Article
Chemistry, Multidisciplinary
Willi M. Amberg, Erick M. Carreira
Summary: This study presents the total synthesis of the complex molecule (+)-aberrarone using an Au-catalyzed-Sn-mediated cascade reaction, which efficiently closes four rings in the molecule. The method offers a stereoselective approach to synthesizing the natural product with a unique tetracyclic skeleton.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Inorganic & Nuclear
Lu Dong, Linke Yu, Xueli Sun, Xiongkai Tang, Xuexin You, Jiaqi Tang, Zi-Ang Nan, Dongxu Cao, Yanyuan Jia, Simin Li, Fengyu Li, Shuo Guo, Hui Shen
Summary: We report a stable gold-copper alloy nanocluster with high catalytic performance. The nanocluster exhibits high thermal stability and contains rich uncoordinated copper sites, which contribute to its extremely high catalytic activity in C-O coupling reactions. This finding is of great significance for understanding the underlying rationale of ligand-functionalized metal nanocatalysts.
INORGANIC CHEMISTRY FRONTIERS
(2023)
Article
Engineering, Environmental
Lulu Kong, Chongchong Wang, Weijie Yang, Lin Zhou, Shaohua Wei
Summary: The detection of mercury is important for assessing its toxicity and health risks. In this study, ultra-thin two-dimensional palladium nanosheets (PdNS) were synthesized for the simple, sensitive, accurate, and cheap detection of Hg2+. The PdNS showed high selectivity and sensitivity, and a detection kit was developed for Hg2+ detection using naked eye or cellphone at a low cost.
JOURNAL OF HAZARDOUS MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Selina K. Kaiser, Adam H. Clark, Lucrezia Cartocci, Frank Krumeich, Javier Perez-Ramirez
Summary: A new synthesis method has been developed to prepare carbon-supported gold nanostructures in bimetallic catalysts, allowing for atomic-level gold dispersion to address the practical applicability of gold single-atom catalysts. Platinum plays a key role in promoting a chlorine-mediated dispersion mechanism, preventing sintering of gold agglomerates and maintaining the activity of Au(I)-Cl active sites.
Article
Chemistry, Multidisciplinary
Chen Zhang, Linli Xu, Wai-Yeung Wong
Summary: Polymetallaynes are a promising branch of metallopolymers with unique skeletons and versatile properties. Both one-dimensional and two-dimensional polymetallaynes have attracted considerable attention due to their excellent electronic, optical, and magnetic properties. The research on molecular metallaynes provides insights for understanding structure-property-activity relationships in organometallic acetylide-containing systems. Recent progress in polymeric and molecular metallaynes containing platinum, mercury, and gold is discussed, highlighting their emerging applications in various fields.
CHINESE JOURNAL OF CHEMISTRY
(2023)
Article
Chemistry, Organic
Dan-Bi Sung, Jong Seok Lee
Summary: This study describes a gold(I)-catalyzed intermolecular formal [2 + 2 + 2] cycloaddition reaction, which selectively synthesizes highly substituted 2H-pyrans using different metal triflate additives. This method provides a new opportunity for the synthesis of other heterocyclic compounds.
Article
Chemistry, Organic
Kenzo Yahata, Raphael J. Zachmann, Alois Fuerstner
Summary: After resolving all the issues surrounding the constitution and stereostructure of prorocentin through a recent total synthesis, a new approach was devised to improve the supply of this scarce marine natural product; this compound is a cometabolite of the phosphatase inhibitor okadaic acid but still lacks detailed biological profiling. The revised method starts from 2-deoxy-D-glucose; the key to success was a telescoped hemiacetal reduction/acetal cleavage and an exquisitely selective gold/Bronsted acid-cocatalyzed spiroacetalization.
Article
Chemistry, Physical
Theo Faverge, Bruno Gilles, Antoine Bonnefont, Frederic Maillard, Christophe Coutanceau, Marian Chatenet
Summary: The mechanisms of oxidation of glucose, gluconic acid, and sorbitol on gold, platinum, and palladium are investigated using cyclic voltammetry, differential electrochemical mass spectrometry, and in situ Fourier transform infrared spectroscopy. The nature of the reactant significantly influences the onset of the oxidation reaction, with glucose's anomeric function oxidized at low potentials on all three surfaces, while gluconic acid and sorbitol poison the surface at low potentials. Different reaction pathways are observed based on the metal surface, and gold features the best activity, selectivity, and specificity for glucose oxidation into gluconate at low potentials. The study highlights the dependence of the mechanism on reactant, catalyst, and potential.
Article
Chemistry, Physical
Theo Faverge, Bruno Gilles, Antoine Bonnefont, Frederic Maillard, Christophe Coutanceau, Marian Chatenet
Summary: The oxidation mechanisms of glucose, gluconic acid, and sorbitol on gold, platinum, and palladium surfaces were studied using cyclic voltammetry, differential electrochemical mass spectrometry, and in situ Fourier transform infrared spectroscopy. The nature of the reactant influenced the onset of the oxidation reaction, with glucose being oxidized at low potentials on all three surfaces, while gluconic acid and sorbitol exhibited poisoning effects. The metal surface also influenced the reaction pathways, with glucose oxidation being initiated through the partial dissociative adsorption of glucose on all three surfaces. Gold demonstrated the highest activity, selectivity, and specificity for glucose oxidation to gluconate at low potentials. The study reveals a reactant, catalyst, and potential-dependent mechanism.
Article
Chemistry, Inorganic & Nuclear
Yulin Xie, Man Wang, Qianqian Sun, Dongmei Wang, Shuiping Luo, Chunxia Li
Summary: In this study, a PtBi-beta-CD-Ce6 nanoplatform was developed to generate sustained O-2 for enhanced tumor therapy. The nanoplatform combines photodynamic therapy, photothermal therapy, photoacoustic imaging, and X-ray computed tomography imaging, showing potential for multimodal imaging-guided therapy.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Organic
Miyu Yokoyama, Yoshinori Okayasu, Yoichi Kobayashi, Hiroki Tanaka, Yohei Haketa, Hiromitsu Maeda
Summary: Dithienylnitrophenols were synthesized to form pi-electron anions, which were stabilized by intramolecular chalcogen bonding and combined with cations to form various ion pairs. The assembly modes of charge-by-charge in the solid state, along with stacking and photoinduced electron transfer behaviors in solution, were modulated by the different ionic species.
Article
Chemistry, Organic
Cunbo Wei, Jiawen Wu, Lizhu Zhang, Zhonghua Xia
Summary: A highly selective synthesis of Z-alkenyl indoles was developed by adding indoles to haloalkynes using a gold catalyst and a cocatalyst, resulting in high yields at room temperature.
Article
Chemistry, Multidisciplinary
Teng Yuan, Qi Tang, Chuan Shan, Xiaohan Ye, Jin Wang, Pengyi Zhao, Lukasz Wojtas, Nicholas Hadler, Hao Chen, Xiaodong Shi
Summary: This study presents a novel method for alkyne trifunctionalization through gold catalysis, achieving consecutive reactions with high efficiency and excellent yields under mild conditions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Rajeshwer Vanjari, Deepanjan Panda, Shaswati Mandal, Ganga B. Vamisetti, Ashraf Brik
Summary: In this study, a novel method for the Au(I)-mediated cyclization of unprotected peptides was proposed. The method involves the rapid addition of an amine on a propargyl group to generate an imine linkage for the synthesis of cyclic peptides. The results demonstrate the successful synthesis of over 35 diverse cyclic peptides with different sequences and lengths, as well as the stereoselective reduction of cyclic imines.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Multidisciplinary
Tingrui Li, Yilitabaier Julaiti, Xiaopeng Wu, Jie Han, Jin Xie
Summary: The gold-catalyzed ring-opening rearrangement of cyclopropenes provides an efficient method for synthesizing polysubstituted naphthols or aryl-substituted furans. The reaction selectivity between naphthols and furans can be switched by using different gold-carbenes or gold-carbocations as catalysts.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Review
Chemistry, Multidisciplinary
Paula Escamilla, Walter D. Guerra, Antonio Leyva-Perez, Donatella Armentano, Jesus Ferrando-Soria, Emilio Pardo
Summary: Since the emergence of metal-organic frameworks (MOFs), a wide range of exciting properties and applications have been reported, mainly due to their porous nature and rich host-guest chemistry. However, the potential rewards offered by other important features of MOFs have been largely unexplored. This feature outlines recent advances in using highly robust and crystalline oxamato- and oxamidato-based MOFs as reactors for the in situ preparation of well-defined catalytically active single atom catalysts (SACS), subnanometer metal nanoclusters (SNMCs), and supramolecular coordination complexes (SCCs).
CHEMICAL COMMUNICATIONS
(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)
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, Multidisciplinary
Yongkun Zheng, Alejandro Vidal-Moya, Juan Carlos Hernandez-Garrido, Marta Mon, Antonio Leyva-Perez
Summary: Commercially available zeolite Y has been used to modulate the catalytic activity and selectivity of ultrasmall silver species during the Buchner reaction and the carbene addition. By exchanging the counter cations of the zeolite framework, the zeolite acts as a macroligand to tune the silver catalytic site. This cheap and recyclable solid catalyst enables the in situ formation of carbenes and selective insertion into C-H and C-O bonds.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Organic
Paloma Mingueza-Verdejo, Jose Pedro Ceron-Carrasco, Judit Oliver-Meseguer, Antonio Leyva-Perez
Summary: This study presents a new synthetic method for the conversion of internal α-methylene ketones and vinyl ethers through formal exchange reactions, providing a one-step synthesis of vinyl ethers from ketones. The method offers mild reaction conditions and utilizes reusable cheap solid catalysts, making it suitable for long-term use in continuous flow reactions.
SYNTHESIS-STUTTGART
(2023)
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, Inorganic & Nuclear
Cristina Bilanin, Paula Escamilla, Jesus Ferrando-Soria, Antonio Leyva-Perez, Donatella Armentano, Emilio Pardo
Summary: Host-guest chemistry within metal-organic frameworks (MOFs) offers great potential for the selective synthesis of industrially relevant products and represents a powerful alternative to current heterogeneous catalysts.
DALTON TRANSACTIONS
(2023)
Article
Multidisciplinary Sciences
Yongkun Zheng, Nuria Martin, Mercedes Boronat, Jesus Ferrando-Soria, Marta Mon, Donatella Armentano, Emilio Pardo, Antonio Leyva-Perez
Summary: Dimers of reduced silver (Ag-2) were successfully synthesized within a metal-organic framework. The resulting catalyst, Ag-2-methioMOF, showed high catalytic activity in the methanation reaction of carbon dioxide under mild reaction conditions.
SCIENTIFIC REPORTS
(2023)
Article
Chemistry, Multidisciplinary
Jordi Ballesteros-Soberanas, Cristina Bilanin, Antonio Leyva-Perez
Summary: This paper proposes two new parameters, adapted sensitivity constant and substrate electronics adaptability, to evaluate the ability of a reaction to transform substrates with opposing electronics. These parameters can help list reactions according to substrate scope, whether catalyzed or not.
ACS ORGANIC & INORGANIC AU
(2023)
