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Two-dimensional (2D) inorganic nanomaterials have garnered extensive attention in the fabrication of inorganic nanofiltration membranes due to their unique structures and properties. In this study, we developed a facile process for fabricating large-scale ultrahydrophilic nanofiltration membranes using layered titanate H 1.07 Ti 1.73 O 4 · n H 2 O nanosheets (HT-ns). A drying deposition process was used to fabricate HT-ns membranes on a poly(tetrafluoroethylene) (TF) substrate. To enhance the bonding strength between the substrate and the deposited HT-ns membrane, the substrate surface was modified with a Cu 2+ -adsorbed silane monomolecular layer, connecting a negatively charged HT-ns membrane and a positively charged substrate surface. The fabricated HT-ns membrane exhibited an excellent rejection performance for inorganic salts and dye molecules. The ultrahydrophilicity of HT-ns membrane with a low water contact angle of 31° results in an ultrafast water permeance, which is approximately 6 times higher than that of a simple graphene-based nanofiltration membrane. The results open a new avenue to a new category of ultrahydrophilic nanofiltration membranes.

β-Ga 2 O 3 is an ultrawide-band gap semiconductor with excellent potential for high-power and ultraviolet optoelectronic device applications. Low thermal conductivity is one of the major obstacles to enable the full performance of β-Ga 2 O 3 -based devices. A promising solution for this problem is to integrate β-Ga 2 O 3 with a diamond heat sink. However, the thermal properties of the β-Ga 2 O 3 /diamond heterostructures after the interfacial bonding have not been studied extensively, which are influenced by the crystal orientations and interfacial atoms for the β-Ga 2 O 3 and diamond interfaces. In this work, molecular dynamics simulations based on machine learning potential have been adopted to investigate the crystal-orientation-dependent and interfacial-atom-dependent thermal boundary resistance (TBR) of the β-Ga 2 O 3 /diamond heterostructure after interfacial bonding. The differences in TBR at different interfaces are explained in detail through the explorations of thermal conductivity value, thermal conductivity spectra, vibration density of states, and interfacial structures. Based on the above explorations, a further understanding of the influence of different crystal orientations and interfacial atoms on the β-Ga 2 O 3 /diamond heterostructure was achieved. Finally, insightful optimization strategies have been proposed in the study, which could pave the way for better thermal design and management of β-Ga 2 O 3 /diamond heterostructures according to guidance in the selection of the crystal orientations and interfacial atoms of the β-Ga 2 O 3 and diamond interfaces.

KNbO 3 (KN) with a perovskite structure is an outstanding representative of lead-free piezoelectric materials, and its mesocrystals have broad application prospects in the fields of catalysis, energy storage, and conversion. However, the formation conditions of KN mesocrystals reported so far are difficult owing to their high aspect ratio and excellent preferred orientation. In this study, the solvothermal process was used successfully to prepare the flake-like potassium salt of Lindquist hexaniobate (K 8 Nb 6 O 19 ·10H 2 O). Subsequently, the precursor niobate was calcined to prepare two-dimensional (2D) plate-like KN mesocrystals. The formation mechanism of the plate-like KN mesocrystals is further revealed from a paired topochemical mesocrystal conversion of K 8 Nb 6 O 19 ·10H 2 O niobate. Finally, the microscopic piezoelectric and photocatalytic responses of the obtained plate-like KN mesocrystals were investigated. The high piezoelectric coefficient of plate-like KN mesocrystals implies that excellent charge separation promotes the photocatalytic performance of rhodamine B (RhB). This study provides a strategy for the efficient application of 2D oriented materials in the field of piezoelectricity and photocatalysis.

As practical interest in the flexible or wearable thermoelectric generators (TEGs) has increased, the demand for the high-performance TEGs based on ecofriendly, mechanically resilient, and economically viable TEGs as alternatives to the brittle inorganic materials is growing. Organic or hybrid thermoelectric (TE) materials have been employed in flexible TEGs; however, their fabrication is normally carried out using wet processing such as spin-coating or screen printing. These techniques require materials dissolved or dispersed in solvents; thus, they limit the substrate choice. Herein, we have rationally designed solvent-free, all carbon-based TEGs dry-drawn on a regular office paper using few-layered graphene (FLG). This technique showed very good TE parameters, yielding a power factor of 97 μW m -1 K -2 at low temperatures. The p-type only device exhibited an output power of up to ∼19.48 nW. As a proof of concept, all carbon-based p-n TEGs were created on paper with the addition of HB pencil traces. The HB pencil exhibited low Seebeck coefficients (-7 μV K -1 ), and the traces were highly resistive compared to FLG traces, which resulted in significantly lower output power compared to the p-type only TEG. The demonstration of all carbon-based TEGs drawn on paper highlights the potential for future low-cost, flexible, and almost instantaneously created TEGs for low-power applications., Competing Interests: The authors declare no competing financial interest., (© 2021 The Authors. Published by American Chemical Society.)

KNbO 3 (KN) piezoelectric polycrystals were prepared by a two-step solvothermal reaction process with the managed organic solvents as reaction mediums at a low temperature for a short time. In the solvothermal reaction system, the formation mechanism of polycrystalline KN is mainly the dissolution-deposition mechanism. The influences of alkalinity, viscosity, and the polarity for reaction mediums on the formation of the niobates were investigated. The chemical reaction mechanisms of niobate products and formation mechanism of niobate crystals from the precursor were clarified. The regulating and controlling mechanism of the phase compositions, the morphologies, and the lattice constants for the niobates obtained in varied reaction mediums were revealed. The obtained KN piezoelectric polycrystals are constructed from oriented KN nanocrystals. Piezoelectric hysteresis loops of cuboid KN polycrystals were detected for the first time. A prepared cuboid KN polycrystal shows an average d 33 * value of 32 pm/V. The study provides a strategy for the development of oriented KN piezoelectric materials to apply the orientation engineering.

A series of isomers of tetranitro-bis-1,2,4-triazoles were designed, and their electronic structures, heats of formation, densities, detonation performances, thermal stabilities, and impact sensitivities were investigated by density functional theory (DFT). The structure and energetic properties of 1,3,5,7-tetranitro-1,3,5,7-tetrazocane (HMX) were also calculated at the same level. On comparing with the detonation velocity and pressure and bond dissociation energy (BDE) of HMX, it was found that four isomers (BT2, BT5, BT6, BT7) have higher detonation performances than HMX and three isomers (BT5, BT6, BT7) have better thermal stabilities than HMX. The calculated results of impact sensitivities indicated that all of the designed isomers have more sensitivity than HMX. The calculated results of energy gaps between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) indicated that all of the designed isomers were more easily excited than HMX in the chemical reaction process. In particular, 3,3',5,5'-tetranitro-1,1'-bis-1,2,4-triazoles (BT5) exhibited excellent detonation performances (9464 m s -1 , 39.44 GPa) and good thermal stability (BDE 256.81 kJ mol -1 ). The results indicated that the isomerization of tetranitro-bis-1,2,4-triazoles could improve their detonation performance or thermal stability and might lead to a promising isomer possessing both good performance and high thermal stability., Competing Interests: The authors declare no competing financial interest., (Copyright © 2020 American Chemical Society.)

Tetrafunctionalized calix[4]resorcinarene cavitands commonly serve as supramolecular scaffolds for construction of coordination-driven self-assembled capsules. However, due to the calix-like shape, the structural diversity of assemblies is mostly restricted to dimeric and hexameric capsules. Previously, we reported a spontaneous heteroleptic complexation strategy based on a pair of self-recognizable terpyridine-based ligands and Cd II ions. Building on this complementary ligand pairing system, herein three types of nanocapsules, including a dimeric capsule, a Sierpiński triangular prism, and a cubic star, could be readily obtained through dynamic complexation reactions between a tetratopic cavitand-based ligand and various multitopic counterparts in the presence of Cd II ions. The dimeric capsular assemblies display the spacer-length-dependent self-sorting behavior in a four-component system. Moreover, the precise multicomponent self-assembly of a Sierpiński triangular prism and a cubic star possessing three and six cavitand-based motifs, respectively, demonstrates that such self-assembly methodology is able to efficiently enhance architectural complexity for calix[4]resorcinarene-containing metallo-supramolecules.

Bacterial populations use a cell-to-cell communication system to coordinate community-wide regulation processes, which is termed quorum sensing (QS). Autoinducer-2 (AI-2) is a universal signal molecule that mediates inter- and intraspecies QS systems among different bacteria. In this study, the effects of exogenous addition of AI-2 synthesized in vitro on physiological behaviors and proteome were investigated in lactic acid bacteria strains. Exogenous AI-2 had a concentration-dependent effect on the Enterococcus faecium 8-3 cell density. There was no significant influence on biofilm formation and individual morphology of cells upon 60 μM AI-2 addition in E. faecium 8-3 and Lactobacillus fermentum 2-1. However, it improved the acid and alkali resistance of E. faecium 8-3. With the addition of AI-2, 15 differentially expressed proteins were identified in E. faecium 8-3, which participate in RNA transport signaling, RNA polymerase, ribosome, oxidative phosphorylation, cysteine and methionine metabolism, pyrimidine metabolism, ATP-binding cassette (ABC) transporters, purine metabolism, biosynthesis of the amino acid pathway, etc. Among them, the expression of 5-methylthioadenosine/ S -adenosylhomocysteine nucleosidase, which is known to be involved in AI-2 synthesis and cysteine and amino acid metabolism, was upregulated. These findings will lay the foundation to clarify the mechanism of cell-to-cell communication and bacterial physiological behaviors mediated by AI-2., Competing Interests: The authors declare no competing financial interest., (Copyright © 2020 American Chemical Society.)

To meet the growing demands in flexible and wearable electronics, various sensors have been designed for detecting and monitoring the physical quantity changes. However, most of these sensors can only detect one certain kind of physical quantity based on a single mechanism. In this paper, we have fabricated a multifunctional sensor made from carbonized electrospun polyacrylonitrile/barium titanate (PAN-C/BTO) nanofiber film. It can detect two physical quantities (pressure and curvature), independently and simultaneously, by integrating piezoresistive, piezoelectric, and triboelectric effects. For flex sensing with the impedance change of PAN-C/BTO nanofiber films during bending, it had a sensitivity of 1.12 deg -1 from 58.9° to 120.2° and a working range of 28°-150°. For self-powered force sensing, it had a gauge factor of 1.44 V·N -1 within the range of 0.15-25 N. The sensor had a long stability over 60 000 cycles at both sensing modes. The inclusion of barium titanate nanoparticles (BTO NPs) into the nanofiber film had an over 2.4 times enhancement of sensitivity for pressure sensing because of the synergy of piezoelectric and triboelectric effects. On the basis of multifunction and modularity, a series of potential applications of the sensor were demonstrated, including sensing human's swallowing, walking gaits, finger flexure, and finger-tapping. The self-powered flexible dual-mode sensor has great application potential in human-computer interactive and smart wearable sensing systems.

Haze events in China megacities involve the rapid oxidation of SO 2 to sulfate aerosol. Given the weak photochemistry that takes place in these optically thick hazes, it has been hypothesized that SO 2 is mostly oxidized by NO 2 emissions in the bulk of pH > 5.5 aerosols. Because NO 2 (g) dissolution in water is very slow and aerosols are more acidic, we decided to test such a hypothesis. Herein, we report that > 95% of NO 2 (g) disproportionates [2NO 2 (g) + H 2 O(l) = H + + NO 3 - (aq) + HONO (R1)] upon hitting the surface of NaHSO 3 aqueous microjets for < 50 μs, thereby giving rise to strong NO 3 - ( m/ z 62) signals detected by online electrospray mass spectrometry, rather than oxidizing HSO 3 - ( m/ z 81) to HSO 4 - ( m/ z 97) in the relevant pH 3-6 range. Because NO 2 (g) will be consumed via R1 on the surface of typical aerosols, the oxidation of S(IV) may in fact be driven by the HONO/NO 2 - generated therein. S(IV) heterogeneous oxidation rates are expected to primarily depend on the surface density and liquid water content of the aerosol, which are enhanced by fine aerosol and high humidity. Whether aerosol acidity affects the oxidation of S(IV) by HONO/NO 2 - remains to be elucidated.

Piezotronics and piezophototronics are emerging fields by coupling piezoelectric, semiconductor, and photon excitation effects for achieving high-performance strain-gated sensors, LEDs, and solar cells. The built-in piezoelectric potential effectively controls carrier transport characteristics in piezoelectric semiconductor materials, such as ZnO, GaN, InN, CdS, and monolayer MoS 2 . In this paper, a topological insulator piezotronic transistor is investigated theoretically based on a HgTe/CdTe quantum well. The conductance, ON/OFF ratio, and density of states have been studied at various strains for the topological insulator piezotronic transistor. The ON/OFF ratio of conductance can reach up to 10 10 with applied strain. The properties of the topological insulator are modulated by piezoelectric potential, which is the result of the piezotronic effect on quantum states. The principle provides a method for developing high-performance piezotronic devices based on a topological insulator.

Innovative secondary organic aerosol (SOA) composition analysis methods normalizing aerosol yield and chemical composition on an aromatic ring basis are developed and utilized to explore aerosol formation from oxidation of aromatic hydrocarbons. SOA yield and chemical composition are revisited using 15 years of University of California, Riverside/CE-CERT environmental chamber data on 17 aromatic hydrocarbons with HC:NO ranging from 11.1 to 171 ppbC:ppb. SOA yield is redefined in this work by normalizing the molecular weight of all aromatic precursors to the molecular weight of the aromatic ring [Formula: see text], where i is the aromatic hydrocarbon precursor. The yield normalization process demonstrates that the amount of aromatic rings present is a more significant driver of aerosol formation than the vapor pressure of the precursor aromatic. Yield normalization also provided a basis to evaluate isomer impacts on SOA formation. Further, SOA elemental composition is explored relative to the aromatic ring rather than on a classical mole basis. Generally, four oxygens per aromatic ring are observed in SOA, regardless of the alkyl substitutes attached to the ring. Besides the observed SOA oxygen to ring ratio (O/R ∼ 4), a hydrogen to ring ratio (H/R) of 6 + 2n is observed, where n is the number of nonaromatic carbons. Normalization of yield and composition to the aromatic ring clearly demonstrates the greater significance of aromatic ring carbons compared with alkyl carbon substituents in determining SOA formation and composition.

Dynamic covalent chemistry (DCC) has become a powerful tool for the creation of molecular assemblies and complex systems in chemistry and materials science. Herein we developed for the first time quantitative reactivity scales capable of correlation and prediction of the equilibrium of dynamic covalent reactions (DCRs). The reference reactions are based upon universal DCRs between imines, one of the most utilized structural motifs in DCC, and a series of O-, N-, and S- mononucleophiles. Aromatic imines derived from pyridine-2-carboxyaldehyde exhibit capability for controlling the equilibrium through distinct substituent effects. Electron-donating groups (EDGs) stabilize the imine through quinoidal resonance, while electron-withdrawing groups (EWGs) stabilize the adduct by enhancing intramolecular hydrogen bonding, resulting in curvature in Hammett analysis. Notably, unique nonlinearity induced by both EDGs and EWGs emerged in Hammett plot when cyclic secondary amines were used. This is the first time such a behavior is observed in a thermodynamically controlled system, to the best of our knowledge. Unified quantitative reactivity scales were proposed for DCC and defined by the correlation log K = S(N) (R(N) + R(E)). Nucleophilicity parameters (R(N) and S(N)) and electrophilicity parameters (R(E)) were then developed from DCRs discovered. Furthermore, the predictive power of those parameters was verified by successful correlation of other DCRs, validating our reactivity scales as a general and useful tool for the evaluation and modeling of DCRs. The reactivity parameters proposed here should be complementary to well-established kinetics based parameters and find applications in many aspects, such as DCR discovery, bioconjugation, and catalysis.