Review
Biochemistry & Molecular Biology
Leonid V. V. Romashov, Fedor A. A. Kucherov, Kirill S. S. Kozlov, Valentine P. P. Ananikov
Summary: The conversion of biomass to C6 furanic compounds is a sustainable technology with high renewable energy utilization efficiency and minimal environmental pollution. This review focuses on naturally occurring substances containing C6 furanic cores and covers the diversity, occurrence, properties, and synthesis of C6 furanic derivatives.
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
(2023)
Review
Chemistry, Multidisciplinary
Wenting Fang, Anders Riisager
Summary: Catalytic transfer hydrogenation/hydrogenolysis is an economically and environmentally friendly method to valorize renewable compounds derived from biomass. This review focuses on recent progress made on important carbohydrate-derived furanic platform chemicals, highlighting catalyst developments and mechanism explanations. Understanding these features can guide the selection of suitable catalysts for specific transformations, improving the selectivity and yield of products.
Article
Chemistry, Physical
Qing-Shan Kong, Xing-Long Li, Hong-Bo Shen, Hua-Jian Xu, Yao Fu
Summary: This study presents an eco-friendly and efficient heterogeneous sodium-doped porous sodium manganese oxide catalyst for the oxidative cleavage of furanic 1,2-diols into medium-chain furanic aldehyde compounds. Various high value-added chemicals were synthesized using this catalytic approach, demonstrating its broad applicability and high selectivity.
GREEN ENERGY & ENVIRONMENT
(2022)
Review
Chemistry, Physical
Ning Li, Min-Hua Zong
Summary: This review summarizes the recent advances in (chemo)biocatalytic conversion of biobased furans, focusing on various reaction types and catalytic mechanisms. The study highlights biocatalyst engineering and reaction engineering strategies to enhance efficiency and drive the development of these processes.
Review
Chemistry, Physical
Chen Li, Jiang Li, Ling Qin, Piaoping Yang, Dionisios G. Vlachos
Summary: This review systematically summarizes recent advances in photocatalytic biomass conversion and the combination of photooxidation with the hydrogen evolution reaction. By investigating the redox potential of photocatalysis, designing more effective catalysts, and broadening reaction types, real industrial production can be achieved. A bright future is foreseen based on explosive reports and numerous promising research topics.
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
Agricultural Engineering
Zhuqian Xiao, Jiajie Li, Hongpeng Wang, Qing Ge, Chuang Xing, Jun Huang, Jianbing Ji, Jianwei Mao
Summary: In this study, a facile method using mechanical force was developed to fabricate a nonmodel supported catalyst with the assistance of chitosan. By applying shear force and plastic deformations, metal precursors were anchored in situ in the chitosan matrix. The resulting catalyst exhibited high catalytic activity and stability in the hydrolysis reaction, indicating its potential for large-scale production.
BIOMASS & BIOENERGY
(2023)
Review
Chemistry, Physical
Hamidreza Arandiyan, Putla Sudarsanam, Suresh K. Bhargava, Adam F. Lee, Karen Wilson
Summary: Biomass is a renewable energy source that is being increasingly utilized due to concerns about climate change caused by fossil fuel consumption. Waste biomass-derived fuels and chemicals offer a solution to reduce reliance on fossil fuels and achieve "Net Zero 2050 CO2 emissions" with environmental, health, and economic benefits. This review focuses on the use of perovskite oxide catalysts for biomass valorization, discussing their structure-reactivity relationships in various reactions. The study highlights the prospects and challenges for the broader application of perovskite oxide catalysts in biomass valorization.
Review
Chemistry, Applied
Lijuan Zhang, Thuppati U. Rao, Jingyi Wang, Dezhang Ren, Suchada Sirisommboonchai, Cheolyong Choi, Hiroshi Machida, Zhibao Huo, Koyo Norinaga
Summary: Research on biomass hydrogenation improves the efficiency of producing high-value chemicals and provides insights into utilizing raw constituents effectively.
FUEL PROCESSING TECHNOLOGY
(2022)
Review
Chemistry, Multidisciplinary
Wenjuan Sun, Haifeng Li, Xiaochen Wang, Anqiu Liu
Summary: Biomass feedstocks are promising candidates of renewable clean energy, and the development and utilization of biomass is in line with the concept of sustainable development and circular economy. Catalysts with appropriate acid-base sites play a crucial role in the efficient synthesis of gamma-valerolactone (GVL) from furfural (FF). In this Mini Review, the research progress of Zr/Hf-based catalysts in the catalytic synthesis of GVL from FF was discussed, focusing on the effects of Lewis acid-base and Bronsted acid sites in the catalysts, as well as the regulation of acid-base sites in the catalysts. The advantages and challenges of Zr/Hf-based catalysts in the FF to GVL system were also proposed.
FRONTIERS IN CHEMISTRY
(2022)
Review
Chemistry, Multidisciplinary
Nathanael C. Ramos, Marc Manye Ibanez, Rupali Mittal, Michael J. Janik, Adam Holewinski
Summary: Despite the challenges in decarbonizing certain industries, renewable carbon can be a promising solution for the synthesis of critical fuels, chemicals, and materials. Biomass, as a renewable carbon source, can capture atmospheric CO2 and undergo chemical transformations to produce valuable final products.
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Article
Chemistry, Physical
Canshuo Gu, Lungang Chen, Yong Liu, Xinghua Zhang, Jianguo Liu, Qi Zhang, Chenguang Wang, Longlong Ma
Summary: The production of furanic biofuel 2-methyltetrahydrofuran (2-MTHF) from biomass-derived levulinic acid (LA) was studied using a bimetallic NiCo/gamma-Al2O3 catalyst. The catalyst with optimal Ni and Co content exhibited high activity, leading to a 73.4% yield of 2-MTHF. Multiple characterizations were performed to evaluate the catalyst properties, and their relationships with 2-MTHF yields were revealed. Additionally, the solvent effect on the conversion of 1,4-pentanediol to 2-MTHF was investigated using molecular dynamics simulations.
MOLECULAR CATALYSIS
(2022)
Article
Polymer Science
Byounghyun Kim, Juhyen Lee, Han Yong Bae, Seung Uk Son, Changsik Song
Summary: A facile synthetic pathway for phthalimide derivatives from biomass-derived furan has been developed in this study, which can generate phthalimides with unique properties such as supramolecular gels formation and sensing abilities for anions.
MACROMOLECULAR RAPID COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Harilal Krishna, Moritz O. Haus, Regina Palkovits
Summary: The gas-phase dehydration of biomass-derived N-(2-hydroxyethyl)-2-pyrrolidone using Na2O/SiO2-type catalysts offers a promising route to producing high-value polyvinylpyrrolidone. Through optimization of the catalysts and in-depth characterization, it was found that the activity of the catalyst is influenced by a balance between weak basic sites and surface hydroxyls, with the optimal synthesis procedure depending on the type of parent silica. This renewed understanding has expanded the application of Na2O/SiO2 materials to the dehydration of other biomass-derived chemicals in the polymer industry.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2021)
Article
Chemistry, Physical
Bin Chen, Zining Zhou, Yuze Li, Kok Bing Tan, Youting Wang, Xiaoping Rao, Jiale Huang, Xiaodong Zhang, Qingbiao Li, Guowu Zhan
Summary: In this study, biomass-derived activated carbon (bio-AC) was synthesized using rice husk as a biotemplate and carbon source. The immobilization of Ni on bio-AC resulted in a highly efficient catalyst for the pyrolysis of fatty acids to paraffin-based biodiesel under H2-free and solvent-free conditions. The N-doped Ni/bio-AC catalyst showed enhanced olefin selectivity due to the inhibition of -COO* dissociation. This research also investigated the catalytic reaction pathways and achieved efficient conversions of plant oils to biofuels and chemicals using Ni/bio-NAC catalysts.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Multidisciplinary
Estefania Bello-Jurado, Daniel Schwalbe-Koda, Mathias Nero, Cecilia Paris, Toni Uusimaki, Yuriy Roman-Leshkov, Avelino Corma, Tom Willhammar, Rafael Gomez-Bombarelli, Manuel Moliner
Summary: A novel methodology based on high-throughput simulations has been developed to design unique biselective organic structure-directing agents (OSDAs) that enable the efficient synthesis of CHA/AEI zeolite intergrowth materials with controlled phase compositions. These materials exhibit outstanding catalytic performance and hydrothermal stability, surpassing even the performance of commercial CHA-type catalysts. This methodology opens up possibilities for synthesizing new zeolite intergrowth materials with more complex structures and unique catalytic properties.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Beatriz Hurtado, Karen S. Arias, Maria J. Climent, Patricia Concepcion, Avelino Corma, Sara Iborra
Summary: In this study, efficient energy conversion of 5-hydroxymethylfurfural (HMF) to 3-hydroxymethylcyclopentylamine was achieved. Platinum-iron (Pt-Factor) nanoparticles were prepared and utilized as catalysts, demonstrating high efficiency in electrochemical CO2 reduction for energy conversion. The unique surface structure and electron modulation effects of Pt-Factor nanoparticles contributed to the efficient conversion of CO2. Additionally, Pt-Factor nanoparticles exhibited excellent resistance to CO2 ionization, prolonging the lifespan of the energy storage system.
Article
Chemistry, Multidisciplinary
Davide Salusso, Silvia Mauri, Gabriele Deplano, Piero Torelli, Silvia Bordiga, Sergio Rojas-Buzo
Summary: The development of Ce-based materials relies on catalyst surface defects caused by calcination for increased structural stability, and the study of cerium's redox properties under reaction conditions is of growing importance. This study presents a simple and cost-effective method for synthesizing homogeneous and stable CeO2 and CeZrOx nanocrystals through the synthesis and subsequent calcination of Ce-UiO-66 and CeZr-UiO-66. The Ce3+/Ce4+ redox properties were investigated using H-2-TPR experiments, in situ FT-IR, and Ce M-5-edge AP-NEXAFS spectroscopy.
Article
Chemistry, Multidisciplinary
S. Rojas-Buzo, D. Salusso, F. Bonino, M. C. Paganini, S. Bordiga
Summary: In this study, Ce3+ presence and formation in Ce-based UiO-66 Metal-Organic Framework (MOF) were investigated using various characterization techniques. The results showed that EPR, UV-Vis, and NEXAFS spectroscopies revealed the conversion between Ce4+ and Ce3+ during sample dehydration. It was also found that the MOF structure remained intact during water loss and radiation, and the oxidation state of Ce was directly related to the water content, providing a new approach for the synthesis and non-invasive characterization of stable and active MOFs. Additionally, laboratory measurements considerations were used to study Ce3+ formation in Zr-doped UiO-66(Ce) samples.
MATERIALS TODAY CHEMISTRY
(2023)
Article
Chemistry, Applied
Cristina Martinez, Alejandro Vidal-Moya, Bilge Yilmaz, C. P. Kelkar, Avelino Corma
Summary: Fluidized Catalytic cracking (FCC) is a main conversion process in refineries, using Y zeolite as the main source of activity and selectivity. A new Y zeolite catalyst, Phinesse(TM), based on partial substitution of RE by P, has been developed and shown to have similar performance to the conventional RE stabilized counterpart. The hydrothermal stability of different USYs with different dealumination degrees, containing P or La alone or a combination of both stabilizing elements, was compared. The results provide insights into the benefits of P-La stabilization observed in the commercial PhinesseTM catalyst.
Review
Chemistry, Multidisciplinary
Lichen Liu, Avelino Corma
Summary: This review discusses the structure, synthesis, and catalytic applications of heterogeneous bimetallic catalysts, including binuclear sites, nanoclusters, and nanoparticles. Recent progress in the field of bimetallic catalysts is highlighted, along with the future research directions and prospects in both fundamental and practical aspects of heterogeneous catalysis.
Article
Multidisciplinary Sciences
Pau Ferri, Chengeng Li, Daniel Schwalbe-Koda, Mingrou Xie, Manuel Moliner, Rafael Gomez-Bombarelli, Mercedes Boronat, Avelino Corma
Summary: Approaching the level of molecular recognition of enzymes with solid catalysts is a challenging goal, achieved in this work for the competing transalkylation and disproportionation of diethylbenzene catalyzed by acid zeolites. The key diaryl intermediates for the two competing reactions only differ in the number of ethyl substituents in the aromatic rings, and therefore finding a selective zeolite able to recognize this subtle difference requires an accurate balance of the stabilization of reaction intermediates and transition states inside the zeolite microporous voids.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Risheng Bai, Guangyuan He, Lin Li, Tianjun Zhang, Junyan Li, Xingxing Wang, Xiumei Wang, Yongcun Zou, Donghai Mei, Avelino Corma, Jihong Yu
Summary: In this work, a carbonization-reduction method was used to create palladium carbide subnanometric species within pure silicate MFI zeolite. The developed catalyst showed superior performance in the selective hydrogenation of alkynes.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Multidisciplinary
Elena Groppo, Sergio Rojas-Buzo, Silvia Bordiga
Summary: Operando IR spectroscopy is a crucial characterization method for studying heterogeneous catalysts under reaction conditions. This review emphasizes the importance of IR spectroscopy by discussing selected case studies that demonstrate its ability to provide relevant information in this field.
Article
Chemistry, Physical
Francisco Gonell, Miriam Rodenes, Santiago Martin, Mercedes Boronat, Ivan Sorribes, Avelino Corma
Summary: Developing precious-metal-free electrocatalysts for the hydrogen evolution reaction (HER) is crucial. Amorphous molybdenum sulfide-based materials provide highly active HER electrocatalysts by introducing active sites at both the edge positions and the typically inactive basal planes. The bottom-up synthesis using molecular complexes with Mo3S4 and Mo3S7 cluster cores enhances the HER activity and allows the modification of the derived materials with atomic-scale precision.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Sergio Rojas-Buzo, Benjamin Bohigues, Davide Salusso, Avelino Corma, Manuel Moliner, Silvia Bordiga
Summary: In this work, a Pt single-atom catalyst supported on a Ce-MOF was synthesized using an efficient electrostatic deposition method. The impregnation process with a basic solution facilitated the interaction between the deprotonated hydroxyl groups and the cationic Pt species. The resulting material, Pt/UiO-66(Ce), exhibited an increase in Ce3+ content, confirming the presence of dispersed Pt single sites. Compared to the Pt/nCeO(2) catalyst, Pt/UiO-66(Ce) showed a six-fold increase in CO oxidation activity. The Pt nature was preserved and the activity was maintained during 14 hours at 100°C without deactivation.
Article
Chemistry, Multidisciplinary
Miriam Rodenes, Frederic Dhaeyere, Santiago Martin, Patricia Concepcion, Avelino Corma, Ivan Sorribes
Summary: A defect-engineered molybdenum sulfide catalyst is used to establish straightforward synthetic processes using alcohols. Developing tandem catalytic strategies based on readily available, stable, and renewable feedstocks is crucial for sustainable chemical industries. The catalyst, defect-engineered basal planes of a molybdenum sulfide nanomaterial ({Mo3S4}( n )), enables one-pot single-step synthesis and facilitates various coupling reactions involving alcohol dehydrogenation and hydrogen activation processes.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Review
Chemistry, Multidisciplinary
Lichen Liu, Avelino Corma
Summary: Heterogeneous bimetallic catalysts are widely used in industrial processes, but understanding the active sites in these catalysts at the atomic and molecular level is challenging due to their structural complexity. Comparing the structural features and catalytic performances of different bimetallic entities can aid in developing a unified understanding of the structure-reactivity relationships and improving current bimetallic catalysts. This review discusses the geometric and electronic structures of three representative types of bimetallic catalysts, as well as the synthesis methods, characterization techniques, and catalytic applications of these catalysts.
Article
Chemistry, Physical
Risheng Bai, Yue Song, Ge Tian, Fei Wang, Avelino Corma, Jihong Yu
Summary: The synthesis of highly efficient nano-sized Ti-rich TS-1 zeolites with controllable titanium species is crucial in zeolite catalytic reactions. A new method was developed using tetrabutyl orthotitanate tetramer as the titanium source, which slowed down the zeolite crystallization process and prevented the formation of anatase species. The Ti-rich TS-1 zeolite prepared with this method exhibited enriched active titanium species, enlarged external surface area, and superior catalytic performance in oxidative desulfurization reactions.
GREEN ENERGY & ENVIRONMENT
(2023)
Review
Chemistry, Multidisciplinary
Alexandra Velty, Avelino Corma
Summary: For many years, capturing, storing or sequestering CO2 from emission sources has been an effective method for reducing atmospheric CO2. The chemical conversion of CO2 into valuable chemicals has gained much attention due to CO2's abundance and renewable nature. Catalysts, particularly zeolite and ordered mesoporous materials, play a critical role in the conversion of CO2. By studying the reactions involving these catalysts, this review aims to explore the potential opportunities for using them to convert CO2 into essential chemicals and fuels.
CHEMICAL SOCIETY REVIEWS
(2023)
Article
Chemistry, Multidisciplinary
Xuemei Liu, Chaonan Cui, Shuoshuo Wei, Jinyu Han, Xinli Zhu, Qingfeng Ge, Hua Wang
Summary: This study presents a new strategy for designing efficient photocatalysts that can convert CO2 into hydrocarbons by utilizing synergistic catalytic sites. The findings provide a solution for the selective photocatalytic reduction of CO2 to CH4.
Article
Chemistry, Multidisciplinary
Chengxian Hu, Dan Wang, Lu Wang, Ying Fu, Zhengyin Du
Summary: A novel one-pot, three-component reaction conducted under electrochemical conditions was studied. The reaction involved 2-aminothiophenols, aldehydes, and malononitrile, using TBABF4 as an electrolyte and CuI as a catalyst. The proposed reaction mechanism suggested that CuI served as an electron relay. This method offers simplified operation, high atom economy, and mild reaction conditions.
Article
Chemistry, Multidisciplinary
Zhi Yang, Yu Chen, Linxi Wan, Yuxiao Li, Dan Chen, Jianlin Tao, Pei Tang, Fen-Er Chen
Summary: A highly enantioselective method for the complete hydrogenation of pyrimidinium salts using Ir/(S,S)-f-Binaphane complex as the catalyst was developed. This method provides easy access to fully saturated chiral hexahydropyrimidines, which are prevalent in many bioactive molecules. The reactions exhibit high yields and enantioselectivities under mild reaction conditions without additives. Successful application of this methodology in a continuous flow fashion further extends its practical utility.
Article
Chemistry, Multidisciplinary
Tina Jeoh, Jennifer Danger Nill, Wujun Zhao, Sankar Raju Narayanasamy, Liang Chen, Hoi-Ying N. Holman
Summary: In this study, the enzymatic hydrolysis of cellulose was investigated using real-time infrared spectromicroscopy. The spatial heterogeneity of cellulose was found to impact the hydrolysis kinetics. Hydration affected cellulose ordering, and Cel7A preferentially removed less extensively hydrogen bonded cellulose.
Article
Chemistry, Multidisciplinary
Tiphaine Richard, Walid Abdallah, Xavier Trivelli, Mathieu Sauthier, Clement Dumont
Summary: An effective method of grafting functionalities onto lignin based on glycerol carbonate has been developed using an efficient nickel-catalysed telomerisation reaction. This method allows lignin to have new reactive functions and reduces the glass transition temperatures of modified lignins, thereby expanding the application range of lignin-based resins.
Article
Chemistry, Multidisciplinary
Jing Qi, Xiyan Wang, Gan Wang, Srinivas Reddy Dubbaka, Patrick ONeill, Hwee Ting Ang, Jie Wu
Summary: This study presents a green and environmentally friendly approach for the synthesis of imides using electrocatalytic oxidation with H2O as the oxygen source. The method eliminates the need for toxic or expensive oxidants and achieves high yields under mild reaction conditions. It shows broad substrate compatibility and potential for industrial applications.
Article
Chemistry, Multidisciplinary
Babasaheb Sopan Gore, Lin-Wei Pan, Jun-Hao Lin, Yi-Chi Luo, Jeh-Jeng Wang
Summary: Here, we report a visible light-promoted intramolecular radical cascade reaction for the construction of fluorenol and naphthalene-fused cyclopropyl carbaldehyde derivatives. This method offers mild reaction conditions, a broad substrate scope, excellent step efficiency, and scalability, without the need for external chemical oxidants. The novelty of this protocol was demonstrated by synthesizing chrysene analogs and performing late-stage functionalizations.
Article
Chemistry, Multidisciplinary
Juho Antti Sirvio, Idamaria Romakkaniemi, Juha Ahola, Svitlana Filonenko, Juha P. Heiskanen, Ari Ammala
Summary: This article discusses the method of using supramolecular interaction between an aromatic hydrogen bond donor and lignin to achieve rapid delignification of softwood at low temperatures.
Article
Chemistry, Multidisciplinary
Yunyan Meng, Chunxiang Pan, Na Liu, Hongjiang Li, Zixiu Liu, Yao Deng, Zixiang Wei, Jianbin Xu, Baomin Fan
Summary: A novel visible light-driven synthesis method for 2,3-diamines has been developed, which has mild conditions, avoids the use of metal reagents, and can synthesize diamines and diols in one pot.
Article
Chemistry, Multidisciplinary
Mingqing Huang, Haiyang Huang, Mengyao You, Xinxin Zhang, Longgen Sun, Chao Chen, Zhichao Mei, Ruchun Yang, Qiang Xiao
Summary: A direct air-oxidized strategy for the synthesis of benzo[b]phosphole oxides was developed in this study. Arylphosphine oxides were transformed into phosphinoyl radicals, which were further combined with various alkynes to achieve the desired products. DFT calculations revealed the mechanism of phosphinoyl radical formation.
Article
Chemistry, Multidisciplinary
Anwei Wang, Jiayin Huang, Chunsheng Zhao, Yu Fan, Junfeng Qian, Qun Chen, Mingyang He, Weiyou Zhou
Summary: This study demonstrates an innovative strategy for the aerobic oxidation of C(sp(3))-H bonds using gamma-valerolactone. By optimizing the reaction conditions and utilizing specific catalysts, efficient oxidation of C(sp(3))-H bonds is achieved with good chemoselectivity in certain cases.
Article
Chemistry, Multidisciplinary
Shun Li, Likai Tong, Zhijian Peng, Bo Zhang, Xiuli Fu
Summary: Sulfide compounds show promise as electrocatalysts for water splitting, but their performance is limited by factors such as limited active sites and hindered substance transport. This study successfully prepared a high-entropy sulfide (ZnCoMnFeAlMg)(9)S-8, which reduced grain size and increased specific surface area, enabling the realization of a dual-functional catalyst with multiple catalytic sites. High entropy also modulated the electronic properties of sulfides, reducing the potential energy barrier for hydrolysis. This research introduces a new approach for functionalizing high entropy nanomaterials and improves the performance of water splitting catalysts.