Article
Chemistry, Multidisciplinary
Thorben Lenk, Valentin Ruess, Janko Gresch, Uwe Schroeder
Summary: This research investigates the use of various Pd- and Pt-containing electrocatalyst materials for electrochemical ring hydrogenation of aromatic compounds. The focus is on selectivity of the reaction based on the composition of the electrocatalyst, as well as understanding the electrocatalytic activity during repetitive electrode use. Different furanic derivatives are used as starting materials for mechanistic considerations. The study finds that furfural, furfuryl alcohol, and furan show high reactivity in ring hydrogenation reactions, while furoic acid and 2-methyl furan do not exhibit this behavior. Selectivities of up to 15.3% (from furfural) and 33% (from furfuryl alcohol) for tetrahydrofurfuryl alcohol are observed.
Article
Chemistry, Physical
Qiang Deng, Honggen Peng, Zhenzhen Yang, Tao Wang, Jun Wang, Zheling Zeng, Sheng Dai
Summary: Developing a powerful bifunctional catalyst is crucial for achieving future carbon neutrality by reducing energy consumption in the chemical industry. This study synthesizes mesoporous zeolite-encapsulated palladium nanoparticles (Pd@meso-ZSM-5) using emulsification-demulsification and dry-gel transformation methods, which exhibit remarkable catalytic performance in the one-pot multiple tandem reaction of cyclic ketones to bicyclic alkanes. Unlike traditional two-step synthesis routes, Pd@meso-ZSM-5 efficiently produces bicyclic alkanes instead of monocyclic alkanes, due to the sufficient space for large molecular intermediates provided by mesoporosity and the promoting effect of the acid-Pd interface on intermediate conversion.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Agricultural Engineering
Song Li, Lele Jin, Haiyong Wang, Xiangqian Wei, Wenzhi Li, Qiying Liu, Xinghua Zhang, Lungang Chen, Longlong Ma, Qi Zhang
Summary: In this study, WOx-decorated catalyst was used to selectively convert microcrystalline cellulose into C-6 alkanes via cellulose hydrolysis, glucose hydrogenation, and sorbitol hydrodeoxygenation. The coupling of WOx and Ir enhanced the catalytic performance by improving hydrogenation and deoxygenation reactions. The interaction between WOx and Ir facilitated electron transfer and improved the reduction capability of Ir and activation of C-O bonds on reduced WOx, resulting in higher yields of C-6 alkanes.
BIORESOURCE TECHNOLOGY
(2022)
Article
Energy & Fuels
Majid Saidi, Pantea Moradi
Summary: The kinetic study of upgrading anisole to jet-grade fuels via catalytic hydrotreatment process reveals that benzene is formed as the primary product through demethoxylation of anisole, with phenol showing the highest selectivity and activation energy in the hydrogenolysis reaction. The comprehensive quantitative reaction network for anisole catalytic hydrotreatment over Cu/gamma-Al2O3 catalyst is consistent with previous studies.
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
(2021)
Article
Chemistry, Multidisciplinary
Tan Li, Jing Su, Linjia Yin, Xiangkun Zhang, Cong Wang, Xinbao Li, Jing Zhang, Kaige Wang
Summary: A Cu-based catalyst was successfully used for the one-step solvent-free synthesis of aviation biofuel from biomass-derived ketones. The catalyst showed high conversion rates and selectivity under optimal conditions, with the synergistic effect of Cu-0 and Cu+ enhancing the formation of the biofuel.
Article
Energy & Fuels
Jin-Xuan Xie, Jing-Pei Cao, Xiao-Yan Zhao, Wei Jiang, Liang Zhao, Ming Zhao, Hong-Cun Bai
Summary: Selective cleavage of C-O bonds in diphenyl ether (DPE), a lignin-derived 4-O-5 linkage, is a challenging topic and of great significance to produce value-added aromatic products for sustainable future. Activated carbon (AC) with different pore structures has different catalytic effects on the reaction. Ni catalysts supported on AC with higher specific surface area and stronger hydrophilicity showed higher catalytic activity in the hydrogenolysis and hydrolysis of DPE.
Article
Chemistry, Multidisciplinary
Fang Lin, Ho-Yin Tse, Hanno C. Erythropel, Predrag Petrovic, Mahlet Garedew, Jinshan Chen, Jason Chun-Ho Lam, Paul T. Anastas
Summary: This study reports a highly selective electrochemical method for the cleavage of benzylic C-O bond in lignin model compounds at room temperature and ambient pressure. Using nickel ions as catalysts in the presence of water molecules, benzyl phenyl ether (BPE) can be converted to toluene and phenol in methanol with high yields.
Article
Energy & Fuels
Wahiba Bendeddouche, Sumeya Bedrane, Asma Zitouni, Redouane Bachir
Summary: Research on eco-responsible energy systems is essential, with biofuels being an interesting way to reduce air pollution. This paper focused on the transformation of lignocellulosic biomass derivative furfural acetone furfural into Jet and Diesel biofuel using ruthenium catalysts supported on silica-alumina. The reaction pathway and products were identified using various characterization techniques.
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
(2021)
Article
Chemistry, Applied
Xiangchen Kong, Chao Liu, Weicong Xu, Yue Han, Yuyang Fan, Ming Lei, Ming Li, Rui Xiao
Summary: This study investigates the depolymerization of stubborn lignin (SL) using Cu/CuMgAlOx catalyst in supercritical methanol, achieving a monomer yield of 37.76% with cyclohexanols identified as the major products. Various analytical techniques confirm the depolymerization of SL and upgrading of its derivatives. Computational determinations of activation energies, chemisorption energies, and bond dissociation energies support the experimental results, providing insights into the cleavage of stubborn linkages within SL.
FUEL PROCESSING TECHNOLOGY
(2021)
Article
Chemistry, Multidisciplinary
Akalanka Tennakoon, Xun Wu, Max Meirow, Daniel Howell, Jarod Willmon, Jiaqi Yu, Jessica V. Lamb, Massimiliano Delferro, Erik Luijten, Wenyu Huang, Aaron D. Sadow
Summary: By embedding active platinum nanoparticles between linear, hexagonal mesoporous silica and gyroidal cubic MCM-48 silica, the new catalyst design emphasizes the pore effect and selectively deconstructs polyolefins into valuable hydrocarbon chains while generating minimal volatile byproducts, including methane.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Energy & Fuels
Majid Saidi, Pantea Moradi
Summary: Recently, there has been a growing focus on the valorization of lignin biomass derived pyrolysis bio-oil to produce a sustainable fuel. Hydrodeoxygenation (HDO) is found to be the most suitable process for generating a high heating value fuel. In this study, the HDO of 4-methylanisole, a model compound of pyrolysis oil, was investigated using a Mo/nano & gamma;-Al2O3 catalyst under a wide range of operating conditions. The main reaction pathways during the upgrading process were identified as hydrogenation, hydrogenolysis of Caliphatic-O, dehydration, deoxygenation of Caromatic-O, alkylation, and tautomerization, which influenced the selectivity of the products.
CHEMICAL ENGINEERING AND PROCESSING-PROCESS INTENSIFICATION
(2023)
Review
Chemistry, Physical
Jingwen Tan, Mei Jiang, Kun Yu, Yuyang Song, Wenbiao Zhang, Qingsheng Gao
Summary: The electrochemical upgradation of biomass feedstock is important for achieving carbon cycle without high-grade heat sources. Notably, Cu-based catalysts enable efficient and selective conversion of furanic molecules through electrochemical hydrogenation and oxidation. This review provides insights into the electrochemical processes and discusses the achievements in catalytic performance, mechanism, and electronic efficiency improvement. Future developments in electrocatalysts and electrolysis techniques are also anticipated.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Shuya Zhang, Xiaochen Liu, Yuanjie Xu, Yu Tang
Summary: This study investigates the production of methane from biomass molecules using hydrogenation techniques. The results show that reaction temperature and the type of nickel catalyst used significantly impact the hydrogenation pathways, with a shift towards hydrodeoxygenation at higher temperatures.
Article
Agricultural Engineering
Yong Liu, Lungang Chen, Yubao Chen, Xinghua Zhang, Jianguo Liu, Qiying Liu, Yuping Li, Chenguang Wang, Qi Zhang, Longlong Ma
Summary: Aviation fuel, a high energy density fuel, is typically produced from refineries in the petroleum industry. The production of renewable aviation fuel from biomass helps alleviate the pressure of carbon emission regulations. This study utilized various operational processes to convert biomass, specifically corn stover, into aviation fuel. The resulting fuel has a low oxygen content, high heat value, and consists mainly of isoparaffins.
BIORESOURCE TECHNOLOGY
(2023)
Article
Energy & Fuels
Cunhao Cui, Xinghua Liu, Chaoqun Zhou, Chunjiang Liu, Zhongyue Zhou, Fei Qi
Summary: By combining an autoclave with online soft photoionization mass spectrometry, this study successfully investigated the catalytic reaction evolution under different hydrogen pressures, providing a new approach to better understand the upgrading process of bio-oil.
Article
Chemistry, Physical
Yoshinao Nakagawa, Hiroki Hayasaka, Takehiro Asano, Masazumi Tamura, Kazu Okumura, Keiichi Tomishige
Summary: The direct synthesis of dioctyl ether by catalytic reduction was investigated using different supported catalysts. The combination of Pd with W on a rutile TiO2 support showed the highest yield of dioctyl ether. The catalytic activity depended on the W loading amount, and a high coverage of W was necessary for good yield. The deactivated catalyst showed no significant difference in characterization compared to the fresh one.
MOLECULAR CATALYSIS
(2022)
Article
Chemistry, Physical
Yo-hei Nagasaki, Masazumi Tamura, Mizuho Yabushita, Yoshinao Nakagawa, Keiichi Tomishige
Summary: The silica-supported molybdenum oxide catalyst showed high efficiency and reusability in the dehydration of various amides. The results of catalyst characterizations and activity tests revealed that the strong acid sites formed by the interaction between silanol groups and molybdenum oxide species, along with the acid-base pair sites, played a crucial role in the dehydration reaction.
Article
Chemistry, Applied
Mii Betchaku, Yoshinao Nakagawa, Masazumi Tamura, Mizuho Yabushita, Yasutomo Miura, Shinya Iida, Keiichi Tomishige
Summary: In toluene reforming, adding a small amount of Rh noble metal can enhance the startability of Ni-Fe/Mg/Al catalyst. Physical mixing of Rh/CeO2 and Ni-Fe/Mg/Al powders results in higher activity, while direct addition of Rh to Ni-Fe/Mg/Al performs less effectively.
FUEL PROCESSING TECHNOLOGY
(2022)
Article
Chemistry, Physical
Ben Liu, Yoshinao Nakagawa, Congcong Li, Mizuho Yabushita, Keiichi Tomishige
Summary: In this study, a regioselective catalyst was developed for the hydrogenolysis of 1,2-butanediol (1,2-BuD) to produce 2-butanol (2-BuOH) from biomass. The addition of iron to the catalyst improved both the activity and selectivity, and the reusability of the catalyst was enhanced through optimization of the preparation method. The catalyst showed high selectivity not only in the hydrogenolysis of 1,2-BuD, but also in the hydrogenolysis of other related alcohols.
Article
Chemistry, Physical
Ryotaro Fujii, Mizuho Yabushita, Daiki Asada, Masazumi Tamura, Yoshinao Nakagawa, Atsushi Takahashi, Akira Nakayama, Keiichi Tomishige
Summary: The synthesis of 2-imidazolidinone (EU) from ethylenediamine carbamate (EDA-CA) using a fixed-bed flow reactor was investigated. CeO2 and EDA were used as the heterogeneous catalyst and reaction solvent, respectively. The flow reaction demonstrated higher selectivity and yield of EU compared to the previous batch system.
Article
Chemistry, Physical
Koki Hashimoto, Kosuke Hatakeyama, Mizuho Yabushita, Keiichi Tomishige, Yoshinao Nakagawa
Summary: The oxidation of 2-hydroxycyclohexanone (2-HCO) using heteropolyacids and oxygen as catalysts and oxidant, respectively, was studied. 2-Hydroxyadipic acid (2-HAA) was obtained in moderate yields, with H4PVW11O40 giving the highest yield (39%). This is the first report of the production of 2-HAA by catalytic oxidation reactions. The oxidation of 1,2-cyclohexanedione (CHDO), a potential intermediate of 2-HCO oxidation, also produced similar yields of 2-HAA even without catalyst. The effects of catalyst amount, oxygen pressure, and the addition of radical scavenger on the 2-HCO oxidation were similar to a related case of 2-methoxycyclohexanone oxidation to adipic acid.
Article
Chemistry, Physical
Ben Liu, Yoshinao Nakagawa, Mizuho Yabushita, Keiichi Tomishige
Summary: This study investigated the hydrogenolysis of 1, 2-diols to primary and secondary alcohols using Ir-FeOx catalysts supported on nonoxides. It was found that BN effectively supported the hydrogenolysis of 1, 2-butanediol to produce 2-butanol, similar to previous findings with rutile TiO2. The addition of Fe species to Ir/BN greatly enhanced catalytic activity, while other supports, such as carbon, mainly produced primary alcohols.
Article
Chemistry, Multidisciplinary
Wen Sun, Peilang Li, Mizuho Yabushita, Yoshinao Nakagawa, Yuqi Wang, Akira Nakayama, Keiichi Tomishige
Summary: This study compared the performance of 2-cyanopyridine and 2-furonitrile in the CeO2-catalyzed synthesis of dialkyl carbonates. The results showed that 2-furonitrile performed better in the synthesis of dialkyl carbonates from bulky or long-chain alcohols compared to 2-cyanopyridine, due to its weaker interaction with the CeO2 surface.
Article
Chemistry, Physical
Ryotaro Fujii, Mizuho Yabushita, Yingai Li, Yoshinao Nakagawa, Keiichi Tomishige
Summary: In this study, Mn-doped CeO2 was found to be a more stable catalyst than pure CeO2 in the flow synthesis of 2-imidazolidinone without gas-phase CO2. The improved stability of Mn-doped CeO2 was attributed to its lower deactivation rate constant and decreased density of acid sites.
Review
Chemistry, Organic
Yoshinao Nakagawa, Mizuho Yabushita, Keiichi Tomishige
Summary: This review explores oxidative carbon-carbon cleavage reactions of non-aromatic oxygenates, focusing on the use of excess base and metal catalysts as well as vanadium as a key component of acidic catalysts. It also highlights recent findings in carbon-carbon dissociation reactions of 1,2-difunctionalized compounds and emphasizes the importance of selective cleavage of bonds between functionalized carbon atoms for the production of useful carboxylic acids or diacids. Overall, this research is valuable for its potential in the valorization of biomass.
ASIAN JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Tao Chang, Mizuho Yabushita, Yoshinao Nakagawa, Norihisa Fukaya, Jun-Chul Choi, Takayoshi Mishima, Seiji Matsumoto, Satoshi Hamura, Keiichi Tomishige
Summary: 2,2-diethoxypropane (DEP) and H-FAU were found to function as an effective dehydrating system to accelerate the synthesis of diethyl carbonate (DEC). A detailed kinetic study and DRIFT spectroscopy revealed that an ethyl carbonate species is formed on the CeO2 surface, while DEP is adsorbed and activated on the H-FAU surface. Additionally, ethanol acts as another ethoxy source in the DEC synthesis.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Ryu Hosaka, Daiki Asada, Ji Cao, Masazumi Tamura, Yoshinao Nakagawa, Keiichi Tomishige, Jun-ya Hasegawa, Akira Nakayama
Summary: The detailed structures of monomeric ReOx catalysts supported on CeO2 surface and the reaction mechanism of the deoxydehydration (DODH) reaction were investigated using density functional theory calculations. The stable structure under experimental conditions was determined to be ReVIIO2 species, and an oxygen vacancy-assisted mechanism was proposed as the most plausible pathway for the reaction.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Review
Chemistry, Multidisciplinary
Keiichi Tomishige, Mizuho Yabushita, Ji Cao, Yoshinao Nakagawa
Summary: Biomass valorization is a sustainable method for increasing the value of chemicals. This review introduces potential biomass platform chemicals and summarizes various catalytic systems for their hydrodeoxygenation.
Article
Chemistry, Organic
Masazumi Tamura, Kohei Yugeta, Yoshinao Nakagawa, Keiichi Tomishige
Summary: SiO2-supported bimetallic Mo and Pt demonstrated high efficiency in hydrogenation of n-octanoic acid at a low temperature in the absence of solvent. Characterization of the catalyst revealed that the MoPt alloy formed by high-temperature reduction was the active site for the reaction.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2022)
Article
Chemistry, Physical
Jia-qi Bai, Masazumi Tamura, Yoshinao Nakagawa, Keiichi Tomishige
Summary: SiO2-supported Ni-Ir alloy is an effective heterogeneous catalyst for the hydrogenation of pyridine, showing high activity and selectivity.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Correction
Chemistry, Applied
Jia Liu, Juntong Dong, Xiaodan Li, Teng Xu, Zhenguo Li, Jeffrey Dankwa Ampah, Mubasher Ikram, Shihai Zhang, Chao Jin, Zhenlong Geng, Tianyun Sun, Haifeng Liu
FUEL PROCESSING TECHNOLOGY
(2024)
Article
Chemistry, Applied
Seba Alareeqi, Daniel Bahamon, Kyriaki Polychronopoulou, Lourdes F. Vega
Summary: This study explores the potential application of single-atom-alloy (SAA) catalysts in bio-oils hydrodeoxygenation refining using density functional theory (DFT) and microkinetic modeling. It establishes the relationships between stability, adsorptive properties, and activity structures for bio-oil derivatives, providing guidance for the synthesis of cost-effective SAA combinations.
FUEL PROCESSING TECHNOLOGY
(2024)
Article
Chemistry, Applied
Bin Hu, Wen -Ming Zhang, Xue-Wen Guo, Ji Liu, Xiao Yang, Qiang Lu
Summary: This study explored the pyrolysis behaviors and mechanisms of different monosaccharides, including arabinose, galactose, galacturonic acid, and glucuronic acid. The roles of structural differences in these monosaccharides were analyzed, and it was found that glucuronic acid undergoes a special C-C bond breaking reaction during pyrolysis. The findings provide a deep understanding of the pyrolysis chemistry of hemicellulose and the role of different branches.
FUEL PROCESSING TECHNOLOGY
(2024)
Review
Chemistry, Applied
Youwei Zhi, Donghai Xu, Guanyu Jiang, Wanpeng Yang, Zhilin Chen, Peigao Duan, Jie Zhang
Summary: Hydrothermal carbonization (HTC) is an effective method for the harmless disposal of municipal sludge (MS) and offers potential applications for the obtained products. Optimizing reaction conditions, coupling with other waste materials, and combining different processes can improve the performance of HTC. Furthermore, HTC contributes to energy recovery and enhances the quality of life cycle assessment.
FUEL PROCESSING TECHNOLOGY
(2024)
Article
Chemistry, Applied
Jia Wang, Jianchun Jiang, Dongxian Li, Xianzhi Meng, Arthur J. Ragauskas
Summary: This study presents a scalable process for converting holocellulose and cellulosic wastes into advanced oxygen-containing biofuels with high furan, cyclic ketone, and ethanol content. By combining hydropyrolysis and vapor-phase hydrodeoxygenation using Pd/Al2O3 as a catalyst, the researchers achieved high yields and conversions. The integrated process holds great promise for biomass waste conversion into advanced biofuels.
FUEL PROCESSING TECHNOLOGY
(2024)
Article
Chemistry, Applied
Florian Held, Jannis Reusch, Steffen Salenbauch, Christian Hasse
Summary: The accurate prediction and assessment of soot emissions in internal combustion engines are crucial for the development of sustainable powertrains. This study presents a detailed quadrature-based method of moments (QMOM) soot model coupled with a state-of-the-art flow solver for the simulation of gasoline engines. The model accurately describes the entire cause-and-effect chain of soot formation, growth and oxidation. Experimental validation and engine cycle simulations are used to identify the root cause of observed soot formation hotspots.
FUEL PROCESSING TECHNOLOGY
(2024)
