Article
Chemistry, Inorganic & Nuclear
Masnun Naher, Chuyi Su, Jeffrey R. Harmer, Craig M. Williams, Paul V. Bernhardt
Summary: The utility and scope of Cu-catalyzed halogen atom transfer chemistry have been exploited in a variety of fields. This study demonstrates the ability to modulate the reactivity of the Cu catalyst using electrochemistry, resulting in unprecedented rate acceleration in Cu-catalyzed bulk electrosynthesis.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Han-Ying Liu, Mary F. Mahon, Michael S. Hill
Summary: The potassium diamidoalumanyl reacts with pinacolato boron esters and B(OMe) to produce potassium (alkoxy)borylaluminate derivatives. The reactivity of these derivatives with heteroallene molecules highlights the kinetic inaccessibility of their Al-B bonds.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Physical
Haiqi Gao, Jing Wang, Yuzhen Liu, Yannan Xie, Petr Kral, Ruifeng Lu
Summary: Molecular dynamics simulations have shown the significant influence of hydration shells on ions passing through ultrathin carbon nanotubes. Electrically-driven ions tend to drag their hydration shells, while pressure-driven ions can be actively driven by their hydration shells. The different binding strengths of hydration shells to ions of various sizes affect the entry rates and driving speeds of ions in CNTs.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Nanoscience & Nanotechnology
Alice Sciortino, Francesco Ferrante, Gil Goncalves, Gerard Tobias, Radian Popescu, Dagmar Gerthsen, Nicolo Mauro, Gaetano Giammona, Gianpiero Buscarino, Franco M. Gelardi, Simonpietro Agnello, Marco Cannas, Dario Duca, Fabrizio Messina
Summary: Carbon dots, when coupled with carbon nanotubes, demonstrate stable electronic coupling and efficient photoinduced electron transfer, leading to high degree of charge separation and conduction. These nanohybrids exhibit significant photocatalytic properties, showing promise for applications in artificial photocatalysis and photosynthesis.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Multidisciplinary
Kayleigh L. Y. Fung, Stephen T. Skowron, Christopher S. Allen, Andrei N. Khlobystov
Summary: This method uses SWNTs as nano test tubes, TEM as an imaging tool, and counts reactant molecules to determine polymerisation reaction rates, resulting in enthalpy of activation of 104 kJ mol(-1) and large entropic contributions to the Gibbs free energy of activation. This experimental methodology bridges reactions at the single-molecule level with macroscopic chemical kinetics parameters by filming the chemical reaction in direct space.
CHEMICAL COMMUNICATIONS
(2021)
Article
Thermodynamics
Yue Chen, Changwei Li, Dachao Yuan, Ying Zhang, Menglin Yang, Kaixuan Tang
Summary: Experiments were conducted on flame spread over cantilevered PMMA composites with addition of CNTs, and the flame spread behavior was analyzed. The results showed that the addition of CNTs enhanced the viscosity of the molten materials, leading to the distinction between the surface flame and the dripping flame regions. The dripping flame, which promotes flame spread, was found to increase the flame height and flame spread rate. Heat transfer analysis revealed that the heat flux from the dripping flame is twice as much as that from pure PMMA at 2.5% CNTs, and it contributes 40% to the total heat flux. The enhancement of the heat feedback of the dripping flame was identified as the main factor for the increased flame spread rate. These findings contrast with the flame retardancy effects of CNTs, suggesting that the application of CNTs as flame retardants in polymers needs to consider fire scenarios.
CASE STUDIES IN THERMAL ENGINEERING
(2023)
Article
Engineering, Environmental
Mengke Li, Zhiguo He, Hui Zhong, Liang Hu, Wei Sun
Summary: A novel catalyst (MT/EMR) was successfully prepared for the high removal efficiency of ROX, demonstrating improved adsorption capacity and accelerated metal transformation. By involving a two-electron pathway for direct ROX oxidation, the catalyst showed increased degradation rate compared to single-EMR, with enhanced stability due to M-O-C (M=Fe or Mn) bonds in MT/EMR. This work provides a new and effective strategy for waste solid-based catalysts and expands the application of adsorption-oxidation technology in tackling organoarsenic pollution.
Article
Engineering, Environmental
Xuxu Wang, Ying Wang, Chun Zhao, Yunhua Zhu, Zhihua Sun, Hua-Jun Shawn Fan, Xuebin Hu, Huaili Zheng
Summary: A novel method for generating free RMnS, with ultrasound enhanced CNTs/permanganate process (UCP), has been proposed for efficient organics removal. CNTs in the UCP process can enrich manganese compounds and target contaminants, acting as an electronic platform for electron transfer. Ultrasound further regulates RMnS generation, converting inactive solid Mn(IV) into free RMnS for rapid contaminants removal.
Article
Engineering, Chemical
Shaohua Chen, Liying Ma, Yaguang Du, Wei Zhan, Tian C. Zhang, Dongyun Du
Summary: The study demonstrates that sulfate radical SO4•- generated by the activation of persulfate (PS) on metal-free carbon-nanotubes (CNTs) effectively degrades the organic contaminant RhB, with natural organic matter (NOM) enhancing the degradation process. The findings suggest a new strategy for treating RhB wastewater with high efficiency without the need for high energy inputs or causing secondary contamination from metal pollution.
SEPARATION AND PURIFICATION TECHNOLOGY
(2021)
Article
Chemistry, Multidisciplinary
Marion Berdal, Sebastien Gouard, Romain Eychenne, Severine Marionneau-Lambot, Mikael Croyal, Alain Faivre-Chauvet, Michel Cherel, Joelle Gaschet, Jean-Francois Gestin, Francois Guerard
Summary: The study investigated the potential of arylboron chemistry as an alternative approach for late stage labelling of antibodies, achieving high radiochemical yields using a copper(ii) catalyst and 1,10-phenanthroline. The CD138 targeting monoclonal antibody labelling retained high RCY and increased specific activities in a preclinical model of multiple myeloma, showing promise for radiotheranostic applications with the radioiodine/At-211 pairs. Overall, the development of radiolabelling kits through this procedure could facilitate its translation to clinical applications.
Article
Engineering, Environmental
Shuiping Yu, Yanhua Peng, Penghui Shao, Yuanyue Wang, Youwen He, Wei Ren, Liming Yang, Hui Shi, Xubiao Luo
Summary: Nanocarbon-based persulfate oxidation technologies show promise for environmentally-friendly removal of phenolic pollutants. Defect-rich carbon nanotubes (CNTs) can induce electron transfer from phenols to peroxymonosulfate (PMS), leading to efficient degradation of phenols. The selective oxidation of phenols via CNT-mediated electron transfer is found to be dependent on the substituent group and position.
JOURNAL OF HAZARDOUS MATERIALS
(2023)
Article
Engineering, Environmental
Jingyan Ming, Hongquan Fu, Guangxing Yang, Hongjuan Wang, Jiangnan Huang, Feng Peng, Yonghai Cao, Hao Yu
Summary: A facile method combining electrochemical and spectroscopic technologies was proposed to evaluate the electron transfer reaction rate on carbon nanotubes with defects. The transferred electrons from CNTs were quantitatively determined through the Beer-Lambert law and coulometric analysis. It was revealed that the edge defects on CNTs are beneficial for the electron transfer reaction rate, leading to higher activity in the electrooxidation of glycerol for Pt/d-CNTs.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Environmental Sciences
Yue Lu, Shoujuan Zhang, Qi Liu, Linrui Zhong, Qingqing Xie, Abing Duan, Zhaohui Yang, Qian Liu, Zhiyi Zhang, Jingru Hao
Summary: The study investigated the effects of the graphite structure on the electron transfer process between bacteria. It found that CNTs exhibited excellent electron shuttle performance, improving the degradation rate of nitrobenzene and shortening the distance of electron transfer.
ENVIRONMENTAL POLLUTION
(2023)
Article
Engineering, Environmental
Xianbao Wang, Tiantian Chen, Chuyue Gao, Yili Xie, Anlong Zhang
Summary: Extracellular polymeric substances (EPS) play an important role in the metabolic activities of activated sludge. This study found that EPS removal deteriorated the denitrification performance of the activated sludge, while re-adding extracted EPS increased the denitrification rate. EPS contains many redox mediators, and re-adding EPS improved the electron transport system activity and key enzymes in biological denitrification. Additionally, EPS re-addition promoted the activities of enzymes related to glycolysis and increased nicotinamide adenine dinucleotide yield, enhancing the denitrification rate of activated sludge.
JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING
(2022)
Article
Chemistry, Physical
Maria Kapsi, Charitomeni M. Veziri, George Pilatos, Georgios N. Karanikolos, George E. Romanos
Summary: This study demonstrates the growth of carbon nanotubes as adsorbents and membranes for hydrogen storage and selective separation. The materials exhibit precise pore sizes and monodispersity, making them promising for practical applications.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Chemistry, Multidisciplinary
Lipiao Bao, Baolin Zhao, Muhammad Ali, Mhamed Assebban, Bowen Yang, Malte Kohring, Dmitry Ryndyk, Thomas Heine, Heiko B. Weber, Marcus Halik, Frank Hauke, Andreas Hirsch
Summary: Structuring distinct building blocks on graphene opens opportunities for constructing 2D architectures and multifunctional devices. However, such structures are rare and existing examples are limited to small addends without easily accessible anchor points.
ADVANCED MATERIALS INTERFACES
(2022)
Article
Nanoscience & Nanotechnology
Christian Dolle, Peter Schweizer, Daniela Dasler, Sebastian Gsaenger, Robert Maidl, Gonzalo Abellan, Frank Hauke, Bernd Meyer, Andreas Hirsch, Erdmann Spiecker
Summary: Covalent functionalisation is an effective approach to tune the properties and processability of graphene. This study successfully observed atomic resolution imaging of dodecyl functionalised monolayer graphene using mechanical filtering method, providing new possibilities for the investigation of this hybrid material.
NPJ 2D MATERIALS AND APPLICATIONS
(2022)
Article
Nanoscience & Nanotechnology
Tobias Dierke, Daniela Dasler, Tamara Nagel, Frank Hauke, Andreas Hirsch, Janina Maultzsch
Summary: In this study, we investigate the degree of covalent functionalization of graphene on different two-dimensional (2D) materials. The underlying substrate has a strong influence on the functionalization of graphene. Patterning the underlying material is a versatile method that preserves the high-quality properties of graphene, allowing for spatially defined functionalization.
ACS APPLIED NANO MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Markus Freiberger, Martin B. Minameyer, Iris Solymosi, Stefan Fruehwald, Marcel Krug, Youzhi Xu, Andreas Hirsch, Timothy Clark, Dirk M. Guldi, Max von Delius, Konstantin Amsharov, Andreas Goerling, M. Eugenia Perez-Ojeda, Thomas Drewello
Summary: We studied the gas-phase chemistry of [10]cycloparaphenylene ([10]CPP) non-covalent complexes with C-60 and C-70 using atmospheric pressure photoionization and electrospray ionization mass spectrometry. The stability and charge distribution of these complexes were analyzed using energy-resolved collision-induced dissociation (ER-CID). It was found that complexes with a C-70 core exhibited greater stability, and the radical cations were more stable than the radical anions. [2:1] complexes of the ([10]CPP2 superset of C-60/70)(+center dot/-center dot) type were observed as isolated solitary gas-phase species for the first time. The stability of these complexes was reduced compared to the [1:1] complexes.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Organic
Johannes Muller, Janina Buck, Andreas Hirsch
Summary: This paper presents nine pi-expanded mono-substituted 5,8,11,14,17-pentakis-(tert-butyl)-hexa-peri-hexabenzocoronenes (HBC) and explores their synthesis method and the influence of substitution groups on their optoelectronic properties.
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Laura von Lueders, Rita Tilmann, Kangho Lee, Cian Bartlam, Tanja Stimpel-Lindner, Tarja K. Nevanen, Kristiina Iljin, Kathrin C. Knirsch, Andreas Hirsch, Georg S. Duesberg
Summary: We present a controllable and specific functionalisation approach for graphene field-effect transistors (GFETs) in order to detect small physiologically active molecules. The key step involves the noncovalent functionalisation of graphene with perylene bisimide (PBI) molecules directly on the growth substrate. This method allows for the homogeneous self-assembly of PBI molecules on graphene, followed by the immobilization of antibodies. The functionalised GFET devices showed excellent performance in terms of atomic force microscopy, Raman spectroscopy, and electrical measurements compared to conventional functionalisation methods. Specific sensing of small molecules such as methamphetamine and cortisol was achieved by monitoring the electrical changes of the functionalised GFET devices. The sensors were able to detect methamphetamine down to a concentration of 300 ng ml(-1).
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Multidisciplinary
Felix Hemauer, Valentin Schwaab, Eva Marie Freiberger, Natalie J. Waleska, Andreas Leng, Cornelius Weiss, Johann Steinhauer, Fabian Duell, Philipp Bachmann, Andreas Hirsch, Hans-Peter Steinrueck, Christian Papp
Summary: This study investigates the surface chemistry of a derivatized norbornadiene/quadricyclane molecule pair and explores their potential as energy storage solutions for renewable energy sources. It demonstrates the success of triggering the release of stored energy on Pt(111) and reveals the decomposition pathways of the two isomers on Ni(111).
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Jovana Jaksic, Iris Solymosi, Andreas Hirsch, M. Eugenia Perez-Ojeda, Aleksandra Mitrovic, Veselin Maslak
Summary: This study presents the synthesis and characterization of four dumbbell-shaped fullerene molecules connected by isosorbide and isomannide moieties. The electrochemical behavior of these molecules and their ability to form complexes with [10]cycloparaphenylene ([10]CPP) were investigated. The results showed a high electron affinity for the fullerene dumbbells, indicating a strong interaction with carbon nanorings.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Organic
Sven Moersel, Rene Kellner, Andreas Hirsch
Summary: The synthesis of novel fluorinated hexa-peri-hexabenzocoronenes (HBCs) and their thioether-substituted analogs was reported, with the reaction time significantly reduced by using microwave assistance. Increasing fluorination or thioether-substituents led to a decrease in the extinction coefficient of the HBCs. Addition of thioether-moieties caused a shift in absorption and emission bands, while the nature of the thioether did not affect the optoelectronic properties. Oxidation to sulfone and formation of sulfonium salts further modified the electronic environment of the HBC core, resulting in decreased extinction coefficients and broadening of absorption and emission bands.
EUROPEAN JOURNAL OF ORGANIC CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Iris Solymosi, Christian Neiss, Harald Maid, Frank Hampel, Thomas Solymosi, Andreas Gorling, Andreas Hirsch, M. Eugenia Perez-Ojeda
Summary: Crystal packing and chromophore communication play vital roles in applications related to light-energy harvesting and conversion. Obtaining crystals with flexible and soluble structures is challenging. However, a crystal structure of a highly flexible perylene-3,4 : 9,10-tetracarboxylic acid bisimide (PBI) cyclophane has been successfully obtained and analyzed, revealing a unique one-dimensional pi-stacking supramolecular polymer-like structure. The findings highlight the importance of crystal packing control for specific applications based on multiexciton generation processes.
Article
Nanoscience & Nanotechnology
Maria Kolesnik-Gray, Laura Meingast, Martin Siebert, Tim Unbehaun, Tobias Huf, Guenter Ellrott, Gonzalo Abellan, Stefan Wild, Vicent Lloret, Udo Mundloch, Julian Schwarz, Michael Niebauer, Maximilian Szabo, Mathias Rommel, Andreas Hutzler, Frank Hauke, Andreas Hirsch, Vojislav Krstic
Summary: In this work, the DC electrical transport characteristics of high-quality black phosphorus (BP) field-effect devices with different thicknesses were studied at room temperature. The experimental data showed that the conductivity and hole density increase non-trivially with a reduced number of layers while maintaining constant field-effect mobility due to electron-phonon scattering. The observed phenomena were found to be a direct consequence of significant interlayer coupling, resulting in a local redistribution of free charge carriers towards the central layers. It was also discovered that a naturally protected 2D hole gas can be encapsulated in BP flakes as thick as 10 nm due to the electrostatic environment.
NPJ 2D MATERIALS AND APPLICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Juan S. S. Rocha-Ortiz, Jianchang C. Wu, Jonas Wenzel, Andreas J. J. Bornschlegl, Jose Dario Perea, Salvador Leon, Anastasia Barabash, Anna-Sophie Wollny, Dirk M. M. Guldi, Jiyun Zhang, Alberto Insuasty, Larry Lueer, Alejandro Ortiz, Andreas Hirsch, Christoph J. J. Brabec
Summary: Dumbbell-shaped systems based on PAHs-BODIPY-triarylamine hybrids TM-(01-04) are designed and employed as hole-transporting materials in planar inverted perovskite solar cells, exhibiting remarkable stability and high power conversion efficiency. The conjugated pi-system's covalent attachment and size are found to influence the energy transfer within the systems. Integrating these systems into the solar cells results in outstanding power conversion efficiency, with TM-02-based devices achieving a PCE of 20.26%. The long-term stability of these devices is also measured, with TM-04-based device showing the highest stability of 94%.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Applied
Juan S. Rocha-Ortiz, Joel Jose Montalvo-Acosta, Yakun He, Alberto Insuasty, Andreas Hirsch, Christoph J. Brabec, Alejandro Ortiz
Summary: Eight novel C60-BODIPY-Triarylamine electroactive triads were synthesized and characterized, and the effect of different linkers and functionalization on the electronic properties were studied. The compounds showed strong absorption of visible light and photo-induced electron transfer, confirmed by solvatochromic effects and redox potentials. The study also found that the pyrrolidine derivatives were more stable than isoxazoline analogs and alkoxy units improved thermal endurance.
Article
Chemistry, Multidisciplinary
Markus Freiberger, Iris Solymosi, Eva Marie Freiberger, Andreas Hirsch, M. Eugenia Perez-Ojeda, Thomas Drewello
Summary: In this study, the stability of [n]cycloparaphenylene (nCPP)-based host-guest complexes with Li+@C-60 and C-60 was compared for the first time in both gas and solution phases. Results showed a significant increase in stability for the complexes featuring [9-12]CPP with Li+@C-60, which was also observed in solution. The formation of [10]CPP superset of Li+@C-60 exhibited a two orders of magnitude larger association constant compared to the C-60 analog, along with an increased binding entropy. This research contributes to a better understanding of host-guest complexes between [n]CPPs and endohedral metallofullerenes at a molecular level.
Article
Chemistry, Multidisciplinary
Wiebke Zika, Andreas Hirsch, Rene Weiss, Simone Pinter, Christoph M. Schuesslbauer, Timothy Clark, Andreas Hirsch, Dirk M. Guldi
Summary: This study investigates the interconversion between QC and NBD and their application in energy storage through photo-assays. An oxidative electron transfer is observed during the QC-to-NBD isomerization using transient absorption spectroscopy. The complementary use of time-resolved and steady-state spectroscopies allows for a complete description of the photoisomerization reaction of NBDs.