Article
Chemistry, Physical
Lucy Hillen, Volkan Degirmenci
Summary: Hierarchical mesoporous-microporous chabazite-type zeolites were synthesized using a dual-templating method in this study, showing fast adsorption-desorption kinetics for carbon dioxide capture with potential for larger-scale application. Template ratios were found to have a significant influence on their structure and performance. These materials are recyclable with minimal loss in crystallinity and carbon dioxide capture capacity.
Article
Materials Science, Multidisciplinary
Yuanchao Shao, Dezhi Wang, Yitong Xu, Takashi Tatsumi, Jingui Wang
Summary: Hierarchical zeolites with improved micropore utilization efficiency due to the introduction of mesopores have become a research hotspot in the fields of zeolites and hetero-catalysis. A foam-like hierarchical zeolite containing many aggregated identical-lattice-direction hollow nanocrystals was successfully synthesized, leading to a new height in catalytic performance for olefin epoxidation.
Article
Chemistry, Applied
Dina G. Boer, Jort Langerak, Benny Bakker, Paolo P. Pescarmona
Summary: A series of binderless zeolite LTA adsorbents in macroscopic bead format with hierarchical porosity were synthesized for CO2 removal from biogas. The ion-exchanged Na58K42-LTA beads exhibited the best performance, with high CO2/CH4 selectivity and substantial CO2 adsorption capacity.
MICROPOROUS AND MESOPOROUS MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Le Xu, Alexander Okrut, Thomas Rea, Kaustav Chaudhuri, Jinyi Han, Alexander Kuperman, Alexander Katz
Summary: Postsynthetic modification of mesoporous Y zeolite (Meso-Y) allows for uniform nanoscale coating of silica, alumina, or aluminosilicate on the interior surface, without causing significant micropore blockage or synthesis of a separate bulk alumina-containing phase. The use of CTAB surfactant as a soft template is crucial for this selective modification under dry conditions. This approach enables control of the surface charge and has important implications for adsorption and catalysis applications.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Chemistry, Physical
Zahra Asgar Pour, Romar Koelewijn, Mustapha El Hariri El Nokab, Patrick C. A. van der Wel, Khaled O. Sebakhy, Paolo P. Pescarmona
Summary: Three zeolites were synthesized in the form of binder-free macroscopic beads using hydrothermal method with anion-exchange resin beads as hard template. The beads consisted of interconnected crystalline zeolite domains, forming a hierarchical porous network. H-Beta beads showed the best catalytic performance in the Friedel-Crafts acylation reaction and could be reused in multiple runs without loss of activity. In continuous-flow tests, H-Beta beads exhibited higher average activity but deactivated more rapidly than the extrudates.
Article
Chemistry, Physical
Junling Liu, Jingnan Wang, Yining Zhang, Wei Zheng, Yongbin Yao, Qiang Liu, Xuejing Zhang, Yongan Yang, Xi Wang
Summary: This study developed an efficient, eco-friendly, and cost-effective catalyst for propane dehydrogenation (PDH), overcoming the toxicity and high cost issues of commercial catalysts. The catalyst exhibited good catalytic performances in PDH reactions.
Article
Chemistry, Multidisciplinary
Yuting Li, Uddhav Kanbur, Jinlei Cui, Guocang Wang, Takeshi Kobayashi, Aaron D. Sadow, Long Qi
Summary: The zeolite-supported lanthanide La(BH4)(x)-HY30 is capable of catalyzing the C-H borylation of benzene with pinacolborane, providing a complementary approach to precious, late transition metal-catalyzed borylations.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Review
Environmental Sciences
Yi Yang, Ruikun Xu, Chenyang Zheng, Yuxi Long, Shuo Tang, Zemin Sun, Binbin Huang, J. Paul Chen
Summary: Hollow zeolite fibers with hierarchical porosity have improved diffusion efficiency and are suitable for catalytic applications. Catalytic zeolite membrane fibers are commonly used due to their stability and selectivity. Further research is needed to develop self-assembly pure hollow zeolite fibers, catalytic substrate incorporated hollow zeolite fibers, hollow zeolite fibers with gradient multicomponent zeolites, and hollow zeolite fibers with nanoscale diameters.
Article
Chemistry, Organic
Santosh Kumar Keshri, Suchithra Madhavan, Manmohan Kapur
Summary: Transition-metal catalysis has revolutionized organic synthesis by enabling efficient C-C and C-heteroatom bond formation. To functionalize nonbiased C-H bonds, various strategies have been developed, including the use of directing groups and substrate modification.
Article
Multidisciplinary Sciences
Yuzhu Ma, Hongjin Zhang, Runfeng Lin, Yan Ai, Kun Lan, Linlin Duan, Wenyao Chen, Xuezhi Duan, Bing Ma, Changyao Wang, Xiaomin Li, Dongyuan Zhao
Summary: In this study, a nanodroplet remodeling strategy is proposed for the synthesis of hierarchical multi-chambered mesoporous silica nanoparticles with tunable architectures. The dual-chambered nanoparticles have a high surface area and two interconnected cavities, allowing for separate anchoring of multiple species without mutual interference. Additionally, the dual-chambered mesoporous nanoreactors prepared using this strategy exhibit efficient mass transfer, leading to improved selectivity of the target product.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Organic
Uros Todorovic, Immo Klose, Nuno Maulide
Summary: Thiocyanates, a versatile building block in organic synthesis, can be easily accessed through an interrupted Pummerer reaction of sulfoxides. This dealkylative functionalization can proceed under mild conditions by electrophilic activation of the sulfoxide partner, and the resulting thiocyanate can be used as a handle for diversification in a straightforward one-pot procedure.
Article
Chemistry, Organic
Hee Chan Noh, Cheol-Eui Kim, Kyungsup Lee, Dongwook Kim, Phil Ho Lee
Summary: A regioselective B(4)-alkenylation method has been developed using o-carboranyl sulfoxonium ylides and alkynes through B(4)-H activation catalyzed by Iridium(I). Sequential B(4)- and B(6)-alkenylation reactions resulted in the synthesis of B(3,5)-dialkenylated o-carboranyl sulfoxonium ylides in one pot. This method allows the introduction of two alkenyl groups at positions 3 and 5 of the carborane, with the sulfoxonium ylide serving as a directing group that can be further functionalized to B-alkenylated o-carboranyl trichloromethyl ketones.
Article
Multidisciplinary Sciences
Ji-Min Yang, Yu-Kun Lin, Tao Sheng, Liang Hu, Xin-Pei Cai, Jin-Quan Yu
Summary: Regiocontrol is challenging in traditional cycloaddition reactions between unsaturated carbon compounds. This study reports a regio-controllable synthesis of benzocyclobutenes (BCBs) through a palladium-catalyzed double C-H activation of adjacent methylene units in carboxylic acids using bidentate amide-pyridone ligands. This method allows for the synthesis of diversely functionalized BCBs and hetero-BCBs found in drug molecules and bioactive natural products.
Article
Energy & Fuels
Min-Yee Choo, Lee Eng Oi, Yu-Chuan Lin, Tau Chuan Ling, Eng-Poh Ng, Wei-Hsin Chen, Chin Kui Cheng, Joon Ching Juan
Summary: Energy is essential in the 21st century, with most of it being supplied by fossil fuels. However, the environmental and sustainability issues associated with burning fossil fuels have led to the production of biofuels. In this study, two synthesis strategies were used to address the diffusion limitation of conventional zeolite Y, resulting in the preparation of hierarchical nanosized zeolite Y. The best hierarchical nanosized zeolite Y (MY0.15) showed good deoxygenation performance and reusability under H-2 free conditions.
Article
Chemistry, Multidisciplinary
Vinayak Hanchate, Sudharshan Nagabhushana Reddy, Anil Kumar, Kandikere Ramaiah Prabhu
Summary: The reactivity of sulfoxonium ylide with allyl carbonates and allyl carbamates diverges. Rh(iii)-catalyzed C-H activation and cyclization of sulfoxonium ylide with ally esters leads to the formation of a cyclopropane-fused tetralone derivative via cascade C-H activation, (4+2) annulation, and cyclopropanation. A similar reaction of sulfoxonium ylide with allyl carbamates forms a C3-substituted indanone derivative through a rare and interesting domino C-H activation and (4+1) annulation in which allyl carbamate acts as a C1-synthon.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Kun-Che Kao, An-Chih Yang, Weixin Huang, Chengshuang Zhou, Emmett D. Goodman, Alexander Holm, Curtis W. Frank, Matteo Cargnello
Summary: The study demonstrates a general approach for depositing hydrophobic ligand-stabilized nanocrystals on hydrophilic oxide supports without ligand exchange, achieving high loadings. Surface functionalization of the supports with primary amine groups using organosilane or bonding with aminoalcohols significantly improves the interaction between nanocrystals and supports.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Engineering, Chemical
Thomas Optenhostert, Sissy Puthenkalam, Niklas Stegmann, Michael Steffen, Wolfgang Schmidt
Summary: The study introduces a hydrogen production process that does not require external hydrogen supply, extracting hydrogen directly from the hydrocarbon matrix for desulfurization, resulting in a simplified process management and superior process startup, thus improving process efficiency.
CHEMIE INGENIEUR TECHNIK
(2021)
Article
Chemistry, Physical
Klara S. Kley, Anna Gruenert, Wolfgang Schmidt, Ferdi Schueth
Summary: Oxymethylene ethers are diesel additives that can be produced from renewable energy and CO2. The sulfonated polymer polyether-ether-ketone (S-PEEK) exhibits outstanding catalytic properties in gas-phase synthesis of OMEn, showing high selectivity to OME1 and OME2.
Article
Chemistry, Multidisciplinary
Ezgi Onur Sahin, Yitao Dai, Candace K. Chan, Harun Tueysuez, Wolfgang Schmidt, Joohyun Lim, Siyuan Zhang, Christina Scheu, Claudia Weidenthaler
Summary: Amorphous TixOy with high surface area has shown higher activity as a photocatalyst in UV light-induced water splitting applications. The molecular titanium alkoxide precursor structure rearranged during hydrolysis, leading to increased connectivity of structure-building units. Upon exposure to UV light, the suspension turned dark corresponding to the reduction of Ti4+ to Ti3+. Temperature-dependent total scattering experiments showed partial ordering in the Ti-O environment below 350 degrees C, with the formation of a distorted anatase core above this temperature.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Editorial Material
Chemistry, Multidisciplinary
Hilke Petersen, Steffen Reichle, Sebastian Leiting, Pit Losch, Wolfgang Kersten, Tobias Rathmann, Jochi Tseng, Martin Etter, Wolfgang Schmidt, Claudia Weidenthaler
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Multidisciplinary Sciences
Weixin Huang, Aaron C. Johnston-Peck, Trenton Wolter, Wei-Chang D. Yang, Lang Xu, Jinwon Oh, Benjamin A. Reeves, Chengshuang Zhou, Megan E. Holtz, Andrew A. Herzing, Aaron M. Lindenberg, Manos Mavrikakis, Matteo Cargnello
Summary: The study showed that high-temperature steam pretreatment can enhance the mass-specific reaction rate for carbon-hydrogen (C-H) activation in methane oxidation on palladium catalysts. Experimental and theoretical methods demonstrated that crystal twinning increased grain boundary density, leading to higher reactivity.
Article
Chemistry, Inorganic & Nuclear
Hilke Petersen, Niklas Stegmann, Michael Fischer, Bodo Zibrowius, Ivan Radev, Wladimir Philippi, Wolfgang Schmidt, Claudia Weidenthaler
Summary: Transition-metal phosphates have a wide range of applications and can be used as catalysts, battery materials, and fuel cell membranes. This study successfully determined the structures of two novel titanium pyrophosphates using experimental data, and found that these compounds exhibit good conductivity and potential for electrochemical device applications.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Applied
Hrishikesh Joshi, Alexander Hopf, Pit Losch, Wolfgang Schmidt, Ferdi Schueth
Summary: The measurement of diffusivity within porous solids is crucial for material characterization. This study presents a method for obtaining trends in gas-phase diffusivity of N-2 within different mesoporous materials by establishing correlations between diffusivity and material properties. The simplified model fitted over transient data allows the identification of trends and correlations. This research has potential applications for other adsorptive molecules or different temperatures.
MICROPOROUS AND MESOPOROUS MATERIALS
(2022)
Article
Chemistry, Physical
Hilke Petersen, Jacopo De Bellis, Sebastian Leiting, Saurabh Mohan Das, Wolfgang Schmidt, Ferdi Schueth, Claudia Weidenthaler
Summary: Mechanochemistry is an excellent green synthesis method for preparing various materials, while mechanocatalysis, a new field of catalysis using mechanical forces, has shown promising potential due to its independence on external temperature and pressure. In this study, high-energy operando X-ray powder diffraction experiments and online gas analysis were used to monitor the processes inside the milling vessel during mechanocatalysis, along with a custom-made milling setup and gas dosing system. The feasibility of the experimental setup was demonstrated through the study of CO oxidation using Au@Fe2O3 as a catalyst, which allowed for monitoring of support morphology changes and crystallite size variations of the gold catalyst.
Article
Chemistry, Inorganic & Nuclear
Linda Zhang, Toshiki Wulf, Florian Baum, Wolfgang Schmidt, Thomas Heine, Michael Hirscher
Summary: In this study, ion-exchanged zeolite has been reported as a promising candidate for hydrogen isotope separation. Through systematic investigation, it has been found that the Ag(I)-exchanged zeolite Y exhibits excellent selectivity and adsorption performance, making it suitable for large-scale applications.
INORGANIC CHEMISTRY
(2022)
Article
Chemistry, Physical
Claudia Weidenthaler, Wolfgang Schmidt, Sebastian Leiting, Jan Ternieden, Alexander Kostis, Tolga Han Ulucan, Eko Budiyanto
Summary: This study focuses on the influence of metal loading and synthesis temperatures on the properties of Co@Al2O3 catalysts. The combination of in situ characterization methods provides insights into the structure-property relation of the Co catalyst on the gamma-Al2O3 support. The experiments also highlight the necessity of in situ studies due to the changes in catalyst state after reaction.
Article
Engineering, Chemical
Ozgul Agbaba, Ioan-Teodor Trotus, Wolfgang Schmidt, Ferdi Schueth
Summary: Acetylene was once the main feedstock for the chemical industry, but it was phased out by ethylene and propylene. However, a novel concept has been presented for producing light olefins based on acetylene using copper-exchanged Y-zeolite. This concept shows promise for diversifying the synthesis of critical C4 bulk chemicals.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Chemistry, Multidisciplinary
Abdurrahman Bilican, Priyanka Sharma, Nguyen Khang Tran, Claudia Weidenthaler, Wolfgang Schmidt
Summary: This article reports a method for synthesizing CXs in a time-efficient manner, requiring only 5 hours using hydrothermal gelation and direct carbonization of the wet polymer. The properties of the CXs obtained via this superfast synthesis route are identical to those obtained via conventional routes.
Meeting Abstract
Chemistry, Multidisciplinary
H. Petersen, N. Stegmann, M. Fischer, B. Zibrowius, W. Schmidt, M. Etter, C. Weidenthaler
ACTA CRYSTALLOGRAPHICA A-FOUNDATION AND ADVANCES
(2021)
Meeting Abstract
Chemistry, Multidisciplinary
T. Rathmann, H. Petersen, S. Reichle, M. Etter, A. P. Amrute, W. Schmidt, C. Weidenthaler
ACTA CRYSTALLOGRAPHICA A-FOUNDATION AND ADVANCES
(2021)