Article
Chemistry, Physical
Maria Ventura, Jaime Mazario, Marcelo E. Domine
Summary: This study achieved the continuous isomerization of glucose to fructose in aqueous media using a new catalyst based on Ca and Al oxides, showing high conversion and selectivity. The catalyst maintained stable activity during continuous operation and slight deactivation could be overcome by thermal regeneration.
Article
Chemistry, Applied
Tingwei Zhang, Haiying Wei, Rongxin Ling, Yongcan Jin, Huining Xiao, Wenzhi Li, Farzad Seidi
Summary: In this study, silica-tin oxide composites and a H3PO4 modified 20SiSnO were synthesized and evaluated for the catalytic dehydration of glucose to 5-hydroxymethylfurfural. The catalysts showed high efficiency, stability, and recyclability, achieving inspiring yields of HMF. The possible reaction pathways of glucose dehydration over the catalysts were also discussed.
MICROPOROUS AND MESOPOROUS MATERIALS
(2021)
Review
Energy & Fuels
Claudia Prestigiacomo, Martina Biondo, Alessandro Galia, Eric Monflier, Anne Ponchel, Dominique Prevost, Onofrio Scialdone, Sebastien Tilloy, Rudina Bleta
Summary: This study successfully fabricates SnO@gamma-Al2O3 composites with tuneable pore size and well-defined octahedral-shape crystal structure using a molecular-colloidal coassembly approach combined with an ultrasonic-assisted precipitation method. The cooperative action of the supramolecular template and gamma-Al2O3 nanoparticles plays a critical role in the growth and orientation of SnO microcrystals and ultimately determines their catalytic performance in ester exchange reactions.
Article
Chemistry, Physical
Mohamed M. M. Kashbor, Dedi Sutarma, James Railton, Naoko Sano, Peter J. Cumpson, Diego Gianolio, Giannantonio Cibin, Luke Forster, Carmine D'Agostino, Xi Liu, Liwei Chen, Volkan Degirmenci, Marco Conte
Summary: In this study, Sn and Ga doped zeolites supported by zeolite Y were synthesized for the isomerization of glucose to fructose. The materials showed activity in methanol and a reaction pathway involving a hydride shift and a Brunsted acid pathway was proposed. The characterizations confirmed that Sn mainly existed as small SnO2 clusters on the external surface of zeolite, while Ga species were highly dispersed inside the zeolite pores. The catalytic activity appeared to be dominated by Brunsted acid sites.
APPLIED CATALYSIS A-GENERAL
(2022)
Article
Chemistry, Physical
Junyan Fu, Feng Shen, Xiaoning Liu, Xinhua Qi
Summary: In-situ MgO-doped ordered mesoporous carbon (OMC@MgO) was fabricated using a formaldehyde-free self-assembly method, with biomass-derived tannin as the carbon precursor and Mg2+ as the cross-linker and catalyst precursor. The OMC@MgO exhibited well-controlled mesoporous structures, high surface area, and good catalytic activity, achieving a high fructose yield with good selectivity from glucose. It also showed tolerance to high glucose concentrations and maintained recyclability.
GREEN ENERGY & ENVIRONMENT
(2023)
Article
Biochemistry & Molecular Biology
Shuai Wang, Dayi Guo, Rui Kang, Junfeng Feng, Hui Pan
Summary: A series of mesoporous carbon/magnesium oxide composites (LDMC@MgO-x) were synthesized with different Mg doping ratios using alkali lignin as the carbon source, potassium chloride as the salt template, and magnesium nitrate as the catalytic site precursor. The as-prepared LDMC@MgO-x exhibited a unique hierarchical porous structure with high specific surface area, rich functional groups, and uniformly distributed MgO nanoparticles. Among them, LDMC@MgO-20% showed the highest catalytic activity, achieving effective isomerization of glucose to fructose with a maximum yield of 34.4% in water at 130 degrees C for 5 minutes under microwave assistance. The activation energy for glucose isomerization catalyzed by LDMC@MgO-20% was estimated to be 43.6 kJ mol(-1), lower than that of most Lewis acid-catalyzed systems.
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
(2023)
Editorial Material
Chemistry, Multidisciplinary
Pannida Dugkhuntod, Narasiri Maineawklang, Chadatip Rodaum, Peerapol Pornsetmetakul, Kachaporn Saenluang, Saros Salakhum, Chularat Wattanakit
Summary: Various metals have been incorporated into MFI nanosheets successfully, resulting in zeolites with high surface area and mesopore volume. The successful introduction of heteroatoms in the framework has been confirmed by UV-Vis absorbance spectra and XRD peaks shift.
Article
Chemistry, Multidisciplinary
Pannida Dugkhuntod, Narasiri Maineawklang, Chadatip Rodaum, Peerapol Pornsetmetakul, Kachaporn Saenluang, Saros Salakhum, Chularat Wattanakit
Summary: Various metals such as Sn, Ge, and Zr were successfully incorporated into MFI nanosheets, resulting in high external surface area and mesopore volume without large metal oxides aggregated on zeolite surfaces. The XRD peaks shifting indicated the successful introduction of heteroatoms in MFI nanosheets, while UV-Vis absorbance spectra showed the tetrahedral coordination of metal species in the zeolite framework. The SnMFI-NS samples demonstrated outstanding catalytic behavior in fructose selectivity (>85%) due to the high dispersion of metal isomorphous species.
Article
Chemistry, Applied
Yayati Naresh Palai, Abhijit Shrotri, Miyuki Asakawa, Atsushi Fukuoka
Summary: A highly efficient Lewis acid catalyst for the isomerization of glucose to fructose was synthesized by controlling the dispersion of Sn on SBA15. The catalyst exhibited high selectivity and fructose yield, while mechanisms involving condensation of Sn with silanol groups on SBA15 were proposed. Despite deactivation due to byproduct deposition in the third cycle, catalyst activity could be restored by calcination.
Review
Chemistry, Physical
Dmitry Yu. Murzin
Summary: This mini-review addresses the kinetic features of single-site catalysis, including both qualitative and quantitative aspects.
Article
Chemistry, Multidisciplinary
Rahul Gautam, Priyanka Pal, Shunmugavel Saravanamurugan
Summary: The study focuses on incorporating Lewis acidic metal Sn into H-ZSM-5 zeolite through desilication and dealumination to generate mesopores, and investigates its catalytic activity for glucose isomerisation. The Sn(4)ZS(180)A(15) catalyst shows enhanced surface area, mesopore volume, and acidic sites compared to the parent H-Z. DRS-UV-Vis and XPS results confirm the incorporation of Sn into the framework of Sn(4)ZS(180)A(15). The Sn(4)ZS(180)A(15) catalyst exhibits high catalytic activity for glucose isomerisation, while the parent H-Z and Sn-incorporated catalysts without desilication-dealumination process show low activity.
Article
Chemistry, Physical
Luke Forster, Mohamed M. M. Kashbor, James Railton, Sarayute Chansai, Christopher Hardacre, Marco Conte, Carmine D'Agostino
Summary: Sn and Ga doped zeolite Y catalysts were studied for the isomerization of glucose to fructose in different solvents. Ethanol favored a Lewis acid site catalyzed pathway, while methanol resulted in an equal distribution of products. The catalysts were inactive in water due to strong solvent adsorption. The results provide evidence of the importance of solvent adsorption properties in zeolites for glucose to fructose isomerization and may aid in designing and optimizing catalytic systems.
JOURNAL OF CATALYSIS
(2023)
Article
Chemistry, Physical
Mario Chiesa, Elio Giamello
Summary: This perspective paper illustrates the potential of EPR techniques in describing critical features of surface structures and reactivity in the fields of surface chemistry and heterogeneous catalysis. Selected examples covering morphological analysis of surfaces to detailed descriptions of chemical bonding and catalytic sites topology are employed. Lastly, the pros and cons related to acquiring EPR instrumentations in an advanced laboratory of surface chemistry and heterogeneous catalysis are briefly considered.
Article
Green & Sustainable Science & Technology
Wanmai Srisuwanno, Kachaporn Saenluang, Anittha Prasertsab, Saros Salakhum, Pinit Kidkhunthod, Supawadee Namuangruk, Chularat Wattanakit
Summary: In this study, bifunctional hafnium-incorporated zeolite catalysts with fine-tuned acidity and hierarchical features were designed for the direct conversion of glucose to 5-hydroxymethylfurfural (HMF). The catalysts demonstrated excellent catalytic performances in glucose conversion and HMF yield, as well as superior catalytic stability compared to a well-known tin-beta zeolite catalyst. Density functional theory calculations further confirmed the catalytic activity and mechanistic studies of the hafnium-incorporated zeolite catalyst.
ADVANCED SUSTAINABLE SYSTEMS
(2023)
Article
Chemistry, Physical
Luca Botti, Sebastian Meier, Ceri Hammond
Summary: This study investigates the catalytic conversion of glucose using Lewis acidic silicates in a continuous flow reactor with operando UV-vis spectroscopy. Transient absorption features related to glucose activation and conversion at various operational conditions are identified, and the deactivation of the stannosilicate catalyst is shown to affect the overall performance of the glucose upgrading reaction during continuous operation. The study highlights the nonuniform deactivation of the catalyst and its implications for improving the selectivity of catalysts for glucose upgrading.
Article
Materials Science, Ceramics
M. R. Cicconi, R. Belli, M. Brehl, J. Lubauer, T. Hayakawa, K. Kimura, T. Hirota, K. Usui, S. Kohara, Y. Onodera, U. Lohbauer, K. Hayashi, D. de Ligny
Summary: The influence of time and temperature on phase stabilisation, crystal phases evolution, and physical properties of lithium-silicate were studied. The effect of nucleation temperature on mineral assemblage and fracture toughness was observed through reverse-engineering a commercial material. The spatial distribution of structural units influenced the final properties.
JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
(2022)
Article
Materials Science, Ceramics
Jayani Kalahe, Yohei Onodera, Yasuyuki Takimoto, Hiroyuki Hijiya, Madoka Ono, Katsuaki Miyatani, Shinji Kohara, Shingo Urata, Jincheng Du
Summary: This study investigated the effects of various simulation parameters on the short and medium range structures of sodium aluminosilicate glasses using molecular dynamics simulations. It was found that different interatomic potentials have different applicability in studying the glass forming process, with fixed-charge and reactive potentials having their own advantages and disadvantages. Moreover, the results demonstrate that the reactive potential provides reasonable structures consistent with experiments.
JOURNAL OF NON-CRYSTALLINE SOLIDS
(2022)
Article
Chemistry, Physical
Anita Zeidler, Philip S. Salmon, Takeshi Usuki, Shinji Kohara, Henry E. Fischer, Mark Wilson
Summary: The structure of molten NaCl was investigated using neutron and x-ray diffraction along with molecular dynamics simulations. The results showed that the rigid-ion approach matched the simple theory qualitatively, while the polarizable ion approach provided a good account of the diffraction results and agreed with experimental data.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Materials Science, Ceramics
Shinya Hosokawa, Jean-Francois Berar, Nathalie Boudet, Wolf-Christian Pilgrim, Laszlo Pusztai, Satoshi Hiroi, Shinji Kohara, Hidemi Kato, Henry E. Fischer, Anita Zeidler
Summary: By comparing the local structures of metallic glasses with different glass-forming abilities, characteristic features related to high GFA were discovered. The larger concentration inhomogeneity of Ni/Cu in PNCP, the increased fraction of pure icosahedral arrangements, and the presence of the largest intermediate-size Cu rings may contribute to the excellent GFA of PNCP.
JOURNAL OF NON-CRYSTALLINE SOLIDS
(2022)
Article
Chemistry, Multidisciplinary
Atsushi Takagaki, Yuta Tsuji, Tatsuya Yamasaki, Sun Kim, Tetsuya Shishido, Tatsumi Ishihara, Kazunari Yoshizawa
Summary: This study demonstrates the importance of low-temperature activation of methane and its conversion into useful compounds. The researchers found that supported platinum oxide can activate methane near room temperature and selectively produce methanol in the presence of oxygen.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Marie-Louise Saboungi, Oleg Borodin, David L. L. Price, Bela Farago, Miguel A. A. Gonzalez, Shinji Kohara, Lucile Mangin-Thro, Andrew Wildes, Osamu Yamamuro
Summary: A new class of electrolytes, hybridizing aqueous with non-aqueous solvents, has been reported. The structure of an electrolyte composed of a mixture of LiTFSI-water and LiTFSI-dimethyl carbonate was measured using high-energy X-ray diffraction and polarized neutron diffraction. The results were compared with molecular dynamics simulations, which showed good agreement except for the prediction of intense scattering in partially deuterated samples, indicating a partial segregation between the two solvents not observed in experimental measurements.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Akihiko Kudo, Yoshihisa Sakata, Junko N. Kondo, Michikazu Hara, Jun Kubota, Shigeru Ikeda, Tsuyoshi Takata, Ryu Abe, Atsushi Takagaki, Takashi Hisatomi
Summary: Professor Kazunari Domen has focused on the research of catalysis, including the development of various photocatalysts, such as layered oxide and oxynitride photocatalysts, as well as oxysulfide photocatalysts with visible-light response. He has also explored water splitting using mechanocatalysis with metal oxides suspended in distilled water. In addition, Professor Domen has advanced the understanding of catalytic mechanisms through spectroscopic techniques such as transmission infrared spectroscopy and interfacial sum-frequency spectroscopy. Furthermore, he has investigated the use of carbon-based and layered solid acid materials as efficient catalysts.
Article
Chemistry, Physical
I. Tyrone Ghampson, Hiroki Miura, Junichi Murakami, Kyoko K. Bando, Tetsuya Kodaira, Atsushi Takagaki, Tatsumi Ishihara, Tetsuya Shishido
Summary: This study investigates the activation of methane with nitric oxide on Au-Pt nanoparticles supported on alumina. The reaction produces HCN through C-H bond cleavage, NO dissociation, and C-N coupling reactions. The catalysts with different Au/Pt ratios have similar particle morphology and bulk properties but exhibit differences in electronic and geometric surface properties due to Au surface enrichment. The relative proportion of electron-deficient Pt sites on the catalysts' surface correlates with their activity for CH4 conversion and HCN formation.
Review
Instruments & Instrumentation
Leighanne C. C. Gallington, Stephen K. K. Wilke, Shinji Kohara, Chris J. J. Benmore
Summary: The popularity of PDF analysis for X-ray total scattering data has increased as access to ex situ synchrotron data has expanded. There is a growing demand for user-friendly software to extract PDFs accessible to non-experts. This review compares the accuracy of different software in analyzing scattering data, emphasizes the importance of normalization and corrections, and highlights the need to understand competing conventions in defining the PDF.
QUANTUM BEAM SCIENCE
(2023)
Article
Chemistry, Physical
Atsushi Takagaki, Kyoko K. Bando, Tatsuya Yamasaki, Junichi Murakami, Nobuya Suganuma, I. Tyrone Ghampson, Tetsuya Kodaira, Tatsumi Ishihara, Tetsuya Shishido
Summary: Methane (CH4) was converted to hydrogen cyanide (HCN) using a commercial Pt/Al2O3 catalyst with nitric oxide (NO) as an oxidant. The yield of HCN was maintained at 1% after 100 hours at 400°C and increased to 3.2% at 425°C but then decreased rapidly. In situ XAFS and FTIR measurements revealed the presence of Pt-CN species, which correlated with the production of HCN. However, these species continuously accumulated at temperatures above 400°C.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Nobuya Suganuma, I. Tyrone Ghampson, Hiroki Miura, Junichi Murakami, Kyoko K. Bando, Tetsuya Kodaira, Tatsuya Yamasaki, Atsushi Takagaki, Tatsumi Ishihara, Tetsuya Shishido
Summary: Platinum nanoparticles supported on various metal oxides were investigated for the catalytic activation of methane with nitric oxide at low temperatures and atmospheric pressure. The presence of hydrogen cyanide (HCN) was detected only on the (theta + gamma)-Al2O3-supported Pt catalyst. The difference in catalytic behavior for C-N coupling was found to be related to the relative concentrations of adsorbed CHx and NO species.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Materials Science, Multidisciplinary
Philip S. Salmon, Anita Zeidler, Motoki Shiga, Yohei Onodera, Shinji Kohara
Summary: The structure of permanently densified silica glass is investigated using neutron and x-ray diffraction and atomistic models. The focus is on the ordering on an intermediate length scale that originates from the formation of n-rings. The densification process affects this ordering, as evidenced by changes to the first sharp diffraction peak. However, the distribution of ring sizes does not directly influence the form of this peak. Instead, a significant contribution to glass densification is from compaction of the n-rings, which is quantified by the radius of gyration and lifetime of the rings.
Article
Materials Science, Multidisciplinary
Mohammad Kassem, Chris J. J. Benmore, Andrey Tverjanovich, Takeshi Usuki, Maxim Khomenko, Daniele Fontanari, Anton Sokolov, Koji Ohara, Maria Bokova, Shinji Kohara, Eugene Bychkov
Summary: Antimony sesquisulfide Sb2S3 is an outstanding advanced functional material in various rapidly growing applications. The high optical and electric contrast between the crystalline and amorphous states of Sb2S3 is due to the different short and intermediate range order. Substitution with anions (Se) or cations (Bi) can further improve the material's performance.
JOURNAL OF MATERIALS CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Hirokazu Masai, Shinji Kohara, Toru Wakihara, Yuki Shibazaki, Yohei Onodera, Atsunobu Masuno, Sohei Sukenaga, Koji Ohara, Yuki Sakai, Julien Haines, Claire Levelut, Philippe Hebert, Aude Isambert, David A. Keen, Masaki Azuma
Summary: Densified amorphous silica (SiO2) fabricated from siliceous zeolite (SZ) remains permanently densified, unlike densified glassy SiO2 (GS) fabricated by cold compression. The topology of the densified SZ retains the characteristics of crystalline SZ, while the densified GS relaxes to pristine GS after thermal annealing. These findings suggest the possibility of designing new functional amorphous materials by tuning the topology of the initial zeolitic crystalline phases.
COMMUNICATIONS CHEMISTRY
(2023)
Article
Chemistry, Physical
Xiao-Feng Shen, Motonori Watanabe, Jun Tae Song, Atsushi Takagaki, Tatsuki Abe, Keiji Tanaka, Tatsumi Ishihara
Summary: This study investigates the effects of -F position substitution and hydrophobicity optimization on the photocatalytic activity of BODIPY dyes. Experimental and theoretical results show that -F substitution and longer alkyl chains enhance the photocatalytic activity, resulting in higher hydrogen production rate and turnover frequency. This study highlights the importance of -F position substitution and hydrophobicity optimization in enhancing the photocatalytic activity of metal-free organic dyes.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
