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Direct air capture (DAC) is a sustainable technology to alleviate the greenhouse effect and a reliable pathway to acquire inexhaustible CO2 for the production of costly chemicals and energy products. Current DAC technologies with amine‐related sorbents rely on chemisorption, while they consume intensive energy for CO2 release and sorbent regeneration by heating. Developing new DAC processes with weak, reversible adsorption can substantially reduce the regeneration energies. Herein, the design of CO2 breathing paper (CBP) is demonstrated toward spontaneous CO2 extraction from ambient air and solar‐driven regeneration. The CBP is fabricated by coupling 2‐ethyl‐4‐methylimidazole to carbon nanotube paper on the basis of density functional theory calculations. At ambient conditions, CBP spontaneously captures atmospheric CO2 with a capacity of 0.14–1.75 mmol g–1 at 0–35 °C through non‐covalent electrostatic interaction. Upon exposure to sunlight, all adsorbed CO2 can be released and converted to concentrated gas for storage. Attractively, the efficiency of solar‐driven CO2 release is much higher than the traditional temperature‐swing method owing to the IR sensitivity of CO2. Besides the reversibility, the mild conditions also ensure the durability of CBP. These findings suggest that the CBP is a promising candidate for cost‐effective DAC. [ABSTRACT FROM AUTHOR]

Although possessing well‐defined nanostructures and excellent multi‐electron redox properties, polyoxometalate clusters have poor intrinsic electrical conductivity and are prone to aggregation due to large surface energy, which makes them difficult to be fully utilized when applying as electrode materials for lithium‐ion batteries. In this paper, monodisperse K7MnV13O38 (MnV13) clusters are achieved by rationally utilizing nano‐sized high conductive carbon dots (CDs) as stabilizers. Benefiting from the fully exposed redox sites of MnV13 clusters (high utilization rate) and sufficient interfaces with carbon dots (extra interfacial energy storage), the optimized MnV13/10CDs anode delivers a high discharge capacity up to 1348 mAh g−1 at a current density of 0.1 A g−1 and exhibits superb rate/cycling capabilities. Density functional theory (DFT) calculations verify that ionic archway channels are formed between MnV13 and CDs, eliminating the bandgap and greatly improving the electron/ion conductivity of MnV13 and CDs. This paper paves a brand‐new way for synthesis of monodisperse clusters and maximization of extra interfacial energy storage. [ABSTRACT FROM AUTHOR]

CuS is an encouraging photoelectrode candidate that meets the essential requirements for efficient solar‐to‐hydrogen production, but it has not been thoroughly studied. A CuS light absorber layer is grown by the self‐assembly of copper and sulfur precursors on a carbon paper (CP) electrode. Simultaneously, rGO is introduced as a buffer layer to control the optical and electrical properties of the absorber. The well‐ordered microstructural arrangement suppresses the recombination loss of electrons and holes owing to enhanced charge‐carrier generation, separation, and transport. The potential reaching 10 mA cm−2 in 1.0 m KOH solution is significantly lowered to 0.87 V, and the photocurrent density at 1.23 V is 94.7 mA cm−2. The computational result reveals that the potential‐determining step is sensitive to O* stability; the lower stability of O* in the thin layer of CuS/rGO decreases the free‐energy gap between the initial and final states of the potential‐determining step, resulting in a lowering of the onset potential. The faradaic efficiency for the photoelectrochemical oxygen evolution reaction in the optimized 2CuS/1rGO/CP photoanode is 98.60%, and the applied bias photon‐to‐current and the solar‐to‐hydrogen efficiencies are 11.2% and 15.7%, respectively, and its ultra‐high performance is maintained for 250 h. These record‐breaking achievement indices may be a trigger for establishing a green hydrogen economy. [ABSTRACT FROM AUTHOR]

The present paper reports a remote carbon‐to‐carbon boryl migration via an intramolecular 1,4‐B/Cu shift, which establishes an in situ stereospecific electrophilic trap on the alkene moiety. The synthetic application is developed to prepare functionalized cyclopentenes by means of a palladium‐catalyzed regioselective intramolecular coupling that completes a strategic cyclopropanation and generates valuable structural bicyclic systems. The mechanism is characterized by DFT (density functional theory) calculations which showed that the 1,4‐migration proceeds through an intramolecular, nucleophilic attack of the copper‐alkyl moiety on the boron atom bonded to the C(sp2), leading to a 5‐membered boracycle structure. The computation of the 1,3‐ and 1,4‐B/Cu shifts is also compared as is the impact of the endo‐ or exocyclic alkene on the reaction kinetics. [ABSTRACT FROM AUTHOR]

The capacity to manipulate magnetization in 2D dilute magnetic semiconductors (2D‐DMSs) using light, specifically in magnetically doped transition metal dichalcogenide (TMD) monolayers (M‐doped TX2, where M = V, Fe, and Cr; T = W, Mo; X = S, Se, and Te), may lead to innovative applications in spintronics, spin‐caloritronics, valleytronics, and quantum computation. This Perspective paper explores the mediation of magnetization by light under ambient conditions in 2D‐TMD DMSs and heterostructures. By combining magneto‐LC resonance (MLCR) experiments with density functional theory (DFT) calculations, we show that the magnetization can be enhanced using light in V‐doped TMD monolayers (e.g., V‐WS2, V‐WSe2). This phenomenon is attributed to excess holes in the conduction and valence bands, and carriers trapped in magnetic doping states, mediating the magnetization of the semiconducting layer. In 2D‐TMD heterostructures (VSe2/WS2, VSe2/MoS2), the significance of proximity, charge‐transfer, and confinement effects in amplifying light‐mediated magnetism is demonstrated. We attributed this to photon absorption at the TMD layer that generates electron–hole pairs mediating the magnetization of the heterostructure. These findings will encourage further research in the field of 2D magnetism and establish a novel design of 2D‐TMDs and heterostructures with optically tunable magnetic functionalities, paving the way for next‐generation magneto‐optic nanodevices. [ABSTRACT FROM AUTHOR]

Understanding the adsorption interactions between carbon materials and sulfur compounds has far‐reaching impacts, in addition to their well‐known important role in energy storage and conversion, such as lithium‐ion batteries. In this paper, properties of intrinsic B or Si single‐atom doped, and B–Si codoped graphene (GR) and graphdiyne (GDY) were investigated by using density functional theory‐based calculations, in which the optimal doping configurations were explored for potential applications in adsorbing sulfur compounds. Results showed that both B or Si single‐atom doping and B–Si codoping could substantially enhance the electron transport properties of GR and GDY, improving their surface activity. Notably, B and Si atoms displayed synergistic effects for the codoped configurations, where B–Si codoped GR/GDY exhibited much better performance in the adsorption of sulfur‐containing chemicals than single‐atom doped systems. In addition, results demonstrated that, after B–Si codoping, the adsorption energy and charge transfer amounts of GDY with sulfur compounds were much larger than those of GR, indicating that B–Si codoped GDY might be a favorable material for more effectively interacting with sulfur reagents. [ABSTRACT FROM AUTHOR]

Transition metal sulfides as anode materials for sodium‐ion batteries (SIBs) have the advantage of high capacity. However, their cycle‐life and rate performance at ultra‐high current density is still a thorny issue that limit the applicability of these materials. In this paper, the carbon‐embedded heterojunction with sulfur‐vacancies regulated by ultrafine bimetallic sulfides (vacancy‐CoS2/FeS2@C) with robust interfacial C‐S‐Co/Fe chemical bonds is successfully synthesized and explored as an anode material for sodium‐ion battery. By changing the ratio of two metal cations, the concentration of anion sulfur vacancies can be in‐situ adjusted without additional post‐treatment. The as‐prepared vacancy‐CoS2/FeS2@C anode material offers ultrahigh rate performance (285.1 mAh g−1 at 200 A g−1), and excellent long‐cycle stability (389.2 mAh g−1 at 40 A g−1 after 10000 cycles), outperforming all reported transition metal sulfides‐based anode materials for SIBs. Both in‐situ and ex‐situ characterizations provide strong evidence for the evolution mechanism of the phases and stable solid‐electrolyte interface (SEI) on the vacancy‐CoS2/FeS2@C surface. The density functional theory calculations show that constructing heterojunction with reasonable concentration of vacancies can significantly increase the anode electronic conductivity. Notably, the assembled vacancy‐CoS2/FeS2@C//Na3V2(PO4)3/C full‐cell shows a capacity of 226.2 mAh g−1 after 400 cycles at 2.0 A g−1, confirming this material's practicability. [ABSTRACT FROM AUTHOR]

With the rapid development of flexible displays and wearable electronics, there are a substantial demand for colorless transparent polyimide (CPI) films with different properties. Traditional trial‐and‐error experimental methods are time‐consuming and costly, and density functional theory based prediction of HOMO‐LUMO gap energy also takes time and is prone to varying degrees of error. Inspired by machine learning (ML) applications in molecular and materials science, this paper proposed a data‐driven ML strategy to study the correlation between microscopic molecular mechanisms and macroscopic optical properties. Based on varying degrees of impact of various molecular features on the cutoff wavelength (λcutoff), the ML algorithm is first used to quickly and accurately predict the λcutoff of CPI. Several new CPI films are then designed and prepared based on the key molecular features, and the predicted values of their λcutoff are effectively verified within the experimental error range. The interpretability provided by the model allows to establish correlations between the nine key descriptors identified and their physicochemical meanings. The contributions are also analyzed to the transparency of polyimide films, thereby giving insight into the molecular mechanisms underlying transparency modulation for CPIs. [ABSTRACT FROM AUTHOR]

van der Waals (vdWs) interchain coupling is a unique feature of 1D vdWs materials, where strong vdWs coupling in 1D vdWs materials leads to the thickness‐dependent physical properties, while weak vdWs coupling can preserve the single‐chain property even in their thick counterparts. Different from 2D vdWs materials, due to their nanoscale widths, identifying and producing ultrathin 1D molecular chains are challenging, severely limit their device applications. Thus, looking for novel 1D vdWs materials with weak interchain coupling is crucial. In this paper, the authors report that the 1D ternary vdWs material, Mo6Se2I8 with non‐centrosymmetric characteristic and strong optical anisotropy, exhibits weak interchain coupling. On one hand, the density functional theory (DFT) calculations theoretically demonstrate its thickness‐independent electronic structure, negligible interchain differential charge density, and weak cleavage energy as low as 0.256 J m−2. On the other hand, the thickness‐independent work function and low first‐order temperature coefficient of −0.0030 cm−1 K−1 further experimentally confirm its weak interchain coupling. Moreover, taking advantage of this weak vdWs coupling characteristic, the in situ exfoliation of the Mo6Se2I8 nanowires is achieved by using a nanoprobe in a scanning electron microscope (SEM), obtaining ultrathin molecular chains with a thickness of ≈1.2 nm. [ABSTRACT FROM AUTHOR]

The attractive physiochemical properties of two dimensional materials demonstrate them to be an emerging class of potential candidates for use in sensing devices. Studies have shown that silicene can act as an excellent chemical sensor; however, no work has been studied about silicene as a glucose sensor. In this paper, using density functional theory, the interaction of pristine silicene and transition metal‐doped (Ag, Au, Cu, Ni, and Pt) silicene is studied with glucose molecules. The calculated adsorption energy, energy gap, and charge transfer value confirmed that the nickel‐doped silicene sheet can be a good glucose sensor with high sensitivity, moderate recovery time, and high conductivity. Further, the electron localization function and the reduced density gradient confirm the physisorption between the glucose molecule and the metal‐doped silicene sheets. [ABSTRACT FROM AUTHOR]

This paper is the first to look at the structural, electronic, mechanical, optical, and thermodynamic properties of the ANiX (ASc, Ti, Y, Zr, Hf; XBi, Sn) half‐Heusler (HH) using DFT based first principles method. The lattice parameters that we have calculated are very similar to those obtained in prior investigations with theoretical and experimental data. The positive phonon dispersion curve confirm the dynamical stability of ANiX (ASc, Ti, Y, Zr, Hf; XBi, Sn). The electronic band structure and DOS confirmed that the studied materials ANiX (ASc, Ti, Y, Zr, Hf; XBi, Sn) are direct band gap semiconductors. The investigation also determined significant constants, including dielectric function, absorption, conductivity, reflectivity, refractive index, and loss function. These optical observations unveiled our compounds potential utilization in various electronic and optoelectronic device applications. The elastic constants were used to fulfill the Born criteria, confirming the mechanical stability and ductility of the solids ANiX (ASc, Ti, Y, Zr, Hf; XBi, Sn). The calculated elastic modulus revealed that our studied compounds are elastically anisotropic. Moreover, ANiX (ASc, Ti, Y, Zr, Hf; XBi, Sn) has a very low minimum thermal conductivity (Kmin), and a low Debye temperature (θD), which indicating their appropriateness for utilization in thermal barrier coating (TBC) applications. The Helmholtz free energy (F), internal energy (E), entropy (S), and specific heat capacity (Cv) are determined by calculations derived from the phonon density of states. [ABSTRACT FROM AUTHOR]

A comprehensive study of the different classes of cycloaddition reactions ([3+2], [2+2], and [2+1]) of SO2 to acetylene and ethylene has been performed using density functional theory (DFT) and composite wavefunction methods. The [3+2] cycloaddition reaction, that was previously explored in the context of the cycloaddition of thioformaldehyde S‐methylide (TSM) to ethylene and acetylene, proceeds in a concerted way to the formation of stable heterocycles. In this paper, we extend our study to the [2+2] and [2+1] cycloadditions of SO2 to acetylene, which would produce 1,1‐oxathiete‐2‐oxide and thiirene‐1,1‐dioxide, respectively. One of the main conclusions is that cyclic 1,1‐oxathiete‐2‐oxide can open through a relatively easy breaking of the SO single bond and rearrange toward sulfinyl acetaldehyde (SA). The SA molecule can easily undergo several internal rearrangements, which eventually lead to sulfenic acid and sulfoxide derivatives of ethenone, 1,2,3‐dioxathiole, and CO plus sulfinylmethane. The most probable path, however, produces 2‐thioxoacetic acid, whose derivatives (or those of the corresponding acetate) are usually obtained by Willgerodt–Kindler‐type sulfuration of acetates. This product can in turn decompose, leading to the final products CO2 and H2CS. Comparison of this decomposition path with that of 2‐amino‐2‐thioxoacetic acid shows that the process occurs through different H‐transfer processes. [ABSTRACT FROM AUTHOR]

Thanks to recent developments in hardware and software, quantum chemical methods are increasingly used for interpreting the complex mechanisms underlying polymerization reaction by homogeneous catalysis. Unfortunately, the dimensions of even the smallest realistic models are too large to permit the use of state‐of‐the‐art composite wave function methods. Under these circumstances, density functional theory still offers the best compromise between cost and accuracy. However, comprehensive benchmarks of different functionals are not yet available for this important research field. The main aim of the present paper is to fill this gap by performing an unbiased comparison of several density functionals and continuum solvent models for the stereo‐control in the propylene polymerization on prototypical catalysts inducing different reaction mechanisms. While it was not possible to define a unique computational protocol providing the best results in all the situations, the B3PW91 functional in conjunction with D3 empirical dispersions and the solvent model density solvent model performs remarkably well for three out of the four investigated catalysts. Under such circumstances, it is recommended to compare the results delivered by different models when approaching additional classes of catalysts. [ABSTRACT FROM AUTHOR]

The kinetics and storage‐capacity of NiCoMg‐ternary layered double hydroxide (NiCoMg‐LDH) are successfully boosted by valence engineering. As the cathode for aqueous magnesium‐ion batteries (AMIBs), the assembled NiCoMg‐LDH//active carbon (AC) delivers a high specific discharge capacity (121.0 mAh·g−1 at 0.2 A·g−1), long‐term cycling stability (85% capacity retention after 2000 cycles at 1.0 A·g−1) and an excellent performance at −30 °C. Moreover, NiCoMg‐LDH//perylenediimide (PTCDI) is assembled, achieving a high specific discharge capacity and long‐term cycling stability. X‐ray absorption spectra (XAS)/X‐ray photoelectron spectroscopy (XPS) analyses and Density functional theory (DFT) calculations disclose that the electrons are redistributed due to the 3d orbital overlap of Co/Ni atoms in NiCoMg‐LDH, which obviously reduces the valence states of Co/Ni atoms, enhances Mg─O bond strength and degree of hybridization of Co/Ni 3d and O 2p orbitals. Hence, the electronic conductivity is significantly enhanced and the electrostatic repulsion between Mg2+ and host layers is greatly reduced, giving rise to the improved diffusion kinetics and storage‐capacity of Mg2+. Furthermore, in situ Raman/X‐ray diffraction (XRD) and ex situ XPS reveal corresponding energy‐storage mechanism. This paper not only demonstrates the feasibility of LDHs as cathode for AMIBs, but also offers a new modification method of valence engineering for high‐performance electrode materials. [ABSTRACT FROM AUTHOR]

In this paper, we examine the cleavage fracture anisotropy in tantalum carbides, namely, TaC, α‐Ta2C, and ζ‐Ta4C3 − x, using density functional theory (DFT) calculations. Our investigation identifies the presence of multiple low‐energy cleavage planes indicating multiple potential pathways for crack propagation in these ceramics, even the low symmetry compounds. The anisotropy characteristics of cleavage fractures exhibited by α‐Ta2C and ζ‐Ta4C3 − x closely align with the intrinsic fracture anisotropy observed in TaC. Notably, there exist at least three pyramidal planes in ζ‐Ta4C3 − x whose cleavage energies are less than those of the carbon‐depleted basal planes, previously reported to have the lowest cleavage energy. The observed preference in experiments for cleavage along carbon‐depleted basal planes, exclusive of other identified low‐energy planes, points to factors beyond cleavage energy influencing cleavage plane preference. [ABSTRACT FROM AUTHOR]

Atom transfer radical addition (ATRA) of halogenated compounds with alkenes is well established but primary alkyl chlorides are understudied because of the difficult C−Cl bond activation. In this paper, we show that TONs of 61 can be achieved in the ATRA of ethyl chloroacetate onto styrene with [Cp*Ru(Cl)2(PPh3)] and 1,1′‐azobis(cyclohexanecarbonitrile) (ACHN) as a radical initiator, representing a three‐fold improvement compared to previous reports. New catalyst precursors of the type [Cp*Ru(Cl)2(PR3)] were synthesized and tested (R=Me, Et, Cy, Ph, p‐CF3C6H4 and p‐MeOC6H4). The kinetic reaction profiles were studied using in situ ATR−FTIR spectroscopy. Among these complexes, [Cp*Ru(Cl)2(PPh3)] gave the best yields while [Cp*Ru(Cl)2(PMe3)] showed the highest rate. While rates correlate with redox potentials (electronics), our investigation reveals that substrate sterics are important for the overall yield. Density functional theory calculations suggest an open‐shell singlet pathway, where polymerization is kinetically disfavored, explaining the selectivity towards ATRA products. [ABSTRACT FROM AUTHOR]

To delve into the microscopic property variations of the ConMoP(n = 1 ~ 5) cluster, this study employs density functional theory at the B3LYP/def2‐TZVP quantum chemistry level. The paper conducts a comprehensive theoretical analysis of the clusters, examining parameters such as bond lengths, bond angles, electronic localization function (ELF), interaction region indicator function (IRI), independent gradient model based on the Hirshfeld partition, deformation density, electronic space range, chemical hardness and softness, polarizability, and dipole moment. The optimization process reveals 16 stable configurations for the ConMoP(n = 1 ~ 5) cluster, predominantly taking on a steric form. As the cluster size increases, the electronic delocalization of Co atoms intensifies, while the electronic properties of Mo atoms remain relatively stable. Notably, P atoms maintain a high degree of electronic delocalization. The interatomic forces within the clusters predominantly exhibit covalent bonding, with no evident repulsive effects observed between atoms. The bonding between metal atoms in the clusters leans toward a preference for covalent interaction. The degree of dispersion in the clusters increases with their growth, particularly evident in configuration 5‐a, which displays a broader spatial distribution. Configuration 3‐a demonstrates the most favorable activity, showcasing a relatively stable structure. Overall, configuration 3‐a emerges as a focal point for catalytic reactions. This article provides a more comprehensive analysis of the ConMoP(n = 1 ~ 5) cluster, yielding diverse results and enhancing the theoretical understanding of this cluster. [ABSTRACT FROM AUTHOR]

This paper reports the principal values of the 13C chemical shift tensors for five nitrogen‐dense compounds (i.e., cytosine, uracil, imidazole, guanidine hydrochloride, and aminoguanidine hydrochloride). Although these are all fundamentally important compounds, the majority do not have 13C chemical shift tensors reported in the literature. The chemical shift tensors are obtained from 1H→13C cross‐polarization magic‐angle spinning (CP/MAS) experiments that were conducted at a high field of 18.8 T to suppress the effects of 14N‐13C residual dipolar coupling. Quantum chemical calculations using density functional theory are used to obtain the 13C magnetic shielding tensors for these compounds. The best agreement with experiment arises from calculations using the hybrid functional PBE0 or the double‐hybrid functional PBE0‐DH, along with the triple‐zeta basis sets TZ2P or pc‐3, respectively, and intermolecular effects modeled using large clusters of molecules with electrostatic embedding through the COSMO approach. These measurements are part of an ongoing effort to expand the catalog of accurate 13C chemical shift tensor measurements, with the aim of creating a database that may be useful for benchmarking the accuracy of quantum chemical calculations, developing nuclear magnetic resonance (NMR) crystallography protocols, or aiding in applications involving machine learning or data mining. This work was conducted at the National High Magnetic Field Laboratory as part of a 2‐week school for introducing undergraduate students to practical laboratory experience that will prepare them for scientific careers or postgraduate studies. [ABSTRACT FROM AUTHOR]

Benzophenone and related derivatives are widely used as photoinitiators for food packaging to cure inks or lacquers with ultraviolet (UV) light on cardboard and paper. However, there are concerns about the potential health risks of their migration into food. Knowing the physical and chemical properties of benzophenone and its derivatives could play a significant role in their quantification and analysis using chemical ionization mass spectrometry (CI‐MS) methods. These parameters are evaluated using B3LYP/6‐311++** density functional theory (DFT) implemented on Gaussian code. Ion–molecule chemistry through the selection of reagent ions, reaction energetics and kinetics, thermodynamic stability, and reactivity of molecules deemed to foster VOC identification and quantification via CI‐MS techniques. The VOCs under study are expected to undergo exothermic reactions from H3O+, NH4+, NO+, and O2+ ions, except endothermic proton transfer from NH4+ to 2‐hydroxy‐4‐methoxybenzophenone and 2,3,4‐trihydroxy benzophenone. These compounds possess less proton affinities than NH3 and are least stable in their protonated forms. The DFT computed properties provide the basis for developing reliable and accurate methods to detect and measure the presence of benzophenone and its derivatives in packaging materials and food products. [ABSTRACT FROM AUTHOR]

The implementation of supported metal catalysts heavily relies on the synergistic interactions between metal nanoparticles and the material they are dispersed on. It is clear that interfacial perimeter sites have outstanding skills for turning catalytic reactions over, however, high activity and selectivity of the designed interface‐induced metal distortion can also obtain catalysts for the most crucial industrial processes as evidenced in this paper. Herein, the beneficial synergy established between designed Pt nanoparticles and MnO in the course of the reverse water gas shift (RWGS) reaction resulted in a Pt/MnO catalyst having ≈10 times higher activity compared to the reference Pt/SBA‐15 catalyst with >99 % CO selectivity. Under activation, a crystal assembly through the metallic Pt (110) and MnO evolved, where the plane distance differences caused a mismatched‐row structure in softer Pt nanoparticles, which was identified by microscopic and surface‐sensitive spectroscopic characterizations combined with density functional theory simulations. The generated edge dislocations caused the Pt lattice expansion which led to the weakening of the Pt−CO bond. Even though MnO also exhibited an adverse effect on Pt by lowering the number of exposed metal sites, rapid desorption of the linearly adsorbed CO species governed the performance of the Pt/MnO in the RWGS. [ABSTRACT FROM AUTHOR]

Solution‐processed ternary‐compound semiconductor AgBiS2 colloidal quantum dots (CQDs) are promising light‐absorbing materials owing to their nontoxicity and high absorption coefficient (>106 cm−1). However, rational strategies to passivate multi‐facet of ternary‐compound CQDs and manufacture stable CQD inks have not yet been proposed. In this paper, a ligand passivation strategy is proposed using a solution‐phase ligand exchange method. A quadruple‐ligand ensemble is employed to demonstrate multifaceted passivation on AgBiS2 CQDs and a highly stable CQD ink. Density functional theory studies reveal the secondary cation adsorption of silver halide passivation, indicating the synergistic passivation of the ligand ensemble. This yields a low trap density in CQD solids, improving the power conversion efficiency to 8.1% by 53% in CQD solar cells. Furthermore, the proposed device exhibits the fastest response time of 400 ns among all reported AgBiS2 devices, demonstrating its potential for efficient lead‐free optoelectronics. [ABSTRACT FROM AUTHOR]

Hydrogen peroxide (H2O2) as relatively stable reactive oxygen species gains considerable attention because it can regulate physiological and pathological processes. In order to better detect H2O2, fluorescent probes were widely applied. Over the past 20 years, a great deal of boronate‐based fluorescent molecular probes appeared due to relatively simple oxidation reaction. However, the reaction mechanisms that boronate derivatives were converted into fluorescent product by H2O2 are poorly studied. In this paper, taking coumarin‐7‐pinacolboronate (CBU) as an example, the oxidation mechanism of boronate‐based probes by various reactive oxygen species was studied by theoretical calculations. The results found that (1) the chemical reaction mechanisms are nearly identical for the reactions of CBU with hydrogen peroxide, hypochlorous acid, peroxynitrite, and tyrosine hydroperoxide, respectively. (2) There is not radical intermediate during the reaction. (3) The different reactive oxygen species has a strong influence on rate limiting step and reaction rate. [ABSTRACT FROM AUTHOR]

The insulating gas and contacts in the arc extinguishing chamber of high‐voltage circuit breakers are the focus of research. In practical applications, the gas may react with the surface of the contacts. In this paper, C5F10O environmental friendly insulating gas, which has one of the potential alternatives, is selected as the research object. The compatibility of C5F10O and its decomposition products with CuW contacts was studied. This article uses the Dmol3 program based on density functional theory. The adsorption energy, transfer charge, and density of electronic states of C5F10O and selected typical decomposition products on the Cu (111) surface and Cu‐W surface were calculated, respectively. It was found that the original CuW metal properties were not changed before and after adsorption. The carbonyl O atom in C5F10O is easily adsorbed on the top of the Cu (111) surface, forming a stable CuO bond, which belongs to chemical adsorption. The interaction of the other three adsorption sites is weaker than that of the top site adsorption, which belongs to physical adsorption. C5F10O exhibits more active charge transfer and forms active W‐O chemical bonds when adsorbed on CuW surfaces than SF6. C5F10O has poorer compatibility with CuW alloy than SF6. C2F4 and C3F6 in the decomposition gas are chemically adsorbed on the Cu‐W surface. CO2, CF4, C2F6, and C3F8 do not form chemical bonds on the CuW surface. The adsorption stability of COF2 is weaker than that of CF4, C2F6, and C3F8. Compared with SF6 adsorption, the compatibility of C5F10O and CO2 on the surface of CuW contact is inferior to that of Cu contact. CF4, C2F6, C3F8, and COF2 in the decomposition gas can be compatible with the surface of the CuW contact. C2F4 and C3F6 cannot be well compatible with the surface of CuW contacts. © 2023 Institute of Electrical Engineer of Japan and Wiley Periodicals LLC. [ABSTRACT FROM AUTHOR]

To find an array of suitable materials for phosphorescent organic light‐emitting diodes (OLEDs), in this paper, we design six blue‐green phosphorescent Ir (III) complexes that have low‐efficiency roll‐off properties. Density functional theory and time‐dependent density functional theory were used to study the properties of (2‐[4‐phenoxyphenyl]pyridine [oppy])2Ir(acetylacetonate [acac]), (oppy)2Ir(picolinate [pic]), (oppy)2Ir(tetraphenylimido‐diphosphinate [tpip]), (5‐fluoro‐2‐(4‐phenoxyphenyl)pyridine [F‐oppy])2Ir(acac), (F‐oppy)2Ir(pic), and (F‐oppy)2Ir(tpip). Here, the main ligands are oppy and F‐oppy, while the auxiliary ligands are acac, pic, and tpip. The advantages of these complexes were analyzed in terms of electronic structure, frontier molecular orbital properties, spectral properties, and OLED display effect. We hope that our research will contribute to the development of the OLED industry. [ABSTRACT FROM AUTHOR]

In this paper, a complete quantum chemical study of propofol molecule has been done by using DFT‐B3LYP/6‐311G (d, p) method. The equilibrium geometry, HOMO–LUMO gap, NBO calculation, and DOS have been studied with the help of density functional theory (DFT) employing 6–311G (d, p) as the basis set. A good correlation is observed between experimental and calculated vibrational frequencies. Its molecular docking with 1B4N receptor shows that propofol can bind and inhibit the receptor enzymes therefore can act as an effective drug. NLO calculation shows that the molecule is good non‐linear optical candidate in future due to its more ICT moment of π–electron. Study shows that title molecule binds well with 1B4N protein. [ABSTRACT FROM AUTHOR]

In this paper, the electronic properties, the adhesive energy, and the interface energy of the MAX phase Ti2SnC(0001)/Ag(111) interface are systematically investigated using first principles based on density functional theory. Four different terminations of Ti2SnC(0001) are considered, and 16 different Ti2SnC(0001)/Ag(111) interface configurations are obtained by varying the stacking positions of the atoms. After calculating the electronic structure, adhesion work, and interface energy of these interface model interfaces with the same terminal but different atomic positions, it is found that the interface of the same terminal has a very limited effect on the interface bonding of the interface model by changing the stacking order of the interface atomic layer. By comparing the adhesion work and interface energy of 16 interface models, it is found that the HCP2 configuration of C‐Ti2SnC(0001)/Ag(111)interface structure has the highest adhesion work and the lowest interface energy. The larger the adhesion work is, the stronger the bonding between the interface atoms is. Meanwhile, the smaller the interface energy (positive value) is, the more stable the interface is. By calculating the electronic structure of the interface, the accuracy of the above results is further verified after analyzing the partial density of states (PDOS) and charge density difference of the interface. [ABSTRACT FROM AUTHOR]

Corannulenes have received much interest due to their electronic properties, which differ between the convex and concave surfaces of the molecule. The ability to control the shapes of corannulenes to optimize charge distribution is therefore important for the development of seminconductors and electronic devices. In this paper, the interactions of corannulenes are modeled inside carbon nanotubes of various sizes using the Lennard–Jones potential and a continuum approach. The major contribution of this work is the analytical expressions for the interaction energy, which are obtained as a function of the nanotube's radius, the offset distance of corannulene from the tube's axis and the orientation of corannulene. Minimizing this energy, the range of nanotube's radii that allow the corannulene to adopt lying, tilting and standing configurations both on‐ and off‐axis of the nanotubes is determined. These results are supported by the density functional theory calculations and agree with previously published work using molecular dynamics simulations for corannulenes located on the nanotube's axis. [ABSTRACT FROM AUTHOR]

In this paper, we study and discuss the structural, and electronic properties of the RbXF3 (X = Co, Mn, V or Fe) Perovskite Materials using the Density Functional Theory (DFT). Also, the origin of both semi‐conductor (SM) and half‐metallic (HM) characters have been outlined. The density functional theory (DFT) has been applied to illustrate the physical properties of the RbXF3 (X = Co, Mn, Fe or V) perovskite materials. The generalized gradient approximation introduced by Perdew–Burke and Ernzerhof (GGA‐PBE) with Hubbard correction has been used for modeling the physical properties of the RbXF3 (X = Co, Mn, V or Fe) perovskite compounds. The total and partial densities of states of each solar perovskite RbVF3 (X = Co, Mn, Fe or V) material have been illustrated and discussed. In addition, the contribution of the different elements: Rb, Co, Mn, Fe, V and F, has been investigated revealing the most contributing ones in the valance and conduction bands. The magnetic behavior of the studied solar perovskites RbVF3 (X = Co, Mn, Fe or V) materials, has been outlined. It is found that the perovskites RbCoF3 and RbFeF3 are half‐metallic, while the materials RbMnF3 and RbVF3 exhibit a semi‐conductor behavior. [ABSTRACT FROM AUTHOR]

Several strategies to synthesize desired 1,2,4‐triazolo[1,5‐a]pyridine‐2‐carboxylate targets have been reported over the years. The most convenient way features the preparation of the precursor triazolopyridine‐N‐oxide through a condensation step between sulfilimines and a nitrile oxide species, followed by a deoxygenation step. This paper presents a detailed work on the synthesis of [1,2,4]triazolo[1,5‐a]pyridine‐2‐carboxylate‐N‐oxide, featuring a synergistic experimental‐theoretical approach. Herein, we report the development of an efficient and straightforward method to prepare ethyl [1,2,4]triazolo[1,5‐a]pyridine‐2‐carboxylate 3‐oxide in continuous flow. The transfer from batch to flow processing resulted in a significant boost in isolated yield (53 % vs. 31 %) and a decrease in the simultaneous presence of starting materials and product in the reaction media from 4 hours to 3.5 minutes. An in‐depth mechanistic study of the reaction using density functional theory provided a deeper understanding of the whole reaction manifold and key indications on how to further improve the process in flow. [ABSTRACT FROM AUTHOR]

Zinc‐based batteries offer good volumetric energy densities and are compatible with environmentally friendly aqueous electrolytes. Zinc‐ion batteries (ZIBs) rely on a lithium‐ion‐like Zn2+‐shuttle, which enables higher roundtrip efficiencies and better cycle life than zinc‐air batteries. Manganese‐oxide cathodes in near‐neutral zinc sulfate electrolytes are the most prominent candidates for ZIBs. Zn2+‐insertion, H+‐insertion, and Mn2+‐dissolution are proposed to contribute to the charge‐storage mechanism. During discharge and charge, two distinct phases are observed. Notably, the pH‐driven precipitation of zinc‐sulfate‐hydroxide is detected during the second discharge phase. However, a complete and consistent understanding of the two‐phase mechanism of these ZIBs is still missing. This paper presents a continuum full cell model supported by density functional theory (DFT) calculations to investigate the implications of these observations. The complex‐formation reactions of near‐neutral aqueous electrolytes are integrated into the battery model and, in combination with the DFT calculations, draw a consistent picture of the cycling mechanism. The interplay between electrolyte pH and reaction mechanisms is investigated at the manganese‐oxide cathodes and the dominant charge‐storage mechanism is identified. The model is validated with electrochemical cycling data, cyclic voltammograms, and in situ pH measurements. This allows to analyze the influence of cell design and electrolyte composition on cycling and optimize the battery performance. [ABSTRACT FROM AUTHOR]

In this paper, the mechanical properties, electronic structures, and thermodynamic properties of Ag2Ga and CuGa2 under pressure are studied using the first‐principles method based on Density functional theory (DFT). With the increase in pressure, the equilibrium lattice constants (a/a0 and c/c0) and volume ratio (V/V0) of Ag2Ga and CuGa2 continuously decrease. The elastic constants show that Ag2Ga and CuGa2 are mechanically stable under pressures of 0–20 GPa, and the increase in pressure improves their deformation resistance. The results of Young's modulus (E) show that the hardness of CuGa2 is higher than that of Ag2Ga. The results of Cauchy pressure (C12 ‐ C44) and B/G ratio show that the plasticity of Ag2Ga and CuGa2 can be maintained with the increase in pressure. By analyzing the density of states (DOS), charge density difference (CDD), and population, the influence of pressure on electronic structure is studied. The calculated Debye temperature (θD) shows that the covalent bond of CuGa2 is stronger. [ABSTRACT FROM AUTHOR]

The stability of hybrid organic–inorganic halide perovskite semiconductors remains a significant obstacle to their application in photovoltaics. To this end, the use of low‐dimensional (LD) perovskites, which incorporate hydrophobic organic moieties, provides an effective strategy to improve their stability, yet often at the expense of their performance. To address this limitation, supramolecular engineering of noncovalent interactions between organic and inorganic components has shown potential by relying on hydrogen bonding and conventional van der Waals interactions. Here, the capacity to access novel LD perovskite structures that uniquely assemble through unorthodox S‐mediated interactions is explored by incorporating benzothiadiazole‐based moieties. The formation of S‐mediated LD structures is demonstrated, including one‐dimensional (1D) and layered two‐dimensional (2D) perovskite phases assembled via chalcogen bonding and S–π interactions. This involved a combination of techniques, such as single crystal and thin film X‐ray diffraction, as well as solid‐state NMR spectroscopy, complemented by molecular dynamics simulations, density functional theory calculations, and optoelectronic characterization, revealing superior conductivities of S‐mediated LD perovskites. The resulting materials are applied in n‐i‐p and p‐i‐n perovskite solar cells, demonstrating enhancements in performance and operational stability that reveal a versatile supramolecular strategy in photovoltaics. [ABSTRACT FROM AUTHOR]

Conjugated polymers exhibit significant potential for use in gas sensors owing to their flexibility and straightforward preparation. However, the performance of organic gas sensors based on such materials is currently suboptimal owing to their poor charge‐transport properties and limited selectivity. To address this limitation, a novel strategy that involves blending a chemically modified metal–organic framework (MOF) material, UiO‐66, with a conjugated polymer is developed. The MOF porous material is chemically modified with polar nitrogen‐containing functional groups (amino and nitro groups) to create gas molecule adsorption sites. To evaluate the impact of these modifications on the sensing performance, experiments that combined the sensing performance with a density functional theory simulation are conducted. The findings reveal that gas sensors fabricated using an amine‐functionalized MOF blended with conjugated polymers exhibit significantly higher sensitivity than home polymer devices, the sensing performance of the UiO‐66‐NH2/P3HT blend film improved by a factor of two with a sensitivity of ≈2%/ppm and an LOD of 0.001 ppt. Additionally, these devices exhibit exclusive NO2‐sensing performance for other gases such as CO2 and SO2. [ABSTRACT FROM AUTHOR]

To attain a circular carbon economy and resolve CO2 electroreduction technology obstacles, single‐atom catalysts (SACs) have emerged as a logical option for electrocatalysis because of their extraordinary catalytic activity. Among SACs, metal–organic frameworks (MOFs) have been recognized as promising support materials because of their exceptional ability to prevent metal aggregation. This study shows that atomically dispersed Ni single atoms on a precisely engineered MOF nanosheet display a high Faradaic efficiency of approximately 100% for CO formation in H‐cell and three‐compartment microfluidic flow‐cell reactors and an excellent turnover frequency of 23,699 h−1, validating their intrinsic catalytic potential. These results suggest that crystallographic variations affect the abundant vacancy sites on the MOF nanosheets, which are linked to the evaporation of Zn‐containing organic linkers during pyrolysis. Furthermore, using X‐ray absorption spectroscopy and density functional theory calculations, a comprehensive investigation of the unsaturated atomic coordination environments and the underlying mechanism involving CO* preadsorbed sites as initial states was possible and provided valuable insights. [ABSTRACT FROM AUTHOR]

By employing metal oxides as oxygen carriers, chemical looping demonstrates its effectiveness in transferring oxygen between reduction and oxidation environments to partially oxidize fuels into syngas and convert CO2 into CO. Generally, NiFe2O4 oxygen carriers have demonstrated remarkable efficiency in chemical looping CO2 conversion. Nevertheless, the intricate process of atomic migration and evolution within the internal structure of bimetallic oxygen carriers during continuous high‐temperature redox cycling remains unclear. Consequently, the lack of a fundamental understanding of the complex ionic migration and oxygen transfer associated with energy conversion processes hampers the design of high‐performance oxygen carriers. Thus, in this study, we employed in situ characterization techniques and theoretical calculations to investigate the ion migration behavior and structural evolution in the bulk of NiFe2O4 oxygen carriers during H2 reduction and CO2/lab air oxidation cycles. We discovered that during the H2 reduction step, lattice oxygen rapidly migrates to vacancy layers to replenish consumed active oxygen species, while Ni leaches from the material and migrates to the surface. During the CO2 splitting step, Ni migrates toward the core of the bimetallic oxygen carrier, forming Fe–Ni alloys. During the air oxidation step, Fe–Ni migrates outward, creating a hollow structure owing to the Kirkendall effect triggered by the swift transfer of lattice oxygen. The metal atom migration paths depend on the oxygen transfer rates. These discoveries highlight the significance of regulating the release–recovery rate of lattice oxygen to uphold the structures and reactivity of oxygen carriers. This work offers a comprehensive understanding of the oxidation/reduction‐driven atomic interdiffusion behavior of bimetallic oxygen carriers. [ABSTRACT FROM AUTHOR]

Aqueous zinc ion batteries (ZIBs) are currently gaining a significant amount of attention as a low‐cost and high safety energy storage option. While mostly inorganic structures are used as cathode materials in aqueous zinc batteries, these materials undergo structural degradation, therefore, alternative organic cathodes are expected to be developed to replace inorganic materials in aqueous zinc ion batteries (AZIBs). In this work, pillar[5]quinone (P5Q) is used as a cathode in AZIBs for the first time. Besides investigating the charge storage mechanism and interfacial property evolution of P5Q by various ex situ analyses, electrochemical quartz crystal microbalance (EQCM) and density functional theory (DFT) demonstrates both Zn2+ and H+ incorporation. The P5Q exhibits >99 % Coulombic efficiency through 10000 cycles at ultra‐fast (500 °C) current density, yielding a capacity value of approximately 120 mAh g−1 at the end of the cycle. When the current density is changed from 500 °C to 120 °C, an initial discharge capacity of approximately 182 mAh g−1 is achieved, demonstrating outstanding performance with over 80 % capacity retention for the subsequent 7000 cycles. [ABSTRACT FROM AUTHOR]

This research article uses density functional theory (DFT) to study photoinduced borylation. This work examined the electron donor‐acceptor complex (EDA) of bis(catecholato)diboron with different redox‐active leaving groups and bis(pinacol)diboron with aryl N‐hydroxyphthalimide. The results of these DFT studies show the complex ratio of B2cat2 and N, N‐dimethylacetamide (DMA) should be 1 : 2 which is consistent with the experimental results in the literature. We further proposed a reaction mechanism and calculated the energies associated with each step. [ABSTRACT FROM AUTHOR]

The technique of plasma processing is beneficial for wafer cleaning and precision etching of integrated circuits and essential in manufacture of advanced semiconductor devices with unmatched perfection. Research on two‐dimensional (2D) materials, such as transition metal dichalcogenides(TMDs), offers a promising solution to the challenges in semiconductor miniaturization. TMDs, with their atomic layer thicknesses and silicon‐like bandgaps, can be integrated using existing plasma systems. Different 2D crystal structures, such as 1T and 2H configurations, exhibit distinctive properties. Computational approaches are also developed to provide guidelines for controlled synthesis and etching of large‐scale and high‐quality 2D materials. Plasma/gas‐surface interactions during the synthesis, etching, and phase transformation of 2D materials are explored using atomistic simulations such as density functional theory and molecular dynamics. The reaction energetics, chemical species, and associated kinetics are discovered in the simulation study. These results decipher various mechanisms of 2D materials processing at the microscopic scale and predict certain optimal process parameters. Plasma/gas‐based semiconductor technologies are crucial in electronics because they enable production of advanced semiconductors. Plasma/gas etching allows precise and selective removal of material and plasma‐enhanced chemical vapor deposition enhances chemical reactions for efficient film deposition; therefore, these processes are majorly important for harnessing 2D materials in electronic applications. [ABSTRACT FROM AUTHOR]

Prussian blue analogs (PBAs) are potential contestants for aqueous Mg‐ion batteries (AMIBs) on account of their high discharge voltage and three‐dimensional open frameworks. However, the low capacity arising from single reaction site severely restricts PBAs' practical applications in high‐energy‐density AMIBs. Here, an organic acid co‐coordination combined with etching method is reported to fabricate defect‐rich potassium‐free copper hexacyanoferrate with structural water on carbon nanotube fiber (D‐CuHCF@CNTF). Benefiting from the high‐valence‐state reactive sites, arrayed structure and defect effect, the well‐designed D‐CuHCF@CNTF exhibits an extraordinary reversible capacity of 146.6 mAh g−1 with two‐electron reaction, nearly close to its theoretical capacity. It is interesting to unlock the reaction mechanism of the Fe2+/Fe3+ and Cu+/Cu2+ redox couples via x‐ray photoelectron spectroscopy. Furthermore, density functional theory calculations reveal that Fe and Cu in potassium‐free D‐CuHCF participate in charge transfer during the Mg2+ insertion/extraction process. As a proof‐of‐concept demonstration, a rocking‐chair fiber‐shaped AMIBs was constructed via coupling with the NaTi2(PO4)3/CNTF anode, achieving high energy density and impressive mechanical flexibility. This work provides new possibilities to develop potassium‐free PBAs with dual‐active sites as high‐capacity cathodes for wearable AMIBs. [ABSTRACT FROM AUTHOR]

Vanadium nitride (VN) is a potential cathode material with high capacity and high energy density for aqueous zinc batteries (AZIBs). However, the slow kinetics resulting from the strong electrostatic interaction of the electrode materials with zinc ions is a major challenge for fast storage. Here, VN clusters with nitrogen‐vacancy embedded in carbon (C) (Nv‐VN/C‐SS‐2) are prepared for the first time to improve the slow reaction kinetics. The nitrogen vacancies can effectively accelerate the reaction kinetics, reduce the electrochemical polarization, and improve the performance. The density functional theory (DFT) calculations also prove that the rapid adsorption and desorption of zinc ions on Nv‐VN/C‐SS‐2 can release more electrons to the delocalized electron cloud of the material, thus adding more active sites. The Nv‐VN/C‐SS‐2 exhibits a specific capacity and outstanding cycle life. Meanwhile, the quasi‐solid‐state battery exhibits a high capacity of 186.5 mAh g−1, ultra‐high energy density of 278.9 Wh kg−1, and a high power density of 2375.1 W kg−1 at 2.5 A g−1, showing excellent electrochemical performance. This work provides a meaningful reference value for improving the comprehensive electrochemical performance of VN through interface engineering. [ABSTRACT FROM AUTHOR]

Due to ever‐increasing concerns about safety issues in using Li ionic batteries, solid electrolytes have extensively explored. The Li‐rich anti‐perovskite Li3OBr has been considered as a promising solid electrolyte candidate, but it still suffers challenges to achieve a high ionic conductivity owing to the high intrinsic symmetry of the crystal lattice. Herein, we presented a design strategy that introduces various point defects and grain boundaries to break the high lattice symmetry of Li3OBr crystal, and their effect and microscopic mechanism of promoting the migration of Li‐ion were explored theoretically. It has been found that Lii· are the dominant defects responsible for the fast Li‐ion diffusion in bulk Li3OBr and its surface, but they are easily trapped by the grain boundaries, leading to the annihilating of the Frenkel defect pair VLi′+Lii· and thus limits the VLi′ diffusion at the grain boundaries. The VBr· defect near the grain boundaries can effectively drive VLi′ across the grain boundary, thereby converting the carrier of Li+ migration from Lii· in the bulk and surface to VLi′ at the grain boundary, and thus improving the ionic conductivity in the whole Li3OBr crystal. This work provides a comprehensive insight into the Li+ transport and conduction mechanism in the Li3OBr electrolyte. It opens a new way of improving the conductivity for all‐solid‐state Li electrolyte material through the defect design. [ABSTRACT FROM AUTHOR]

Non‐fullerene acceptors (NFAs) have recently emerged as pivotal materials for enhancing the efficiency of organic solar cells (OSCs). To further advance OSC efficiency, precise control over the energy levels of NFAs is imperative, necessitating the development of a robust computational method for accurate energy level predictions. Unfortunately, conventional computational techniques often yield relatively large errors, typically ranging from 0.2 to 0.5 electronvolts (eV), when predicting energy levels. In this study, the authors present a novel method that not only expedites energy level predictions but also significantly improves accuracy , reducing the error margin to 0.06 eV. The method comprises two essential components. The first component involves data cleansing, which systematically eliminates problematic experimental data and thereby minimizes input data errors. The second component introduces a molecular description method based on the electronic properties of the sub‐units comprising NFAs. The approach simplifies the intricacies of molecular computation and demonstrates markedly enhanced prediction performance compared to the conventional density functional theory (DFT) method. Our methodology will expedite research in the field of NFAs, serving as a catalyst for the development of similar computational approaches to address challenges in other areas of material science and molecular research. [ABSTRACT FROM AUTHOR]

In the backdrop of today's environmental priorities, where toxicity and stability hinder lead‐based perovskite solar cell (PSC) progress, the emergence of lead‐free alternatives like Cs2AgBiBr6 perovskites has gained significance. This study revolves around the comprehensive evaluation of Cs2AgBiBr6 as a potential photovoltaic (PV) material, using density functional theory (DFT) calculations with CASTEP. Revealing a vital bandgap of 1.654 eV and emphasizing the contributions of Ag‐4d and Br‐4p orbitals, this analysis also underscores Ag atoms' dominance in charge distribution. Optically, Cs2AgBiBr6 exhibits UV absorption peaks around 15 eV, intensifying with photon energy up to 3.75 eV, hinting at its promise for solar applications. Guided by DFT, forty configurations involving various electron transport layers (ETLs) and hole transport layers (HTLs) are explored. Among these, CNTS emerges as the prime HTL due to ideal absorber alignment. The spotlight architecture, FTO/AZnO/Cs2AgBiBr6/CNTS/Au, boasts exceptional efficiency (23.5%), Voc (1.38 V), Jsc (21.38 mA cm−2), and FF (79.9%). In contrast, FTO/CdZnS/Cs2AgBiBr6/CNTS/Au achieves a slightly lower 23.15% efficiency. Real‐world intricacies are probed, encompassing resistances, temperature, current–voltage (J–V) traits, and quantum efficiency (QE), enhancing practical relevance. These findings are thoughtfully contextualized within prior literature, showcasing the study's contributions to non‐toxic, inorganic perovskite solar technology. This work aspires to positively steer sustainable PV advancement. [ABSTRACT FROM AUTHOR]

A CoMoS composite is synthesized to combine the benefits of cobalt and molybdenum sulfides as an anodic material for advanced lithium‐ion batteries (LIBs). The synthesis is accomplished using a simple two‐step hydrothermal method and the resulting CoMoS nanocomposites are subsequently encapsulated in a carbonized polydopamine shell. The synthesis procedure exploited the self‐polymerization ability of dopamine to create nitrogen‐doped carbon‐coated cobalt molybdenum sulfide, denoted as CoMoS@NC. Notably, the de‐lithiation capacity of CoMoS and CoMoS@NC is 420 and 709 mAh g⁻1, respectively, even after 100 lithiation/de‐lithiation cycles at a current density of 200 mA g⁻1. Furthermore, excellent capacity retention ability is observed for CoMoS@NC as it withstood 600 consecutive lithiation/de‐lithiation cycles with 94% capacity retention. Moreover, a LIB full‐cell assembly incorporating the CoMoS@NC anode and an NMC‐532 cathode is subjected to comprehensive electrochemical and practical tests to evaluate the performance of the anode. In addition, the density functional theory showcases the increased lithium adsorption for CoMoS@NC, supporting the experimental findings. Hence, the use of dopamine as a nitrogen‐doped carbon shell enhanced the performance of the CoMoS nanocomposites in experimental and theoretical tests, positioning the material as a strong candidate for LIB anode. [ABSTRACT FROM AUTHOR]

Ice accumulation and proliferation adversely affect the activities of various residential, commercial, and polar research stations. Although significant efforts are devoted to preventing ice adhesion to various surfaces by developing various anti‐icing coatings, it is still necessary to enhance overall performance and durability. Herein, a facile approach is proposed for fabricating an icephobic coating on an aluminum 6061 (Al) substrate, by coating a poly(dimethylsiloxane) (PDMS)/ poly(tetrafluoroethylene) (PTFE) composite through a spin‐coating method, followed by sprinkling of SiO2 nanoparticles (NPs). Crosslinker/binder‐free adhesion between PDMS and PTFE is achieved by utilizing secondary‐induced electrostatic dipole‐dipole interactions, these interactions are supported by density functional theory (DFT) calculations as well as structural studies. Moreover, the controlled addition of PTFE powder to PDMS improves the water‐repellency, mechanical strength, and surface roughness of the coating. The self‐formation of the superhydrophobic state of the PDMS/PTFE composite is achieved by sprinkling SiO2 NPs. The sprinkled SiO2 NPs are protected by the PDMS/PTFE composite, which serves as a stress concentrator to achieve low ice adhesion. Furthermore, freezing at low temperatures can be delayed by controlling the heat flow rate, interfacial contact area, and surface texture. This indicates the feasibility of the proposed method for various promising anti‐icing applications. [ABSTRACT FROM AUTHOR]

Amorphous tin oxide (a‐SnOx) is a potential transparent oxide semiconductor candidate for future large‐area electronic applications. The thin‐film transistor (TFT) mobilities reach ≈100 cm2 Vs−1, a mobility higher than other multiple cation‐based oxide semiconductor TFTs. Few optical properties have been reported so far and therefore both the effect of visible light and negative bias illumination stress (NBIS) on a‐SnOx TFT performances, known to dramatically impact oxide semiconductor‐based TFTs, have been investigated. The variation of density of states (DOS) due to NBIS by device simulation is analyzed, and a fourfold increase of the donor‐like states and a decrease in the band edge DOS from 2.3 to 2.0 × 1019 cm−3 eV−1 are showed. The evaluation of the effect of neutral, singly, and doubly ionized oxygen vacancies by density functional theory using 95 atoms reveals not only states in the gap of SnO2, but also variations in the electron density, and modifications in the crystal parameters compared to a structure without an oxygen vacancy. Material and device simulation analysis reveal that the oxygen vacancies have a dramatical impact on the DOS in the gap of SnO2 and can explain the NBIS phenomenon observed in a‐SnOx TFT. [ABSTRACT FROM AUTHOR]

Atomically‐dispersed copper sites coordinated with nitrogen‐doped carbon (Cu–N–C) can provide novel possibilities to enable highly selective and active electrochemical CO2 reduction reactions. However, the construction of optimal local electronic structures for nitrogen‐coordinated Cu sites (Cu–N4) on carbon remains challenging. Here, we synthesized the Cu–N–C catalysts with atomically‐dispersed edge‐hosted Cu–N4 sites (Cu–N4C8) located in a micropore between two graphitic sheets via a facile method to control the concentration of metal precursor. Edge‐hosted Cu–N4C8 catalysts outperformed the previously reported M–N–C catalysts for CO2‐to‐CO conversion, achieving a maximum CO Faradaic efficiency (FECO) of 96%, a CO current density of –8.97 mA cm–2 at –0.8 V versus reversible hydrogen electrode (RHE), and over FECO of 90% from –0.6 to –1.0 V versus RHE. Computational studies revealed that the micropore of the graphitic layer in edge‐hosted Cu–N4C8 sites causes the d‐orbital energy level of the Cu atom to shift upward, which in return decreases the occupancy of antibonding states in the *COOH binding. This research suggests new insights into tailoring the locally coordinated structure of the electrocatalyst at the atomic scale to achieve highly selective electrocatalytic reactions. [ABSTRACT FROM AUTHOR]

In the process of photocatalytic synthesis of ammonia, the kinetics of carrier separation and transport, adsorption of nitrogen, and activation of the NN triple bond are key factors that directly affect the efficiency of converting nitrogen to ammonia. Here, we report a new strategy for anchoring MXene quantum dots (MXene QDs) onto the surface of ZnIn2S4 by forming TiS bonds, which provide a channel for the rapid separation and transport of charge carriers and effectively extend the lifespan of photogenerated carriers. The unique charge distribution caused by the sulfurization of the MXene QDs further enhances the performance of the photocatalysts for the adsorption and activation of nitrogen. The photocatalytic ammonia synthesis efficiency of MXene QDs–ZnIn2S4 can reach up to 360.5 μmol g−1 h−1. Density functional theory calculations, various in situ techniques, and ultrafast spectroscopy are used to characterize the successful construction of TiS bonds and the dynamic nature of excited state charge carriers in MXene QDs–ZnIn2S4, as well as their impact on nitrogen adsorption activation and photocatalytic ammonia synthesis efficiency. This study provides a new example of how to improve nitrogen adsorption and activation in photocatalytic material systems and enhance charge carrier dynamics to achieve efficient photocatalytic nitrogen conversion. [ABSTRACT FROM AUTHOR]

The electrochemical reduction of CO2 into C2+ products represents a promising solution to completing the carbon cycle, thereby fostering a sustainable energy supply. Single‐atom electrocatalysts (SAECs) have garnered significant attention as efficient electrocatalysts for the CO2 reduction reaction. Herein, we carried out a first‐principles study on the mechanism of C−C bond formation on single‐Cu‐atom‐modified covalent triazine frameworks (Cu‐CTFs), which are a promising platform for SAECs. Static density functional calculations indicated that the dimerization of CO, which is the main mechanism for C−C bond formation on bulk Cu metals, was not favorable for Cu‐CTFs because of the lack of adjacent Cu sites for co‐adsorption of CO molecules. Rather than CO dimerization, the reaction between adsorbed *CHO and CO to produce *COCHO has a relatively low reaction energy barrier. Constrained ab initio molecular dynamics analyses revealed that the C−C bond‐forming reaction proceeds via insertion of CO at the *CHO intermediate, which has a modest activation energy of 0.09 eV. Specifically, when CO molecule is constrained to be brought close to *CHO, CO insertion between *CHO and Cu occurs at a C−C distance of 1.8 Å. This insertion reaction is the transition step for this C−C bond formation. [ABSTRACT FROM AUTHOR]

Herein, a remarkable achievement in the synthesis and characterization of an atomically precise copper‐hydride nanocluster, [Cu41(SC6H3F2)15Cl3(P(PhF)3)6(H)25]2− via a mild one‐pot reaction is presented. Through X‐ray crystallography analysis, it is revealed that [Cu41(SC6H3F2)15Cl3(P(PhF)3)6(H)25]2− exhibits a unique shell–core–shell structure. The inner Cu29 kernel is composed of three twisted Cu13 units, connected through Cu4 face sharing. Surrounding the metal core, two Cu6 metal shells, resembling a protective sandwich structure are observed. This arrangement, along with intracluster π···π interactions and intercluster C─H···F─C interactions, contributes to the enhanced stability of [Cu41(SC6H3F2)15Cl3(P(PhF)3)6(H)25]2−. The presence, number, and location of hydrides within the nanocluster are established through a combination of experimental and density functional theory investigations. Notably, the addition of a phosphine ligand triggers a fascinating nanocluster‐to‐nanocluster transformation in [Cu41(SC6H3F2)15Cl3(P(PhF)3)6(H)25]2−, resulting in the generation of two nanoclusters, [Cu14(SC6H3F2)3(PPh3)8H10]+ and [Cu13(SC6H3F2)3(P(PhF)3)7H10]0. Furthermore, it is demonstrated that [Cu41(SC6H3F2)15Cl3(P(PhF)3)6(H)25]2− exhibits catalytic activity in the hydrogenation of nitroarenes. This intriguing nanocluster provides a unique opportunity to explore the assembly of M13 units, similar to other coinage metal nanoclusters, and investigate the nanocluster‐to‐nanocluster transformation in phosphine and thiol ligand co‐protected copper nanoclusters. [ABSTRACT FROM AUTHOR]