Article
Chemistry, Physical
Christopher C. McAtee, Daniel J. Nasrallah, Ho Ryu, Michael R. Gatazka, Rory C. McAtee, Mu-Hyun Baik, Corinna S. Schindler
Summary: We describe a regioselective Lewis-acid-catalyzed method for the synthesis of highly functionalized cyclopentadienes incorporating diverse subunits. Insightful studies suggest that the mechanism involves Lewis-acid-catalyzed cycloadditions followed by stepwise oxetane fragmentation, resulting in the formation of functionalized cyclopentadienes. This work provides new insights into the design of catalytic carbonyl-olefin metathesis reactions.
Article
Chemistry, Physical
Zhen Li, Yao Yang, Zhenglei Yin, Xing Wei, Hanqing Peng, Kangjie Lyu, Fengyuan Wei, Li Xiao, Gongwei Wang, Hector D. Abruna, Juntao Lu, Lin Zhuang
Summary: By using a nitrogen-doped carbon overlayer on the Cu surface, the selectivity and efficiency of the CO2 reduction reaction can be significantly improved, directing towards valuable products such as ethylene and ethanol. Additionally, the overlayer also protects the stability of the copper substrate.
Article
Chemistry, Multidisciplinary
Itay Raz, Roman Dobrovetsky
Summary: The synthesis of a dicationic Zn+2-based complex with a tripodal tris(2-pyridylmethyl)amine (TPA) ligand is reported, which serves as a highly chemoselective catalyst for hydrosilylation reactions of alkynes. Unlike typical Zn-catalyzed hydrosilylation reactions, this system activates C equivalent to C triple bonds instead of Si-H bonds, which explains its high chemoselectivity.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Physical
Yingying Cheng, Wenjing Xu, Jing Hou, Peng Kang
Summary: Electrosynthesis of multi-carbon chemicals from oxalic acid offers a sustainable pathway for chemical production. A series of gallium tin oxide catalysts were used for selective electroreduction of oxalic acid to glyoxylic acid and glycolic acid. The product distribution can be controlled by adjusting the reaction temperature, and the catalysts showed high efficiency and stability in acidic media.
Article
Chemistry, Multidisciplinary
Surajit Panda, Amareshwar Nanda, Rakesh R. Behera, Rahul Ghosh, Bidraha Bagh
Summary: Commercially available Co-2(CO)(8) is an effective catalyst for the hydrosilylation of nitroarenes under thermal and photochemical conditions. This protocol selectively reduces a wide variety of nitroarenes with different functionalities to aromatic amines, expanding its potential utility in drug synthesis. Experimental evidence supports a radical pathway for this reaction.
CHEMICAL COMMUNICATIONS
(2023)
Article
Engineering, Environmental
Shahi Mulk, Muhammad Sajid, Lei Wang, Feng Liu, Gang Pan
Summary: This study investigated the synthesis of 5-hydroxymethylfurfural (HMF) from excess sucrose using an environmentally friendly and cost-effective technology. The results showed that the combination of p-toluenesulfonic acid and chromium chloride was the most effective dehydrating catalyst, with temperature, time, and concentration affecting the yields. The isomerization of glucose to fructose was identified as a major barrier to achieving high process yields.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2022)
Article
Materials Science, Multidisciplinary
S. R. Kunst, A. C. V. Bianchin, L. T. Mueller, J. A. Santana, T. M. Volkmer, F. D. P. Morisso, C. L. P. Carone, J. Z. Ferreira, I. L. Mueller, C. T. Oliveira
Summary: In this study, anodizing was used to improve the corrosion resistance of Zamak by forming oxide layers on its surface. The research found that anodizing promotes better corrosion resistance by creating oxide layers that fill the cracks generated during the anodizing process.
JOURNAL OF MATERIALS RESEARCH AND TECHNOLOGY-JMR&T
(2021)
Article
Chemistry, Inorganic & Nuclear
Agustin A. de la Fuente-Olvera, Franciso J. Ruiz-Mendoza, Jose M. Vasquez-Perez, Myriam Melendez-Rodriguez, Alejandro Alvarez-Hernandez, Veronica Salazar-Pereda, Daniel Mendoza-Espinosa
Summary: We report the synthesis and characterization of a novel series of rhodium(I) complexes supported by hydroxyl-functionalized 1,2,3-triazolylidenes. These complexes exhibit excellent catalytic activity in the hydrosilylation of terminal alkynes and the 1,4-addition of boronic acid to 2-cyclohexenone.
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
(2022)
Article
Environmental Sciences
Srinivas Bikkina, Kimitaka Kawamura, Yosuke Sakamoto, Jun Hirokawa
Summary: Oxidation of isoprene can lead to the production of oxalic acid, with methylglyoxal identified as an important intermediate. The relative abundances of methylglyoxal and oxalic acid fluctuate significantly during the reaction, suggesting a complex pathway of oxalic acid formation under dry conditions. The study proposes new reaction schemes for interpreting the ambient SOA composition and highlights the stable character of C-2 towards oxidation by hydroxyl radicals.
SCIENCE OF THE TOTAL ENVIRONMENT
(2021)
Article
Engineering, Environmental
Zhixiong Yang, Zhuangzhuang Wang, Junting Wang, Yuan Li, Gaoke Zhang
Summary: In this study, a magnetic recyclable greigite material (Fe3S4) with the exposed {011} facet was successfully prepared using a facile hydrothermal method. The activated oxalic acid (OA) under visible light irradiation showed promising potential for fast degradation of pollutants. The removal efficiency of metronidazole (MNZ) and hexavalent chromium using the Fe3S4 material with the exposed {011} facet was significantly higher compared to that of the material with the exposed {112} facet. Theoretical calculations and analyses provided insights into the mechanism of enhanced OA activation by facet engineering and the degradation mechanism of MNZ.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Multidisciplinary
Qiuying Zhu, Yuying Hu, Hongyu Chen, Chen Meng, Yizhu Shang, Chengcheng Hao, Shuxian Wei, Zhaojie Wang, Xiaoqing Lu, Siyuan Liu
Summary: This study proposes a simple method to construct a graphdiyne (GDY) supported Ag-Cu nanocluster as a selective electrocatalyst for producing C2+ products. Compared to Cu/GDY, the Ag-Cu/GDY tandem scheme exhibits superior performance in CO2RR to C2+ products. Theoretical calculations show that CO has a higher adsorption energy on Cu than on Ag, promoting the drift of *CO from Ag to Cu. Additionally, the key C-C coupling reaction of *CO with *COH is more favored on Ag-Cu/GDY, contributing to the formation of C2+ products.
Article
Chemistry, Physical
Jiajun Wu, Subash Nethaji Narayanasamy, Christophe Darcel
Summary: This contribution described the first iron-catalyzed chemoselective reduction of secondary carboxamides to aldimines under hydrosilylation conditions. The reaction is catalyzed by the well defined Fe(CO)4(IMes) complex, in the presence of 2.5 equiv. of diphenylsilane under UV irradiation (350 nm) at room temperature.
Review
Chemistry, Multidisciplinary
Oleksandr S. Liashuk, Vladyslav A. Andriashvili, Andriy O. Tolmachev, Oleksandr O. Grygorenko
Summary: The chemoselective transformations of functionalized sulfonyl fluorides and chlorides have been comprehensively surveyed. Sulfonyl fluorides show excellent selectivity control in their reactions, while sulfonyl chlorides typically react at the SO2Cl moiety except for a few exceptions.
Article
Engineering, Environmental
Huifen Yin, Jing Liu, HanLu Shi, Lei Sun, Xiangjuan Yuan, Dongsheng Xia
Summary: A series of Ag2CO3 doping g-C3N4 composites were synthesized by a precipitation method, and the effects of hydrothermal temperature on their structure and performance were investigated. The decoration of Ag2CO3 provided more active sites, improving the catalytic ozonation performance. The AgCN0.4-10 0 composite showed the best performance and good reusability.
PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
(2022)
Article
Chemistry, Multidisciplinary
Yan Yan, Jiayun Li, Ying Bai, Jiajian Peng
Summary: A series of polyethylene glycol phosphine ligands with N donor were synthesized and coordinated with Co(BF4)2 to catalyze the hydrosilylation of olefins and silanes. The best catalytic effect was achieved when the amount of catalyst was 0.5 mol% and the temperature was 90 degrees C with a reaction time of 5 hours. The catalytic cycle performance was also studied, and it was found that after 8 times, its yield could still reach> 90%.
ARABIAN JOURNAL OF CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Louise Ponsard, Emmanuel Nicolas, Ngoc Huan Tran, Sarah Lamaison, David Wakerley, Thibault Cantat, Marc Fontecave
Summary: A system coupling high-pressure CO2 electrolysis with thermal catalysis using high-pressure CO has been developed to convert CO2 into beta-butyrolactone, achieving a high reaction yield. This strategy enables the production of lactones from CO2 for polyester synthesis, expanding the range of chemicals derived from CO2.
Article
Chemistry, Multidisciplinary
Marie Kobylarski, Jean-Claude Berthet, Thibault Cantat
Summary: Homogeneous reductive depolymerization of polyesters and polycarbonates with hydroboranes can be achieved using f-metal complex catalysts, resulting in the transformation of these polymeric materials into valuable alcohol compounds with high selectivity.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Inorganic & Nuclear
Gabriel Durin, Jean-Claude Berthet, Emmanuel Nicolas, Pierre Thuery, Thibault Cantat
Summary: This study reports the catalytic hydrogenolysis of R3SiOTf species to R3SiH in the presence of a base using hydride complexes. The mechanisms of these reactions were examined using DFT studies, revealing different active species for the reduction of Si-OTf and Si-Cl bonds.
Article
Chemistry, Physical
Caroline Genre, Idir Benaissa, Timothe Godou, Mathieu Pinault, Thibault Cantat
Summary: Formic acid is used as the only source of carbon and hydrogen in the methylation of aromatic and aliphatic amines to methylamines. The reaction proceeds over a solid Pd/In2O3 catalyst via a formylation/transfer hydrogenation pathway without the need for any additive.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Materials Science, Multidisciplinary
Jose Enrico Q. Quinsaat, Elias Feghali, Daniel J. van de Pas, Richard Vendamme, Kirk M. Torr
Summary: Depolymerized native lignin was used as a polyol in the synthesis of rigid bio-based polyurethane foams, which showed similar densities and thermal properties but substantially improved compression properties compared to traditional foams. Incorporating dimeric-rich lignin-derived polyols led to significant enhancements in compression modulus and strength in the resulting foams. These findings suggest that a lignin-first approach can be a valuable strategy for producing rigid PU foams with enhanced mechanical robustness and bio-based content.
ACS APPLIED POLYMER MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Gabriel Durin, Albane Fontaine, Jean-Claude Berthet, Emmanuel Nicolas, Pierre Thuery, Thibault Cantat
Summary: The metal-free catalytic hydrogenolysis of silyl triflates and halides to hydrosilanes is achieved using arylborane Lewis acids as catalysts. The catalyst acts as a Frustrated Lewis Pair and is able to split H-2 and generate a boron hydride intermediate capable of reducing (pseudo)halosilanes. This metal-free organocatalytic system competes with metal-based catalysts and enables the formation of a variety of hydrosilanes at room temperature in high yields under low hydrogen pressure.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Liam J. Donnelly, Jean-Claude Berthet, Thibault Cantat
Summary: This study describes a zirconium-catalyzed synthesis of imines through the reductive deoxygenation of secondary amides, achieving high yields and excellent chemoselectivity. The reaction utilizes Schwartz's reagent and (EtO)(3)SiH as a mild stoichiometric reductant, with stoichiometric mechanistic investigations suggesting the regeneration of the active catalyst through the metathesis of Si-H and Zr-OR sigma-bonds.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Etienne Crochet, Lucile Anthore-Dalion, Thibault Cantat
Summary: Investigation was conducted on the reactivity of alkyl formates as novel transfer hydroalkylation reagents in the transfer hydroalkylation of imines. By using a ruthenium-based catalyst and LiI as promoter to cleave the C-O sigma-bond of the formate scaffold, tertiary amines were produced with divergent regioselectivity compared to previously reported strategies.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Biochemistry & Molecular Biology
Jose Enrico Q. Quinsaat, Elias Feghali, Daniel J. van de Pas, Richard Vendamme, Kirk M. Torr
Summary: In this work, isocyanate-free polyurethane/epoxy hybrid thermosets with high biobased content were prepared. The materials exhibited high flexural modulus and flexural strength by optimizing the composition and curing agent. These novel biobased hybrid materials outperformed epoxy-only thermosets and hybrid materials produced from petrochemicals.
Article
Chemistry, Physical
Marie-Helene Pietraru, Nicolas Lentz, Louise Ponsard, Emmanuel Nicolas, Thibault Cantat
Summary: In order to reduce our reliance on fossil feedstock, alternative sources for polymeric materials have been sought in recent years. This study presents a new approach to the formation of a useful monomer for polyesters, succinic anhydride, through the catalytic carbonylation of bio-sourced acrylic acid. The use of an Earth-abundant metal catalyst, [Co-2(CO)(8)], along with a bidentate ligand, 1,2-bis(dicyclohexylphosphino)ethane (dcpe), and H-2, successfully tackles the challenging carbonylation of unsaturated carboxylic acids.
Article
Chemistry, Multidisciplinary
Xin Liu, Marie Kobylarski, Jean-Claude Berthet, Thibault Cantat
Summary: This study reports the catalyst-free depolymerization of polycaprolactone with iodosilanes, leading to the formation of valuable functionalized monomer derivatives.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Xin Liu, Marie Kobylarski, Jean-Claude Berthet, Thibault Cantat
Summary: Catalyst-free depolymerization of polycaprolactone with iodosilanes (Me3SiI and SiH2I2) can generate valuable functionalized monomer derivatives.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Alexia Ohleier, Antoine Sallustrau, Bouchaib Mouhsine, Fabien Caille, Davide Audisio, Thibault Cantat
Summary: This study reports a method for synthesizing high-value building blocks from carbon dioxide. By using a new nucleophilic labeled source, methoxyborane, a catalytic methoxylation reaction on aryl halides can be achieved directly, leading to the successful labeling of a series of substrates.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Marie Kobylarski, Liam J. Donnelly, Jean-Claude Berthet, Thibault Cantat
Summary: Cp2Zr(H)Cl has been used as a stoichiometric reagent for the reduction of unsaturated organic molecules. Recently, it has been developed as a catalyst by turnover of the [Zr]-X intermediates formed upon reaction with an organic substrate, using hydride reagents. In this study, a new catalytic pathway for the reduction of esters using Cp2Zr(H)Cl as the catalyst and a bench-stable silane, Me(OMe)(2)SiH (DMMS), as a mild stoichiometric reductant is reported. The methodology showed high yields of alcohols and proved effective for the depolymerisation of polyesters found in household plastic waste.
Article
Chemistry, Multidisciplinary
R. Martin Romero, Neethu Thyagarajan, Nora Hellou, Clement Chauvier, Timothe Godou, Lucile Anthore-Dalion, Thibault Cantat
Summary: This article presents a transfer hydrosilylation of ketones using silyl formates as hydrosilane surrogates under mild conditions. A total of 24 examples of ketones were successfully converted to their corresponding silyl ethers with yields ranging from 61% to 99% in the presence of a (PNP)-P-H-based ruthenium catalyst and silyl formate reagent. The crucial role of the ligand in the transformation was demonstrated.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Zi-Ye Liu, Qian-Yu Wang, Ji-Ming Hu
Summary: In this study, a layered carbon dot composite catalyst (NiFe LDH@CDs) was prepared using a one-step coprecipitation method, without the need for heating or hydrothermal treatment. The CD-functionalized catalyst facilitated rapid charge transfer and accelerated the oxygen evolution reaction. Additionally, the heterojunction structure formed between NiFe LDH and CDs efficiently suppressed photoelectron-hole recombination.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Rohit Kumar, Ankit Kumar Srivastava, Palaniyappan Nagarasu, Vedichi Madhu, Ekambaram Balaraman
Summary: We designed and synthesized a NN-CoII bidentate complex and used it for the amination of alcohols under mild and solventless conditions. The complex exhibited good reactivity towards both primary and sterically hindered secondary alcohols, providing high yields of amines. The pyrazole moiety in the ligand played a crucial role in the reaction. Furthermore, we demonstrated the reusability of the complex as a homogeneous cobalt catalyst.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Shivanand Chettri, Liang-Ting Wu, Sagarmani Rasaily, Debesh Sharma, Bikram Gurung, Rajani Dewan, Sudarsan Tamang, Jyh-Chiang Jiang, Anand Pariyar
Summary: Replicating the enzymatic surface microenvironment in vitro is challenging, but constructing an analogous model could facilitate our understanding of surface effects and aid in developing an efficient bioinspired catalytic system. In this study, five unique Cu2O morphologies were generated, and the surface morphology variations were found to be a consequence of differences in the exposure of low-index facets. The reactivity of Cu2O was found to be influenced by the proportion of {110} planes, with r-Cu2O exhibiting the highest reactivity.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Yong Tang, Jianhao Qiu, Dingliang Dai, Guanglu Xia, Lu Zhang, Jianfeng Yao
Summary: Defect engineering has been shown to improve the photocatalytic performance. This study investigated the use of defect-rich UiO-66-NH2 wrapped by ZnIn2S4 as a catalyst for photocatalytic H2O2 production. The defects in UiO-66-NH2 enhanced O-2 adsorption and charge separation, leading to higher H2O2 yield. The insights from this work can advance the research in defect engineering of MOFs and photocatalytic H2O2 synthesis.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Ruiyang Qu, Shuxin Mao, Jana Weiss, Vita A. Kondratenko, Evgenii V. Kondratenko, Stephan Bartling, Haifeng Qi, Annette-Enrica Surkus, Kathrin Junge, Matthias Beller
Summary: The hydrogenation of amides, a challenging reaction usually performed at high temperatures, has been achieved under milder conditions using a new Pt-MoOx/TiO2 catalyst. This catalyst system enables the selective hydrogenation of various amides and imides.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Xiaoran Niu, Ao Wang, Lei Tong, Lei Wang, Yuan Kong, Chenliang Su, Hai-Wei Liang
Summary: This study introduces a novel intermetallic PdCu3 catalyst supported on defective nanodiamond-graphene (ND@G), which exhibits high selectivity (95%) and remarkable activity (turnover frequency: 2940 h(-1)), six times higher than that of the commercial Lindlar catalyst.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Review
Chemistry, Physical
Zhiyuan Zheng, Yiming Yue, Hongying Zhuo, Qinggang Liu, Yanqiang Huang
Summary: This review presents the recent research advances on single-atom catalysis for deep reduction of CO2. Detailed introductions and summaries were classified into three categories based on proton-coupled multi-electron transfer approaches: strengthening metal-support interaction, rational design and regulation of coordination environment, and development of SACs with multi-atom active sites. The challenges and future research directions in the field of SACs for CO2 reduction are also proposed.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
Shiv Kumar, Paramita Datta, Anup Bhunia, Swadhin K. Mandal
Summary: This article reports a transition-metal-free process for in situ denitrogenation of tosylhydrazones, resulting in the production of various sulfones. The authors used a phenalenyl-based odd alternant hydrocarbon as a photoredox catalyst, which acted as a potent oxidant to facilitate the denitrogenation reaction. The method showed wide functional-group tolerance and high yields, making it suitable for late-stage modification of natural products.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)
Article
Chemistry, Physical
L. A. Luque-Alvarez, J. Gonzalez-Arias, F. Romero-Sarria, T. R. Reina, L. F. Bobadilla, J. A. Odriozola
Summary: Currently, the production of acetic acid through the carbonylation reaction of methanol has limitations, leading to the exploration of alternative methods using heterogeneous catalysts. This study investigates the methanol carbonylation reaction over a Cu-H-MOR catalyst and proposes a reaction mechanism based on the catalytic behavior and performance of the catalyst. The results provide insights into the reaction mechanism and the involvement of acid and redox centers.
CATALYSIS SCIENCE & TECHNOLOGY
(2024)