Article
Chemistry, Physical
Jingsheng Niu, Chuanqi Zhao, Chun Liu, Jinsong Ren, Xiaogang Qu
Summary: Bacterial infections pose a significant threat to global health annually. Despite efforts to improve existing antibiotics, the development of multi-drug resistance remains a challenge. The design and synthesis of biomimetic sea urchin-like PdCu nanoparticles show promise in enhancing antibacterial therapy through increased interactions with bacteria and decreased antibiotic overuse.
CHEMISTRY OF MATERIALS
(2021)
Article
Engineering, Environmental
Alejandro Cabrera-Garcia, Vincent Blay, Ruben Blay-Roger, Angel G. Ravelo, Javier Gonzalez-Platas, M. Carmen Arevalo, Joaquin Sanchiz, Pedro Martin-Zarza
Summary: The novel dinuclear Ni(II) complexes, Ni-PATIO and Ni-PACO, show high catalytic activity and promise in producing hydrogen from water at significantly reduced potentials without the need for any additives.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Nanoscience & Nanotechnology
Gulcihan Gulseren, Aytul Saylam, Antoine Marion, Salih Ozcubukcu
Summary: The introduction of fullerene nanocatalysts into biocatalysis represents a novel approach to mimic enzymatic activity, offering potential for the design of high-efficiency artificial nanocatalysts through self-assembled nanostructures.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Multidisciplinary
Francesco Vaghi, Giorgio Facchetti, Isabella Rimoldi, Matteo Bottiglieri, Alessandro Contini, Maria Luisa Gelmi, Raffaella Bucci
Summary: Multiple studies have shown that the pyrrolidine nucleus is more efficient as organocatalysts for the condensation of aldehydes with electrophiles via enamine, compared to piperidine or morpholine. The low reactivity of morpholine-enamines is due to the presence of oxygen on the ring and the pyramidalisation of nitrogen, which decreases the nucleophilicity of the enamine. Therefore, finding efficient morpholine organocatalysts is a challenging task.
FRONTIERS IN CHEMISTRY
(2023)
Review
Chemistry, Multidisciplinary
Fujie Tanaka
Summary: This article discusses catalysts and catalyst systems that use amino acids, primary, secondary, and/or tertiary amines as key catalytic functional groups to accelerate chemical transformations. It also explores strategies and methods that utilize amine derivatives as catalysts. The understanding of dynamics and kinetic controls in amine-catalyzed reactions has enabled the synthesis of complex molecules in stereocontrolled manners.
Article
Chemistry, Multidisciplinary
Mao Cai, Runze Zhang, Chunming Yang, Sanzhong Luo
Summary: This article summarizes the efforts of chemists to explore uncharted chemical spaces by taking inspiration from nature. The authors categorize their research on bio-inspired small molecular catalysis into different strategies and provide insights into the biological origins, catalyst design, methodology development, and mechanistic insights. They emphasize the importance of nature's catalytic mechanisms in guiding the development of new catalysts for synthetic and energy chemistry.
CHINESE JOURNAL OF CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
P. Rani, N. Pundir, Heena, A. Husain, A. K. K. Bhasin, K. K. Bhasin, G. Kumar
Summary: Two new doubly interpenetrated MOFs were studied and found to be effective in amino acid sensing and catalytic reactions.
MATERIALS TODAY CHEMISTRY
(2023)
Review
Chemistry, Physical
Dan Xiao, Jennifer Gregg, K. Lakshmi, Peter J. Bonitatibus
Summary: The catalytic tetranuclear manganese-calcium-oxo cluster in photosynthetic reaction center, photosystem II, provides an excellent blueprint for light-driven water oxidation. Water oxidation reaction has attracted intense interest due to its potential as a renewable, clean energy source. Numerous synthetic bio-inspired molecular catalysts incorporating cheap and abundant metals such as Mn, Fe, Co, Ni, and Cu, as well as Ru and Ir, are being developed.
Article
Engineering, Chemical
Junfan Liu, Shuai Wang, Rujie Yang, Lu Li, Shanshan Liang, Liang Chen
Summary: In this study, a nacre-like structure membrane based on graphene oxide (GO) cross-linked by amino acid was fabricated. The membrane exhibited high water permeance and metal ions rejection, and showed stable separation performance for a long time.
JOURNAL OF MEMBRANE SCIENCE
(2022)
Article
Multidisciplinary Sciences
Insoo Ro, Ji Qi, Seungyeon Lee, Mingjie Xu, Xingxu Yan, Zhenhua Xie, Gregory Zakem, Austin Morales, Jingguang G. Chen, Xiaoqing Pan, Dionisios G. Vlachos, Stavros Caratzoulas, Phillip Christopher
Summary: This study investigates the catalytic mechanism of ethylene hydroformylation using supported, atomically dispersed Rh-WOx pair sites. Through Rh-assisted WOx reduction, transfer of ethylene from WOx to Rh, and H2 dissociation at the Rh-WOx interface, the pair sites exhibit high activity and selectivity, demonstrating the potential of oxide-supported pair sites in industrial reactions performed with homogeneous catalysts.
Article
Multidisciplinary Sciences
Terry Z. H. Gani, Zachariah J. Berkson, Ran Zhu, Jong Hun Kang, John R. Di Iorio, Ka Wing Chan, Daniel F. Consoli, Sohel K. Shaikh, Christophe Coperet, Yuriy Roman-Leshkov
Summary: The authors identify a dynamic site renewal and decay cycle, mediated by proton transfers involving proximal BrOnsted acidic OH groups, which operates concurrently with the Chauvin cycle and could address roadblocks associated with industrial metathesis processes. This cycle can be manipulated using small quantities of promoter olefins to drastically increase steady-state propylene metathesis rates, with negligible promoter consumption, showing potential applicability to other reactions. The increase in activity and reduction of operating temperature requirements were also observed on MoOx/SiO2 catalysts, indicating the broad scope of this strategy in addressing major challenges in industrial metathesis processes.
Article
Chemistry, Multidisciplinary
Jingsheng Niu, Liangpeng Wang, Tingting Cui, Zhao Wang, Chuanqi Zhao, Jinsong Ren, Xiaogang Qu
Summary: Artificial antibodies with bio-orthogonal catalytic activity were designed and synthesized to recognize specific bacteria and synthesize drugs in live bacteria, providing a strategy for disease diagnosis and treatment. Both in vitro and in vivo experiments demonstrated that the designed antibodies can distinguish and selectively bind to specific pathogens, eliminating them on site with activated drugs.
Article
Chemistry, Multidisciplinary
Alexander Seitz, Raffael C. C. Wende, Peter R. R. Schreiner
Summary: We describe the site-selective acetylation of partially protected monosaccharides using immobilized oligopeptide catalysts, synthesized via solid-phase peptide synthesis. The catalysts exhibit a reversed selectivity compared to N-methylimidazole and show high selectivity for various pyranosides. The catalysts demonstrate stability for multiple reaction cycles and can be easily reused after separation from the reaction solution. They can also be used in flow without any loss of reactivity and selectivity.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Jose J. Garrido-Gonzalez, Estela Sanchez-Santos, Asmaa Habib, Angel Cuevas Ferreras, Francisca Sanz, Joaquin R. Moran, Angel L. Fuentes de Arriba
Summary: In recent decades, there has been much interest in synthesizing small molecules that can mimic the active site of hydrolytic enzymes, but it remains challenging to prepare suitable small-molecule mimics. The newly proposed synthetic artificial enzymes are able to perform transesterification of non-activated esters under mild and neutral reaction conditions.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Biochemistry & Molecular Biology
Henry C. Wilkinson, Paul A. Dalby
Summary: This study explores the effects of site-specific saturation mutagenesis within enzyme active sites and the potential benefits of incorporating noncanonical amino acids (ncAA) on improving enzyme activity and stability simultaneously. By fine-tuning residue 385 with different aromatic ring substituents, the researchers were able to significantly enhance specific activity, catalytic performance, and stability of the enzyme, showcasing the advantages of expanding designer libraries to include ncAAs.
Article
Materials Science, Multidisciplinary
Matthew E. Potter, Daniel J. Stewart, Konstantin Ignatyev, Tom Bradley, Pier J. A. Sazio, Robert Raja
Summary: Optical fiber technology has the potential to revolutionize the efficiency of photoreactors in chemistry, enhancing key reactions and demonstrating feasibility for large-scale industrial applications.
ADVANCED OPTICAL MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Priyanka Verma, Matthew E. Potter, Alice E. Oakley, Panashe M. Mhembere, Robert Raja
Summary: In this study, PdAu bimetallic nanostructures supported on hierarchically porous silicoaluminophosphates (SAPOs) show significantly enhanced catalytic activities, highlighting the benefits of introducing hierarchical porosity in the SAPO support matrix.
Article
Chemistry, Physical
Hamza Annath, Jinesh C. Manayil, Jillian Thompson, Andrew C. Marr, Robert Raja
Summary: A comparative study of catalytic active sites in amorphous and crystalline aluminophosphates and their iron-containing analogues revealed that secondary porosity generated via soft templating and large mesopores significantly improve mass-transport and conversion of carbonyls. The active acidic sites play a crucial role in activating carbonyl groups and enhancing catalytic performance. Amorphous aluminophosphate (5) showed promising potential in industrial and pharmaceutical applications, outperforming hierarchical porous FeAlPO-5.
APPLIED CATALYSIS A-GENERAL
(2021)
Article
Chemistry, Multidisciplinary
Matthew E. Potter, Joshua J. M. Le Brocq, Alice E. Oakley, Evangeline B. McShane, Panashe M. Mhembere, Marina Carravetta, Bart D. Vandegehuchte, Robert Raja
Summary: The diverse applications of metal nanoparticle systems have individual demands on their properties, requiring novel synthetic methods for optimization. Utilizing strong thiol-Pd binding as a precursor for small, uniform Pd nanoparticle formation shows significant improvements in catalytic reactions. The presence of thiol groups offers greater control over nanoparticle formation, potentially allowing more targeted procedures.
CHEMISTRY-AN ASIAN JOURNAL
(2021)
Article
Chemistry, Multidisciplinary
Ivana Miletto, Marta Meazza, Geo Paul, Maurizio Cossi, Enrica Gianotti, Leonardo Marchese, Ramon Rios, Marc Pera-Titus, Robert Raja
Summary: In this study, a designed N-heterocyclic carbene (NHC) catalyst was anchored on mesoporous and hierarchical supports of varying pore sizes to investigate the influence on the benzoin condensation of furfural. The characteristics of the anchored catalysts were examined to rationalize their stability and recyclability using molecular dynamics simulations. The results showed that the catalysts maintained quantitative yields (99%) and complete recyclability after multiple cycles, validating the design rationale.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Engineering, Chemical
Stylianos Kyrimis, Kathryn E. Rankin, Matthew E. Potter, Robert Raja, Lindsay -Marie Armstrong
Summary: The optimization of large-scale fixed particle bed catalytic reactors requires a deep understanding of the various scales of bed structure, even down to the micrometre scale. Theoretical studies offer a cost-effective approach to support the optimization process, but they rely on simplified assumptions for the particles, which differ from real particle preparations. This study evaluates the impact of sieving on particle properties and the overall structural morphology of catalytic beds, providing valuable insights for the development of more accurate computational models.
ADVANCED POWDER TECHNOLOGY
(2023)
Article
Chemistry, Physical
Priyanka Verma, Kohsuke Mori, Yasutaka Kuwahara, Maela Manzoli, Sara Morandi, Choji Fukuhara, Robert Raja, Hiromi Yamashita
Summary: Over the past decade, plasmonic catalysis has shown improved product yield and selectivity in various chemical transformation reactions. This study investigates the effect of tertiary amine functionalization on the surface of hierarchically-porous zeotype materials to enhance plasmon-mediated catalysis. The presence of tertiary amine enhances the turnover number significantly under light irradiation conditions.
Article
Chemistry, Physical
Matthew E. Potter, Jonas Amsler, Lucas Spiske, Philipp N. Plessow, Theresah Asare, Marina Carravetta, Robert Raja, Paul A. Cox, Felix Studt, Lindsay-Marie Armstrong
Summary: Catalytic transformations are crucial for chemical technologies as we shift towards renewable bio-based systems. The dehydration of short-chain alcohols using solid acid catalysts is of interest to multiple industries. Microporous aluminophosphates, such as SAPO-34 and SAPO-5, show promising potential due to their size matching with alcohols and various framework topologies.
Article
Chemistry, Multidisciplinary
Priyanka Verma, Panashe M. Mhembere, Paolo Tallone, Maela Manzoli, Giuseppina Cerrato, Ryo Watanabe, Choji Fukuhara, Robert Raja, Hiromi Yamashita
Summary: The research focuses on the combination of Au nanoparticles and catalytically active nanoparticles to form hybrid plasmonic nanocatalysts with interesting properties and efficient catalysis under visible light irradiation. By varying the ratio of AuxPdy prepared on the CuClP framework, the optimized catalysis in the Suzuki-Miyaura coupling reaction was achieved. The results show the superior catalytic performance of Au1Pd1/CuClP under visible light irradiation and its potential for recycling and reusability, providing important insights for the design of new plasmonic photocatalysts combined with unique support materials.
Article
Engineering, Chemical
Stylianos Kyrimis, Robert Raja, Lindsay-Marie Armstrong
Summary: To achieve emission reduction goals, the production of carbon-neutral fuels and chemicals through heterogeneous fixed bed chemical reactors is crucial. Accurate CFD models are needed to optimize and scale-up these reactors. Image processing plays a significant role in CFD simulations by affecting the flow characteristics and pore connectivity of the bed.
ADVANCED POWDER TECHNOLOGY
(2023)
Article
Chemistry, Physical
Matthew E. Potter, Alice E. Oakley, Joshua J. M. Le Brocq, Lauren N. Riley, Marina Carravetta, Stephen M. King, Cara M. Doherty, Bart D. Vandegehuchte, Robert Raja
Summary: By modifying traditional synthetic procedures, this study successfully synthesized hierarchical solid-acid zeotypes by adding a hydrocarbon surfactant. The porosity of these materials was qualitatively described using small angle neutron scattering, positron annihilation lifetime spectroscopy, and porosimetry measurements. The results revealed that the size and nature of the mesopores can be finely tuned by varying the quantity of mesoporogen, and small angle neutron scattering showed a silica layer lining the mesopores, which strongly influenced the accessibility of the micropores.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Matthew E. Potter, Alice E. Oakley, Joshua J. M. Le Brocq, Lauren N. Riley, Marina Carravetta, Stephen M. King, Cara M. Doherty, Bart D. Vandegehuchte, Robert Raja
Summary: In this study, hierarchical solid-acid zeotypes were synthesized by modifying traditional synthetic procedures and adding a hydrocarbon surfactant. Small angle neutron scattering, positron annihilation lifetime spectroscopy, and porosimetry were used to qualitatively describe the porosity and investigate the connectivity of micropores and mesopores in the hierarchical materials. By varying the quantity of the mesoporogen, the size and nature of the mesopores could be finely tuned. Catalytic studies revealed distinct acid sites in the micropores and weaker silanol groups lining the mesopores, influencing the catalytic performance in n-butane isomerization and ethanol dehydration reactions.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Matthew E. Potter, J. J. M. Le Brocq, A. E. Oakley, H. Cavaye, Bart D. Vandegehuchte, Robert Raja
Summary: In this study, the molecular interactions between n-butane and mordenite catalyst were investigated using experimental and theoretical methods. The results revealed that the solid-acid sites induced conformer changes in the catalyst, which could be crucial for the design of optimized catalysts for hydrocarbon transformations.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Priyanka Verma, Yasutaka Kuwahara, Kohsuke Mori, Robert Raja, Hiromi Yamashita
Summary: Plasmonic nanostructures offer unique opportunities for enhancing chemical reactions under light irradiation. However, challenges such as lower efficiency, stability, and understanding of reaction mechanisms still exist. This review explores plasmonic catalysis, including trends, challenges, and applications, using advanced characterization techniques to establish the structure-property relationship of plasmonic hybrid nanostructures based on noble metals in hydrogen generation and CO2 reduction reactions.
Article
Chemistry, Physical
Stylianos Kyrimis, Matthew E. Potter, Robert Raja, Lindsay-Marie Armstrong
Summary: This study focuses on the kinetics of methanol synthesis from a mixture of CO2/CO/H-2, including the role of direct CO hydrogenation. A computational fluid dynamics model was developed, demonstrating that including CO hydrogenation in the kinetic model can more accurately predict inhibitions caused by the reactions.
FARADAY DISCUSSIONS
(2021)
Article
Chemistry, Applied
Qingyuan Zheng, Jack H. Williams, Scott Elgersma, Mick D. Mantle, Andrew J. Sederman, G. Leendert Bezemer, Constant M. Guedon, Lynn F. Gladden
Summary: In this study, a pilot-scale fixed-bed reactor compatible with NMR/MRI was developed for Fischer-Tropsch synthesis. Multiple magnetic resonance techniques were applied to quantitatively characterize different product species within catalyst pellets, providing valuable information for catalyst and reactor optimization.
Article
Chemistry, Applied
Lisa Ramisch, Sebastian Pfaff, Sabrina M. Gericke, Edvin Lundgren, Johan Zetterberg
Summary: We present a combination of optical operando techniques that allow simultaneous measurement of adsorbed species on catalyst surfaces, monitoring of surface oxide formation, and imaging of the gas phase above the catalyst surface. The experimental setup was validated by studying CO oxidation on Pd(100) at different pressures, revealing the effects of pressure on the heterogeneous catalytic reaction.
Article
Chemistry, Applied
Marta Paniagua, Gabriel Morales, Juan A. Melero, Daniel Garcia-Salgado
Summary: The influence of common impurities in levulinic acid on the catalytic performance of different acid catalysts for bio-jet fuel production was studied. It was found that furfural had the greatest detrimental effect on catalyst performance, while propyl-sulfonic acid-modified SBA-15 and sulfonic acid resin Amberlyst-70 showed good regeneration ability.
Article
Chemistry, Applied
Jesus Tapiador, Pedro Leo, Guillermo Calleja, Gisela Orcajo
Summary: This study presents a new MOF material, Zn-URJC-13, with acid and basic sites, permanent porosity, and high affinity to CO2 molecules. The Zn-URJC-13 catalyst exhibits efficient performance in CO2 cycloaddition reactions and can be reused multiple times.
Article
Chemistry, Applied
Dan Zhao, Vita A. Kondratenko, Dmitry E. Doronkin, Shanlei Han, Jan-Dierk Grunwaldt, Uwe Rodemerck, David Linke, Evgenii V. Kondratenko
Summary: This study demonstrates the potential of cheap and commercially available Zr or Ti-based supports and ZnO to serve as active and selective catalysts for propane dehydrogenation (PDH). The catalytically active species formed in situ under PDH conditions consist of isolated ZnOx. ZnOx on the surface of LaZrOx shows the highest rate of propene formation.
Article
Chemistry, Applied
Hanbyeol Kim, Jung Rae Kim, Young-Kwon Park, Jeong-Myeong Ha, Jungho Jae
Summary: In this study, metal phosphates were used as catalysts for biomass conversion to produce sustainable aromatics through DielsAlder cycloaddition reactions. The effects of synthesis method, activation method, and P/Ti molar ratio on the structure and acid properties of titanium phosphate catalysts were systematically studied. The mesoporous titanium phosphate catalyst synthesized by hydrothermal method at 180℃ for 12 h followed by ethanol refluxing at 60℃ for 24 h at a molar P/Ti ratio of 1 showed the highest surface area and acid site density.
Article
Chemistry, Applied
Yasin Khani, Sumin Pyo, Kwang-Eun Jeong, Chul-Ung Kim, Moonis Ali Khan, Byong-Hun Jeon, Kun-Yi Andrew Lin, Siyoung Q. Choi, Young-Kwon Park
Summary: A protonated form of Zeolite Socony Mobil-5 (H-ZSM-5) catalyst was synthesized through a hydrothermal method using different sources of silica. The effect of loading the catalyst with yttrium, samarium, and gadolinium on the acidic properties was investigated. Among the metal-loaded catalysts, the Sm/LHZ catalyst showed the best performance in the methanol to propylene conversion due to its high amount of weak and intermediate acid sites, while the Gd-LHZ catalyst increased the selectivity towards ethane and propane.
Article
Chemistry, Applied
Michael Franc, Ivana Cisarova, Jan Vesely
Summary: The present study investigates an enantioselective cyclization of enals with imidazolone derivatives catalyzed by a combination of achiral Pd(0) complex and chiral secondary amine. Corresponding spirocyclic imidazolones were produced in high yields with moderate diastereoselectivity and excellent enantioselectivity. The developed co-operative catalytic methodology provides a highly substituted spirocyclic scaffold with four stereogenic centers under mild conditions.
Article
Chemistry, Applied
Mauro Alvarez, Jennifer Cueto, David P. Serrano, Pablo Marin, Salvador Ordonez
Summary: This study focuses on improving the formulation and preparation methods of catalysts for the production of dimethyl carbonate. By using suitable catalyst preparation methods and copper salt precursors, the researchers successfully produced catalysts with optimal performance for dimethyl carbonate formation.
Article
Chemistry, Applied
Claudia J. Keijzer, Luc C. J. Smulders, Dennie Wezendonk, Jan Willem de Rijk, Petra E. de Jongh
Summary: This study investigates the catalytic behavior of alpha-alumina supported silver catalysts in the presence of chloride. It is found that the particle size of silver can affect the selectivity of the catalyst, but different strategies lead to different results. In this size range, the selectivity of ethylene oxide is correlated to the Ag : Al2O3 surface ratio.
Article
Chemistry, Applied
Takeshi Aihara, Wataru Aoki, Michikazu Hara, Keigo Kamata
Summary: The development of acid-base bifunctional catalysts is important for promoting specific chemical transformations. In this study, Ti-based perovskite oxides were synthesized and used as catalysts for two C-C bond-forming reactions (cyanosilylation and Knoevenagel condensation). The highly pure SrTiO3 nanoparticles with a high specific surface area exhibited the highest catalytic performance, and could be easily recovered and reused.
Article
Chemistry, Applied
Olga Gorlova, Petra Pribylova, Eliska Vyskocilova, Katerina Peroutkova, Jan Kohout, Iva Paterova
Summary: This study investigates the Baeyer-Villiger oxidation of beta-cyclocitral using tin-modified mixed oxides as catalysts. The optimal reaction conditions and the effects of various factors on the reaction course and selectivity were determined. The results show that tin-modified mixed oxides exhibit high activity and selectivity in the oxidation reaction.
Article
Chemistry, Applied
M. I. Avila, M. M. Alonso-Doncel, L. Briones, G. Gomez-Pozuelo, J. M. Escola, D. P. Serrano, A. Peral, J. A. Botas
Summary: The catalytic fast pyrolysis of lignin using ion-exchanged zeolite catalysts showed significant improvements in bio-oil quality and the production of aromatic hydrocarbons and oxygenated compounds.
Article
Chemistry, Applied
Enrico Catizzone, Giorgia Ferrarelli, Paolo Bruno, Girolamo Giordano, Massimo Migliori
Summary: The acid-catalysed alcohol conversion reaction is a promising route for de-fossilization strategies. Research on pure alcohol conversion and simultaneous dehydration of mixed alcohols have shown different product compositions, with the type and distribution of acid sites affecting the reaction mechanism.
Article
Chemistry, Applied
Alireza Ranjbari, Juho Kim, Jihee Yu, Jiyun Kim, Mireu Park, Nayoung Kim, Kristof Demeestere, Philippe M. Heynderickx
Summary: This study investigated a novel kinetic model for the adsorption and photocatalytic degradation of methyl orange using commercial ZnO and reduced ZnO photocatalysts. The results provided new insights into the interaction of catalysts with molecules of different charges and compared with a previous study on methylene blue. The presence of oxygen vacancies in ZnO and their effects on adsorption and photocatalytic degradation were analyzed, and the photocatalytic degradation rate of reduced ZnO was found to increase significantly.