI, were successfully prepared via in situ hydrothermal route followed by oxidative treatment. The as-prepared Pd@MFI samples exhibit promising activity and stability as catalysts in methane combustion. Strong interaction between Pd sites and zeolite framework, as well as the presence of Bronsted acid sites, play key roles in enhancing methane activation efficiency and catalytic performance.
CHINESE JOURNAL OF CATALYSIS
(2021)
Article
Chemistry, Applied
Byung Jin Lee, Jae Hwan Lee, Do Heui Kim, Young Gul Hur, Kwan-Young Lee
Summary: Heteroatoms such as gallium can influence the catalytic properties of zeolite-based catalysts, particularly in ethane activation. The optimal Ga/Al ratio of 1-4 can achieve high activity and stability for ethane dehydroaromatization by enhancing dehydrogenation ability while weakening acidity. Trade-off exists for the production of aromatic compounds in Ga-Al-MFI catalysts.
MICROPOROUS AND MESOPOROUS MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Mohsen Rostami Sakha, Parya Halimitabrizi, Saeed Soltanali, Fatemeh Ektefa, Zeinab Hajjar, Dariush Salari
Summary: The aim of this study was to investigate green and sustainable chemistry approaches in current industrial processes, such as methanol to olefin (MTO) and hexane to olefin (HTO), in order to minimize environmental pollution. The synthesis of multifunctional catalysts for simultaneous use in both processes was studied, along with the effect of different metals on product strengthening. The investigation showed that propylene production efficiency in microchannels for HTO was higher than ideal value, indicating significant improvement for future sustainable technologies. Ga-ZM exhibited the best overall performance in both processes due to a high P/E ratio, and Ga was found to have a significant effect on increasing propylene in MTO.
Article
Chemistry, Physical
Peng Liu, Jingjing Zhang, Shaozhong Peng, Wei Liu, Donghai Mei
Summary: The hydrocracking process of aromatic rings in the petrochemical industry has been studied using density functional theory. It is found that the Lewis acid site composed of a single extraframework-Al3+ atom is the most stable mononuclear extraframework aluminum species. Molecular dynamics simulations show that this site is the most efficient catalytic center for hydrogen splitting, leading to the formation of the stable tetrahydroanthracen-1-ylium cation. The reactivity of the hydrogen splitting process on different catalytic centers is influenced by the local electric field generated by the hydride acceptor and proton acceptor within the frustrated Lewis pair sites.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Engineering, Chemical
Mahesh Dumpalapally, Sasikumar Boggala, Rohitha Chozhiyath Nappuni, Shirisha Varimalla, Venugopal Akula
Summary: A cerium sulfate doped ZrO2 solid acid catalyst was prepared and its efficiency for the synthesis of polyoxymethylene dimethyl ethers (PODE) was tested. The surface Bronsted acidity played a significant role in improving the selectivity of desired PODE3-5 and higher PODEn>5. The overall acidity of the catalyst was related to the dispersion of CeO2 and the sulfate moiety.
CHEMICAL ENGINEERING SCIENCE
(2023)
Article
Chemistry, Applied
Haimei Xu, Peng Lu, Guangying Fu, Jifa Miao, Jiaqi Zhao, Ruiqin Ding, Lei Zhao, Zhirong Lang, Xiaobo Yang, Valentin Valtchev
Summary: The zeolite community successfully synthesized high-silica LTA-type zeolites after 50 years of research, and found strong interactions between organic structure-directing agents and the framework. Removing the structure-directing agents is difficult and can only be done at high temperatures.
MICROPOROUS AND MESOPOROUS MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Dong-Huang Liu, Hai-Long He, Jun-Jie Wang, Si-Yu Zhou, Tengwu Zeng, Xiang-Yu Gao, Yao Xiao, Xianfeng Yi, Anmin Zheng, Yue-Biao Zhang, Zhi Li
Summary: This study demonstrates a method using nanoporous acidic metal-organic frameworks for precise hydrodeoxygenation reactions, achieving efficient and highly selective hydrocarbon production. The superior performance of this method is mainly attributed to the preferential adsorption of oxygenate precursors and expulsion of deoxygenated intermediates facilitated by Lewis acid sites.
Article
Chemistry, Physical
Wenqian Fu, Chengyou Yin, Yu Feng, Lei Zhang, Feng Cheng, Zhongxue Fang, Chaojie Zhu, Tiandi Tang
Summary: The Cu/Beta-M catalyst exhibits superior catalytic performance in the difunctionalization of styrenes, attributed to the synergistic effect of Bronsted acid, copper species, and mesoporosity. Substrates with high electron density show increased reactivity towards the Cu/Beta-M catalyst.
APPLIED CATALYSIS A-GENERAL
(2021)
Article
Chemistry, Physical
Yaojie Li, Bo Qin, Wenming Hao, Yanze Du, Jinghong Ma, Ruifeng Li
Summary: The influence of acid sites with different spatial locations of USY zeolite with different micro-/mesoporous structures and Si/Al ratio on catalytic cracking reactions was investigated. The hierarchical USY zeolites exhibited increased numbers of accessible strong Brønsted acid sites and enhanced diffusion ability. This led to mainly monomolecular protolytic scission in cracking reactions and less bimolecular hydrogen transfer.
Article
Thermodynamics
Raissa Carvalho Martins, Simone Pereira da Silva Ribeiro, Michelle Jakeline Cunha Rezende, Regina Sandra Veiga Nascimento, Marco Antonio Chaer Nascimento, Jose-Marie Lopez-Cuesta
Summary: This study investigates the impact of montmorillonite acidity on the thermal degradation and cone calorimeter parameters of an intumescent composite. The results indicate that the absence of moderate-strength acidic sites leads to an increase in the peak heat release rate. Furthermore, the addition of clay minerals helps preserve char at higher temperatures and excessive Bronsted sites contribute to increased esterification reactions. Additionally, the mechanical properties of the composites remain unaffected by the presence of clay minerals.
JOURNAL OF THERMAL ANALYSIS AND CALORIMETRY
(2023)
Article
Chemistry, Physical
Nihad Omer Hassan, Mohamed Challiwala, Dhallia Mamoun Beshir, Nimir O. Elbashir
Summary: This paper investigates the use of HZSM-5 zeolite catalyst to reduce the acidity of crude oil by removing naphthenic acids. The results show that the catalyst can effectively remove naphthenic acids via decarboxylation. The removal efficiency is enhanced with increasing temperature and residence time. Additionally, a kinetic model is developed to predict the performance of the catalyst.
Article
Chemistry, Multidisciplinary
Aiyong He, Qinyin Gu, Xinming Shen, Jingyi Zheng, Lei Hu, Xiaoyu Wang, Yetao Jiang, Zhen Wu, Jiaxing Xu, Jinliang Song
Summary: A bifunctional catalyst was developed in this study which achieved the one-pot conversion of 5-hydroxymethylfurfural to 2,5-bis(hydroxymethyl)furan. The catalyst, sulfonic acid-functionalized zirconium-based coordination catalyst (Zr-BDC-S-60), exhibited excellent catalytic activity and stability, and could be reused for at least three cycles.
Article
Chemistry, Physical
Han K. Chau, Quy P. Nguyen, Ana Carolina Jerdy, Dai-Phat Bui, Lance L. Lobban, Bin Wang, Steven P. Crossley
Summary: Selective dehydration of polyalcohols over zeolites containing Bri nsted acids is a promising approach for purifying and recycling multilayer polymer films. Water plays a positive role in facilitating the dehydration reactions by delocalizing surface-bound protons and allowing dehydration rates to occur even in the presence of inhibiting solvents. The presence of hydronium ion clusters as delocalized acid sites enhances surface coverage of the reactant and improves dehydration activity in the presence of solvent molecules, which could have significant implications for polymer recycling and upcycling.
Article
Chemistry, Physical
Tram N. Pham, Vy Nguyen, Huy Nguyen-Phu, Bin Wang, Steven Crossley
Summary: Extra-framework aluminum (EFAL) species generated during the hydrolysis of framework Al play a crucial role in alkane cracking activity on zeolites. Water treatment facilitates the mobility of EFAL species without framework hydrolysis. The proximity and location of framework Al influence the generation of synergistic sites in MFI zeolites.
Article
Nanoscience & Nanotechnology
Cao Wu, Jing Wang, Xiaohang Zhang, Lixing Kang, Xun Cao, Yongyi Zhang, Yutao Niu, Yingying Yu, Huili Fu, Zongjie Shen, Kunjie Wu, Zhenzhong Yong, Jingyun Zou, Bin Wang, Zhou Chen, Zhengpeng Yang, Qingwen Li
Summary: This study proposes a microwave absorber with nanoscale gradient structure, using an inorganic-organic competitive coating strategy to adjust the thermodynamic and kinetic reactions of iron ions. The results show that this absorber offers outstanding reflection loss value, broadband wave absorption, and flexible adjustment ability, surpassing other structures and meeting the requirements of lightweight equipment. In addition, the study elucidates the microwave regulation mechanism of the multiscale hybrid electromagnetic wave absorber.
NANO-MICRO LETTERS
(2023)
Article
Chemistry, Physical
Ana Carolina Jerdy, Tram Pham, Miguel Angel Gonzalez-Borja, Pascale Atallah, David Soules, Ron Abbott, Lance Lobban, Steven Crossley
Summary: Chemical recycling of waste plastics has gained global attention recently, but the role of polymer additives in depolymerization reactions remains unclear. This study investigates the impact of typical additives on the reaction rate of pyrolysis and catalytic decomposition over zeolites. It is found that all tested additives hinder the activity of ZSM-5 catalysts, and some additives can be fully removed from the catalyst, while others may permanently deposit and modify sites. The deposition of impurities on zeolites can affect their alkane cracking capabilities.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Vinicius Martins, Bryan E. G. Lucier, Kuizhi Chen, Ivan Hung, Zhehong Gan, Christel Gervais, Christian Bonhomme, Heng-Yong Nie, Wanli Zhang, Yining Huang
Summary: Porous metal-organic frameworks (MOFs) have diverse applications in various fields, and post synthetic modification (PSM) approaches can enhance their properties. In this study, high-field solid-state NMR techniques were used to gain molecular-level insights into a prototypical aluminum MOF and its interactions with metal guests. The results provide detailed information about the oxygen environment, intermolecular interactions, and host-guest connectivity in the MOF.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Shuo Tao, Lei Wang, Zhili Wang, Xiaolei Li, Xue Li, Yujie Wang, Bo Wang, Wenwen Zi, Ying Wei, Kuizhi Chen, Zhijian Tian, Guangjin Hou
Summary: Due to the interest in applications of zeolitic materials and challenges associated with traditional synthesis methods, a new synthesis approach for aluminophosphate (AlPO) zeotypes has been developed. By calcinating amorphous precursors at moderate temperatures and short reaction times, highly crystalline AlPO zeotypes with various topologies have been successfully synthesized. Multinuclear multidimensional solid-state NMR techniques combined with complementary characterizations reveal the catalytic role of fluoride and the directing role of organic structure-directing agents in the synthesis process. This novel synthesis strategy not only shows excellent efficiency, but also sheds new light on the crystallization mechanism of zeolitic materials.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Laura A. Gomez, Caleb Q. Bavlnka, Tianhao E. Zhang, Daniel E. Resasco, Steven P. Crossley
Summary: The study investigates the selective deoxygenation of carboxylic acid on promoted MoO3, revealing the potential for synthesizing valuable renewable products. The results suggest that the deoxygenation of pentanoic acid on an oxygen vacancy of MoO3 can be explained by a Langmuir-Hinshelwood mechanism. The incorporation of Pt shifts the reaction order with respect to hydrogen and alters the rate-determining step.
Article
Chemistry, Physical
Zhili Wang, Dong Xiao, Kuizhi Chen, Caiyi Lou, Lixin Liang, Shutao Xu, Guangjin Hou
Summary: Increasing research has revealed the complexity of active sites in zeolite catalysts, making it challenging to effectively characterize them, especially for a molecular-level understanding. Trimethylphosphine (TMP) is found to have strong catalytic meanings as proven by NMR-assisted 31P-27Al internuclear distance measurement and comprehensive 2D heteronuclear correlation (HETCOR) NMR experiments. The TMP-binding site is identified as special Al-OH groups, originating from partially bonded framework Al(IV)-2 species.
Article
Engineering, Biomedical
Ming Pei, Yixuan Amy Pei, Sheng Zhou, Elmira Mikaeiliagah, Christopher Erickson, Benjamin Giertych, Halima Akhter, Lei Wang, Amanda Stewart, Joshua Parenti, Bin Wang, Sijin Wen, Sotcheadt Sim, Eric Quenneville, Kirk C. Hansen, Steven Frisch, Gangqing Hu
Summary: Articular cartilage has limited self-healing capacity. Tissue-specific stem cells can be used for cartilage regeneration, but ex vivo expansion leading to cell senescence is a challenge. Cell-derived extracellular matrix (C-dECM) has been shown to rejuvenate stem cells and promote cartilage regeneration. In this study, the authors evaluated the rejuvenation of rabbit stem cells by C-dECM in both ex vivo and in vivo models, and identified potential cellular and molecular mechanisms involved.
BIOACTIVE MATERIALS
(2023)
Article
Chemistry, Physical
Ismaeel Alalq, Huy Nguyen-Phu, Steven Crossley
Summary: This study investigates the acylation reaction between 2-methylfuran and acetic acid over HZSM-5 catalysts at different temperatures, revealing the significant impact of surface coverage of acetic acid on catalyst deactivation behavior.
JOURNAL OF CATALYSIS
(2023)
Review
Chemistry, Physical
Victor Fung, Michael Janik, Steven Crossley, Ya-Huei Cathy Chin, Aditya Savara
Summary: Metal oxides have diverse adsorption site types on their complex surfaces, enabling catalytic transformations of organic molecules through various routes. This Perspective updates recent advances and future directions for organic reactions on metal oxide catalyst surfaces, particularly focusing on C-H activation of alkanes and C-C bond formation with organic oxygenate reactants. Molecular scale details, active site structures, energetic descriptors, and contemporary ideas for low activation energies are emphasized. This progress is enabled by specialized experiments and advanced electronic structure calculations.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Quy P. P. Nguyen, Han K. K. Chau, Lance Lobban, Steven Crossley, Bin Wang
Summary: Multi-layered plastic films have excellent properties for food packaging, but their recycling is challenging due to the complicated chemistry of the hydrophobic substrates and hydrophilic layers. In this study, the acid-catalyzed conversion of functional groups in polyalcohols was investigated to improve the recyclability of these films. The conversion pathways of ethylene vinyl alcohol, a common copolymer in multi-layered plastic films, were analyzed, providing insights for its selective conversion.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Tien Le, Taha Salavati-fard, Bin Wang
Summary: In this study, density functional theory calculations were performed on Cu2O to investigate the interfacial charge transfer and bond dynamics during CO2 reduction under plasmonic excitation. The presence of oxygen vacancies lowers the activation barrier for C-O bond cleavage, and this barrier can be further reduced or eliminated by plasmon-excited states when Cu2O is integrated with plasmonic metals.
Article
Chemistry, Multidisciplinary
Tien Le, Bin Wang
Summary: This study investigates the effect of different protic solvent molecules on interfacial charge transfer by calculating excitation energy. The research finds that H-bonds between water and NH3, as well as methanol (or phenol) and ammonia, can alter the direct interfacial charge transfer. The study provides valuable insights for tuning the excitation energy and controlling photon energy in plasmonic catalysis.
NANOSCALE ADVANCES
(2023)