Article
Chemistry, Physical
Xiao Kong, Xiao-jie Wei, Lu-ping Li, Zhen Fang, Hanwu Lei
Summary: Aldol condensation of furfural with acetone over basic catalysts produces furanic adducts that can be transformed into diesel fuels. This study synthesized La2O2CO3-promoted ZnO-Al2O3 catalysts with medium strength basic sites, showing improved catalytic performance. The medium strength basic sites were found to be especially active for aldol condensation reactions.
CATALYSIS COMMUNICATIONS
(2021)
Article
Chemistry, Physical
Lu-ping Li, Zhen Fang, Xiao Kong, Wen-Jie Cong
Summary: Efficient La2O2CO3-Al2O3 catalyst was successfully prepared and showed improved catalytic activity in aldol condensation reactions. The catalyst achieved a total conversion of furfural with high yields of F2Ac and FAc at optimal conditions.
MOLECULAR CATALYSIS
(2021)
Article
Chemistry, Applied
Valeriia Korolova, Oleg Kikhtyanin, Evgeniya Grechman, Vincenzo Russo, Johan Warna, Dmitry Yu. Murzin, David Kubicka
Summary: The influence of temperature, furfural to acetone ratio, and catalyst loading on the furfural condensation with acetone over hydrotalcite materials was studied. Concentration profiles showed limiting conversion values depending on the catalyst amounts, and thermodynamic calculations demonstrated the absence of any thermodynamic restrictions, indicating catalyst deactivation, especially at lower catalyst concentrations. Deactivation is more likely to affect the first step of aldol condensation rather than subsequent dehydration. A kinetic model, including catalyst deactivation, was developed and confirmed an adequate description of the experimental data with the advanced model.
Article
Chemistry, Physical
Kempanna S. Kanakikodi, Sathyapal R. Churipard, Rama Bai, Sanjeev P. Maradur
Summary: The study presents a sustainable protocol for the condensation of furfural with acetone over gamma-Al2O3 supported sodium aluminate catalyst, showing excellent conversion and selectivity under mild reaction conditions. The catalytic activity is attributed to the properties of the catalyst, including active sites distribution, specific surface area, and mesoporosity. Comparison with other catalysts shows superior performance, and recycling experiments demonstrate the stability of the catalyst with consistent catalytic activity.
MOLECULAR CATALYSIS
(2021)
Article
Chemistry, Multidisciplinary
Hochan Chang, Ishan Bajaj, Ali Hussain Motagamwala, Arun Somasundaram, George W. Huber, Christos T. Maravelias, James A. Dumesic
Summary: The study demonstrates a method for producing HMF through enzymatic catalysis and chromatographic separation, with chromatographic separation having lower operating costs and minimum selling price compared to extraction. It also shows that the HMF process can be integrated with the HFCS process, and retrofitting existing HFCS facilities is a promising short-term low-risk strategy to advance HMF production technology.
Article
Chemistry, Applied
O. Kikhtyanin, V Korolova, A. Spencer, L. Dubnova, B. Shumeiko, D. Kubicka
Summary: The study shows that the furfural conversion depends on the acidity of the furfural source, and storing freshly distilled furfural may lead to a decrease in its conversion rate. Distillation of furfural can improve the conversion rate for some furfurals in aldol condensation, but careful storage is required to prevent re-oxidation.
Article
Chemistry, Physical
Liyuan Yuan, Mengran Liu, Shanshan Liu, Guoli Fan, Lan Yang, Feng Li
Summary: By tuning the surface acid-base properties of alumina-zirconia composite catalysts, a high catalytic performance in the aldol condensation reaction of furfural with acetone to produce furfurylidene acetone was achieved, with a yield of FAc exceeding 90.0%.
CATALYSIS COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Chuncheng Lin, Jiamin Zhou, Zhangfan Zheng, Jinzhu Chen
Summary: This research demonstrates a highly efficient and convenient strategy for the synthesis of various biomass-based tertiary amines using a rhodium phosphide catalyst. The one-pot reaction achieves excellent yields and offers a sustainable approach to extend amine chemistry.
JOURNAL OF CATALYSIS
(2022)
Article
Thermodynamics
Shanshan Shao, Zian Ye, Chengyue Liu, Xinggang Hu, Jiayuan Sun, Xiaohua Li, Huiyan Zhang, Rui Xiao
Summary: This study explores the production of jet fuel using catalytic pyrolysis products from holocellulose. The integrated process of carbonylation and aldol condensation and hydrogenation achieves high carbon yield and energy density in aviation fuel. The quality of the final oil is also confirmed to meet aviation fuel standards.
ENERGY CONVERSION AND MANAGEMENT
(2022)
Article
Energy & Fuels
Lungang Chen, Yong Liu, Xinghua Zhang, Jianguo Liu, Qi Zhang, Longlong Ma
Summary: A method for converting biomass-derived furfural and levulinic acid into long-chain hydrocarbon fuels was developed. A C20 oxygenate with 95% mol yield was synthesized through condensation-polymerization reactions catalyzed by NaOH. Various techniques were used to verify the chemical structure of the C20 oxygenate. The condensation mixture was then subjected to hydrodeoxygenation reaction using a catalytic system of Pd/C and H3PO4 in aqueous phase, resulting in a 57.1% weight yield of liquid fuel with main products of C12, C14, and C18 hydrocarbons. The carbon and hydrogen mass percent in the fuel were significantly improved to 95.91%, and the high heat value increased to 47.04 MJ/kg.
Article
Chemistry, Multidisciplinary
Changqu Lin, Hao Yang, Xin Gao, Yue Zhuang, Caojian Feng, Hongli Wu, Haifeng Gan, Fei Cao, Ping Wei, Pingkai Ouyang
Summary: In this study, a process for the selective conversion of N-acetyl-D-glucosamine (NAG) into unsubstituted 3-acetamidofuran (3AF) is developed. The yield of 3AF from NAG catalyzed by a ternary Ba-(OH)(2)-H3BO3-NaCl catalytic system in N-methylpyrrolidone at 180 degrees C for 20 min can reach 73.9%. Mechanistic studies reveal that the pathway to 3AF starts with a base-promoted retro-aldol condensation of the ring-opened NAG, affording the key intermediate N-acetylerythrosamine.
Article
Chemistry, Applied
Kun Yuan, Huangxian Zhang, Qiao Sun, Xiaohua Zhang, Dan Hou, Jing Chen, Changxiang Liu, Jinzhu Chen, Wanming Xiong
Summary: By using a series of diimidazole ILs, furfural can be upgraded to furoin effectively. Factors affecting the yield include the solvent composition, the structure of the cation and anion of the ILs. The study suggests that extending the side chain and transforming ethyl group into unsaturated vinyl group can greatly enhance the production yield.
FUEL PROCESSING TECHNOLOGY
(2022)
Article
Chemistry, Multidisciplinary
Bharath Velaga, Nageswara Rao Peela
Summary: A novel, rapid, and green route for levulinic acid (LA) production from bio-derived furfural was developed using a microwave reactor. The process involved hydroxymethylation followed by rehydration and achieved high yields of LA under specific temperature conditions. Microwave heating significantly improved the conversion rate and yield compared to conventional heating. Techno-economic analysis showed that this process could produce LA at a lower cost.
Article
Chemistry, Multidisciplinary
Kun Yuan, Wen Zhao, Yaohong Zhou, Xiaohua Zhang, Shangxing Chen, Jing Chen, Changxiang Liu, Wanming Xiong
Summary: A novel strategy for preparing 1,13-tridecanediol by using furfural was proposed. The catalytic performance of Raney Ni and Pd/TiO2-ZrO2 was investigated, and the synergistic effect of TiO2-ZrO2 and Pd was found to play a crucial role in improving the yield.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Multidisciplinary Sciences
Haifeng Qi, Yurou Li, Zhitong Zhou, Yueqiang Cao, Fei Liu, Weixiang Guan, Leilei Zhang, Xiaoyan Liu, Lin Li, Yang Su, Kathrin Junge, Xuezhi Duan, Matthias Beller, Aiqin Wang, Tao Zhang
Summary: A unique catalyst has been developed to transform bio-based compound furfural into N-heterocyclic piperidine. The catalyst enables efficient synthesis of the desired product under mild conditions via a cascade reaction process.
NATURE COMMUNICATIONS
(2023)
Review
Chemistry, Multidisciplinary
Dmytro Dedovets, Qingyuan Li, Loic Leclercq, Veronique Nardello-Rataj, Jacques Leng, Shuangliang Zhao, Marc Pera-Titus
Summary: This article provides a systematic overview of recent progress in liquid-liquid and gas-liquid dispersions stabilized by solid particles as microreactors for engineering eco-efficient reactions, focusing on biobased reagents. It discusses physicochemical driving parameters, challenges, and strategies for destabilizing/stabilizing dispersions for product recovery/catalyst recycling. Advanced concepts such as cascade and continuous flow reactions, compartmentalization of incompatible reagents, and multiscale computational methods for accelerating particle discovery are also addressed.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Shi Zhang, Dmytro Dedovets, Andong Feng, Kang Wang, Marc Pera-Titus
Summary: Oil foams stabilized by surface-active catalytic particles bearing fluorinated chains and Pd nanoparticles enable fast and efficient aerobic oxidation of various alcohols. The stability of the foam greatly affects the catalytic performance, and the particles can be conveniently recycled.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Andong Feng, Dmytro Dedovets, Shi Zhang, Jin Sha, Renate Schwiedernoch, Jie Gao, Yunjiao Gu, Marc Pera-Titus
Summary: This study unravels the foaming properties of Aquivion(TM) PFSA resin and designs a catalytic foam system for efficient conversion reactions. The foam system shows a significant increase in interfacial area and preferential location of catalytic acid centers, leading to enhanced reaction efficiency.
ADVANCED MATERIALS INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Walid Lamine, Frederic Guegan, Francois Jerome, Gilles Frapper
Summary: This study investigates the reaction mechanism of cellulose depolymerization under non-thermal plasma conditions. The degradation of glycosidic bonds triggered by reaction with hydroxyl radicals is explored. It is found that the hydrogen abstraction reactions by hydroxyl radicals on different sites of the pyranose ring are nonselective and exergonic, resulting in the formation of cellobiosyl carboradicals. These carboradicals protect against direct hydrolysis and a homolytic bond cleavage process allows the desired monomer to be obtained. Through molecular simulation and analysis, three feasible reaction pathways are identified based on their kinetics and thermodynamics.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Pablo G. Argudo, Lea Spitzer, Francois Jerome, Henri Cramail, Luis Camacho, Sebastien Lecommandoux
Summary: Sugar-based amphiphiles are a natural alternative to synthetic ones with biodegradable properties. An investigation of their structure-assembly relationship was conducted using various techniques in aqueous media. The results showed that the average degree of polymerization (DP) and the addition of a hydroxyl group to the hydrophobic tail affected their self-assembly. The critical micelle concentration was more influenced by changes in the hydrophobic molecular region than by variations in (DP) over bar. Amphiphiles with high (DP) over bar formed spherical micelles regardless of the presence of a hydroxyl group, while those with low (DP) over bar and only one hydrophilic moiety formed cylindrical micelles, and the addition of a hydroxyl group to the tail resulted in a spherical shape.
Article
Chemistry, Multidisciplinary
Dmytro Dedovets, Shi Zhang, Jacques Leng, Marc Pera-Titus
Summary: A polydimethylsiloxane-based microfluidic device allows monitoring local oxidation events in organic solvents at the level of an individual air bubble armored with surface-active low-surface energy catalytic particles. This new technique permits tunable design of microreactors for gas-liquid-solid reactions.
ADVANCED MATERIALS INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Anaelle Humblot, Tony Chave, Prince N. Amaniampong, Stephane Streiff, Francois Jerome
Summary: With the progressive defossilization of our industry, hydrogen (H-2) has been identified as a central molecule to store renewable electricity. In this context, ammonia (NH3) is now rapidly emerging as a promising hydrogen carrier for the future. This study demonstrates a novel method of cleaving the N-H bond of NH3 within cavitation bubbles, generated by ultrasonic irradiation, leading to the in situ formation of a diimide, which then catalyzes the hydrogenation of alkenes. This work offers a potential solution for hydrogenation reactions using ammonia directly, without the need for transition metals and with N-2 as the sole co-product.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Biochemistry & Molecular Biology
Somia Haouache, Yu Chen, Clara Jimenez-Saelices, Fabrice Cousin, Pan Chen, Yoshiharu Nishiyama, Francois Jerome, Isabelle Capron
Summary: This study compares the organization of nanocelluloses on oil-water interfaces. Both native and mercerized cellulose nanocrystals form strongly adsorbed layers at the interface, but the layer thickness depends on the concentration. Molecular dynamics simulations show that the migration of nanocelluloses to the interface is spontaneous and irreversible.
Review
Chemistry, Physical
Sophie Hameury, Hana Bensalem, Karine De Oliveira Vigier
Summary: This review provides an overview of the use of Borrowing Hydrogen methodology with bio-based alcohols, highlighting key parameters and remaining scientific hurdles in biomass amination.
Article
Chemistry, Multidisciplinary
Yaoyao Feng, Jean-Francois Dechezelles, Quentin D'Acremont, Emmanuel Courtade, Vincent De Waele, Marc Pera-Titus, Veronique Nardello-Rataj
Summary: In this study, an emulsion system combining plasmonic Au-loaded amphiphilic silica nanoparticles and tri(dodecyltrimethylammonium) phosphotungstate nanoparticles was developed for oxidation reactions at near-room temperature. The system showed a 5-fold increase in activity compared to thermal reactions, with potential energy savings of 74% compared to thermally heated reactors.
Article
Chemistry, Physical
Fan Jiang, Zhen Yan, Xuan Chen, Xinlei Li, Stephane Streiff, M. Pera-Titus
Summary: An alternative non-toxic route for the synthesis of pentamethyldiethylenetriamine using methanol as a greener and cheaper methylating reagent is presented. The reaction proceeds fast and selectively over composite copper catalysts, yielding pentamethyldiethylenetriamine with a yield of 75% and resistance to sintering.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Multidisciplinary
Hang Hu, Muhammad Akif Ramzan, Raphael Wischert, Francois Jerome, Carine Michel, Karine de Oliveira Vigier, Marc Pera-Titus
Summary: The direct amination of biomass-derived isohexides over a Ru/C catalyst showed that the presence of hydrogen gas (H-2) and ammonia gas (NH3) played important roles in the selectivity of isohexide conversion to diamines and aminoalcohols. Isohexides with an exo-OH group formed aminoalcohols, while isohexides with two endo-OH groups produced a moderate yield of diamines due to higher reactivity. The adsorption of NH3 on the catalyst strongly suppressed isomerization of isohexides and discouraged the formation of byproducts promoted by H-2.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Physical
Teseer Bahry, Shang Jiang, Umesh Jonnalagadda, Wen Liu, Benoit Teychene, Francois Jerome, Samir H. Mushrif, Prince N. Amaniampong
Summary: This study presents a novel catalytic chemistry for the demethylenation of benzyl alcohol to phenol using a combination of an earth-abundant transition metal oxide (CuO) catalyst and high frequency ultrasound (HFUS). The reaction takes place in water and at room temperature. By characterizing the catalyst, analyzing the chemistry and acoustics, using isotope labelling and density functional theory computations, the researchers unveil the molecular reaction mechanism, which involves benzaldehyde as an intermediate. Water is not only a benign solvation medium, but also directly participates in the reaction by undergoing dissociation due to sonolysis. The adsorption of the OH from water on the catalyst surface inhibits recombination and activates the C-H bond in benzyl alcohol, leading to the formation of benzaldehyde and its incorporation into the phenyl ring to form phenol.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Chemistry, Physical
Shi Zhang, Dmytro Dedovets, Marc Pera-Titus
Summary: A novel amphiphilic polyhedral oligomeric silsesquioxane (POSS) was synthesized and combined with surface-active catalytic organosilica particles to create a dual particle system capable of generating foam in pure organic solvents. The foamability and foam stability could be adjusted by varying the concentration of POSS. The catalytic activity was significantly enhanced in the aerobic oxidation of pure aromatic alcohols, and the particles could be easily recycled with high foamability for at least 7 consecutive runs.
JOURNAL OF MATERIALS CHEMISTRY A
(2022)
