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3,133 result(s) for "140/58"
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Laboratory confirmation of C60+ as the carrier of two diffuse interstellar bands
Laboratory measurements of the gas-phase spectrum of C 60 + confirm that the diffuse interstellar bands observed at 9,632 ångströms and 9,577 ångströms arise as a result of C 60 + in the interstellar medium. Fullerene C 60 identified in the Milky Way Lick Observatory astronomer Mary Lea Heger first observed what were to be called 'diffuse interstellar bands' in 1919. These are absorption lines seen towards reddened stars, and although hundreds are now known, until now none of the molecules giving rise to them have been conclusively identified. In 1994, Bernard Foing and Pascale Ehrenfreund reported two diffuse interstellar bands with wavelengths close to those of the absorption bands of fullerene C 60 + measured in a neon matrix. A more certain identification awaited the gas-phase spectrum of C 60 + . John P. Maier and colleagues now present laboratory measurements of the gas-phase spectrum of C 60 + and confirm that the diffuse interstellar bands that Foing and Ehrenfreund observed do arise from C 60 + . As C 60 has already been detected in various nebulae by detection of its infrared spectrum, this new observation in the Milky Way can only add to current interest in the role of astronomical fullerenes. The diffuse interstellar bands are absorption lines seen towards reddened stars 1 . None of the molecules responsible for these bands have been conclusively identified 2 . Two bands at 9,632 ångströms and 9,577 ångströms were reported in 1994, and were suggested to arise from C 60 + molecules (ref. 3 ), on the basis of the proximity of these wavelengths to the absorption bands of C 60 + measured in a neon matrix 4 . Confirmation of this assignment requires the gas-phase spectrum of C 60 + . Here we report laboratory spectroscopy of C 60 + in the gas phase, cooled to 5.8 kelvin. The absorption spectrum has maxima at 9,632.7 ± 0.1 ångströms and 9,577.5 ± 0.1 ångströms, and the full widths at half-maximum of these bands are 2.2 ± 0.2 ångströms and 2.5 ± 0.2 ångströms, respectively. We conclude that we have positively identified the diffuse interstellar bands at 9,632 ångströms and 9,577 ångströms as arising from C 60 + in the interstellar medium.
Thermal runaway of Lithium-ion batteries employing LiN(SO2F)2-based concentrated electrolytes
Concentrated electrolytes usually demonstrate good electrochemical performance and thermal stability, and are also supposed to be promising when it comes to improving the safety of lithium-ion batteries due to their low flammability. Here, we show that LiN(SO 2 F) 2 -based concentrated electrolytes are incapable of solving the safety issues of lithium-ion batteries. To illustrate, a mechanism based on battery material and characterizations reveals that the tremendous heat in lithium-ion batteries is released due to the reaction between the lithiated graphite and LiN(SO 2 F) 2 triggered thermal runaway of batteries, even if the concentrated electrolyte is non-flammable or low-flammable. Generally, the flammability of an electrolyte represents its behaviors when oxidized by oxygen, while it is the electrolyte reduction that triggers the chain of exothermic reactions in a battery. Thus, this study lights the way to a deeper understanding of the thermal runaway mechanism in batteries as well as the design philosophy of electrolytes for safer lithium-ion batteries. Concentrated electrolytes display superior thermal stability due to their non-flammability nature. Here, the authors show that LiN(SO 2 F) 2 -based concentrated electrolytes are incapable of solving the safety issues due to heat release during reaction between the lithiated graphite and electrolyte.
Activating lattice oxygen in high-entropy LDH for robust and durable water oxidation
The oxygen evolution reaction is known to be a kinetic bottleneck for water splitting. Triggering the lattice oxygen oxidation mechanism (LOM) can break the theoretical limit of the conventional adsorbate evolution mechanism and enhance the oxygen evolution reaction kinetics, yet the unsatisfied stability remains a grand challenge. Here, we report a high-entropy MnFeCoNiCu layered double hydroxide decorated with Au single atoms and O vacancies (Au SA -MnFeCoNiCu LDH), which not only displays a low overpotential of 213 mV at 10 mA cm −2 and high mass activity of 732.925 A g −1 at 250 mV overpotential in 1.0 M KOH, but also delivers good stability with 700 h of continuous operation at ~100 mA cm −2 . Combining the advanced spectroscopic techniques and density functional theory calculations, it is demonstrated that the synergistic interaction between the incorporated Au single atoms and O vacancies leads to an upshift in the O 2 p band and weakens the metal-O bond, thus triggering the LOM, reducing the energy barrier, and boosting the intrinsic activity. The unsatisfied stability of the oxygen evolution reaction electrocatalysts remains a great challenge. The authors activate the lattice oxygen in high-entropy layered double hydroxide, exhibiting durable and robust performance due to the high-entropy effect and optimized electronic structure.
Covalent organic frameworks for direct photosynthesis of hydrogen peroxide from water, air and sunlight
Solar-driven photosynthesis is a sustainable process for the production of hydrogen peroxide, the efficiency of which is plagued by side reactions. Metal-free covalent organic frameworks (COFs) that can form suitable intermediates and inhibit side reactions show great promise to photo-synthesize H 2 O 2 . However, the insufficient formation and separation/transfer of photogenerated charges in such materials restricts the efficiency of H 2 O 2 production. Herein, we provide a strategy for the design of donor-acceptor COFs to greatly boost H 2 O 2 photosynthesis. We demonstrate that the optimal intramolecular polarity of COFs, achieved by using suitable amounts of phenyl groups as electron donors, can maximize the free charge generation, which leads to high H 2 O 2 yield rates (605 μmol g −1 h −1 ) from water, oxygen and visible light without sacrificial agents. Combining in-situ characterization with computational calculations, we describe how the triazine N-sites with optimal N 2p states play a crucial role in H 2 O activation and selective oxidation into H 2 O 2 . We further experimentally demonstrate that H 2 O 2 can be efficiently produced in tap, river or sea water with natural sunlight and air for water decontamination. Solar-driven photosynthesis is a green and sustainable process for hydrogen peroxide production. Here the authors report that optimizing the intramolecular polarity of COFs can greatly boost H 2 O 2 photosynthesis from water, air, and sunlight.
Double-slit photoelectron interference in strong-field ionization of the neon dimer
Wave-particle duality is an inherent peculiarity of the quantum world. The double-slit experiment has been frequently used for understanding different aspects of this fundamental concept. The occurrence of interference rests on the lack of which-way information and on the absence of decoherence mechanisms, which could scramble the wave fronts. Here, we report on the observation of two-center interference in the molecular-frame photoelectron momentum distribution upon ionization of the neon dimer by a strong laser field. Postselection of ions, which are measured in coincidence with electrons, allows choosing the symmetry of the residual ion, leading to observation of both, gerade and ungerade , types of interference. The wave nature of light and particles is of interest to the fundamental quantum mechanics. Here the authors show the double-slit interference effect in the strong-field ionization of neon dimers by employing COLTRIMS method to record the momentum distribution of the photoelectrons in the molecular frame
Genome-wide association analysis of plasma lipidome identifies 495 genetic associations
The human plasma lipidome captures risk for cardiometabolic diseases. To discover new lipid-associated variants and understand the link between lipid species and cardiometabolic disorders, we perform univariate and multivariate genome-wide analyses of 179 lipid species in 7174 Finnish individuals. We fine-map the associated loci, prioritize genes, and examine their disease links in 377,277 FinnGen participants. We identify 495 genome-trait associations in 56 genetic loci including 8 novel loci, with a considerable boost provided by the multivariate analysis. For 26 loci, fine-mapping identifies variants with a high causal probability, including 14 coding variants indicating likely causal genes. A phenome-wide analysis across 953 disease endpoints reveals disease associations for 40 lipid loci. For 11 coronary artery disease risk variants, we detect strong associations with lipid species. Our study demonstrates the power of multivariate genetic analysis in correlated lipidomics data and reveals genetic links between diseases and lipid species beyond the standard lipids. The human plasma lipidome captures risk for cardiometabolic diseases. Here, the authors perform univariate and multivariate genome-wide analyses of 179 lipid species in 7174 Finnish individuals, revealing genetic links between diseases and lipid species beyond the standard lipids HDL-Cholesterol, LDL-Cholesterol, Triglycerides, and total Cholesterol.
Small reorganization energy acceptors enable low energy losses in non-fullerene organic solar cells
Minimizing energy loss is of critical importance in the pursuit of attaining high-performance organic solar cells. Interestingly, reorganization energy plays a crucial role in photoelectric conversion processes. However, the understanding of the relationship between reorganization energy and energy losses has rarely been studied. Here, two acceptors, Qx-1 and Qx-2, were developed. The reorganization energies of these two acceptors during photoelectric conversion processes are substantially smaller than the conventional Y6 acceptor, which is beneficial for improving the exciton lifetime and diffusion length, promoting charge transport, and reducing the energy loss originating from exciton dissociation and non-radiative recombination. So, a high efficiency of 18.2% with high open circuit voltage above 0.93 V in the PM6:Qx-2 blend, accompanies a significantly reduced energy loss of 0.48 eV. This work underlines the importance of the reorganization energy in achieving small energy losses and paves a way to obtain high-performance organic solar cells. Minimising energy loss is important for achieving high-performance organic solar cells. Here, the authors design and synthesise two acceptors with small reorganisation energies and reveal the relationship between reorganisation energy and energy losses.
A pyridinic Fe-N4 macrocycle models the active sites in Fe/N-doped carbon electrocatalysts
Iron- and nitrogen-doped carbon (Fe-N-C) materials are leading candidates to replace platinum catalysts for the oxygen reduction reaction (ORR) in fuel cells; however, their active site structures remain poorly understood. A leading postulate is that the iron-containing active sites exist primarily in a pyridinic Fe-N 4 ligation environment, yet, molecular model catalysts generally feature pyrrolic coordination. Herein, we report a molecular pyridinic hexaazacyclophane macrocycle, (phen 2 N 2 )Fe, and compare its spectroscopic, electrochemical, and catalytic properties for ORR to a typical Fe-N-C material and prototypical pyrrolic iron macrocycles. N 1s XPS and XAS signatures for (phen 2 N 2 )Fe are remarkably similar to those of Fe-N-C. Electrochemical studies reveal that (phen 2 N 2 )Fe has a relatively high Fe(III/II) potential with a correlated ORR onset potential within 150 mV of Fe-N-C. Unlike the pyrrolic macrocycles, (phen 2 N 2 )Fe displays excellent selectivity for four-electron ORR, comparable to Fe-N-C materials. The aggregate spectroscopic and electrochemical data demonstrate that (phen 2 N 2 )Fe is a more effective model of Fe-N-C active sites relative to the pyrrolic iron macrocycles, thereby establishing a new molecular platform that can aid understanding of this important class of catalytic materials. Iron- and nitrogen-doped carbon materials are effective catalysts for the oxygen reduction reaction whose active sites are poorly understood. Here, the authors establish a new pyridinic iron macrocycle complex as a more effective active site model relative to legacy pyrrolic model complexes.
Iron-mediated organic matter decomposition in humid soils can counteract protection
Soil organic matter (SOM) is correlated with reactive iron (Fe) in humid soils, but Fe also promotes SOM decomposition when oxygen (O 2 ) becomes limited. Here we quantify Fe-mediated OM protection vs. decomposition by adding 13 C dissolved organic matter (DOM) and 57 Fe II to soil slurries incubated under static or fluctuating O 2 . We find Fe uniformly protects OM only under static oxic conditions, and only when Fe and DOM are added together: de novo reactive Fe III phases suppress DOM and SOM mineralization by 35 and 47%, respectively. Conversely, adding 57 Fe II alone increases SOM mineralization by 8% following oxidation to 57 Fe III . Under O 2 limitation, de novo reactive 57 Fe III phases are preferentially reduced, increasing anaerobic mineralization of DOM and SOM by 74% and 32‒41%, respectively. Periodic O 2 limitation is common in humid soils, so Fe does not intrinsically protect OM; rather reactive Fe phases require their own physiochemical protection to contribute to OM persistence. Reactive iron minerals protect vast amounts of terrestrial carbon from decomposition and release as CO 2 . Here the authors show that reactive iron alone does not provide sufficient protection except under strict oxic conditions—instead, iron itself promotes carbon decomposition.
Unraveling oxygen vacancy site mechanism of Rh-doped RuO2 catalyst for long-lasting acidic water oxidation
Exploring durable electrocatalysts with high activity for oxygen evolution reaction (OER) in acidic media is of paramount importance for H 2 production via polymer electrolyte membrane electrolyzers, yet it remains urgently challenging. Herein, we report a synergistic strategy of Rh doping and surface oxygen vacancies to precisely regulate unconventional OER reaction path via the Ru–O–Rh active sites of Rh-RuO 2 , simultaneously boosting intrinsic activity and stability. The stabilized low-valent catalyst exhibits a remarkable performance, with an overpotential of 161 mV at 10 mA cm −2 and activity retention of 99.2% exceeding 700 h at 50 mA cm −2 . Quasi in situ/operando characterizations demonstrate the recurrence of reversible oxygen species under working potentials for enhanced activity and durability. It is theoretically revealed that Rh-RuO 2 passes through a more optimal reaction path of lattice oxygen mediated mechanism-oxygen vacancy site mechanism induced by the synergistic interaction of defects and Ru–O–Rh active sites with the rate-determining step of *O formation, breaking the barrier limitation (*OOH) of the traditional adsorption evolution mechanism. Exploring highly active and durable Ru-based electrocatalysts for acidic water oxidation is challenging. Here authors reported an ion-exchange adsorption strategy to regulate oxygen vacancies and Rh dopant, with a corresponding fundamental investigation on the lattice oxygen oxidation and the oxygen vacancy site.