Abstract Decoupling the electronic and geometric effects has been a long cherished goal for heterogeneous catalysis due to their tangled relationship. Here, novel orthogonal decomposition method is firstly proposed settle this issue in p -chloronitrobenzene hydrogenation reaction on size- shape-controlled Pt nanoparticles (NPs) carried various supports. Results suggest Fermi levels of catalysts can be modulated by supports with varied work function ( W f ). And selectivity NPs similar size...

Single-crystal semiconductor-based photocatalysts exposing unique crystallographic facets show promising applications in energy and environmental technologies; however, crystal facet engineering through solid-state synthesis for photocatalytic overall water splitting is still challenging. Herein, we develop a novel strategy recrystallization to synthesize uniform SrTiO3 single crystals tailored {111} facets. The presynthesized low-crystalline precursors enable the formation of well-defined...

The identification of deep-level defects that act as detrimental nonradiative recombination centers is critical for optimizing the optoelectronic performance hybrid perovskites. Although extensive studies have been devoted to revealing nature in perovskites, it still unclear what are responsible experimentally observed rates. Employing first-principles approaches, we quantitatively show iodine interstitial a dominant center methylammonium-lead iodide. This important insight points target...

Slow radiative recombination due to a slightly indirect band gap has been proposed explain the high efficiency of lead-halide perovskite solar cells. Here, we calculate rate from first principles for prototypical lead halide perovskite, MAPbI3 (MA = CH3NH3). Because structure is dynamic, with MA molecule rotating even at room temperature, determine momentum mismatch between edges as function orientation molecule. Our results demonstrate that nature suppresses by less than factor two and...

Phosphoglycerate kinase-1 (PGK1) has been recently documented in various malignancies; however, the molecular mechanisms of variable PGK1 expression and its clinical significance terms survival status remain unclear. Real-time quantitative PCR (real-time qPCR) western blotting were used to verify 46 fresh breast cancer tissues matched normal tissues. A tissue microarray (TMA) comprising 401 123 was investigated by immunohistochemistry for expression. Then, correlation between...

The notion of "defect tolerance" has often been invoked to explain the excellent performance halide perovskites in optoelectronic applications. However, this concept not rigorously defined or assessed. A common interpretation is that all energetically favorable intrinsic defects are shallow. On basis examples prototypical perovskite CsPbI3, we show case. antisite PbI and IPb favorable, but also have levels deep band gap. Still, because strong anharmonicity, they efficient nonradiative...

In recent years, the impressive photovoltaic performance of halide perovskites has been commonly attributed to their defect tolerance. This attribution is seemingly intuitive and widely promoted in field, though it not rigorously assessed. this Perspective, we critically discuss proposition tolerance based on first-principles calculations. We show that actually do suffer from defect-assisted nonradiative recombination, i.e., they are tolerant. The recombination rates comparable or even...

It has been experimentally observed that light-induced lattice expansion could enhance the solar conversion efficiency in hybrid perovskites, but origin remains elusive. By performing rigorous first-principles calculations for a prototypical hybrid-perovskite FAPbI_{3} (FA: formamidinium), we show 1% already reduce nonradiative capture coefficient by one order of magnitude. Unexpectedly, suppressed is not caused changes band gap or defect transition level due to expansion, originates from...

As a prototypical photocatalyst, TiO <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline" overflow="scroll"> <mml:msub> <mml:mrow /> <mml:mn>2</mml:mn> </mml:msub> </mml:math> has been extensively studied. An interesting yet puzzling experimental fact was that P25—a mixture of anatase and rutile —outperforms the individual phases; origin this mysterious fact, however, remains elusive. Employing rigorous first-principles calculations, here we uncover metastable...

Cu chalcopyrites exhibit excellent thermoelectric performance because of their high thermopower and low thermal conductivity. Conversely, despite that Ag have even lower conductivity than the Cu-based ones, they generally display performance. The underlying physics for disparity between Cu- Ag-based materials remains unclear. In this work we investigate transport ternary $AM{\mathrm{Se}}_{2}$ $(A=\mathrm{Cu}/\mathrm{Ag}; M=\mathrm{Ga}/\mathrm{In})$ using first-principles methods. We reveal...

Abstract Rechargeable magnesium-metal batteries (RMMBs) are promising next-generation secondary batteries; however, their development is inhibited by the low capacity and short cycle lifespan of cathodes. Although various strategies have been devised to enhance Mg 2+ migration kinetics structural stability cathodes, they fail improve electronic conductivity, rendering cathodes incompatible with anodes. Herein, we propose a dual-defect engineering strategy, namely, incorporation...

The signals that determine the size and duration of primary T cell immune response are not well defined. We studied CD4 cells at an important checkpoint in their development: when they have become effectors ready to rapidly mediate effector functions, both via direct interaction with antigen (Ag)-presenting cytokine production. determined effects specific Ag cytokines interleukin (IL) 2 transforming growth factor (TGF) beta 1 on helper type (Th2) apoptosis versus expansion. Th2-polarized...

Abstract The emergence of halide perovskites for photovoltaic applications has triggered great interest in these materials solid‐state light emission. Higher order electron–hole recombination processes can critically affect the efficiency such devices. In present work, Auger coefficients are computed prototypical perovskite, CH 3 NH PbI (MAPbI ), using first‐principles calculations. It is demonstrated that responsible exceptionally high third‐order coefficient observed experiment. large...

Structural transformations in Fe–C alloys are decisive for the mechanical properties of steels, but their modeling remains a challenge due to simultaneous changes Fe lattice and redistribution C. With combination orientation relationships between austenite, ferrite cementite, we identify metastable intermediate structure (MIS), which can serve as link three phases. Based on this framework, different mechanisms depending local conditions (C concentration, strain, magnetism) revealed from ab...

Abstract In recent years, there have been remarkable developments in halide perovskites, which are used highly efficient optoelectronic devices and exhibit intriguing materials physics. Detailed knowledge of carrier recombination mechanisms is essential for understanding their excellent performance to further increase efficiency. Obtaining such challenging however, different studies reached divergent conclusions some cases. This progress report outlines the critical perovskites from a...

A cobalt-catalyzed asymmetric sequential hydroboration/isomerization/hydroboration of 2-aryl vinylcyclopropanes was for the first time reported preparation valuable chiral 1,5-bis(boronates) in good yields with excellent enantioselectivity via isomerization/hydroboration a trisubstituted alkene intermediate. The reaction carried out smoothly and this protocol used syntheses (-)-preclamol gram-scale. two primary C(sp3) -B bonds could be distinguished iterative Suzuki-Miyaura cross-coupling...

Phase transitions are a common phenomenon in condensed matter and act as critical degree of freedom that can be employed to tailor the mechanical or electronic properties materials. Understanding fundamental mechanisms thermodynamics kinetics phase is, thus, at core modern materials design. Conventionally, studies have, large extent, focused on pristine bulk phases. However, realistic exist complex form; their microstructures consist different point extended defects. The presence defects...

The electronic structure of halide perovskites is central to their carrier dynamics, enabling the excellent optoelectronic performance. However, experimentally resolved transient absorption spectra exhibit large discrepancies from commonly computed by density functional theory. Using pseudocubic CsPbI3 as a prototype example, here, it unveiled with both ab initio molecular dynamics simulations and transmission electron microscopy that there exists pronounced dynamical lattice distortion in...

Abstract Structural search and feature extraction are a central subject in modern materials design, the efficiency of which is currently limited, but can be potentially boosted by machine learning (ML). Here, we develop an ML-based prediction-analysis framework, includes symmetry-based combinatorial crystal optimization program (SCCOP) additive attribution model, to significantly reduce computational costs extract property-related structural features. Our method highly accurate predictive,...

Constructing carbonaceous materials with versatile surface structures still remains a great challenge due to limited self-assembly methods, especially at high temperatures. This study presents an innovative template evolution induced relay (TEIRSA) for the fabrication of large polyoxometalate (POM)-mixed nanosheets featuring mesoporous through hydrothermal carbonization (HTC). The method employs POM and acetone as additives, cleverly modulating Ostwald ripening-like process P123-based...