Article
Chemistry, Physical
Ida Ziccarelli, Raffaella Mancuso, Francesco Giacalone, Carla Calabrese, Valeria La Parola, Alex De Salvo, Nicola Della Ca', Michelangelo Gruttadauria, Bartolo Gabriele
Summary: This article reports the successful heterogenization of the classical PdI(4)(2-)carbonylation catalyst on multi-walled carbon nanotubes. The newly developed heterogeneous catalyst shows good activity and recyclability in the oxidative monoaminocarbonylation reaction, with limited metal contamination in the final organic compounds.
JOURNAL OF CATALYSIS
(2022)
Article
Chemistry, Multidisciplinary
Yandi Shi, Fan Liao, Wenxiang Zhu, Huixian Shi, Kui Yin, Mingwang Shao
Summary: This study presents a new and efficient nickel-based catalyst with an anodized nickel passivation film formed on the surface of nickel sheet using carbon dots as a co-catalyst. The catalyst exhibited low overpotential and high output energy under current density conditions, with the main advantage being the increase in charge-transfer capacity and promotion of oxidation of carbonaceous intermediates.
CHINESE JOURNAL OF CHEMISTRY
(2021)
Article
Chemistry, Multidisciplinary
Yandi Shi, Fan Liao, Wenxiang Zhu, Huixian Shi, Kui Yin, Mingwang Shao
Summary: In this study, a high efficient nickel-based catalyst for ethanol oxidation, Ni-APF/CDs, was shown to have low overpotential and high peak current density at a current density of 110 mA·cm(-2), reducing electrode thermal loss and increasing output energy. The carbon dots (CDs) in the system mainly function in increasing charge-transfer capacity and promoting the oxidation of carbonaceous intermediates.
CHINESE JOURNAL OF CHEMISTRY
(2021)
Article
Chemistry, Physical
Shi He, Yufeng Chen, Mengdi Wang, Hanggai Nuomin, Peter Novello, Xueqian Li, Siyuan Zhu, Jie Liu
Summary: Ammonia is a promising hydrogen mediator that reduces the cost of hydrogen transportation, but improvements are needed for extracting hydrogen. Ammonia electrolysis is a convenient method for low-cost hydrogen production. Nickel-cobalt nitride nanosheets show high electrocatalytic activity for the ammonia oxidation reaction in non-aqueous solutions.
Article
Chemistry, Physical
M. Nur Hossain, Syed Ahmad, Heinz-Bernhard Kraatz
Summary: A facile one-step synthesis route was reported to fabricate coinage metal nano-dendrites through a tailored galvanic replacement reaction, exhibiting unique morphology and superior catalytic activity, especially the Au NDs showing the highest performance.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2021)
Article
Chemistry, Multidisciplinary
Lucy J. T. Metzroth, Elisa M. Miller, Andrew G. Norman, Sadegh Yazdi, Gerard Michael Carroll
Summary: Exploiting the high surface-area-to-volume ratio of nanomaterials to store energy in the form of electrochemical alloys shows promise, but nanoscale-specific properties affect the absorption and desorption of energy carrying equivalents. Adding an ultrathin platinum shell to the surface of palladium can greatly enhance hydrogen absorption rates and facilitate diffusion across the entire surface.
Article
Energy & Fuels
Haoyu Xiao, Shujiang Li, Zhen Shi, Cunhao Cui, Sunwen Xia, Yingquan Chen, Zhongyue Zhou, Xin Tu, Xu Chen, Haiping Yang, Hanping Chen
Summary: Plasma-catalytic pyrolysis is a promising technology for upgrading plastic waste and producing hydrogen and high-value carbon materials. This study investigated the role of plasma in the pyrolysis of polypropylene (PP) and found that plasma can further activate and cleave the pyrolysis volatiles, resulting in more active carbon species for the growth of carbon nanotubes (CNTs). Compared to conventional catalytic pyrolysis, plasma addition significantly reduced the formation temperature of CNTs and promoted the conversion of liquid and gaseous products to CNTs and hydrogen. The addition of plasma also improved the graphitization degree of CNTs and reduced their defectivity. The findings highlight the potential of plasma-catalytic pyrolysis for the valorization of plastic waste.
Article
Chemistry, Multidisciplinary
Dan Wu, Jie Hao, Weilin Wang, Yan Yu, Xian-Zhu Fu, Jing-Li Luo
Summary: An efficient strategy was developed for concurrent H-2 production and refining oxidative alcohols into value-added formate using self-supported Ni2P-CoP bifunctional electrocatalysts. This method enabled high-efficiency hydrogen production under low voltage conditions and demonstrated excellent durability.
Article
Chemistry, Multidisciplinary
Bibhudatta Malik, Sumit Majumder, Roberto Lorenzi, Ilana Perelshtein, Michal Ejgenberg, Alberto Paleari, Gilbert Daniel Nessim
Summary: This work presents a composite of Ni doped Fe2O3 (Ni-Fe2O3) with mildly oxidized multi-walled CNT (O-CNT) as an exceptional Mott-Schottky catalyst for electrochemical oxygen evolution reaction (OER) and methanol oxidation reaction (MOR). The O-CNT acts as a co-catalyst to regulate charge transfer in Ni-Fe2O3, enhancing electrocatalytic performance. The Ni-Fe2O3/O-CNT composite exhibits low onset potential and overpotential for OER and delivers high MOR current density in the presence of 1 M CH3OH.
Article
Chemistry, Multidisciplinary
Ruxue Fan, Haiyan Wang, Xiaozhong Zheng, Jiadong Chen, Yang Ou, Yong Wang, Shanjun Mao
Summary: The synthesis of Fe-2 dimers has been found to effectively activate non-polar diatomic molecule O-2 and enhance its catalytic activity. Additionally, Fe-2 dimers promote the direct breaking of O=O bonds, leading to lower H2O2 yield and higher specific activity.
Article
Chemistry, Physical
Samuel S. Hardisty, Kobby Saadi, Samala Nagaprasad Reddy, Ilya Grinberg, David Zitoun
Summary: Catalyst poisoning and leaching is a common issue in catalyst applications. In the case of hydrogen bromine redox flow battery, the degradation of the hydrogen oxidation/evolution catalyst caused by bromide ions crossing the membrane hinders its performance. However, the synthesis of Pt nanoparticles inside single-walled carbon nanotubes has been proven to enhance the stability and activity of the catalyst.
MATERIALS TODAY ENERGY
(2022)
Review
Engineering, Environmental
Abir Azara, Salma Belbessai, Nicolas Abatzoglou
Summary: Waste plastics pose challenges to the environment and ecosystems due to their non-biodegradable nature. Thermochemical recycling can convert waste plastics to high-value products and produce filamentous carbon nanomaterials. While progress has been made in the synthesis of filamentous carbon nanomaterials, a complete understanding of the growth mechanism is still lacking.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2022)
Article
Chemistry, Multidisciplinary
Di Zhang, Youyuan Xiong, Yingjie Guo, Lei Zhang, Zheng Wang, Kuiling Ding
Summary: In this study, a Pd-catalyzed enantioselective domino Heck carbonylation reaction was developed using o-iodoacrylanilides, terminal alkynes, and water as nucleophiles. The reaction afforded a diverse range of beta-carbonylated 2-oxindole derivatives with a 3,3-disubstituted all-carbon quaternary stereocenter in high yields and good to excellent enantioselectivities. The synthetic utility of the methodology was demonstrated through gram-scale synthesis of various compounds, showcasing its potential for efficient chiral 2-oxindole synthesis.
CHEMISTRY-A EUROPEAN JOURNAL
(2022)
Article
Chemistry, Multidisciplinary
Zisheng Zhang, Tsugunosuke Masubuchi, Philippe Sautet, Scott L. Anderson, Anastassia N. Alexandrova
Summary: We studied the size-dependent activity and stability of supported Pt-1, Pt-4, Pt-7, and Pt-8 for electrocatalytic hydrogen evolution reaction and found that clusters have higher activity than polycrystalline Pt, along with size-dependent stability. DFT calculations were used to understand the size effects by studying the structural fluxionality under different potentials. Our research showed that the clusters can reshape under H coverage, leading to a diverse ensemble of states with varying stoichiometry, structure, and reactivity. Both experimental and theoretical results suggest that the electrocatalytic species are hydridic states of the clusters (2 H/Pt). An ensemble-based kinetic model reproduced the experimental activity trend and highlighted the role of metastable states. The stability trend was rationalized through chemical bonding analysis. Our joint study showcases the potential- and adsorbate-coverage-dependent fluxionality of subnano clusters of different sizes and provides a systematic modeling strategy to tackle the complexities.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Review
Chemistry, Multidisciplinary
Shizhi Dong, Yanshuai Li, Zhilong Zhao, Ruichuan Li, Jiaqi He, Jinpeng Yin, Bing Yan, Xing Zhang
Summary: This paper reviews the research progress of hydrogen production from water electrolysis as a significant part of clean energy in the future. It focuses on the development of heterogeneous electrocatalysts, measurement parameters of electrocatalytic hydrogen evolution reaction, and the hydrogen evolution mechanisms in different environments. The paper also highlights the essential development direction and challenges in this field.
Article
Chemistry, Multidisciplinary
Zhibin Liu, Hatem M. A. Amin, Yuman Peng, Manuel Corva, Rossitza Pentcheva, Kristina Tschulik
Summary: This study investigates the influence of nanocatalyst morphology on their catalytic activity in the oxygen evolution reaction (OER). The results show that nanocubes with predominant (001) facets exhibit higher activity compared to multi-faceted spheroids. Density functional theory calculations confirm the higher activity of (001) surfaces, attributed to a change in active sites and potential-determining steps.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Anna Rabe, Maximilian Jaugstetter, Felix Hiege, Nicolas Cosanne, Klaus Friedel Ortega, Julia Linnemann, Kristina Tschulik, Malte Behrens
Summary: A computer-controlled microemulsion-assisted co-precipitation method is established to control the pore size of catalysts for the electrochemical oxygen evolution reaction. It is found that when the pore size reaches a certain threshold, the overpotential increases significantly and the oxygen release mechanism changes. These findings are of great importance for the development of better catalysts.
Article
Chemistry, Physical
Steffen Murke, Kevin Wonner, Serena R. Alfarano, Christian Rurainsky, Paolo Cignoni, Kristina Tschulik, Martina Havenith
Summary: Due to their unique surface properties, gold-enriched porous nanoparticles fabricated by electrochemical dealloying show enhanced catalytic performance for the electrochemical oxygen evolution reaction (OER) compared to monometallic gold nanoparticles or bare electrodes. Surface-enhanced Raman spectroscopy (SERS) combined with electrochemistry confirmed the formation of Au-O-O-H species, a known intermediate of OER, at a specific potential. These results highlight the potential application of dealloying-derived nanoparticles as promising catalyst materials.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Chenglong Luan, Manuel Corva, Ulrich Hagemann, Hongcai Wang, Markus Heidelmann, Kristina Tschulik, Tong Li
Summary: Co-based electrocatalysts undergo dynamic surface changes during oxygen evolution reaction, which affects their performance. A multimodal characterization approach is used to study the structural and compositional evolution of the CoOOH layer and its impact on OER activity.
Review
Chemistry, Physical
Christopher Batchelor-McAuley
Summary: The onset potential is widely used to measure the electrocatalytic activity but lacks a single and agreed definition or a standard measurement procedure. This review discusses the different definitions used in the literature. However, regardless of how it is measured, the onset potential is sensitive to catalyst loading and specific surface area, making the mass-activity or specific-activity a better method for measuring the activity of an electrocatalyst.
CURRENT OPINION IN ELECTROCHEMISTRY
(2023)
Article
Chemistry, Physical
Paolo Cignoni, Niclas Blanc, Kristina Tschulik
Summary: The advancement of electrocatalysis from fundamental research to application requires seamless collaboration between researchers from different fields. This mini review highlights the common problems faced when evaluating the performance of complex electrode assemblies made of nanostructured materials. Applying classical kinetic descriptors to these assemblies often makes it challenging to distinguish and attribute material properties to electrode performance. Recent advancements in discerning and analyzing electrocatalysis on composite or nanostructured electrodes are discussed, with emphasis on detecting and addressing inhomogeneities in the electrocatalytic activity of three-dimensional electrodes.
CURRENT OPINION IN ELECTROCHEMISTRY
(2023)
Review
Chemistry, Physical
Mahnaz Azimzadeh Sani, Kristina Tschulik
Summary: In this article, we discuss the capabilities of nanoimpact electrochemistry for studying properties of colloidal nanoparticles, electrocatalytic activity, and particle reactivity at a single entity level. These capabilities provide a better understanding of the role of solid/liquid interfaces in various chemical and biological systems. The article reviews the effects of particle properties and particle-electrode interactions on electrochemical signals and resulting scientific insights.
CURRENT OPINION IN ELECTROCHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Jiahao Yu, Minjun Yang, Christopher Batchelor-McAuley, Samuel Barton, Rosalind E. M. Rickaby, Heather A. Bouman, Richard G. Compton
Summary: A fluorescence-electrochemical method is used to study the response of phytoplankton to electro-generated oxidants, allowing for high-throughput species analysis.
CELL REPORTS PHYSICAL SCIENCE
(2023)
Article
Chemistry, Physical
K. Koeble, M. Jaugstetter, M. Schilling, M. Braig, T. Diemant, K. Tschulik, R. Zeis
Summary: Thermal activation at different temperatures was investigated for its impact on the structure, surface composition, wettability, and electrochemical activity of rayon-based carbon felt electrodes for VRFBs. Novel techniques including AFM, DVS, EIS, and DRT analysis were used to study these properties. The results showed that higher activation temperatures improved the wettability and reduced process impedances, but also caused severe carbon decomposition. The optimum electrochemical performance was observed at an activation temperature of 400 degrees C.
JOURNAL OF POWER SOURCES
(2023)
Article
Chemistry, Analytical
Christoph J. Bondue, Marc T. M. Koper, Kristina Tschulik
Summary: Online techniques for quantitative analysis of reaction products have limitations in coupling with electrochemistry due to the low product formation rates. However, differential electrochemical mass spectrometry (DEMS), combined with a dual thin-layer cell, provides high time resolution and addresses some challenges arising from the vacuum-electrolyte interface. To accurately translate signals observed in the mass spectrometer into electrochemical product formation rates, a calibration constant considering both DEMS sensitivity and dual thin-layer cell transfer efficiency is required. We propose a two-point calibration method based on the dependence of transfer efficiency on analyte diffusion coefficient, which offers a versatile and easy approach for a wide range of electrode-electrolyte combinations.
ACS MEASUREMENT SCIENCE AU
(2023)
Article
Chemistry, Multidisciplinary
Chen Ma, C. Alexander Schrage, Juliana Gretz, Anas Akhtar, Linda Sistemich, Lena Schnitzler, Han Li, Kristina Tschulik, Benjamin S. Flavel, Sebastian Kruss
Summary: Small perturbations in material structures can significantly affect their properties. By modifying single wall carbon nanotubes (SWCNTs) with quantum defects using diazonium salts, the photophysics of the nanotubes can be determined. The presence of multiple chiralities in SWCNT samples complicates the identification of defect-related emission features. This study shows that quantum defects do not affect aqueous two-phase extraction of different SWCNT chiralities, indicating a low number of defects. The results demonstrate the importance of stochasticity in the optical properties of SWCNTs and highlight the discrepancy between ensemble and single particle experiments/properties of nanomaterials.
Article
Chemistry, Multidisciplinary
Christoph J. J. Bondue, Marius Spallek, Lennart Sobota, Kristina Tschulik
Summary: To date, the electroactive species for selective aldehyde oxidation to carboxylates at gold electrodes is usually assumed to be the diolate, which is formed in high concentration only in very alkaline electrolytes. However, OH--induced aldehyde decomposition in these electrolytes hinders its industrial application for biomass upgrading. In this study, we demonstrate the successful oxidation of aliphatic aldehydes at a rotating gold electrode at pH 12, where only 1% of the aldehyde exists as the diolate species. This insight allows developing strategies for selective aldehyde oxidation without aldehyde decomposition, making its future industrial application viable.
Article
Electrochemistry
Paolo Cignoni, Pouya Hosseini, Christoph Kaiser, Oliver Trost, Dean-Robin Nettler, Lisa Trzebiatowski, Kristina Tschulik
Summary: Accurate normalization of electrochemical active surface area (ECSA) is crucial for determining and comparing catalyst activity. In this study, we propose a versatile approach to validate different ECSA determination techniques for nanoparticle-modified or nanostructured electrodes, using AuxPdy nanoparticles as an example. By combining surface oxide reduction and volume determination, we can estimate the nanoparticle diameter and assess the accuracy of the obtained ECSA values. Experimental conditions for determining AuxPdy nanoparticle ECSA using surface oxide reduction are provided and compared to those for macroelectrodes. This approach can be applied to different alloy systems, offering a widely applicable method for determining electrochemical surface areas and validating the transferability of existing macroelectrode characterization techniques to nanostructured or nanoparticle-modified electrodes.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Physics, Applied
Steffen Schuettler, Ludwig Jolmes, Emanuel Jess, Kristina Tschulik, Judith Golda
Summary: A humid atmospheric pressure plasma jet was used to treat an aqueous liquid, and the transport of hydrogen peroxide and hydroxyl from the plasma to the liquid was analyzed. Two in situ liquid diagnostics for each species were compared and validated. The results showed good agreement between the different methods used for detection.
PLASMA PROCESSES AND POLYMERS
(2023)
Article
Chemistry, Physical
Stefan M. Piontek, Dennis Naujoks, Tadneem Tabassum, Mark J. DelloStritto, Maximilian Jaugstetter, Pouya Hosseini, Manuel Corva, Alfred Ludwig, Kristina Tschulik, Michael L. Klein, Poul B. Petersen
Summary: Water is essential in electrochemistry and plays a crucial role in the electric double layer and interfacial electric fields. Investigating the molecular-level structure of interfacial water near working electrode surfaces has been challenging. However, using sum-frequency-generation (SFG) spectroscopy, it is now possible to probe the structure of water at buried electrode-electrolyte interfaces. Thin gold layers were found to effectively remove the limitation of obscuring the SFG spectra. This newfound ability to probe interfacial solvent structure may contribute to more efficient electrolyte composition and electrode design.
ACS PHYSICAL CHEMISTRY AU
(2023)
