Table_1_Acquisition of non-canonical word orders in Mandarin Chinese.DOCX

To better understand Mandarin-speaking children’s acquisition of non-canonical word orders, we tested comprehension and production of Mandarin non-canonical active ba-construction and passive bei-construction, in comparison with canonical active SVO sentences among 180 children between three and 6 years of age. Our results showed that children had more difficulties with bei-construction compared to SVO sentences in both comprehension and production, but early problems of ba-construction only lied in production. We discussed these patterns in connection with two accounts of language acquisition which attribute language development to the maturation of grammar or to the exposure to the input, respectively.</p

Electronic Structure Theory Study of the Microsolvated F^–(H₂O) + CH₃I S_N2 Reaction

The potential energy profile of microhydrated fluorine ion reaction with methyl iodine has been characterized by extensive electronic structure calculations. Both hydrogen-bonded F^–(H₂O)---HCH₂I and ion–dipole F^–(H₂O)---CH₃I complexes are formed for the reaction entrance and the PES in vicinity of these complexes is very flat, which may have important implications for the reaction dynamics. The water molecule remains on the fluorine side until the reactive system goes to the S_N2 saddle point. It can easily move to the iodine side with little barrier, but in a nonsynchronous reaction path after the dynamical bottleneck to the reaction, which supports the previous prediction for microsolvated S_N2 systems. The influence of solvating water molecule on the reaction mechanism is probed by comparing with the influence of the nonsolvated analogue and other microsolvated S_N2 systems. Taking the CCSD­(T) single-point calculations based on MP2-optimized geometries as benchmark, the DFT functionals B97-1 and B3LYP are found to better characterize the potential energy profile for the title reaction and are recommended as the preferred methods for the direct dynamics simulations to uncover the dynamic behaviors

Theoretical Prediction of Chemically Bound Compounds Made of Argon and Hydrocarbons

Equilibrium structures, vibrational properties, and stabilities of organo-argon compounds, HArC4H and HArC6H, are studied at the MP2=full/6-311++G(2d,2p) level of theory. Ab initio calculations show that the two molecules are metastable, but protected against the Ar + HY (Y = C4H or C6H) dissociation by high barriers, and these species are energetically stable with respect to the three separate fragments (H + Ar +Y). The implied kinetic stability of HArC4H and HArC6H molecules suggests that these species should very likely be candidates for experimental observation. The results may open possibilities of organic chemistry of light noble gas elements

Predicted Organic Noble-Gas Hydrides Derived from Acrylic Acid

The Ar-, Kr-, and Xe-insertion compounds into acrylic acid, i.e., C₂H₃COONgH (Ng = Ar, Kr, and Xe), have been studied by ab initio calculations. The geometry optimization, frequency calculation, and stability were investigated at the MP2/aug-cc-pVTZ (aug-cc-pVTZ-PP) level of theory. Two configuration isomers, i.e., <i>s-cis syn</i> (isomer A) and <i>s-cis anti</i> (isomer B), were optimized for each molecule. Using the <i>s-cis syn</i> structure (isomer A) as an example, we performed natural bond orbital (NBO) analysis, natural energy decomposition analysis (NEDA), and atom-in-molecules (AIM) analysis to investigate the bonding nature of these noble-gas compounds. Our study predicts the existence of Kr- and Xe-derivatives of acrylic acid and the instability of Ar-related compounds

Janus Silica Hollow Spheres Prepared via Interfacial Biosilicification

A poly­(ethylene glycol)<i>-<i>b</i>-</i>poly­(_L-lysine)<i>-<i>b</i>-</i>poly­(styrene) (PEG-PLL-PS) triblock copolymer, which contains a cationic PLL block as the middle block, is synthesized via a combination of ring-opening polymerization (ROP) and atom-transfer radical polymerization (ATRP). The PEG-PLL-PS (ELS) triblock is employed as a macromolecular surfactant to form a stable oil-in-water (O/W) emulsion, which is subsequently used as the template to prepare Janus silica hollow spheres (JHS) via a one-pot biosilicification reaction. For the emulsion template, the middle PLL block assembles at the O/W interface and directs the biomimetic silica synthesis in the presence of phosphate buffer and silicic acid precursors. This biosilicification process takes place only in the intermediate layer between water and the organic interior phase, leading to the formation of silica JHSs with hydrophobic PS chains tethered to the inner surface and PEG attached to the outer surface. The three-layer JHSs, namely, PEG/silica-polylysine/PS composites, were verified by electron microscopy. Upon further breaking these JHSs into species, polymer-grafted Janus silica nanoplates (JPLs) can be obtained. Our studies provide an efficient one-step method for preparing hybrid silica Janus structures within minutes

Hydrolysis of Ammonia Borane on a Single Pt Atom Supported by N‑Doped Graphene

The hydrolysis of ammonia borane (NH3BH3 or AB) at room temperature is a promising method to produce hydrogen, but the complete reaction mechanism is still less investigated. Herein, the full hydrolysis process of the AB molecule on single Pt atom coordinated by two carbon atoms and one nitrogen atom (Pt1–C2N1) on nitrogen doped graphene is investigated using the density functional theory (DFT) method. Our results demonstrate that the rate-limiting step is the formation of *BH2NH3 by breaking the first B–H bond in AB with an energy barrier of 0.68 eV, implying that Pt1–C2N1 is a potential room-temperature catalyst for the full hydrolysis of AB. In addition, 27 more types of M1–C2N1 (M represents transiton metal atom) and Pt1 supported on nitrogen-doped graphene with different local coordination environments (Pt1–CxNy, x and y are the number of carbon and nitrogen atoms that coordinated with the platinum atom) are considered to screen out potential single-atom catalysts for AB hydrolysis. The screening results further show that Pt1–C1N2 is another potential catalyst for AB hydrolysis. In particular, two hydrogen atoms precovered on Pt1–C1N2, resulting in a lower energy barrier for the rate-limiting step than that on Pt1–C2N1. This study provides a prototype of Pt1–C1N2 and Pt1–C2N1 for catalytic full hydrolysis of AB at room temperature

Data-Driven Discovery of a Covalent Organic Framework Heterojunction as Efficient Photocatalysts for Overall Solar Water Splitting

Searching for highly efficient visible-light photocatalysts is a high-cost and time-consuming process in the water splitting field. The integration of data-driven screening based on the database and density functional theory calculations represents a promising approach. In this study, we first present a topologically assembled single-layer covalent organic framework (COF) that is used to build a COF heterojunction database via AA stacking. Then we propose a systematic search procedure for COF heterojunctions as overall solar water splitting photocatalysts, including suitable band gap (screen 1), appropriate band edge position (screen 2), spontaneous catalytic reactions for water splitting (screen 3), and efficient separation of photogenerated electrons and holes (proof). Finally, we successfully identify 1 heterojunction from the pool of 222 items as an efficient photocatalyst for overall solar water splitting. Clearly, this kind of data-driven screening procedure, based on a COF heterojunction database, opens up new avenues and inspires the development of high-performance photocatalysts

Identified OTUs for hand surface bacteria data.

<p>Identified OTUs for hand surface bacteria data.</p

Bipolar Rashba Semiconductors: A Class of Nonmagnetic Materials for Electrical Spin Manipulation

The realization of the electrical control of spin is highly desirable. One promising approach is by regulating the Rashba spin–orbit coupling effect of materials through external electric fields. However, this method requires materials to possess either a high electric field response and a large Rashba constant or the simultaneous presence of Rashba splitting and ferroelectric polarization. These stringent requirements result in a scarcity of suitable materials. In order to surpass these limitations and exploit a new prospect for spin manipulation via the Rashba effect, a conceptual class of materials named bipolar Rashba semiconductors (BRS) is proposed, whose valence band and conduction band possess opposite spin texture directions when approaching the Fermi level. The unique electronic structure of BRS makes it feasible to reverse the spin precession by simply applying a gate voltage. The existence of BRS is confirmed through first-principles calculations on the two-dimensional (2D) material AlBiS3

Data_Sheet_1_Serum Chloride Is Inversely Associated With 3 Months Outcomes in Chinese Patients With Heart Failure, a Retrospective Cohort Study.docx

BackgroundSerum chloride was recently found to be associated with prognosis of heart failure in western countries. However, the evidence was scarce in Asia. We aimed to investigated the relationship between serum chloride and clinical outcomes in a Chinese cohort with hospitalized heart failure.MethodsWe retrospectively analyzed the data from PhysioNet, involving 1996 patients who were admitted with heart failure between December 2016 and June 2019. Outcome was a composite endpoint of all-cause death or rehospitalization at 3 months.ResultsThe incidence of the composite endpoint was 26.8% (535/1,996); it was 32.2% (213/662), 25.0% (165/661), and 23.3% (157/673) by chloride tertiles (from the lowest to the highest), respectively. The serum chloride at admission was independently and inversely associated with the composite endpoint risk (hazard ratio: 0.967; 95% confidence interval: 0.939 to 0.996; p = 0.026) in contrast to sodium, which was no longer significant (p > 0.05) after multivariable adjustment. Pearson correlation between serum chloride and sodium was 0.747 (p ConclusionsLow serum chloride at admission was associated with poor outcomes in Chinese hospitalized patients with heart failure. These findings warrant future studies for tackling the potential pathophysiological mechanisms and correction methods of hypochloremia in heart failure.</p