Article
Multidisciplinary Sciences
Felix M. Kirchberger, Yue Liu, Philipp N. Plessow, Markus Tonigold, Felix Studt, Maricruz Sanchez-Sanchez, Johannes A. Lercher
Summary: The presence of water critically influences the kinetics of methanol autocatalytic conversion to hydrocarbons in acid zeolites. The main reactions at the initiation stage involve hydrogen transfer from methanol and DME to surface methoxy groups, leading to methane and formaldehyde in a 1:1 stoichiometry. The kinetic analysis of CH4 formation rates can be used as a unique quantitative parameter to characterize catalyst activity in the methanol-to-hydrocarbon process.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Engineering, Chemical
Tianyu Mo, Miao Yu, Hongyan Li, Songnan Li, Bin Lu, Jingxiang Zhao, Qinghai Cai
Summary: CrOx nanoparticle-and H+-modified NaZSM5 composites were prepared and characterized. The composites showed moderate surface acidity and basicity, resulting from the substitution of Cr species or H+ for counter Na+ and the highly dispersed CrOx nanoparticles on zeolites. The composites exhibited excellent performance in catalyzing methanol dehydration to dimethyl ether, with over 90% conversion and nearly 100% selectivity at lower reaction temperature. The activity remained stable over 500 hours of continuous operation, indicating excellent running stability.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Chemistry, Physical
Xinde Sun, Yue Yang, Yanli He, Shukui Zhu, Zhongmin Liu
Summary: By optimizing Si/Al ratio and hydrothermal treatment temperature, a high performance HZSM-5 catalyst was developed for liquid phase dehydration of methanol to dimethyl ether (DME). During a long term test of 6788 hours, DME selectivity remained above 99.96% with only slight deactivation observed, primarily attributed to coking and decline of HZSM-5 crystallinity.
Article
Energy & Fuels
Jianqing Li, Dezhi Han, Zhongyue Zi, Tao He, Guangbo Liu, Zhiqi Wang, Jingli Wu, Jinhu Wu
Summary: This study investigated the effects of crystallization time on the physicochemical properties of H[Fe,Al]ZSM-5 zeolite catalysts for the dimethyl ether to gasoline (DTG) reaction. The results showed that nanocrystalline H[Fe,Al]ZSM-5 zeolites with high crystallinity could be synthesized in a short time of 4 hours. The catalyst with a crystallization time of 24 hours exhibited the best catalytic performance, achieving a DME conversion rate of 100% for about 125 hours, a gasoline yield of 77%, and an isoparaffin selectivity of 35.5%.
Article
Chemistry, Multidisciplinary
Andrey Trypolskyi, Alexey Zhokh, Valentina Gritsenko, Mengyao Chen, Jianguo Tang, Peter Strizhak
Summary: The intrinsic kinetics of methanol dehydration to dimethyl ether over commercial ZSM-5 zeolite was studied theoretically and experimentally to establish the rate equation. Kinetic models based on Langmuir-Hinshelwood and Eley-Rideal formalism were proposed, with experimental verification showing a good correspondence with the L-H kinetics. In contrast, the E-R models provided an insufficient description of the methanol dehydration kinetics.
Article
Chemistry, Multidisciplinary
Alexey Zhokh, Andrey Trypolskyi, Valentina Gritsenko, Peter Strizhak
Summary: A series of H-ZSM-5/Al2O3 molded catalysts with different zeolite/alumina ratios were prepared and studied for catalytic activity in methanol dehydration to dimethyl ether. It was found that the mechanism of methanol adsorption is not sensitive to catalyst composition, while catalyst composition affects activation energy and methanol adsorption enthalpy.
REACTION CHEMISTRY & ENGINEERING
(2022)
Article
Energy & Fuels
Tingyu Liang, Jialing Chen, Zhangfeng Qin, Sen Wang, Pengfei Wang, Fang Jin, Mei Dong, Jianguo Wang, Weibin Fan
Summary: A series of H-ZSM-5 catalysts with different Si/Al ratios were prepared and their Methanol to Olefin (MTO) performance was investigated. The results showed that the density of Brønsted acid sites (BAS) significantly influenced the reaction pathways, but had little effect on the activity of aromatic hydrocarbon pool (HCP) species.
Article
Engineering, Chemical
Pei He, Jianhao Wang, Ying Li, Shouying Huang, Mei-Yan Wang, Yue Wang, Jing Lv, Xinbin Ma
Summary: Microporous zeolites are commonly used as industrial catalysts, with Bronsted acidity playing a crucial role in their performance and stability. This study demonstrates an efficient synthesis method for MOR zeolite, which maintains specific acidity while shortening the synthesis period. The ultrafast synthesis method shows no negative impact on the textural and acidic properties of zeolites, resulting in improved catalytic activity and stability for MOR.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2021)
Article
Chemistry, Applied
Yasin Khani, Sumin Pyo, Kwang-Eun Jeong, Chul-Ung Kim, Moonis Ali Khan, Byong-Hun Jeon, Kun-Yi Andrew Lin, Siyoung Q. Choi, Young-Kwon Park
Summary: A protonated form of Zeolite Socony Mobil-5 (H-ZSM-5) catalyst was synthesized through a hydrothermal method using different sources of silica. The effect of loading the catalyst with yttrium, samarium, and gadolinium on the acidic properties was investigated. Among the metal-loaded catalysts, the Sm/LHZ catalyst showed the best performance in the methanol to propylene conversion due to its high amount of weak and intermediate acid sites, while the Gd-LHZ catalyst increased the selectivity towards ethane and propane.
Review
Chemistry, Multidisciplinary
Xiujuan Gao, Junfeng Zhang, Faen Song, Qingde Zhang, Yizhuo Han, Yisheng Tan
Summary: Methanol and dimethyl ether (DME) serve as important platform compounds in the coal chemical, petrochemical, and fine chemical industries. The synthesis of methanol/DME has been industrialized, but with a production capacity exceeding market demand. To make better use of these compounds, the selective oxidation of methanol/DME to produce high value-added chemicals has gained significant attention for its green and environmentally friendly nature. This article provides a summary of recent advancements in the synthesis of formaldehyde, methyl formate, dimethoxymethane, and polyoxymethylene dimethyl ethers through selective oxidation of methanol/DME. The article also explores the challenges and prospects in catalyst design and application, aiming to provide theoretical guidance for activating and cleaving C-O, C-H, or O-H bonds in other alcohol/ether molecules and low-carbon alkanes to synthesize high value-added chemicals.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Mansoor Ali, Jong Jin Kim, Faisal Zafar, Dongming Shen, Xu Wang, Jong Wook Bae
Summary: The synthesis of gasoline-range hydrocarbons was studied using different ZSM-5 zeolites with various morphologies and Fe contents. Nanostructured N-ZSM-5 showed the highest C5+ selectivity and aromatics selectivity, attributed to its larger strong Bronsted acidic sites and smaller crystallite sizes. Fe-impregnated N-ZSM-5 exhibited an enhanced C5+ selectivity and suppressed cracking reactions, resulting in smaller C1-C4 selectivity. However, excessive Fe blocked active acidic sites, leading to lower DME conversion and C5+ selectivity.
Article
Chemistry, Physical
Jasper van Kampen, Jurriaan Boon, Martin van Sint Annaland
Summary: Separation enhanced reaction processes are promising for carbon dioxide utilisation. In situ water removal results in high conversions and avoids the drawbacks of conventional methods. Membrane and adsorption technologies have shown great advancements in the direct production of methanol and dimethyl ether.
JOURNAL OF MATERIALS CHEMISTRY A
(2021)
Article
Chemistry, Applied
Youming Ni, Wenliang Zhu, Zhongmin Liu
Summary: Metal-modified H-ZSM-5 has high selectivity of aromatics in methanol to aromatics (MTA) reaction, with HCHO formed by methanol dehydrogenation participating in aromatics synthesis, and methanol conversion producing more aromatics than olefins conversion.
JOURNAL OF ENERGY CHEMISTRY
(2021)
Article
Engineering, Chemical
Maria Magomedova, Mikhail Afokin, Anastasiya Starozhitskaya, Ekaterina G. Galanova
Summary: The process of olefin synthesis from dimethyl ether was tested on a pilot unit with nitrogen and synthesis gas as diluent gases. The study compared results with a laboratory unit's kinetic study to estimate the effectiveness of the porous catalyst Mg-HZSM-5/Al2O3 based on experimental data and theoretical equations.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2021)
Article
Multidisciplinary Sciences
Yanxia Guo, Sen Wang, Rui Geng, Pengfei Wang, Shiying Li, Mei Dong, Zhangfeng Qin, Jianguo Wang, Weibin Fan
Summary: Various FER zeolite nanosheets were prepared with different organic templates, and FER-MORP sample synthesized with morpholine showed the highest DME conversion and methyl acetate space-time yield. The study also revealed that morpholine can enhance the carbonylation activity and suppress the formation of coke species.
Article
Chemistry, Physical
J. Sirijaraensre, J. Limtrakul
APPLIED SURFACE SCIENCE
(2016)
Article
Chemistry, Physical
Patanachai Janthon, Francesc Vines, Jakkapan Sirijaraensre, Jumras Limtrakul, Francesc Illas
JOURNAL OF PHYSICAL CHEMISTRY C
(2017)
Article
Chemistry, Physical
Yuwanda Injongkol, Thana Maihom, Piti Treesukul, Jakkapan Sirijaraensre, Bundet Boekfa, Jumras Limtrakul
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2017)
Article
Chemistry, Multidisciplinary
J. Sirijaraensre, J. Limtrakul
STRUCTURAL CHEMISTRY
(2018)
Article
Chemistry, Physical
Patanachai Janthon, Francesc Vines, Jakkapan Sirijaraensre, Jumras Limtrakul, Francesc Illas
CATALYSIS SCIENCE & TECHNOLOGY
(2017)
Article
Chemistry, Physical
J. Sirijaraensre, P. Khongpracha, J. Limtrakul
APPLIED SURFACE SCIENCE
(2019)
Article
Chemistry, Multidisciplinary
Jakkapan Sirijaraensre
Summary: The sensing properties of paddlewheel-type metal dimers (M-BTC: M = Fe, Ni, Cu, Zn, and Pd) towards SO2 gas were investigated using density functional theory. Among the studied systems, Ni-BTC and Zn-BTC paddlewheels showed the highest sensitivity towards SO2 gas, suggesting their great potential as SO2 sensors.
Article
Engineering, Environmental
Sirapat Munpollasri, Yingyot Poo-arporn, Waleeporn Donphai, Jakkapan Sirijaraensre, Winyoo Sangthong, Sirapassorn Kiatphuengporn, Pongsakorn Jantaratana, Thongthai Witoon, Metta Chareonpanich
Summary: For the first time, the effects of an external magnetic field on metal phase transformation, CO2 conversion, and C-2 + C-3 hydrocarbons selectivity of Fe-Cu/MCM-41 catalysts were investigated using time-resolved X-ray absorption spectroscopy and online quadrupole mass spectrometry. The results showed that the magnetic field stabilized the active forms of FeO and Fe3O4 within the catalysts, leading to increased CO2 conversion and improved concentrations of C-2 + C-3 hydrocarbons.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Physical
Jakkapan Sirijaraensre
Summary: The catalytic performance of palladium atom deposited on the cavity of the g-C3N4 sheet for the formic acid (FA) dehydrogenation was investigated. It was found that the hydrocarboxyl intermediate is the preferable pathway for H2 production. Boron doping enhances the basicity of g-C3N4, leading to stronger interaction between the deposited Pd atom and FA. The reaction mechanism on Pd1/B-doped g-C3N4 proceeds preferentially through the formate pathway.
APPLIED SURFACE SCIENCE
(2022)
Article
Biochemical Research Methods
Winyoo Sangthong, Jakkapan Sirijaraensre
Summary: In this study, density functional theory calculations were used to investigate the cycloaddition reaction of ethylene oxide (EO) with CO2 in the absence of a co-catalyst. The influence of exchanged metals on the adsorption of EO was found to be significant. The proposed reaction mechanism involves the concerted mechanism, with the metals initiating the EO ring opening and the formation of two new C-O bonds between the adsorbed EO and CO2. The Cu-FAU catalyst exhibited the lowest activation energy, which can be attributed to moderate adsorption of EO and larger electron transfer at the transition state.
JOURNAL OF MOLECULAR GRAPHICS & MODELLING
(2022)
Article
Chemistry, Organic
Poomsith Thangsan, Thanya Rukkijakan, Bongkotrat Thanaussavadate, Kanyapat Yiamsawat, Jakkapan Sirijaraensre, Kevin P. P. Gable, Pitak Chuawong
Summary: Alkylphenylacetylene derivatives were synthesized and used in the Larock heteroannulation reaction to investigate the steric influence on regioselectivity. The results showed that large alkyl groups favored the formation of 2-alkyl-3-phenylindole products, while smaller alkyl groups preferred 3-alkyl-2-phenylindole. Various steric parameters, especially Charton values, exhibited good correlations with the regioisomeric product ratios.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Jakkapan Sirijaraensre
Summary: This study used DFT calculations to investigate the adsorption and sensitivity of six M-HITP units (M = Cr, Mn, Fe, Co, Ni, and Cu) as active sensor materials for SO2 gas. The results showed that there were two modes of adsorption on the metal center, namely O-bound and S-bound configurations. Among them, Cr-HITP exhibited significant response to SO2 gas, while the remaining systems were almost insensitive. Therefore, Cr-HITP has great potential in the application of SO2 gas sensors.
Article
Chemistry, Multidisciplinary
Jakkapan Sirijaraensre
NEW JOURNAL OF CHEMISTRY
(2019)
Article
Chemistry, Multidisciplinary
Patipan Charoenwiangnuea, Thana Maihom, Pipat Kongpracha, Jakkapan Sirijaraensre, Jumras Limtrakul
Article
Chemistry, Multidisciplinary
Jakkapan Sirijaraensre
Summary: DFT calculations were used to investigate the structure and electronic properties of bimetallic paddlewheels, revealing the importance of substituted metal in the adsorption of SO and CO2 molecules. Highly exposed Cu active sites in Al-Cu-BTC and Ga-Cu-BTC play a crucial role in activating the SO in the chemical reaction compared to Mg-Cu-BTC and Ca-Cu-BTC nodes.
NEW JOURNAL OF CHEMISTRY
(2021)