Article
Chemistry, Multidisciplinary
Yongwei Chen, Sol Ahn, Mohammad Rasel Mian, Xingjie Wang, Qing Ma, Florencia A. Son, Lifeng Yang, Kaikai Ma, Xuan Zhang, Justin M. Notestein, Omar K. Farha
Summary: Solid supports play a crucial role in heterogeneous catalysis, but their specific effects remain challenging to elucidate. In this study, metal-organic frameworks (MOFs) with 8-connected Zr-6 nodes were used as supports to deposit molybdenum(VI) and investigate the effects of pore environment and topology on the resulting catalysts. It was found that by modulating the chemical environments of the deposited molybdenum species, the catalytic activity and structure can be changed. This work demonstrates the importance of using MOF supports to construct heterogeneous catalysts and elucidate structure-activity relationships in reactions.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Review
Chemistry, Physical
Iuliana M. Chirica, Anca G. Mirea, Stefan Neatu, Mihaela Florea, Michel W. Barsoum, Florentina Neatu
Summary: MAX phases and MXenes are materials with great potential in heterogeneous catalytic applications, as evidenced by their unique properties and proven effectiveness in various processes.
JOURNAL OF MATERIALS CHEMISTRY A
(2021)
Review
Chemistry, Multidisciplinary
Kai Wang, Chen Han, Zongping Shao, Jieshan Qiu, Shaobin Wang, Shaomin Liu
Summary: This review comprehensively elaborates the advances of perovskite oxides in advanced oxidation processes (AOPs) for water remediation, providing insights into their performance, structure, and tuning methods. Strategies for designing novel perovskite oxides to enhance catalytic activities in AOPs have been highlighted.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Nanoscience & Nanotechnology
Hengzhou Liu, Jiaqi Yu, Yifu Chen, Jungkuk Lee, Wenyu Huang, Wenzhen Li
Summary: Electrocatalytic oxidative dehydrogenation (EOD) of aldehydes allows for the production of bipolar H-2 at ultra-low voltage with carboxylic acid co-generation. This study presents a simple galvanic replacement method to prepare CuM (M = Pt, Pd, Au, and Ag) bimetallic catalysts, enabling industrially relevant current densities in the EOD of furfural. The incorporation of noble metals onto the Cu surface and the subsequent enlargement of its surface area significantly improve the EOD performance, with CuPt achieving a record-high current density of 498 mA cm(-2) and a Faradaic efficiency of >80% to H-2 at a low cell voltage of 0.6 V. Further research is required to understand the synergistic effects of Cu-M on furfural EOD and enhance the catalyst stability, thus facilitating the future production of green hydrogen and carbon chemicals with practical rates and low-carbon footprints.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Hannah Rogers, Isaac T. Daniel, Simon J. Freakley
Summary: In this study, a novel catalyst Pd/TiO2 is reported for the acceptorless dehydrogenation of 1-phenylethanol, leading to the production of acetophenone and molecular hydrogen. The catalyst exhibits significantly higher catalytic activity and comparable selectivity compared to commercially available catalysts.
CATALYSIS COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Akash Kaithal, Basujit Chatterjee, Christophe Werle, Walter Leitner
Summary: The acceptorless dehydrogenation of methanol to carbon monoxide and hydrogen using homogeneous molecular complexes, particularly those containing ruthenium and manganese with the MACHO ligand framework, showed promising catalytic activities. The metal complex was found to mediate the initial fast dehydrogenation of methanol to formaldehyde and methyl formate followed by subsequent slow decarbonylation, resulting in gas mixtures with varying CO/H2 ratios.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Samira Zafarnak, Ali Bakhtyari, Hamed Taghvaei, Mohammad Reza Rahimpour, Adolfo Iulianelli
Summary: This study evaluates the carbon-dioxide-assisted dehydrogenation over alumina-supported catalysts, with particular focus on the performance of cobalt and molybdenum oxide catalysts in ethylene production. Time on steam effect on catalyst performance was also investigated.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Chemistry, Physical
Zhongliang Yu, Yanyan Yang, Song Yang, Jie Zheng, Xiaogang Hao, Guoqiang Wei, Hongcun Bai, Abuliti Abudula, Guoqing Guan
Summary: Efficient dehydrogenation of aqueous formic acid (FA) for hydrogen production using non-noblemetal-based heterogeneous catalysts remains challenging. In this study, a biomass-derived multifunctional gamma-Mo2N catalyst was synthesized and showed high dehydrogenation activity for aqueous FA, without significant deactivation during stability testing. Mechanism investigations revealed that the catalyst's active sites and cooperation played a crucial role in the dehydrogenation activity.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2022)
Article
Chemistry, Physical
Qian Wang, Jialing Lan, Rong Liang, Yihao Xia, Lei Qin, Lung Wa Chung, Zhiping Zheng
Summary: In this study, a new application of the Grubbs catalysts in hydrogen production from aqueous-phase methanol reforming was reported, showing that the G-III catalyst achieved the best performance among those tested and can also be used for other dehydrogenation reactions. Mechanistic studies and DFT calculations revealed an unusual substrate-assisted metathesis pathway, shedding light on the reaction mechanism and suggesting new opportunities in catalyst design for clean and renewable energies.
Article
Engineering, Chemical
Xia Zhang, Haibo Wang, Lianke Gou, Lanpeng Li, Aijun Duan, Zhengkai Cao
Summary: The study showed that serial VPO catalysts with different activation temperatures exhibited varying species proportions and surface properties, with the S-405 catalyst demonstrating the highest conversion and selectivity for n-butane oxidation.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2021)
Article
Chemistry, Multidisciplinary
Ali Bakhtyari, Samira Zafarnak, Hamed Taghvaei, Mohammad Reza Rahimpour, Adolfo Iulianelli
Summary: The demand for hydrogen and olefins production has driven the exploration of new and multipurpose processes, with a focus on utilizing carbon dioxide emissions. This study examines the carbon-dioxide-assisted conversion of ethane to ethylene and hydrogen over alumina-supported cobalt-molybdenum catalysts. The highest initial conversions and hydrogen yield were achieved at 700℃ and GHSV = 2250 Lreactant/kgcatalyst.hr.
JOURNAL OF CO2 UTILIZATION
(2021)
Article
Chemistry, Multidisciplinary
Jian Wang, He Liu, Shiguang Fan, Shuai Wang, Guanjun Xu, Aijun Guo, Zongxian Wang
Summary: In this study, a series of active metals loaded on nitrogen-doped carbon were prepared to investigate their roles in the dehydrogenation of cycloalkanes, with Pt/CN showing the highest catalytic activity. The differences in catalytic activity between different active metals diminish with increasing temperature, indicating a thermodynamic effect. Additionally, optimizing the alkyl substituents on cyclohexane can enhance the dehydrogenation activity and hydrogen production rate.
Article
Chemistry, Applied
Natalia Llopis, Patricia Gisbert, Alejandro Baeza, Jara Correa-Campillo
Summary: This study describes the oxidative dehydrogenation of N-heterocyclic compounds using H2O2 as an oxidant in combination with polar solvents such as 1,1,1,3,3,3-hexafluoroisopropanol (HFIP) and H2O. The best yields for heteroaromatic compounds were generally achieved in HFIP, but it is surprising that using a non-toxic solvent like H2O also gave good yields. Additionally, this method can be implemented on a larger scale and the HFIP solvent can be reused.
ADVANCED SYNTHESIS & CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
Md Arifur Rahim, Jianbo Tang, Andrew J. Christofferson, Priyank Kumar, Nastaran Meftahi, Franco Centurion, Zhenbang Cao, Junma Tang, Mahroo Baharfar, Mohannad Mayyas, Francois-Marie Allioux, Pramod Koshy, Torben Daeneke, Christopher F. McConville, Richard B. Kaner, Salvy P. Russo, Kourosh Kalantar-Zadeh
Summary: Understanding the interactions between metal and matrix in metal-matrix catalytic systems can enhance the catalytic activity of isolated metal atoms. In this study, it was found that a trace amount of platinum dissolved in liquid gallium can drive catalytic reactions with enhanced kinetics at low temperature. Molecular simulations showed that the platinum atoms remained unchanged in the gallium matrix and activated the surrounding gallium atoms for catalysis. The liquid catalyst system exhibited significantly higher activity compared to existing solid platinum catalysts, setting a foundation for future exploration of high-throughput catalysis.
Article
Chemistry, Physical
Huafan Li, Nan Zhou, Tianli Zhu, Hailian Tang, Guoyi Bai
Summary: This study reported a Ni-catalyst supported on H2O2 modified nanodiamonds (NDs) which exhibited much improved catalytic activity and stability for the phenol hydrogenation reaction compared to the other two catalysts with untreated NDs and high temperature N-2 treated NDs as supports. The interaction between the ND support and nickel species was enhanced by simple H2O2 pretreatment while maintaining the excellent structural stability of the ND. This study emphasizes the importance of support selection and pretreatment, and offers new insights for the design and development of supported catalysts.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Article
Materials Science, Multidisciplinary
Thierry K. Slot, Fang Yue, Hualong Xu, Enrique Ramos-Fernandez, Antonio Sepulveda-Escribano, Zdenek Sofer, Gadi Rothenberg, N. Raveendran Shiju
Summary: This study investigates the use of MXenes as supports for platinum nanoparticles in the hydrolysis of ammonia borane. Oxidizing the surface of MXene can modify the electronic environment of platinum, enhancing its catalytic activity. These findings provide a new approach to developing active catalysts for energy-related reactions.
Article
Physics, Applied
E. J. Devid, M. Ronda-Lloret, D. Zhang, E. Schuler, D. Wang, C-H Liang, Q. Huang, G. Rothenberg, N. R. Shiju, A. W. Kleyn
Summary: Introducing metal meshes into radio frequency-driven plasma reactors significantly increases the relative reaction yield of CO2 splitting, while supported metal oxide catalysts have no effect. The metal mesh plays a dual role as a catalyst for both direct CO2 dissociation and oxygen recombination.
JOURNAL OF APPLIED PHYSICS
(2021)
Article
Energy & Fuels
Jasper Biemolt, John C. Douglin, Ramesh K. Singh, Elena S. Davydova, Ning Yan, Gadi Rothenberg, Dario R. Dekel
Summary: This study presents a unique anion-exchange membrane fuel cell (AEMFC) that only contains affordable and abundant materials, with high catalytic activity without the use of precious metals and critical raw materials, marking it as one of the best CRM-free AEMFCs reported to date.
Article
Materials Science, Multidisciplinary
Thierry K. Slot, Varun Natu, Enrique Ramos-Fernandez, Antonio Sepulveda-Escribano, Michel Barsoum, Gadi Rothenberg, N. Raveendran Shiju
Summary: MXenes are a new family of two-dimensional carbides and/or nitrides with O, OH and/or F atoms terminating their 2D surfaces. Ti3C2Tx, the most studied compound of the MXene family, is demonstrated to be a good acid catalyst for various reactions, with the catalytic activity and selectivity being influenced by surface modifications. A thin oxide layer on the Ti3C2Tx surface is essential for catalyzing ring-opening reactions.
Article
Chemistry, Physical
Thierry K. Slot, Paula Oulego, Zdenek Sofer, Yuelei Bai, Gadi Rothenberg, N. Raveendran Shiju
Summary: MAX phases, including MXenes, demonstrate potential for high-temperature catalysis, while an open, disordered structure as a support can enhance catalytic activity at metal active sites.
Article
Chemistry, Multidisciplinary
Maria Ronda-Lloret, Liuqingqing Yang, Michelle Hammerton, Vijaykumar S. Marakatti, Moniek Tromp, Zdenek Sofer, Antonio Sepulveda-Escribano, Enrique Ramos-Fernandez, Juan Jose Delgado, Gadi Rothenberg, Tomas Ramirez Reina, N. Raveendran Shiju
Summary: MAX phases are attractive for catalysis applications due to their unique set of properties, such as high thermal stability and good conductivity like metals. The Ti(3)AlC(2) MAX phase as a support for molybdenum oxide showed better performance in the reverse water-gas shift reaction compared to traditional materials, due to its outstanding electronic properties and the charge transfer effect from the MAX phase to the catalyst surface.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2021)
Article
Multidisciplinary Sciences
Xiaoyu Yan, Jasper Biemolt, Kai Zhao, Yang Zhao, Xiaojuan Cao, Ying Yang, Xiaoyu Wu, Gadi Rothenberg, Ning Yan
Summary: Electrochemical water splitting is a sustainable method for generating hydrogen, but traditional and emerging electrolyzers face efficiency and cost challenges. The membrane-free flow electrolyzer designed by the authors allows for efficient water splitting at high current densities. By combining the advantages of different electrolyzer concepts, the study paves the way for sustainable hydrogen generation.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Physical
Frances Pope, Noe Watson, Antoine Deblais, Gadi Rothenberg
Summary: Alkali metal borohydrides are promising materials for large-scale hydrogen storage. This study investigates the physical and chemical properties of self-hydrolysis solutions by monitoring the hydrogen evolution, pH changes, and reaction intermediates using NMR. Higher concentrations of borohydride lead to significant changes in the system's microstructure and result in non-Newtonian behavior.
Article
Chemistry, Physical
Petrus C. M. Laan, Felix J. de Zwart, Emma M. Wilson, Alessandro Troglia, Olivier C. M. Lugier, Norbert J. Geels, Roland Bliem, Joost N. H. Reek, Bas de Bruin, Gadi Rothenberg, Ning Yan
Summary: In this study, the reactivity and selectivity of two forms of NiOOH (beta-NiOOH and gamma-NiOOH) were examined using three typical alcohols as model reactions. The results showed that the solvent had an effect on the reaction rate of beta-NiOOH but not on its selectivity. Moreover, high concentrations of OH(-) in aqueous solvent promoted the conversion of benzyl alcohol to benzoic acid. The mechanism of oxidative dehydrogenation of benzyl alcohol to benzaldehyde was also elucidated. This work highlights the unique oxidative and catalytic properties of NiOOH in alcohol oxidation reactions and contributes to the mechanistic understanding of electrochemical alcohol conversion using NiOOH-based electrodes.
Article
Chemistry, Physical
Martijn J. Mekkering, Gadi Rothenberg, Hong Zhang, Ning Yan
Summary: Single-atom catalysts (SACs) have high metal loading and strong metal-support interaction, making them advantageous for photochemical conversions.
Article
Chemistry, Multidisciplinary
Petrus C. M. Laan, Eduard O. Bobylev, Felix J. de Zwart, Joppe A. Vleer, Alessandro Troglia, Roland Bliem, Gadi Rothenberg, Joost N. H. Reek, Ning Yan
Summary: Controlling the coordination sphere of heterogeneous single-metal-site catalysts is a difficult task, but immobilizing supramolecular cages to control the ligand design of the primary- and secondary coordination spheres allows for fine-tuning of catalytic properties. The study of the hydrolysis of ammonia borane revealed that placing a well-defined reaction pocket around the active site can enhance catalytic performance, resulting in diffusion-controlled reaction kinetics.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Jasper Biemolt, Eva J. Meeus, Felix J. de Zwart, Jeen de Graaf, Petrus C. M. Laan, Bas de Bruin, Thomas Burdyny, Gadi Rothenberg, Ning Yan
Summary: Immobilizing molecular catalysts on electrodes is crucial for electrochemical applications. The study demonstrates a bottom-up approach for constructing a conjugated C-C bond between the Vulcan carbon electrode and an organometallic catalyst without introducing any foreign elements. The synthesized catalyst exhibits high activity and selectivity for the oxygen reduction reaction compared to the homogeneous counterpart, making it a promising candidate for electrochemical applications.
Article
Chemistry, Multidisciplinary
Frances Pope, Jeffrey Jonk, Millie Fowler, Petrus C. M. Laan, Norbert J. Geels, Larissa Drangai, Vitaly Gitis, Gadi Rothenberg
Summary: The safety concern of using large amounts of compressed or liquid hydrogen in a transition to a hydrogen economy can be addressed by using chitosan as a catalyst support. Chitosan spheres encapsulating cobalt catalysts remain stable at high reaction pH, and show high catalytic activity and reusability.
Article
Chemistry, Multidisciplinary
Zheng Wei, Tanja Knaus, Yuxin Liu, Ziran Zhai, Andrea F. G. Gargano, Gadi Rothenberg, Ning Yan, Francesco G. G. Mutti
Summary: We developed a highly efficient biosensor for uric acid detection by immobilizing modified urate oxidase on gold nanoparticles deposited on a carbon-glass electrode. This biosensor exhibits a low limit of detection (9.16 nM), a high sensitivity (14 mu A/mu M), a wide linear range (50 nM-1 mM), and a long lifetime of over 28 days.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Martijn J. Mekkering, Jasper Biemolt, Jeen de Graaf, Yi-An Lin, Nicolaas P. van Leest, Alessandro Troglia, Roland Bliem, Bas de Bruin, Gadi Rothenberg, Ning Yan
Summary: This study demonstrates that the agglomeration of isolated atom sites can be prevented by dissolution/exsolution of metal atoms into/from the support in the case of Rh/Al2O3 single-atom catalysts. A series of catalysts are designed, synthesised and characterised to study the impact of exsolution in the dry reforming of methane. The catalysts' performance improves with increasing reaction time due to the migration of rhodium atoms from the subsurface to the surface. The main factor affecting catalyst performance is atom migration, despite the changes in rhodium oxidation state during catalysis. The implications of these results for real-life catalyst preparation are discussed.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)