We have synthesized the products of fluoroethylene carbonate (FEC) and vinylene (VC) via lithium naphthalenide reduction. By analyzing resulting solid precipitates gas evolution, our results confirm that both FEC VC decomposition include HCO2Li, Li2C2O4, Li2CO3, polymerized VC. For FEC, experimental data supports a reduction mechanism where reduces to form LiF, followed by subsequent In product, Li2CO3 were found in smaller quantities than with no additional fluorine environments being...

Amorphous silicon (a-Si) is a widely studied noncrystalline material, and yet the subtle details of its atomistic structure are still unclear. Here, we show that accurate structural models a-Si can be obtained using machine-learning-based interatomic potential. Our best network by simulated cooling from melt at rate 1011 K/s (that is, on 10 ns time scale), contains less than 2% defects, agrees with experiments regarding excess energies, diffraction data, 29Si NMR chemical shifts. We this...

To elucidate the role of fluoroethylene carbonate (FEC) as an additive in standard carbonate-based electrolyte for Li-ion batteries, solid interphase (SEI) formed during electrochemical cycling on silicon anodes was analyzed with a combination solution and solid-state NMR techniques, including dynamic nuclear polarization. facilitate characterization via 1D 2D NMR, we synthesized 13C-enriched FEC, ultimately allowing detailed structural assignment organic SEI. We find that soluble...

The parasitic reactions associated with reduced oxygen species and the difficulty in achieving high theoretical capacity have been major issues plaguing development of practical nonaqueous Li-O2 batteries. We hereby address above by exploring synergistic effect 2,5-di-tert-butyl-1,4-benzoquinone H2O on chemistry a battery. Water stabilizes quinone monoanion dianion, shifting reduction potentials to more positive values (vs Li/Li+). When water are used together (largely) battery, cell...

We report the exfoliation of layered Na2Ti3O7, a promising anode material for Na-ion batteries, and restacking using HNO3 NaOH to form H-[Ti3O7] Na(x)-[Ti3O7] compositions, respectively. The materials were characterized by range techniques (SEM, TEM, solid-state NMR, XRD, PDF). Although formation aggregated nanoparticles is favored under acidic conditions, use basic conditions can lead control over adherence between exfoliated layers. Pair distribution function (PDF) analysis confirms that...

LiI-promoted LiOH formation in Li-O2 batteries with wet ether electrolytes has been investigated by Raman, nuclear magnetic resonance spectroscopy, operando pressure tests, and molecular dynamics simulations. We find that is a synergistic effect involving both H2O LiI additives, whereas either alone Li2O2 forms. generated via nominal four-electron oxygen reduction reaction, the hydrogen coming from O2 H2O, fewer side reactions than typically associated formation; presence of parasitic...

In this work, we present a quantum algorithm for ground-state energy calculations of periodic solids on error-corrected computers. The is based the sparse qubitization approach in second quantization and developed Bloch Wannier basis sets. We show that functions require less computational resources with respect to because: (i) L$_1$ norm Hamiltonian considerably lower (ii) translational symmetry can be exploited order reduce amount classical data must loaded into computer. resource...

The determination of the nature and structure surface sites after chemical modification large area oxides such as silica is a key point for many applications challenging from spectroscopic view. This has been, instance, long-standing problem reacted with alkylaluminum compounds, system typically studied model supported methylaluminoxane aluminum cocatalyst. While (27)Al solid-state NMR spectroscopy would be method choice, it been difficult to apply this technique because quadrupolar...

Triisobutylaluminum reacts with silica yielding three different Al sites according to high-field aluminum-27 NMR and first principle calculations: a quadruply grafted dimeric surface species two incorporated Al(O)x (x = 4 or 5). This result is in stark contrast the bis-grafted that forms during Et3Al grafting. Thus isobutyl ligands, which render R3Al monomeric, lead greater reactivity towards surface.

This study explores an innovative photocatalytic approach using pristine graphitic carbon nitride (C

Understanding the structural origins of properties amorphous materials remains one most important challenges in science. In this study, we demonstrate that local ``structural simplicity'', embodied by degree to which atomic environments within a material are similar each other, is powerful concept for rationalizing structure silicon ($a$-Si) canonical material. We show, restraining reverse Monte Carlo refinement against pair distribution function (PDF) data be simpler, simplest model...

Redox flow batteries (RFBs) rely on the development of cheap, highly soluble, and high-energy-density electrolytes. Several candidate quinones have already been investigated in literature as two-electron anolytes or catholytes, benefiting from fast kinetics, high tunability, low cost. Here, an investigation nitrogen-rich fused heteroaromatic was carried out to explore avenues for electrolyte development. These were synthesized screened by using electrochemical techniques. The most promising...

Double conjugate addition leads to an increased stability and voltage for this amine functionalised quinoidal anolyte designed basic aqueous redox flow batteries, suggesting that such a reaction does not always lead degradation.

(27)Al NMR is the method of choice for studying grafted Al species on a large area solid support, such as co-catalysts α-olefin oligomerization involving mesoporous silica materials. Here, we show how to interpret solid-state spectrum and parameters various types monomeric dimeric alkyl halogen compounds silica, based trends obtained from first-principles calculations. Since most alkylaluminum tend form dimers in gas phase, chose prototypes both AlMe3 monomer Al2Me6 dimer. On top that...

Abstract An der Redox‐Polymerisation von Acrylnitril mit H 2 O /Rongalit wird gezeigt, daß es nicht stets OH‐Radikale sein müssen, die derartige Reaktionen auslösen. Zieht man Möglichkeit Anlagerungsverbindungen als Zwischenstufen in Betracht, so ergeben sich interessante Ausblicke hinsichtlich Spezifität Redox‐Systemen und anderen technisch bedeutsamen Fragen.

The parasitic reactions associated with reduced oxygen species and the difficulty in achieving high theoretical capacity have been major issues plaguing development of practical non-aqueous Li-O2 batteries. We hereby address above by exploring synergistic effect 2,5-di-tert-butyl-1,4- benzoquinone H2O on chemistry a battery. Water stabilizes quinone monoanion dianion, shifting reduction potentials to more positive values (vs. Li+). When water are used together (largely) battery, cell...

Abstract We present a new software to easily perform QM:MM and QM:QM' calculations called QMX. It follows the subtraction scheme it is implemented in Atomic Simulation Environment (ASE). Special attention paid couple molecular with periodic boundaries approaches. QMX inherits flexibility versatility of ASE package: any combination methods namely force field, semiempirical, first principle, ab initio , can be used as hybrid potential energy surface (PES). Its ease use demonstrated by...

Amorphous silicon (a-Si) is a widely studied non-crystalline material, and yet the subtle details of its atomistic structure are still unclear. Here, we show that accurate structural models a-Si can be obtained by harnessing power machine-learning algorithms to create interatomic potentials. Our best network cooling from melt in molecular-dynamics simulations, at rate 10$^{11}$ K/s (that is, on 10 ns timescale). This shows defect concentration below 2% agrees with experiments regarding...

In this work, we present a quantum algorithm for ground-state energy calculations of periodic solids on error-corrected computers. The is based the sparse qubitization approach in second quantization and developed Bloch Wannier basis sets. We show that functions require less computational resources with respect to because: (i) L$_1$ norm Hamiltonian considerably lower (ii) translational symmetry can be exploited order reduce amount classical data must loaded into computer. resource...