Article
Multidisciplinary Sciences
Wei Wang, Sai Chen, Chunlei Pei, Ran Luo, Jiachen Sun, Hongbo Song, Guodong Sun, Xianhui Wang, Zhi-Jian Zhao, Jinlong Gong
Summary: By coupling chemical looping-selective hydrogen combustion and multifunctional catalysts, we achieved high propylene selectivity in the direct propane dehydrogenation reaction. The reaction mechanism is influenced by the proximity between the dehydrogenation and combustion sites.
Article
Chemistry, Multidisciplinary
Bo Sheng, Yangen Xie, Qi Zhao, Hua Sheng, Jincai Zhao
Summary: This study presents a specific strategy for optimizing H2O2 photosynthesis by modulating proton supplementation. By synthesizing a photocatalyst with enriched hydroquinone content, it demonstrates higher efficiency and more efficient utilization of oxygen.
ENERGY & ENVIRONMENTAL SCIENCE
(2023)
Article
Chemistry, Analytical
Fuxing Kang, Wei Yang, Mengwen Guo, Lars Borregaard Pedersen, Lars Peter Nielsen
Summary: Monitoring PH3 flux at the Earth's surface-atmosphere interface is a challenging task. A new amperometric PH3 microsensor with high selectivity and sensitivity is developed for in situ detection in aquatic or sedimentary environments. The sensor uses a Au-coated Pt working electrode and a Pt guard electrode, and employs a two-layer silicone membrane to selectively oxidize PH3 into H3PO4, producing a current proportional to the PH3 concentration (>2 nmol center dot L-1). The sensor is designed to eliminate interferences from H2S and other gases, making it suitable for environmental monitoring. A sedimentary profile example demonstrates the presence of high PH3 accumulations 13 mm below the sediment surface.
ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Analytical
Fuxing Kang, Wei Yang, Mengwen Guo, Lars Borregaard Pedersen, Lars Peter Nielsen
Summary: Developing a PH3 microsensor with high selectivity and sensitivity is crucial for monitoring PH3 in aquatic or sedimentary environments. The sensor utilizes an Au-coated Pt working electrode and Pt guard electrode to selectively oxidize PH3, generating a current proportional to its concentration. By eliminating major H2S disruptors, the effects of other gases on the microsensor can be ignored.
ANALYTICAL CHEMISTRY
(2023)
Review
Chemistry, Physical
Chinedu J. Okere, James J. Sheng
Summary: To achieve net-zero emissions by 2050, the conversion of petroleum reservoirs into hydrogen sources through in-situ combustion, gasification, and biodegradation is a promising option. This technique involves hydrogen separation using a hydrogen-permeable membrane installed in the wellbore. However, there are challenges to overcome, such as developing efficient downhole membranes, optimizing reservoir temperature, and preventing hydrogen-consuming reactions. Extensive pilot studies and collaborative efforts are needed to realize sustainable and clean hydrogen production from petroleum reservoirs.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2023)
Article
Chemistry, Multidisciplinary
Princewill M. Ikpeka, Johnson O. Ugwu
Summary: Researchers from the University of Calgary have developed an innovative method of producing hydrogen from hydrocarbon reservoirs while keeping the associated by-products in the reservoir. This method has many beneficial properties to the environment and could be used as a framework to design experimental analysis. The combustion model reveals an upward trending sinusoidal relationship between steam-carbon ratio and the amount of hydrogen yield from an in situ hydrogen production study.
Article
Thermodynamics
Florian Meyer, Christian Eigenbrod, Volker Wagner, Wolfgang Paa, James C. Hermanson, Shion Ando, Marc Avila
Summary: The combustion of liquid oxygen droplets in gaseous hydrogen under microgravity conditions is investigated experimentally. The study provides insights into spray combustion processes in rocket engines, discussing the effects of pressure on the flame standoff ratio and burning rate constant.
COMBUSTION AND FLAME
(2022)
Article
Engineering, Biomedical
Andre J. van der Vlies, Masoud Ghasemi, Bernadette M. Adair, James H. Adair, Enrique D. Gomez, Urara Hasegawa
Summary: Hydrogen sulfide (H2S) is a gaseous signaling molecule with regulatory roles in cancer cell proliferation and migration, making it of interest in cancer therapy. Controlled delivery of H2S has been a challenge, but polymeric micelles containing H2S donating groups offer a solution. These micelles release H2S upon oxidation by reactive oxygen species (ROS) present inside cancer cells, with the release profiles controlled by changing the polymer design. In vitro and in vivo experiments demonstrate that micelles with moderate H2S release rates have the strongest anti-proliferative effect in human colon cancer cells and the chick chorioallantoic membrane cancer model, while not affecting human umbilical vein endothelial cell proliferation. This study highlights the importance of fine-tuning H2S release profiles using a micelle approach for maximizing the therapeutic potential of H2S in cancer treatment.
ADVANCED HEALTHCARE MATERIALS
(2023)
Article
Chemistry, Physical
Xiao Huang, Min Song, Jian Zhang, Jingjing Zhang, Wei Liu, Chang Zhang, Wang Zhang, Deli Wang
Summary: This study investigates the H2O2 electrosynthesis performance of three MXene materials and finds that MXenes exhibit excellent two-electron ORR catalytic activity and high stability. Among them, Nb2CTx catalyst shows the best performance with high H2O2 production and rapid organic dye decoloration ability.
Article
Thermodynamics
Beilin Zuo, Shuai-Zhong Wang, Sulan Yang, Peijin Liu, Qi-Long Yan
Summary: Si@NC/AP and Si@PVDF/CL-20 composites with different Si contents were fabricated by spray-drying technique. Their flame structure, ignition delay time, and combustion process were investigated. The results showed that the Si-based fuel with 40 wt% of Si had the shortest ignition delay time. The core-shell structured composites exhibited better combustion performance with lower burn rate and slightly lower pressure exponent, as well as more fluffy combustion products.
COMBUSTION AND FLAME
(2022)
Article
Thermodynamics
Mohamed Amine Ifticene, Keju Yan, Qingwang Yuan
Summary: This paper introduces an emerging technology for hydrogen production, which generates hydrogen directly from petroleum reservoirs through in-situ combustion gasification. By using hydrogen-selective membranes to separate pure hydrogen, this technology achieves zero carbon emissions. It shows promising potential for large-scale environmentally friendly hydrogen production and discusses the scientific challenges and key aspects of its application.
ENERGY CONVERSION AND MANAGEMENT
(2023)
Article
Chemistry, Physical
Hongcen Yang, Fei Ma, Niandi Lu, Shuhao Tian, Guo Liu, Ying Wang, Zhixia Wang, Di Wang, Kun Tao, Hong Zhang, Shanglong Peng
Summary: By embedding transition metal single atoms (TM SAs) in g-C3N4 nanosheets (CNNS), the selectivity and activity for the 2e(-) ORR can be enhanced, leading to the production of H2O2. Ni0.10 SA/CNNS exhibits the best selectivity and highest yield among the TM SA/CNNS catalysts.
NANOSCALE HORIZONS
(2023)
Article
Energy & Fuels
Fatih Gulec, Jude A. Okolie, Peter T. Clough, Ahmet Erdogan, Will Meredith, Colin E. Snape
Summary: Chemical looping combustion is an advanced combustion process that uses metal oxides as oxygen carriers for fuel combustion and re-oxidizes reduced metal oxides in an air reactor. This research comprehensively studied the low-temperature oxidation of hydrogen using CuO, Co3O4, and Mn2O3 as oxygen carriers, and proposed potential reduction stages for safe hydrogen combustion for space heating.
JOURNAL OF THE ENERGY INSTITUTE
(2023)
Article
Chemistry, Inorganic & Nuclear
Baijie Xu, Qian Xu, Quanzhong Wang, Zhen Liu, Ruikun Zhao, Dandan Li, Pengtao Ma, Jingping Wang, Jingyang Niu
Summary: The copper-containing polyoxometalate-based metal-organic framework HENU-7 showed excellent catalytic performance for the oxidation of diphenylmethane, with high conversion rate and selectivity to benzophenone. In addition, the material demonstrated stability for multiple reuses and the ability to catalyze the oxidation of different benzylic compounds.
INORGANIC CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Xiang Zheng, Chuanhui Zhang, Dongsen Mao, Haifang Mao, Jun Yu
Summary: A series of Mn3Co16Ox composite oxide catalysts were prepared using different manganese precursors, which showed variable catalytic activities and physicochemical properties depending on the precursors. The optimal catalytic performance of Mn3Co16Ox-A was attributed to its larger surface area, higher reducibility and oxygen mobility, and more oxygen vacancies.
NEW JOURNAL OF CHEMISTRY
(2022)
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)
Article
Chemistry, Multidisciplinary
Xuemei Liu, Chaonan Cui, Shuoshuo Wei, Jinyu Han, Xinli Zhu, Qingfeng Ge, Hua Wang
Summary: This study presents a new strategy for designing efficient photocatalysts that can convert CO2 into hydrocarbons by utilizing synergistic catalytic sites. The findings provide a solution for the selective photocatalytic reduction of CO2 to CH4.
Article
Chemistry, Multidisciplinary
Chengxian Hu, Dan Wang, Lu Wang, Ying Fu, Zhengyin Du
Summary: A novel one-pot, three-component reaction conducted under electrochemical conditions was studied. The reaction involved 2-aminothiophenols, aldehydes, and malononitrile, using TBABF4 as an electrolyte and CuI as a catalyst. The proposed reaction mechanism suggested that CuI served as an electron relay. This method offers simplified operation, high atom economy, and mild reaction conditions.
Article
Chemistry, Multidisciplinary
Zhi Yang, Yu Chen, Linxi Wan, Yuxiao Li, Dan Chen, Jianlin Tao, Pei Tang, Fen-Er Chen
Summary: A highly enantioselective method for the complete hydrogenation of pyrimidinium salts using Ir/(S,S)-f-Binaphane complex as the catalyst was developed. This method provides easy access to fully saturated chiral hexahydropyrimidines, which are prevalent in many bioactive molecules. The reactions exhibit high yields and enantioselectivities under mild reaction conditions without additives. Successful application of this methodology in a continuous flow fashion further extends its practical utility.
Article
Chemistry, Multidisciplinary
Tina Jeoh, Jennifer Danger Nill, Wujun Zhao, Sankar Raju Narayanasamy, Liang Chen, Hoi-Ying N. Holman
Summary: In this study, the enzymatic hydrolysis of cellulose was investigated using real-time infrared spectromicroscopy. The spatial heterogeneity of cellulose was found to impact the hydrolysis kinetics. Hydration affected cellulose ordering, and Cel7A preferentially removed less extensively hydrogen bonded cellulose.
Article
Chemistry, Multidisciplinary
Tiphaine Richard, Walid Abdallah, Xavier Trivelli, Mathieu Sauthier, Clement Dumont
Summary: An effective method of grafting functionalities onto lignin based on glycerol carbonate has been developed using an efficient nickel-catalysed telomerisation reaction. This method allows lignin to have new reactive functions and reduces the glass transition temperatures of modified lignins, thereby expanding the application range of lignin-based resins.
Article
Chemistry, Multidisciplinary
Jing Qi, Xiyan Wang, Gan Wang, Srinivas Reddy Dubbaka, Patrick ONeill, Hwee Ting Ang, Jie Wu
Summary: This study presents a green and environmentally friendly approach for the synthesis of imides using electrocatalytic oxidation with H2O as the oxygen source. The method eliminates the need for toxic or expensive oxidants and achieves high yields under mild reaction conditions. It shows broad substrate compatibility and potential for industrial applications.
Article
Chemistry, Multidisciplinary
Babasaheb Sopan Gore, Lin-Wei Pan, Jun-Hao Lin, Yi-Chi Luo, Jeh-Jeng Wang
Summary: Here, we report a visible light-promoted intramolecular radical cascade reaction for the construction of fluorenol and naphthalene-fused cyclopropyl carbaldehyde derivatives. This method offers mild reaction conditions, a broad substrate scope, excellent step efficiency, and scalability, without the need for external chemical oxidants. The novelty of this protocol was demonstrated by synthesizing chrysene analogs and performing late-stage functionalizations.
Article
Chemistry, Multidisciplinary
Juho Antti Sirvio, Idamaria Romakkaniemi, Juha Ahola, Svitlana Filonenko, Juha P. Heiskanen, Ari Ammala
Summary: This article discusses the method of using supramolecular interaction between an aromatic hydrogen bond donor and lignin to achieve rapid delignification of softwood at low temperatures.
Article
Chemistry, Multidisciplinary
Yunyan Meng, Chunxiang Pan, Na Liu, Hongjiang Li, Zixiu Liu, Yao Deng, Zixiang Wei, Jianbin Xu, Baomin Fan
Summary: A novel visible light-driven synthesis method for 2,3-diamines has been developed, which has mild conditions, avoids the use of metal reagents, and can synthesize diamines and diols in one pot.
Article
Chemistry, Multidisciplinary
Mingqing Huang, Haiyang Huang, Mengyao You, Xinxin Zhang, Longgen Sun, Chao Chen, Zhichao Mei, Ruchun Yang, Qiang Xiao
Summary: A direct air-oxidized strategy for the synthesis of benzo[b]phosphole oxides was developed in this study. Arylphosphine oxides were transformed into phosphinoyl radicals, which were further combined with various alkynes to achieve the desired products. DFT calculations revealed the mechanism of phosphinoyl radical formation.
Article
Chemistry, Multidisciplinary
Anwei Wang, Jiayin Huang, Chunsheng Zhao, Yu Fan, Junfeng Qian, Qun Chen, Mingyang He, Weiyou Zhou
Summary: This study demonstrates an innovative strategy for the aerobic oxidation of C(sp(3))-H bonds using gamma-valerolactone. By optimizing the reaction conditions and utilizing specific catalysts, efficient oxidation of C(sp(3))-H bonds is achieved with good chemoselectivity in certain cases.
Article
Chemistry, Multidisciplinary
Shun Li, Likai Tong, Zhijian Peng, Bo Zhang, Xiuli Fu
Summary: Sulfide compounds show promise as electrocatalysts for water splitting, but their performance is limited by factors such as limited active sites and hindered substance transport. This study successfully prepared a high-entropy sulfide (ZnCoMnFeAlMg)(9)S-8, which reduced grain size and increased specific surface area, enabling the realization of a dual-functional catalyst with multiple catalytic sites. High entropy also modulated the electronic properties of sulfides, reducing the potential energy barrier for hydrolysis. This research introduces a new approach for functionalizing high entropy nanomaterials and improves the performance of water splitting catalysts.