Review
Chemistry, Physical
Sarah Freeburne, Brock Hunter, Kirsten Bell, Christian W. Pester
Summary: Heterogeneous photocatalysis combines light chemistry with catalytic platforms to enable re-use of photocatalysts, providing economic, sustainable, safe, and user-friendly chemical syntheses. This review outlines recent developments in heterogeneous photocatalyst design and their use in mediating polymerizations. Four prevalent classes of materials, including nanoparticles, polymer networks, metal organic frameworks (MOFs), and immobilized photocatalysts on solid supports, are explored for their potential in light-mediated reversible deactivation radical polymerization.
Article
Chemistry, Physical
Carlos Lizandara-Pueyo, Xinyuan Fan, Carles Ayats, Miquel A. Pericas
Summary: This study involved the controlled synthesis of calcium carbonate particles surface-functionalized with azido groups, followed by copper-catalyzed alkyne-azide cycloaddition reactions to prepare novel catalytic materials. The immobilized catalyst demonstrated high selectivity and efficiency in catalyzing Michael addition reactions of aldehydes, with the added advantage of being reusable and adaptable to continuous-flow operation for increased productivity.
JOURNAL OF CATALYSIS
(2021)
Review
Chemistry, Multidisciplinary
Chiara Bisio, Fabio Carniato, Matteo Guidotti
Summary: This review provides an overview of the use and role of coordination complexes as precursors for the generation of hybrid catalysts in oxidation reactions for fine chemical synthesis. The understanding of active site formation in hybrid catalysts is emphasized, and different families of coordination precursors are considered. Each example includes a brief analysis of synthesis, characterization, and catalytic performance. Special attention is given to the chemical environment of the active metal center's first coordination sphere. By integrating advantages of both homogeneous and heterogeneous systems, catalysts obtained through heterogenization, grafting, or anchoring of homogeneous catalysts exhibit enhanced catalytic performance. Deposition of coordination complexes onto preformed supports offers a versatile strategy for designing novel catalysts with tailored and controlled properties.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Engineering, Electrical & Electronic
Asif Rasool, R. Amiruddin, Shahnaz Kossar, Mc Santhosh Kumar
Summary: The current research focuses on a hybrid device based on n-ZnO/MoO3/PEDOT:PSS, which can be used for UV light detection and non-volatile resistive switching memory applications. Through the deposition of multi-layered thin films, the fabricated device exhibits good performance characteristics, such as high photoresponsivity and stable endurance.
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
(2022)
Article
Chemistry, Multidisciplinary
Jens Moons, Alexandra Loosen, Charlotte Simms, Francisco de Azambuja, Tatjana N. Parac-Vogt
Summary: Materials with enzyme-like activities and proteolytic potential, such as the Hf6O8-based NU-1000 metal organic framework, are showing promise as robust and effective alternatives to natural enzymes. The Hf-MOF exhibited high selectivity in cleaving protein substrates and maintained hydrolytic activity efficiently. In comparison to the Zr-NU-1000, the Hf variant showed slightly slower reaction rates but greater stability and recyclability, attributed to intrinsic differences between Hf-IV and Zr-IV centers and the lower surface area of Hf-NU-1000.
Article
Chemistry, Applied
Qian Gu, PingPing Jiang, Yirui Shen, Kai Zhang, Phyu Thin Wai, Agus Haryono
Summary: Highly dispersed molybdenum trioxide was loaded into three-dimensional dendritic mesoporous silica nanospheres (MoO3@3D-DMSNs) via a one-pot method. These MoO3@3D-DMSNs showed better catalytic performance for olefin epoxidation, with optimal conditions at a Mo/Si molar ratio of 5%. The catalysts maintained their activity and stability after five reaction-regeneration cycles, demonstrating good potential for catalytic reactions.
JOURNAL OF POROUS MATERIALS
(2021)
Article
Chemistry, Physical
Yo-hei Nagasaki, Masazumi Tamura, Mizuho Yabushita, Yoshinao Nakagawa, Keiichi Tomishige
Summary: The silica-supported molybdenum oxide catalyst showed high efficiency and reusability in the dehydration of various amides. The results of catalyst characterizations and activity tests revealed that the strong acid sites formed by the interaction between silanol groups and molybdenum oxide species, along with the acid-base pair sites, played a crucial role in the dehydration reaction.
Article
Chemistry, Multidisciplinary
Yunlong Zhao, Chen-Fei Liu, Leroy Qi Hao Lin, Albert S. C. Chan, Ming Joo Koh
Summary: In this study, a N-heterocyclic carbene-Ni-I catalytic species was used to achieve highly substituted alkenes from abundant monosubstituted substrates with excellent regio- and stereoselectivities. Trimethylsilyl triflate and trimethylamine additives were added to mediate the reaction, resulting in the generation of trisubstituted boron- and arene-containing trans alkenes. This method represents a significant addition to the toolbox of reactions for the concise synthesis of unsaturated biologically active compounds.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Polymer Science
Eduard Karakhanov, Anton Maximov, Anna Zolotukhina
Summary: This article reviews the recent advances and applications of dendritic catalysis in the past two decades, with a focus on heterogeneous dendrimer-based catalysts. Three main approaches to synthesizing immobilized heterogeneous dendrimer-based catalysts are considered, and magnetically separable dendritic catalysts are also discussed. These dendritic catalysts can be stored as powders and easily separated from the reaction medium, maintaining efficiency similar to homogeneous dendritic catalysts.
Article
Chemistry, Physical
Kaijian Xing, Wei Li, Enrico Della Gaspera, Joel van Embden, Lei Zhang, Steve A. Yianni, Daniel L. Creedon, Tony Wang, Jeffrey C. McCallum, Linjun Wang, Jian Huang, Christopher Pakes, Dong-Chen Qi
Summary: The study demonstrates a simple solution-processed method for depositing a MoO3 layer on H-terminated diamond surface to achieve surface transfer doping, leading to a reduction in sheet resistivity and an increase in hole density. The hole accumulation layer induced by sp-MoO3 is thermally stable up to 450 degrees C and exhibits metallic conductivity with strong spin-orbit interaction in the induced 2D surface conducting layer.
Article
Chemistry, Physical
Rosaria Ciriminna, Mario Pagliaro, Rafael Luque
Summary: This study suggests that the fine chemical and pharmaceutical sectors may soon begin to widely adopt supported transition metal catalysts, thanks to the emergence of new generation supported metal catalysts and flow chemistry. In the future, both heterogenized metal nanoparticles as well as single-site molecular and single-atom catalysts are expected to become common.
GREEN ENERGY & ENVIRONMENT
(2021)
Review
Chemistry, Multidisciplinary
Yiqi Liu, Amol Agarwal, Yosi Kratish, Tobin J. Marks
Summary: In this minireview, we analyze and summarize a less conventional type of SSHC in which molybdenum dioxo species are grafted onto unusual carbon-unsaturated scaffolds, such as activated carbon, reduced graphene oxide, and carbon nanohorns. The choice of earth-abundant, low-toxicity, versatile metal constituents, and various carbon supports illustrates catalyst by design principles and yields insights into new catalytic systems of both academic and technological interest. Here, we summarize experimental and computational investigations of the bonding, electronic structure, reaction scope, and mechanistic pathways of these unusual catalysts.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Energy & Fuels
Adriano Lima da Silva, Ana Flavia Felix Farias, Joao Baptista da Costa Agra de Melo, Alisson Mendes Rodrigues, Simoni Margareti Plentz Meneghetti, Ana Cristina Figueiredo de Melo Costa
Summary: The MoO3 catalyst was successfully synthesized on a pilot scale by combustion reaction, and showed promising catalytic performance in the production of biodiesel, with high conversion to ethyl esters and long activity life. These catalysts have the potential to have positive impacts on the environment and society.
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
(2022)
Article
Chemistry, Physical
Gianvito Vile, Giovanni Di Liberto, Sergio Tosoni, Alessandra Sivo, Vincenzo Ruta, Maarten Nachtegaal, Adam H. Clark, Stefano Agnoli, Yajun Zou, Aleksandr Savateev, Markus Antonietti, Gianfranco Pacchioni
Summary: This study reports the high catalytic performance of a family of Cu-based single-atom catalysts for triazole synthesis. The use of a carbon nitride carrier as a ligand for atomically dispersed copper species improves the catalyst activity and selectivity.
Article
Chemistry, Multidisciplinary
Michael G. J. Doyle, Alexis L. Gabbey, Wesley McNutt, Rylan J. Lundgren
Summary: In this study, electron-deficient arylacetates were utilized as benzyl nucleophile surrogates to successfully generate enantioenriched acyclic molecules containing quaternary carbon centers via a two-step substitution-decarboxylation process. Products were often obtained with >90% ee using a commercially available catalyst.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Inorganic & Nuclear
Siqi Li, Zhipeng Huang, Huifang Liu, Meijiang Liu, Chaofeng Zhang, Feng Wang
Summary: An efficient approach for the synthesis of arylamines from nitroarenes and hydrazine using an iron-molybdenum sulfide catalyst has been presented. The study reveals that the reduction of the nitro group to the nitroso group is the rate-determining step, and it is confirmed that the active H* should be in polar states.
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Multidisciplinary
Lulu Sun, Yike Huang, Shiyang Liu, Xiumei Liu, Nengchao Luo, Feng Wang
Summary: In this study, we show the scission of strong ether C-O bonds promoted by low-work-function Cd single atoms and clusters as photocatalysts. Their loading on ZnS facilitates the breaking of C-H bonds, thus weakening the C-O bond for chemical bond breaking.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Fengan Han, Yanting Liu, Guangyi Li, Lin Yuan, Aiqin Wang, Feng Wang, Tao Zhang, Ning Li
Summary: Zinc molybdate with a disordered layered stacking structure was prepared using an evaporation method and demonstrated excellent catalytic performance for selectively converting lignocellulose-derived ketones to olefins. The outstanding catalytic performance was attributed to its porous structure, higher oxygen vacancy concentration, and higher acidity. Additionally, it also exhibited good catalytic performances for other lignocellulose-derived ketones.
Article
Chemistry, Physical
Puning Ren, Zhuyan Gao, Tiziano Montini, Zhitong Zha, Na Ta, Yike Huan, Nengchao Luo, Emiliano Fonda, Paolo Fornasiero, Feng Wang
Summary: Biomass reforming using solar energy allows for the production of green hydrogen. Current biomass photoreforming inefficiently produces hydrogen due to intermittent solar light and incomplete degradation of biomass C-C bonds. This study overcomes these issues by converting carbohydrates into liquid hydrogen carriers (LHCs) suitable for transportation. The LHCs are then fully decomposed, releasing only H2 and CO2. By prioritizing complete scission of carbohydrate C-C bonds, this process yields 44 g of H2 per kg of glucose. This work demonstrates the production and storage of hydrogen through the complete breakdown of biomass C-C bonds.
Review
Chemistry, Multidisciplinary
Min Wang, Feng Wang, Hongru Zhou
Summary: Biomass exploration is an important topic in renewable energy research. Photocatalytic valorization of biomass into fuels and chemicals is a promising and sustainable method. This article provides a comprehensive review of the research direction of photocatalytic reforming of biomass into syngas (CO + H2) and discusses various strategies and challenges in this field.
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Article
Chemistry, Multidisciplinary
Qingchun Xu, Puning Ren, Yang Peng, Nengchao Luo, Zhuyan Gao, Caixia Meng, Jian Zhang, Feng Wang
Summary: In this study, a catalytic Ni complex was designed to work synergistically with TiO2, enabling the reductive coupling of IEO powered by photo-energy. This photocatalytic process provides 1,4-butanediol with high selectivity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Multidisciplinary
Chaofeng Zhang, Yongcan Jin, Feng Wang, Xiaojun Shen, Jinlan Cheng, Cheng Cai
Summary: This review summarizes the strategies and methods for lignin depolymerization into aromatic chemicals, including traditional methods such as pyrolysis, gasification, liquid-phase reforming, solvolysis, chemical oxidation, and newly developed processes like redox-neutral, biocatalysis, and combinatorial strategies. The mechanisms and key intermediates involved in these strategies are discussed. This review provides a comprehensive overview of lignin depolymerization research, offering useful suggestions for further advancements in this field.
Article
Chemistry, Physical
Kun Zhang, Qiang Guo, Yehong Wang, Pengfei Cao, Jian Zhang, Marc Heggen, Joachim Mayer, Rafal E. Dunin-Borkowski, Feng Wang
Summary: In this work, selective ethylene carbonylation to 3-pentanone was achieved using in situ produced hydrogen via a water-gas shift (WGS) reaction on a defective ceria-supported Rh catalyst. The interface of Rh/CeO2 activates water, CO, and ethylene, facilitating the WGS reaction and ethylene carbonylation. A redox pathway for the WGS reaction was proposed based on in situ FTIR results, and water was confirmed as the hydrogen source for ethylene carbonylation through mass spectrometry (MS) study.
Article
Chemistry, Multidisciplinary
Yafei Liang, Yehong Wang, Zhixin Zhang, Jianyu Han, Jian Zhang, Yuda Zhang, Feng Wang
Summary: A Sn-modified CeO2 catalyst with high catalytic performance in the selective conversion of biomass-derived acetone-n-butanol-ethanol (ABE) fermentation was synthesized via a facile ball milling-pyrolysis strategy. The conversion rate of ABE reached 95% with a liquid selectivity of 82% for 4-heptanone, which was superior to other Sn-modified CeO2 catalysts obtained by conventional methods.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Puning Ren, Yue Zhou, Kaiyi Su, Lulu Sun, Nengchao Luo, Feng Wang
Summary: In this study, a CuOx-loaded Nb2O5 photocatalyst was designed, which selectively catalyzes the oxidation of furfural to produce maleic anhydride and its precursor. By loading CuOx and forming a complex, the catalyst can efficiently absorb visible light to activate furfural, leading to C-C bond cleavage and CO generation. This method provides a mild approach for the production of renewable maleic anhydride.
CHEMISTRY-AN ASIAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Jianyu Han, Jingyi Yang, Zhixin Zhang, Xunzhu Jiang, Wei Liu, Botao Qiao, Junju Mu, Feng Wang
Summary: This research presents a holistic design strategy for multicomponent alloy catalysts and demonstrates the importance of strong metal-support interaction. By establishing a metal atom transport pathway, PtPdCoFe MA with excellent catalytic activity and stability is successfully synthesized at low reduction temperature, and the role of SMSI in the formation of alloy nanoparticles on reducible oxides is revealed.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Xuke Chen, Yu Xia, Zhenyuan Zhang, Lei Hua, Xiuquan Jia, Feng Wang, Richard N. Zare
Summary: Contact between water and oil can result in new chemical reactions, producing CO2, H·, H2, and short-chain hydrocarbons. This reaction is caused by contact electrification at the water-oil microdroplet interface, generating reactive oxygen species.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Yuting Liu, Huifang Liu, Ning Li, Feng Wang
Summary: This study reports a novel photocatalytic strategy for the oxidative C-C cleavage of lignin and β-O-4 derivatives using photoredox organocatalysts. High yields of aromatic aldehydes and phenyl formate were obtained, and mixed binary organic solvents were shown to promote bond cleavage and inhibit over-oxidation side reactions. The absorbance, excitation, and interaction with the lignin model of the photocatalyst in different solvents were investigated, and a C-centered radical intermediate was captured, providing evidence for the direct Cα-Cβ bond cleavage mechanism.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Chemistry, Physical
Jianyu Han, Zhixin Zhang, Zhuoran Xu, Lunhua He, Feiran Shen, Yehong Wang, Xuebin Liu, Meiling Guo, Zaihong Guan, Feng Wang
Summary: The interfaces in heterogeneous catalysts have a crucial role in their performances by providing active sites through synergistic effects or modulating the state of active sites. Constructing abundant interfaces in heterogeneous catalysts is challenging due to the high dispersion required for all catalyst compositions involved in substrate activation. A surface reduction strategy is proposed as a solution to this challenge, where a pyramid-type catalyst, (Pt/4nmCeO(2))/SiO2, with maximized interfacial Pt-CeO2 sites is created. This work aids in the development of heterogeneous catalysts by enabling a high level of control over the local chemical environment within nanomaterials.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Physical
Kun Zhang, Qiang Guo, Yehong Wang, Pengfei Cao, Jian Zhang, Marc Heggen, Joachim Mayer, Rafal E. Dunin-Borkowski, Feng Wang
Summary: In this study, selective ethylene carbonylation to 3-pentanone was achieved using in situ produced hydrogen via a water-gas shift reaction. The interface of Rh/CeO2 activates water, CO, and ethylene and promotes subsequent reactions, including the water-gas shift reaction and ethylene carbonylation. The hydrogen generated from the water-gas shift reaction suppresses hydrogenation and promotes ethylation.
