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The integrity of the hydrogenated amorphous silicon/crystalline silicon (a‐Si:H/c‐Si) interface is essential for the enhanced performance of a‐Si:H/c‐Si heterojunction‐based devices. However, during annealing processes aimed at passivating silicon dangling bonds, unexpected Si epitaxy and nanotwin formation tend to emerge, even under low‐temperature conditions. Therefore, understanding the influence of such annealing on the a‐Si:H/c‐Si interfacial structure is therefore pivotal for device optimization. In this study, the atomic‐scale structural transformation of the a‐Si:H/c‐Si heterointerface subjected to low‐temperature annealing is delved into. The dynamic evolution of this interface is captured by employing in situ spherical aberration (CS)‐corrected transmission electron microscopy (TEM), molecular dynamics (MD) simulations, and density functional theory (DFT) calculations. The TEM observations indicated that Si epitaxy initiated before Si nanotwin formation, and these nanotwins are inclined to revert to epitaxial structures upon sustained annealing. Through MD and DFT insights, the thermodynamic and kinetic intricacies driving the concerted tri‐layer atomic shift characterizing the Si nanotwin‐to‐epitaxy transition are decoded. The findings shed light on the thermal behavior of a‐Si:H/c‐Si interfaces, offering new perspectives on the thermal management in silicon heterojunction devices. [ABSTRACT FROM AUTHOR]

Owing to kinetic‐sluggish nature of electrocatalytic oxygen transformation processes, it is pivotal to develop durable and efficient bifunctional air electrode catalysts for fabricating high‐performance Zn–air batteries (ZABs). In this work, oxygen vacancy (Ov) induced Mn(III) sites optimization is achieved via nano‐micro structure modulation. Protonated carbon nitride (p‐C3N4) is applied as a structure‐stiffening module to immobilize α‐MnO2 on N/P‐doped active carbon (NPAC) and induce Ov construction. X‐ray adsorption spectra (XAS) disclose the formation of Ov and Mn(III) sites in MCC, the unit coordination structure is well maintained with the aid of a dual‐carbon strategy. Mn(III) sites efficiently catalyze oxygen reduction/evolution reaction (ORR/OER), MCC shows high half‐wave potential (E1/2) of 0.88 V for ORR and low potential at 10 mA cm−2 (Ej = 10) of 1.64 V for OER. According to density functional theory (DFT) simulations analysis, the gorgeous bifunctional activity is owing to that optimized charge distribution facilitates the intermediates transformation. Aqueous ZABs based on MCC manifests high peak power density of 452 mW cm−2 and durable cycling stability of 1640 h. Quasi‐solid‐state ZABs based on MCC also show satisfactory performances (175 mW cm−2, 105 h). This work provides the route to develop efficient and durable electrocatalyst for constructing ZABs with long lifespan and high‐power‐density. [ABSTRACT FROM AUTHOR]

Urea oxidation reaction (UOR) is an ideal alternative to oxygen evolution reaction (OER) for efficient hydrogen production but is immensely plagued by slow kinetics. Herein, a multilayer hole amorphous boron‐nickel catalyst (a‐NiBx) is fabricated through a simple chemical plating method, which displays intriguing catalytic activity toward UOR, demanding a low working potential of 1.4 V to reach 100 mA cm−2. The high performance is credited to the formation of metaborate (BO2−), which can promote the formation of high‐oxidation‐state NiOOH active phase and optimize the adsorption of urea molecules. This can be confirmed by the operando spectroscopy characteristics and density functional theory calculations. Consequently, the assembled electrolyzer utilizing NiBx as bifunctional catalysts exhibited splendid catalytic activity, requiring an evidently lower voltage of 1.66 V to reach a current density of 100 mA cm−2 and 1.57 V when using Pt/C as a cathode catalyst. Moreover, the assembled electrolyzer secured a robust stability of over 200 h, as well as a four times higher hydrogen production rate than traditional water electrolysis. [ABSTRACT FROM AUTHOR]

Transition metal sulfides are emerging as promising anode materials for sodium‐ion batteries (SIBs) due to their high theoretical capacity and low cost, their practical application yet face critical issues of sluggish kinetics and poor cycling stability. In this study, a reliable approach is introduced to overcome these challenges by fabrication of Se0.75‐Fe1‐xS0.25@SC hollow nanospheres thanks to the enriched robust Fe─S─C, C─S, and C─Se bonding, which greatly benefit for enhancing both reaction kinetics and structural stability. Kinetic study combining with in situ characterization reveals that the incorporation of rich‐Se into FeSx induces the formation of cationic Fe and Se vacancies, leading to abundant sites and optimized path for sodium storage. Density functional theory calculations also demonstrate how Se‐rich engineering weakens carbonaceous polar C─S─Fe bonds and accelerates reaction dynamics. The as‐prepared Se0.75‐Fe1‐xS0.25@SC can deliver a high reversible capacity of 515 mAh g−1 at 2 A g−1 over 1250 cycles and achieve superior rate capability with maintaining capacity of 418 mAh g−1 at 10 A g−1. This work pioneers the concept of vacancy‐rich functionalized nanostructures, offering a new pathway for designing advanced electrode materials for energy storage devices. [ABSTRACT FROM AUTHOR]

Chloride–ion batteries (CIBs) offer a compelling alternative to conventional battery systems, particularly in applications demanding cost‐effectiveness and resource sustainability. However, the development of tailored electrode materials remains a critical bottleneck for CIB advancement. In this study, an untapped class of perovskite‐based material, potassium hexachlorostannate (K2SnCl6, denoted as KSC) is synthesized via a facile mechanochemical route for the first time. The prepared KSC is subjected to various characterization techniques to confirm its crystal structure and morphology. Herein, KSC exhibits intriguing electrochemical performance in a non‐aqueous CIB configuration, utilizing a lithium metal counter electrode. Furthermore, ex situ X‐ray diffraction (XRD) and X‐ray photoelectron spectroscopy (XPS) analysis, reveal a conversion reaction mechanism involving chloride ion shuttling and provide insights into structural evolution during cycling. Moreover, the density functional theory (DFT) studies support additional degradation products that can potentially limit the performance of these materials as potential battery electrodes in CIBs. [ABSTRACT FROM AUTHOR]

Electrocatalytic nitrate reduction reaction (NO3RR) can convert nitrate contaminants into ammonia with higher added value. However, due to the NO3RR involving complex multi‐electron reactions, there is an urgent need to develop efficient electrocatalysts. Herein, CoCu Janus nanoparticles loaded on Ti3C2Tx MXene (CoCu‐Ti3C2Tx) is synthesized via the combination of molten salt etching and galvanic replacement strategy. The tandem catalysis of CoCu Janus NPs can maintain the balance between nitrogenous intermediates and active hydrogen (Hads). CoCu‐Ti3C2Tx exhibits a high NH3 yield of 8.08 mg h−1 mgcat.−1 and a satisfactory Faradaic efficiency of 93.6% at −0.7 V versus reversible hydrogen electrode (RHE). The Zn‐NO3− battery assembled with CoCu‐Ti3C2Tx shows an excellent power density of 10.33 mW cm−2, an NH3 yield of 1.52 mg h−1 mgcat.−1 and a Faradaic efficiency of 95.3% at 10 mA cm−2, which enables the simultaneous elimination of nitrate pollutants, ammonia production, and energy supply. Moreover, a series of verification experiments and density functional theory calculation are combined to reveal the reaction path and tandem catalytic mechanism. This work not only provides a new inspiration for the design of tandem catalysts but also promotes the development of Zn‐nitrate battery. [ABSTRACT FROM AUTHOR]

In order to address imminent energy and environmental challenges, photocatalytic water splitting emerges as a promising way for harnessing solar radiation to generate clean chemical energy. 2D arsenene (β‐As) has notable catalytic activity in hydrogen production. Based on first principles calculations and non‐adiabatic molecular dynamics (NAMD) simulations, the β‐As/Ti2CO2 heterojunction is predicted to be a promising Z‐scheme photocatalyst for overall solar water splitting. It has a desirable energy band structure with the valence band maximum of Ti2CO2 and the conduction band minimum of β‐As well below and above the redox potentials of H2O. Both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) can proceed spontaneously under light irradiation. NAMD simulations confirm that it is a Z‐scheme photocatalyst with fast electron–hole combination dynamics. Instead of by intrinsic electric field, such a fast electron–hole combination is driven by a large nonadiabatic coupling. The heterojunction exhibits strong optical absorption in the visible and ultraviolet regions. The estimated solar‐to‐hydrogen (STH) efficiency limit of β‐As/Ti2CO2 reaches 32%, which is the highest among all β‐As based junctions reported in the literature. These results suggest that β‐As/Ti2CO2 is a promising photocatalyst for achieving overall water splitting. [ABSTRACT FROM AUTHOR]

Many ligands commonly used to prepare nanoparticle catalysts with precise nanoscale features contain nitrogen (e.g., oleylamine); here, it is found that the use of nitrogen‐containing ligands during the synthesis of metal oxide nanoparticle catalysts substantially impacts product analysis during photocatalytic studies. These experimental results are confirmed via hybrid Density Functional Theory (DFT) computations of the materials’ electronic properties to evaluate their viability as photocatalysts for nitrogen reduction. This nitrogen ligand contamination, and subsequent interference in photocatalytic studies is avoidable through the careful design of synthetic pathways that exclude nitrogen‐containing constituents. This result highlights the urgent need for careful evaluation of catalyst synthesis protocols, as contamination by nitrogen‐containing ligands may go unnoticed since the presence of nitrogen is often not detected or probed. [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]

Given the pronounced dissolution of electrocatalysts in acidic environments, the quest for effective oxygen evolution reaction (OER) electrocatalysts suitable for proton exchange membrane (PEM) water electrolyzers persists as a formidable challenge. In this investigation, catalysts are synthesized by creating oxygen vacancies within various metal oxides (Nb2O5‐x, Ta2O5‐x, ZrO2‐x, TiO2‐x) through plasma‐assisted method, thereby facilitating the immobilization of IrO2 onto these defect‐rich surfaces. The findings unveil that IrO2/Nb2O5‐x manifests reduced overpotentials during acidic OER, achieving an overpotential down to 225 mV@10 mA cm−2, coupled with outstanding durability at multicurrent densities exceeding 200 h, attributed to strong oxide‐support interaction (SOSI) between the IrO2 catalyst and Nb2O5‐x substrate. Density functional theory (DFT) computations uncover intensified binding affinities between IrO2 and Nb2O5‐x, thus modulating the central energy levels of Ir's d orbitals toward favorable OER conditions, consequently bolstering the electrocatalytic activity and stability of the composite catalyst. Furthermore, employing IrO2/Nb2O5‐x as a PEM electrolyzer anode enables consistent operation at 1000 mA cm−2 for 200 h, with an Ir content of only 0.2852 mg cm−2 and an energy consumption of 4.34 kWh Nm−3 H2. This achievement substantially lowers the cost of hydrogen production to US$ 0.96 per kilogram, underscoring its potential for practical applications. [ABSTRACT FROM AUTHOR]

The manifestation of mechanical phenomena in quantum materials at the macroscopic level is intricately linked to pronounced electron‐electron interactions within their lattices, a relationship that becomes especially evident in low‐dimensional materials. Violet phosphorous (VP), a nascent 2D material distinguished by its unique vertically aligned tubular structures, has garnered considerable attention owing to its layer‐dependent electronic bandgap, exceptional carrier mobility, and robust air stability. Herein, a comprehensive exploration of the phonon modes exhibited by few‐layer VP through an integrated experimental‐theoretical approach, focusing on the modulation of their Raman response under the uniaxial strain along a‐axis, b‐axis, and tube direction, respectively, is undertaken. Density functional theory calculations highlight when strain is applied along the a‐ or b‐axis direction, the strain is predominantly mitigated through tube rotational adaptations instead of the change of bond length and bond angle, culminating in a pronounced anisotropic Raman response. Moreover, the strain engineering can effectively optimize the photoelectric response performance of VP, including increase the responsivity ≈2500% and elevate the anisotropic ratio from 2.26 to 3.38. This investigation not only confirms the superior stretchability and impact resistance properties of cross‐structured VP but also establishes the groundwork for exploring the strain‐induced anisotropic optoelectric properties to VP. [ABSTRACT FROM AUTHOR]

Porous organic polymers (POPs) as electrode materials for sodium‐ion batteries (SIBs) are attracting increasing attention. However, the application of porous organic radical polymers (PORPs) with unique properties in SIBs is still in an infancy. Herein, two 3D germanium‐based POPs with conjugated diacetylene units (Ge‐DA) and acetylene units (Ge‐A) are designed and synthesized. Carbon radicals in Ge‐DA are verified by electron paramagnetic resonance and the resonance structure is calculated by density functional theory, showing a lower lowest unoccupied molecular orbital (LUMO) energy level (−5.46 eV) and a narrow energy gap (ca. 1.64 eV). In contrast, Ge‐DA as an anode for SIBs shows superior electrochemical properties to that of Ge‐A counterpart, including a higher specific discharge capacity of 349 mAh g−1 at 200 mA g−1, excellent cyclability with a capacity of 112 mAh g−1 at 5 A g−1 for at least 5000 cycles and high rate performance of 135 mAh g−1 at 20 A g−1, proving that the different electronic structures of the diacetylene and monoacetylene units affect the properties of materials. [ABSTRACT FROM AUTHOR]

Halide perovskites emerge as promising candidates for thermoelectrics due to their ultralow thermal conductivity. The conventional theory based on the phonon gas model, which treats thermal transport as particle‐like behavior, shows limitations to describe the unusual thermal transport property in some halide perovskites with strong anharmonicity. Here, the significance of phonon coherence effect on thermal transport of bismuth‐halide perovskite Cs3Bi2Br9 is reported by inelastic neutron scattering and simulations including density functional theory and machine‐learning potential based molecular dynamics. This study shows that the restrictive low‐energy acoustic phonons lead to the limited particle‐like thermal conductivity, which seriously underestimates the lattice thermal conductivity of Cs3Bi2Br9. The significant contribution of wave‐like optical phonon modes, driven by the coherence effect, accounts for an additional ≈50% wave‐like thermal conductivity. Besides, the experimental weak temperature dependence of thermal conductivity along z direction (κ ≈T−0.35) is well reproduced by calculation (κ ≈T−0.37) when including phonon coherence. This work highlights the critical role of phonon coherence in Cs3Bi2Br9 and enhances understanding on the unusual thermal transport properties in halide perovskites and other related materials with strong anharmonicity. [ABSTRACT FROM AUTHOR]

Photocatalytic conversion of CO2 to methane faces challenges due to the stability of CO2, unpredictable intermediates, and complex electron transfer steps. Herein, a spatial In2S3/In2O3 heterojunction with abundant S vacancies (ISIO(VS)) is obtained through facile Polyvinylpyrrolidone (PVP) treatment to reach a methane yield of 16.52 µmol·g−1·h−1 with a selectivity of 95.93%, which is the highest among reported In2S3 and In2O3 based catalysts. The work function (Wf), differential charge density, and Kelvin Probe Force Microscopy (KPFM) results confirm that S vacancies strengthen the built‐in electric field (BEF) of In2S3/In2O3 (ISIO) heterojunctions, improving carrier separation. Density functional theory (DFT) calculations reveal that S vacancies induce electron redistribution, facilitating adsorption and activation of CO2 and *CO intermediate, thus promoting hydrogenation to yield *CHO. The reaction pathway of photocatalytic CO2 reduction is revealed by in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and Gibbs free energy (ΔG). The S vacancies modify electronic orbitals and the highest occupied molecular orbital (HOMO) of In atom, resulting in a stronger interaction between the catalyst and *CHO, which reduces ΔG*CHO and regulates the selectivity of CH4. This study paves a new avenue for the design of photocatalysts with highly selective reduction of CO2 to CH4 through defect engineering. [ABSTRACT FROM AUTHOR]

Progress is made in the advancement of efficient and durable electrocatalysts for the ethylene glycol oxidation reaction (EGOR), which is a critical breakthrough in the conversion of waste plastic into high‐value‐added chemicals. Here, an organic ligand‐modified PdNi bimetallenes (PdNi O‐BMs) catalyst is designed and constructed through the one‐pot method. Benefiting from the frizzy and porous surface structure and inorganic–organic hybrid interface modification, PdNi O‐BMs undergo electrocatalytic reforming of ethylene glycol (EG) derived from polyethylene terephthalate (PET) to form formic acid. The unique structural advantages result in high EGOR performance. Meanwhile, the influence of Ni and organic ligand on the catalyst performance is confirmed through density functional theory calculations. This study reveals an advanced strategy for the synthesis of inorganic–organic hybrid bimetallenes, providing a green and sustainable new approach for PET value‐added transformation. [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]

Tuning the lattice strain of catalysts represents a powerful strategy to alter their electronic structures and ultimately regulate catalytic performance. Electrocatalytic CO2 reduction is a promising avenue to accomplish the carbon‐neutral cycle, however, there still lacks a distinct and systematic understanding of the lattice strain effect in CO2 electrochemical conversion. In this work, the influence of lattice strain on Bi (012) facets to formate production is studied. The pre‐executed density functional theory (DFT) calculations reveal that lattice compression promotes the wrinkling of exposed Bi surface and increases the total density of state (DOS) of active sites at the Fermi level. As the gradual intensification of lattice contraction, the selectivity of CO2 reduction exhibits a volcanic alteration, with an optimal lattice contraction of 3%. Experimentally synthesized Bi2O2CO3/Bi heterogeneous catalyst confirms the effect of lattice compression. When compression reaches −3.04% on Bi (012) facets, the catalyst possesses the highest Faraday efficiency (FE) of 96.17% at −1.2 VRHE and an industrially scalable current density of −600 mA cm−2. Additionally, in seawater‐based electrolysis, the catalyst also exhibits excellent remarkable FE of 95.43% of formate production. [ABSTRACT FROM AUTHOR]

Sustaining the steady state for highly active non‐stoichiometric iridium (Ir)‐based oxide (IrOx) at low Ir loading remains challenging primarily due to the continuous oxidation and sequent dissolution of Ir active sites during the oxygen evolution reaction (OER). In this context, a new iridium–cerium (Ce) substitution solid solution oxide (SSO) has been developed, featuring uniformly dispersed Ir atoms within Ce dioxide (CeO2) matrix as electron buffer, which delivers remarkable acidic OER catalytic activity and enhanced stability. The electron‐buffering capacity of CeO2 facilitates the charge transfer toward Ir atoms, leading to abundant active low‐valence Ir sites and effectively prevent their oxidation and dissolution. As a result, Ir─Ce SSO demonstrates an overpotential of merely 238 mV@10 mA cm−2. Proton exchange membrane water electrolyzer employing Ir─Ce SSO at a low Ir loading of 396 µgIr cm−2 operates consistently for over 100 h@500 mA cm−2. Density functional theory (DFT) calculations corroborate that the electron‐buffering effect of CeO2 enriches the density of IrIII and substantially increases the dissolution energy barrier of Ir atoms. This study presents a viable approach to addressing the issues of instability and low efficiency in Ir‐based OER electrocatalysts for acidic water electrolysis. [ABSTRACT FROM AUTHOR]

Electrochemical nitrogen reduction reaction (NRR) for ammonia synthesis has attracted great interest in recent years, which presents a carbon‐free alternative to the energy‐intensive Haber–Bosch process. Besides, NRR also provides a promising coverage route of renewable energy since NH3 is considered the second generation of hydrogen energy while possessing established technologies of liquefaction, storage, and transport. However, there are long‐term challenges in catalyst design for NRR due to its low intrinsic activity and unsatisfied selectivity. Fortunately, by conducting extensive explorations in this field, much progress is achieved in boosting the NRR performance. Herein, from a view of the atomic/electronic level, three promotion effects are summarized for NRR (i.e., electron effect, geometry effect, and ligand effect), which tackle the challenges of activity and selectivity. Representative studies with taking fully advantages of the promotion effects are reviewed, which realized remarkable NRR performance. Finally, the future research directions and prospects are discussed. It is highly expected that this review will enable the advancement of NRR catalysts and promote the further development of electrochemical NRR. [ABSTRACT FROM AUTHOR]

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]

Developing highly effective transition metal‐based bifunctional electrocatalysts remains a tremendously challenging task for large‐scale overall water splitting. Herein, a multiheterostructured Mo‐doped Ni2P/FexP electrocatalyst on NiFe foam with P vacancy (denoted as Mo─Ni2P/FexP‐V/NFF) is developed to serve as an efficient dual‐pH electrocatalyst. Due to the synergistic effect of multiple strategies (heteroatom doping, heterointerface, and P vacancy), the Mo─Ni2P/FexP‐V/NFF possesses remarkable hydrogen evolution reaction (HER) catalytic activity in alkaline/acidic and excellent oxygen evolution reaction (OER) in alkaline media, along with encouraging durability. The mechanisms of improved electrocatalytic activity combining multicharacterizations and density functional theory (DFT) calculations are elucidated. Specifically, X‐ray absorption fine structure experimental analysis confirms that the Mo doping can optimize the electronic structure of electrocatalyst. In situ Raman spectroscopy demonstrates that the evolved oxyhydroxides are the real active substances for the OER. DFT calculations reveal that the conductivity of as‐prepared samples can be enhanced through multiple strategy synergy. Moreover, in the HER process, multiple strategies can not only reduce the hydrogen binding energy to near zero but also enhance the H2O dissociation and *OH desorption. In the OER process, DFT calculations also verify that Mo doping and interface engineering can optimize the adsorption of the rate‐determining step, achieving the lowest theoretical overpotential. [ABSTRACT FROM AUTHOR]

Metal oxides with spinel structure have garnered increasing attention as promising alternatives to noble metal‐based electrocatalysts. However, these electrocatalysts often fail to simultaneously exhibit high activity and stability for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), limiting their applications in electrocatalytic water splitting. Herein, crystalline/amorphous heterogeneous interfaces are successfully introduced into spinel NiCo2O4 nanosheets, which are grown in situ on carbon cloth (CC), denoted as NiCo2O4‐B‐CC. The amorphous/crystalline heterostructures combine the advantages of both phases in electrocatalysts. The amorphous phase of the spinel NiCo2O4 nanosheets modulates the electron density, provides abundant oxygen single vacancies as active sites, and enhances the corrosion resistance, while the crystalline phase improves conductivity. Density functional theory (DFT) calculations are performed to investigate the influence of surface oxygen single vacancy (SVO) on the activity of the OER and HER processes. The NiCo₂O₄‐B‐CC exhibits overpotentials of only 26 mV for HER and 215 mV for OER at a current density of 10 mA cm−2. It exhibits excellent electrocatalytic performance for water splitting, achieving a current density of 400 mA cm−2 at an applied voltage of 2.0 V. The construction of crystalline/amorphous heterogeneous interfaces in electrocatalysts provides novel approach for enhancing the electrocatalytic performance of metal oxides in water splitting. [ABSTRACT FROM AUTHOR]

A comprehensive understanding of atomic fracture mechanisms in 2D materials is essential for their practical applications, yet this knowledge is currently limited. To address this gap, an aberration‐corrected scanning transmission electron microscope (STEM) to induce new cracks in suspended monolayer transition metal dichalcogenides (TMDs) using broad electron beam illumination, is employed. During characterization, a low‐dose electron beam to avoid irradiation damage, allowing to observe the atomic fracture behavior in these materials, is utilized. The STEM experiments reveal a novel atomic fracture pattern along the zigzag direction, resulting in a distribution where half of the chalcogen atoms (S or Se) adhered to the molybdenum‐terminated (Mo‐T) edge and the other half to the chalcogen‐terminated (S‐T or Se‐T) edge. Density functional theory (DFT) calculations suggest that this fracture mode produces a pair of edges with the lowest formation energy. Additionally, molecular dynamics (MD) simulations support the observed fracture behavior under a mixed mechanical loading mode of “I+III” with both in‐plane and out‐of‐plane stress, originating from the ultrathin nature and nonplanar deformation in suspended 2D materials. This research offers new insights for the development of 2D fracture mechanics and is pivotal for designing devices incorporating 2D materials. [ABSTRACT FROM AUTHOR]

Interfacial defects between perovskite and adjacent charge transport layers present a significant obstacle, hindering the enhancement of power conversion efficiency (PCE) and stability in perovskite solar cells (PSCs). To address this challenge, a dual‐interface modification is proposed to aim at improving the performance of mixed‐halide PSCs. Specifically, the hole‐collecting side is modified with 5‐Aminopyridine‐2‐carboxylic Acid (APC), while the electron‐collecting side is modified with 2‐thiopheneethylammonium chloride (TEACl). The multifunctional APC enhances charge transfer by tailoring the interface between the perovskite and poly(triarylamine) (PTAA) through multiple bonding interactions, thereby suppressing interfacial nonradiative recombination. Density functional theory studies reveal that APC on the perovskite surface induces uniform adsorption energy, promoting homogenous crystallization without residual stress. Additionally, APC interlayer eliminates the localized edge states induced by the iodine vacancies near the conduction band edge. Further improvement in the device performance is achieved by passivating the top perovskite surface with TEACl, leading to well‐matched energy bands and reduced vacancy trap states. As a result, champion cell achieves a PCE of 24.87% with an open‐circuit voltage of 1.188 V. Furthermore, The dual‐interface modification improves thermal stability due to enhanced ion‐migration activation energy. [ABSTRACT FROM AUTHOR]

Transition metal‐nitrogen‐carbon single‐atom catalysts (M─N─C SACs) exhibit outstanding catalytic activity for the oxygen reduction reaction (ORR). However, these catalysts still face the dual challenges of low density and low utilization of active sites in practical applications. Hence, a simultaneous modulation strategy to construct high‐density and accessible Co‐N4 sites on nitrogen‐doped porous carbon (CoH SA/NC), is reported. As expected, the optimized CoH SA/NC catalyst exhibits superior ORR activity with a half‐wave potential value of 0.874 V, outperforming that of the benchmark Pt/C catalyst. Importantly, the mass activity and turnover frequency of CoH SA/NC are 14.7 and 13.3 times higher than that of low‐density Co single atom catalyst (CoL SA/NC), respectively. Structural characterization and density functional theory (DFT) reveal that the porous structure and the high dense Co‐N4 sites synergistically improve the ORR performance, in which the high dense Co‐N4 sites induced a redistribution of the d orbital, resulting in dz2 orbital has enough electron to interact with the OOH* specie, thereby facilitating the kinetic process of ORR. Moreover, CoH SA/NC‐based Zn–Air Battery (ZAB) also showed excellent device performance, including a high‐power density (191.7 mW cm−2), high specific capacity, and outstanding stability (250 h), significantly superior to benchmark Pt/C‐based ZABs. [ABSTRACT FROM AUTHOR]

Fine control over the graphitization level of carbonized nanostructures can play a strategic role in tuning the crystallization of supported nanocatalysts, thereby modulating the kinetics of catalysis. However, realizing the synergistic interplay of graphitization‐tunable support and supported catalysts poses a significant challenge. This study proposes a current pulse‐induced ultrafast strategy for developing MOF‐derived graphitic nano‐leaves (GNL) and supported ultrafine ruthenium nanoclusters exhibiting selective crystallization states depending on the tunable graphitization level of GNL. The resulting ultrafine (≈0.7 nm) amorphous‐ruthenium nanoclusters linked with GNL (a‐Ru@GNL500) exhibit state‐of‐the‐art performance in the hydrogen evolution reaction (HER), requiring very low overpotentials of only 23.0 and 285.0 mV to achieve current densities of 10 and 500 mA cm−2, respectively. Furthermore, a‐Ru@GNL500 demonstrates exceptional operational stability for 100 h under high HER currents of 200 and 400 mA cm−2. Density functional theory reveals that the unique electronic structure of a‐Ru and the cooperative effect of cobalt embedded in the graphitic layer lower the occupancy of the antibonding orbital, resulting in an accelerated HER process. Additionally, the unique electronic structure, highly conducting GNL, and efficient bubble release dynamics of super‐aerophobic a‐Ru@GNL500 contribute to reduced overpotentials, particularly at high HER current densities. [ABSTRACT FROM AUTHOR]

Research on high‐efficiency and cost‐efficient catalysts for oxygen reduction reaction (ORR) is still a vital but challenging issue for commercializing metal–air batteries. Herein, a single‐molecule/atom hybrid catalyst is developed to boost the ORR, in which iron phthalocyanine molecules containing molecular Fe─N4 moieties couple with atomic Co─N4 sites on the surface of polyhedral carbon. Density functional theory calculations reveal that face‐to‐face laminated construction of Fe─N4 and Co─N4 in the hybrid catalyst can effectively modulate the electronic structure of active iron atoms and reduce the energy barrier of the rate‐determining step for ORR. As a result, this hybrid catalyst demonstrates excellent ORR performance, featuring a half‐wave potential of 0.904 V, a peak power density of 238.3 mW cm−2 for zinc–air battery, and outstanding electrocatalytic stability. This work offers a distinctive and robust molecular/atomic engineering approach to creating efficient electrocatalysts, advancing the fields of metal–air batteries. [ABSTRACT FROM AUTHOR]

Highly active Pt‐based intermetallic nanoparticles (i‐NPs) loaded on stable supports have garnered considerable interest as promising oxygen reduction reaction (ORR) catalysts for proton‐exchange‐membrane fuel cells (PEMFCs). Herein, thermostable tellurium (Te) is vapor‐deposited onto commercial conductive carbon to anchor high‐temperature‐synthesized Pt3Co i‐NPs. Advanced characterization and density functional theory (DFT) calculations demonstrate that the binding energy of Pt 4f and Co 2p shift positively by 0.12 and 0.95 eV after the introduction of Te in carbon support, promoting the formation of Pt─Te bonds, which enhances the metal–support interactions (MSIs) in Pt3Co/Te‐C (with a more negative binding energy of −10.28 eV). The average size of well‐dispersed Pt3Co i‐NPs (≈3.9 nm) on Te─C is considerably smaller than that of Pt3Co i‐NPs (≈9.1 nm) on commercial carbon. The specific activity of Pt3Co/Te‐C decreases by only 1.5% after 100,000 ultra‐long voltage‐accelerated cycles, while the morphology remains almost unchanged. The membrane electrode assembly using Pt3Co/Te‐C as a cathode demonstrates impressive activity (power density of 2.32 W cm−2@4 A cm−2 and mass activity of 0.50 A mgPt−1@0.9 V) and robust durability (mass activity@0.9 V loss of 26% after 30,000 cycles with intact L12 ordered structure) in H2–O2 operation, significantly exceeding the DOE 2025 requirements. [ABSTRACT FROM AUTHOR]

Garnet electrolyte Li6.5La3Zr1.5Ta0.5O12 (LLZTO) has been identified as a promising candidate for solid‐state batteries (SSBs). However, the implementation of garnet‐based SSBs is severely restricted owing to the Li dendrite originating from the uneven Li+ deposition and the electron leakage. Herein, one high‐performance garnet‐based SSB is proposed through the enhancement of interfacial dynamics and the inhibition of electron penetration, induced by an artificial harmonized interphase (LSF). The formation of a tightly bonded LLZTO|Li interface is facilitated by the Li3Sb with lower interfacial energies against LLZTO and Li, elucidated by the density functional theory (DFT) calculations. Furthermore, electron leakage and dendrite infiltration are effectively suppressed by the LiF with the electron‐insulating nature and an exceptional γE value. Therefore, a low interfacial resistance of 4.8 Ω cm2 is successfully achieved by the utilization of the functional LSF interphase layer, and the Li|LLZTO‐LSF|Li symmetric cell displayed prolonged Li plating/stripping stability over 1200 h at 0.3 mA cm−2. Moreover, the LFP|LLZTO‐LSF|Li full cell also exhibited notable cycling performance (93.1% capacity retention after 200 cycles at 1 C). The utilization of a synergistic interlayer has been identified as an effective strategy for the advancement of garnet‐based solid‐state lithium batteries. [ABSTRACT FROM AUTHOR]

Ammonia, as a high‐energy‐density carrier for hydrogen storage, is in great demand worldwide. Electrocatalytic nitrate reduction reaction (NO3RR) provides a green NH3 production process. However, the complex reaction pathways for NO3RR to NH3 and the difficulty in controlling intermediate products limit the reduction process. Herein, by incorporating atomic‐level bismuth (Bi) into CuCo2O4 hollow carbon nanofibers, the catalytic activity of the electrocatalyst for NO3RR is enhanced. The maximum Faradaic efficiency of Bi1‐CuCo2O4 is 95.53%, with an NH3 yield of 448.74 µmol h−1 cm−2 at −0.8 V versus RHE. Density Functional Theory calculations show that the presence of Bi lowers the reaction barrier for the hydrogenation step from *NO2 to *NO2H, while promoting mass transfer on the release of *NH3 and the reactivation of surface‐active sites. Differential charge density calculations also show that after Bi doping, the charge supplied by the catalyst to NO3− increases from 0.62 to 0.72 e‐, thus reasoned for enhanced NO3RR activity. The established nitrate‐Zn battery shows an energy density of 2.81 mW cm−2, thus implying the potential application. [ABSTRACT FROM AUTHOR]

Lithium–sulfur (Li–S) batteries, as one of the most promising “post‐Li‐ion” energy storage devices, encounter several intrinsic challenges: polysulfide dissolution and shuttle effect, poor sulfur utilization, lithiation‐induced sulfur expansion, and lithium dendritic growth. These challenges must be resolved, and the associated mechanisms must be completely understood before the practical applications of Li–S batteries. Despite significant progress in enhancing battery capacities, experimental studies on the working mechanisms of Li–S batteries remain challenging. Alternatively, computational methods are proven useful for understanding Li–S electrochemistry and designing high‐performance Li–S batteries. This review presents recent advances in computational methods (density functional theory, molecular dynamics simulations, and finite element analysis) for Li–S batteries, compares their advantages, and summarizes their favorable applications in addressing the challenges of Li–S batteries. Computational methods should find more applications in the development of Li–S batteries. [ABSTRACT FROM AUTHOR]

Sodium metal is regarded as an optimal anode material for high‐energy‐density sodium‐ion batteries (SIBs). However, during the processes of sodium deposition and stripping, the failure of the solid electrolyte interphase (SEI) film leads to the continuous accumulation of inactive sodium, thereby compromising the cycling reversibility of the battery. Here, a novel metal fluoride heterointerface layer is generated and constructed through in situ manipulation of the continuous reaction between TiF4 and metal Na. The reconstructed NaF/TiF3 interface layer, which tightly anchors the sodium metal, effectively suppresses the formation of sodium dendrites during the charge‐discharge process. The highly sodium‐philic TiF3 component exhibits strong binding with Na ions, while NaF reduces the Na+ diffusion energy barrier, significantly enhancing the reaction kinetics. Due to the successful artificial construction of this interface layer, the Na/TiF4 composite electrode demonstrates an exceptional ultra‐long cycling stability of 2370 h in symmetric cells (0.5 mAh cm−2). Density functional theory (DFT) calculations further validate the functionality of each component in the Na/TiF4 protective layer. When paired with NaNi1/3Fe1/3Mn1/3O2 cathode in a pouch cell, it exhibits stability up to 2000 cycles at current densities of 2 C and 4 C, with a maximum energy density output of 483.1 Wh kg−1 (power density: 320.8 W kg−1). [ABSTRACT FROM AUTHOR]

The sluggish kinetics of alkaline hydrogen evolution reaction (HER) hinders practical exploitation of water splitting. Catalysts, known as platinum single atoms (Pt‐SAs) anchored in Ni4Mo/Ni alloys on nickel foam (Pt SAs‐Ni4Mo/Ni@NF) with ultralow Pt mass loading (mPt = 0.3 wt.%) derived from self‐reconstruction, with boosted atomic utilization in alkaline HER are demonstrated. In situ characterizations confirm the leaching of Mo species during the self‐reconstruction of NiMoO4, which facilitates the anchoring of Pt‐SAs through the generation of atomic defects. Further, density functional theory (DFT) calculations indicate that the atomic defects can effectively capture Pt2+ in salt solution, aiding in the distribution of Pt‐SAs. Besides, theoretical results emphasize that Pt SAs‐Ni4Mo/Ni with unique Pt‐Ni interaction can accelerate the desorption of hydroxides in alkaline electrolytes during HER, as well as lower energy barriers for reaction steps. Pt SAs‐Ni4Mo/Ni@NF shows remarkable catalytic activity toward alkaline HER with a low overpotential of 17 mV (j = 10 mA cm−2), together with high atomic utilization of Pt (8.92 A mgPt−1 at 30 mV) and excellent durability. This work not only provides a scalable preparation for efficient and robust low‐Pt catalysts but also establishes in‐depth understanding of the synergistic interaction between Pt SAs and Ni‐Mo alloys in alkaline HER, which is likely to accelerate the development of water‐splitting technique. [ABSTRACT FROM AUTHOR]

Nano‐single‐atom‐catalysts have the potential to combine the respective advantages of both nano‐catalysts and single‐atom‐catalysts and thus exhibit enhanced performance. Generally, the separation of active sites in space limits the interaction between single atoms and nanoparticles. Heterointerface engineering has the potential to break this limitation. Regretfully, studies on the interface effect between single atoms and nanoparticles are rarely reported. Herein, an unprecedented nano‐single‐atom heterointerface composed of Fe single‐atoms and carbon‐shell‐coated FeP nanoparticles (Fe SAC/FeP@C) is demonstrated as an efficient electrocatalyst for the nitrate reduction process from alkaline to acidic. Compared with typical nano‐single‐atom‐catalysts (Fe SAC/FePO4) and single‐atom‐catalysts (Fe SAC), the constructed Fe SAC/FeP@C heterostructure exhibits dramatically enhanced nitrate‐to‐ammonia performance. Especially in acidic media, the maxmium Faradaic efficiency of ammonia (NH3) can reach 95.6 ± 0.5%, with a maximum NH3 yield of 36.2 ± 3.1 mg h−1 mgcat−1 (pH = 1.2), which is considerably higher than previously reported. Density functional theory calculations and in situ spectroscopic investigations indicate that the unique charge redistribution at the interface, together with the optimized electronic structure of Fe single‐atoms, strengthens intermediate adsorption and catalytic activity. This work provides a feasible strategy for designing nano‐single‐atom‐catalysts with unique heterointerfaces, as well as valuable insights into nitrate conversion under environmentally relevant wastewater conditions. [ABSTRACT FROM AUTHOR]

Atomically thin, mechanically flexible, memory‐functional, and power‐generating crystals play a crucial role in the technological advancement of portable devices. However, the adoption of these crystals in such technologies is sometimes impeded by expensive and laborious synthesis methods, as well as the need for large‐scale, mechanically stable, and air‐stable materials. Here, an instant‐in‐air liquid metal printing process utilizing liquid bismuth (Bi) is presented, forming naturally occurring, air‐stable, atomically thin, mechanically flexible nanogenerators and ferroelectric oxides. Despite the centrosymmetric nature of the monoclinic P21/c system of achieved α‐Bi2O3‐δ the high kinetics of liquid metal synthesis leads to the formation of vacancies that disrupt the symmetry which is confirmed by density functional theory (DFT) calculations. The polarization switching is measured and utilized for ferroelectric nanopatterning. The exceptional attributes of these atomically thin multifunctional stable oxides, including piezoelectricity, mechanical flexibility, and polarizability, present significant opportunities for developing nano‐components that can be seamlessly integrated into a wide range of devices. [ABSTRACT FROM AUTHOR]

Tumor microenvironment (TME)‐responsive nanozymes‐based catalytic therapy shows great potential in combating malignant tumor. However, their biological application still suffers from deficient catalytic activity. Herein, the MoOx‐Rh metallene nanozyme demonstrates highly efficient multiple enzymatic catalytic activities, where MoOx species atomically dispersed on Rh metallene surface. The resulting structures enable MoOx‐Rh metallene with maximally exposed active oxide‐metallene interface and more atoms sites around interface can be well finely regulated. Results of experiment and density functional theory (DFT) simulations support the notion that atomic interface structure facilitates multiple enzyme‐like reactions. As a TME‐responsive nanozyme, MoOx‐Rh metallene exhibits remarkable therapeutic effect of tumor due to intrinsic near‐infrared photothermal effect and laser‐enhanced multiple enzymatic catalytic activities. This study illustrates the great promise of atomic interface engineering strategy in tumor catalytic therapy. [ABSTRACT FROM AUTHOR]

In this work, the potential of 2D semi‐metallic PtSe2 as source/drain (S/D) contacts for 2D material field‐effect‐transistors (FETs) through theoretical and experimental investigations, is explored. From the density functional theory (DFT) calculations, semi‐metallic PtSe2 can inject electrons and holes into MoS2 and WSe2, respectively, indicating the feasibility of PtSe2 contacts for both n‐ and p‐metal‐oxide‐semiconductor FETs (n‐/p‐MOSFETs). Indeed, experimentally fabricated flake‐level MoS2 n‐MOSFETs and WSe2 p‐MOSFETs exhibit a significant reduction in contact resistance with semi‐metallic PtSe2 contacts compared to conventional Ti/Au contacts. To demonstrate the applicability for large‐area electronics, MoS2 n‐MOSFETs are fabricated with semi‐metallic PtSe2 contacts using chemical vapor deposition‐grown MoS2 and PtSe2 films. These devices exhibit outstanding performance metrics, including high on‐state current (≈10−7 A/µm) and large on/off ratio (>107). Furthermore, by employing these high‐performance MoS2 n‐MOSFETs, vertically stacked n‐MOS inverters are successfully demonstrated, suggesting that 3D integration of 2D material FETs is possible using semi‐metallic PtSe2 contacts. [ABSTRACT FROM AUTHOR]

This study unveils a novel concept of symmetric protonic ceramic fuel cells (symm‐PCFCs) with the introduction of a self‐recoverable electrode design, employing the innovative material BaCo0.4Fe0.4Zr0.1Y0.1O3‐δ (BCFZY). This research marks a significant milestone as it demonstrates the bi‐functional electrocatalytic activity of BCFZY for the first time. Utilizing density functional theory simulations, the molecular orbital interactions and defect chemistry of BCFZY are explored, uncovering its unique capability for the reversible exsolution and dissolution of Co‐Fe nanoparticles under redox conditions. This feature is pivotal in promoting both hydrogen oxidation and oxygen reduction reactions. Leveraging this insight, a cell is fabricated exhibiting high electrocatalytic activity and fuel flexibility as evidenced by the peak power densities of ≈350, 287, and 221 mW cm−2 (at 600 °C) with hydrogen, methanol, and methane as fuels, respectively. Experiments also show that the reversible exsolution/dissolution mitigates performance degradation, enabling prolonged operational life through self‐recovery. This approach paves the way for novel, advanced, durable, and commercially viable symm‐PCFCs. [ABSTRACT FROM AUTHOR]

Diamond is a material with promising electronics applications but with challenges in effective doping. Cubic boron nitride (cBN), due to its similar lattice structure, is ideal for forming heterostructures with diamond, to modify electronic properties and especially shift the band positions. Here it is demonstrated how integrating cBN layers of finite thickness in diamond can induce an electronic band offset near the polarized diamond‐cBN interface. Beyond the direct density functional theory computations, an analytical model is developed for rapid examination of the band offset, for a broad number of crystallographic orientations, in excellent agreement with ab initio calculations. Results show that near [100] and [111] crystal directions, the diamond|cBN|diamond heterostructure displays a 3–4 eV band offset which is expected to facilitate effective modulation doping of diamond. [ABSTRACT FROM AUTHOR]

In recent years, it has become possible via on‐surface bottom‐up synthesis to engineer the topological character of carbon nanostructures. Graphene nanoribbons and 1D conjugated polymers (1DCPs) have thus tailored so as to host either topologically trivial or non‐trivial phases. Molecular design is the primary means to set the topological class of these nanomaterials. However, external control over topology is also demonstrated via electric fields or top‐down hydrogenation. Inspired by the connection between topology and π‐conjugation, here it is demonstrated via first‐principles calculations that aryl ring twist angles also serve as topological knobs. Focusing on rationally designed 1DCPs composed of triarylmethyl (TAM) units, it is shown that rotation of certain aryl rings enables a transition from the trivial to the topologically non‐trivial phase. Accordingly, fixing a particular twist angle configuration (e.g., via chemical functionalization) is equivalent to robustly setting a targeted topological phase. It is also found that in considered 1DCPs, the quantum phase transition occurs without the electronic band gap closing, due to a multiradical antiferromagnetic phase emerging at the transition point. All in all, this study highlights the potential of aryl ring twisting for engineering topological properties in carbon nanomaterials and establishes TAM 1DCPs as exotic topological 1D systems. [ABSTRACT FROM AUTHOR]

A conversion‐chemistry‐based zinc–selenium aqueous battery is reported that delivers high specific capacity, good rate capability, and excellent cycle life. In this work, an electronically conjugated covalent triazine framework is used to physicochemically lock selenium (Se8) clusters. As a control sample, the traditional melt‐diffusion approach is used to physically lock Se8. While the melt‐diffused selenium cathode exhibited a precipitous drop in capacity with cycling, the physicochemically locked selenium cathode can be cycled in a stable manner and delivered a specific capacity of ≈600 mAh g−1 with a capacity retention of ≈70% after 1000 continuous charge/discharge steps. Ab initio density functional theory calculations and various structural and morphological characterizations indicate that the superiority of the physicochemically locked selenium cathode stems from its ability to suppress the polyselenide shuttle phenomenon and thus prevent loss of active material during cycling. This work opens the door toward the development of conversion chemistries for high performing, non‐flammable, and low‐cost zinc‐based rechargeable batteries. [ABSTRACT FROM AUTHOR]

Developing effective descriptors for perovskite oxygen evolution reaction (OER) electrocatalysts is crucial for advancing clean energy technologies, which are often constrained by incomplete theoretical calculations. Herein, using step‐wise strained (−3–3%) NdNiO3 as a model, the density functional theory (DFT) is employed, considering both bulk superlattice model (B‐model) and surface slab models (S‐model) to garner a set of electronic descriptors. The S‐model‐derived metal─oxygen orbital hybridization is found to agree with the X‐ray absorption spectroscopy (XAS) results, which, however, are disentangled from the observed OER activity trend. Further detailed analysis discovers that the alignment of the calculated O 2p band position with the OER redox potential on an absolute scale can serve as a hitherto unexplored descriptor for comprehending the activity of lattice oxygen and its bonding strength to OH*. Combined DFT and XAS data reveals that excessive strain hinders surface oxygen exchange, slows down the rate‐determining step of OH* adsorption, and impairs the durability of the electrocatalyst by altering the random electron occupancy in frontier orbitals. The work sheds light on the rational design of cost‐effective, high‐performance perovskite‐based electrocatalysts. [ABSTRACT FROM AUTHOR]

The rational design of heteronuclear dual‐atom catalyst (DAC) is intricate due to the random dispersion of metal atoms under thermal treatment. Herein, a novel precursor pre‐orientation strategy is reported to construct Fe‐Co diatomic sites atomically dispersed on nitrogen doped carbon (Fe‐Co‐NC) via cubic Prussian blue analogue as metal source. Due to the specific synergy between Fe and Co centers, the obtained Fe‐Co‐NC catalyst renders outstanding oxygen reduction reaction (ORR) performance with positive half‐wave potential and good durability in wide pH range. Density functional theory further clarifies the active centers and reveals that the Fe‐Co‐NC dual atomic catalyst follows the modulation mechanism, where the intermediates tended to adsorb on Fe site, while the neighboring Co atom can assist by lowering the d‐band center of Fe site. Experimentally and theoretically emphasizes the priority of heteronuclear diatomic Fe‐Co catalysts over homonuclear Fe‐Fe‐NC and Co‐Co‐NC DAC. Moreover, the Zn‐Air battery (ZAB) and microbial fuel cell (MFC) assembled with Fe‐Co‐NC cathodes both exhibit splendid power density (382 mW cm−2 for ZAB, 2034 ± 103 mW m−2 for MFC) as well as excellent stability. This work provides a new perspective for rational construction and precise regulation for heteronuclear dual‐atom catalysts. [ABSTRACT FROM AUTHOR]

The cost‐effective synthesis of high‐performance hard carbons (HCs) is a key step of sodium‐ion batteries toward practical applications. Considering the rich resource of low‐value aromatic hydrocarbons (e.g., pitch), there is tremendous interesting in its conversion into value‐added HCs. Unfortunately, it still lacks an efficient way for the synthesis, in addition to the time‐consuming oxygen contamination of the carbon framework. Herein, a universal strategy is reported that enables the efficient synthesis of HCs from pitch by modulating hydrogen transfer using metal chlorides. CuCl2 is selected as the model modulator and the effect of different metal chlorides (FeCl3, AlCl3, ZnCl2, and MgCl2) are further explored. Based on material characterizations and density functional theory calculation employing 1‐methylnaphthalene as the model molecule, it shows that the hydrogen capture and chlorination reactions mediated by CuCl2 and FeCl3 are thermodynamically favored, which promote the crosslinking of pitch to form HCs. After optimization, the derived HC exhibits superior performance of reversible capacity of 304.8 mAh g−1 and a high initial Columbic efficiency of 88.4%. These discoveries provide new insights into the synthesis of HCs from aromatic hydrocarbons, facilitating their utilization in electrochemical energy storage. [ABSTRACT FROM AUTHOR]

Topological defects are ubiquitous, they manifest in a wide variety of systems such as liquid crystals, magnets or superconductors. The recent quest for non‐abelian anyons in condensed matter physics stimulates the interest for topological defects since they can be hosted in vortices in quantum magnets or topological superconductors. In addition to these vortex defects, this study proposes to investigate edge dislocations in 2D magnets as new building blocks for topological physics since they can be described as vortices in the structural phase field. It demonstrates the existence of higher order topological dislocations within the higher order moiré pattern of the van der Waals 2D magnet CrCl3 deposited on Au(111). Surprisingly, these higher order dislocations arise from ordinary simple edge dislocations in the atomic lattice of CrCl3. This study provide a theoretical framework explaining the higher order dislocations as vortices with a winding Chern number of 2. It is expected that these original defects can stabilize some anyons either in a 2D quantum magnet or within a 2D superconductor coupled to it. [ABSTRACT FROM AUTHOR]

This work proposes a europium‐based metal–organic framework ([Eu2(HNCP)4Cl4(H2O)2]n, named ZL‐1), featuring dinuclear Eu2(COO)2 clusters as connecting nodes, linked by benzimidazolyl tridentate ligand 2‐(4‐carboxyphenyl)‐imidazo[4,5‐f]‐1,10‐phenanthroline (HNCP) for efficient self‐electrochemiluminescence (self‐ECL). The cathodic ECL emission shows two peaks with a maximum intensity of 7500 a.u.at 0 ∼ −1.8 V in pH 9.0 phosphated buffered solution (PBS) without extra coreactant. The cleavage of N─H bond in benzimidazolyl group can occur under alkaline conditions to generate neutral radical ZL‐1•. After applying voltage, the ZL‐1 can be reduced twice to form ZL‐1Re1•− and ZL‐1Re2•−. Then, ZL‐1Re1•− and ZL‐1Re2•− react with ZL‐1•, accompanied by transferring energy from HNCP to central Eu3+ to produce excited ZL‐1Re1* and ZL‐1Re2* for ECL1 and ECL2 emissions. The local excitation in the HNCP unit is demonstrated with cyclic voltammetry (CV) and stepping pulse ECL. The stimulated and luminous species are confirmed by density functional theory calculations and ECL spectra. This design approach of self‐ECL materials, which coordinated functional ligands with lanthanide metal ions as 3D‐structured MOF, broadened the applications of ECL systems to loose conditions and facilitated mechanistic exploration of ECL processes. [ABSTRACT FROM AUTHOR]

The solid electrolyte interphase (SEI) is a thin heterogeneous layer formed at the anode/electrolyte interface in lithium‐ion batteries as a consequence of the reduction of the electrolyte. The initial formation of the SEI inhibits the direct contact between the electrode and the electrolyte and thus protects the battery. However, the composition, structure, and size of the SEI evolve over time and the growth of the SEI is considered the primary mechanism leading to the gradual deterioration of the battery performance. Despite the importance of the SEI and its growth, the atomistic understanding of the underlying elementary reaction steps remains partial. Molecular modeling of the electrolyte decomposition is key to gain detailed insights that are complementary to experiments for the reactions occurring in this heterogenous interphase. In this perspective, the electron transport mechanisms are first described from the anode to the electrolyte through the SEI and highlight the importance of the inorganic/organic interface within the heterogeneous SEI: it is where the electrolyte decomposition reactions are likely to occur. Finally, a view is provided on the current progress on molecular modeling techniques (e.g., Density Functional Theory, force fields, machine learning potentials) of the SEI and the challenges each method faces. [ABSTRACT FROM AUTHOR]

The moisture‐enabled electricity generators (MEGs) represent an appealing clean power strategy within the realm of hydrovoltaic technology. However, their stable operation under all‐weather conditions is still challengeable due to the effect of ambient humidity. Herein, a self‐water‐storage MEGs with multifunctionality was developed. Gel textiles are employed as the proton‐release layer, while graphite fibers loaded with tin‐bismuth alloy liquid metal serve as water‐storing electrode. The gel textiles absorb water permeating down from the electrodes, releasing protons, which then react with the active electrode to enhance output performance. The experiment demonstrates that a device can generate a voltage of 0.55 V and a current of 7.08 μA after water storage, with a maximum power density of 1.14 μW·cm‐². The device's performance output can remain stable within a wide temperature range. The experiment confirms that the electrical output of the device originates from ionic diffusion, while density functional theory (DFT) and molecular dynamics (MD) calculations reveal the importance of the strong hydrolysis ability of the polymer and the high adsorption energy of the liquid metal for H3O+ on the output performance of the device. Furthermore, the integrated device has demonstrated effective applications in driving microelectronic devices, charging capacitors and, self‐powered health monitoring. [ABSTRACT FROM AUTHOR]

The compelling demand for laser protection both for civil and defense use calls for new‐generation nonlinear optical materials. Chemical vapor deposition (CVD) techniques provide extra tricks to modulate crystal optical nonlinearity through fractal growth. The synthesized 2D NbSe2 and its fractal structures exhibit giant, broadband laser attenuation behaviors extending into the near Infrared (NIR) range. Particularly, the optical limiting performance generally correlates with the fractal dimension, where Fractal NbSe2 demonstrates enhanced third‐order optical nonlinearity at a huge nonlinear absorption coefficient of 9.7 × 10−4 m W−1 and an ultralow starting threshold of 5 mJ cm−2 at 532 nm. Various techniques include femtosecond spectroscopy, Density functional theory (DFT) calculation and Kelvin probe force microscopy disclose the origin of the strong nonlinearity of the 2D NbSe2 crystals, and suggest the formation of edge states and overall faster carrier dynamics, larger surface contact potential difference NbSe2 fractals contribute to their even augmented nonlinear responses. Fractal engineering thus opens new avenues to fabricate highly efficient laser protection materials, and the blocking of intense beam (a large attenuation factor over 13.3 dB at 532 nm) while allowing transmission of weak one (a high linear optical transmittance over 80%) fulfills the much desired "smart" defense. [ABSTRACT FROM AUTHOR]