Silver cluster-assembled materials (SCAMs), by virtue of their tunable structure, accessible surface area and excellent stability, hold great promise as highly efficient catalysts. Herein, we report a new SCAM [Ag12(StBu)6(CF3COO)3(TPyP)]n (denoted Ag12TPyP) composed Ag12 chalcogenolate cluster core stabilized porphyrinic ligands. Ag12TPyP showed superior sulfur mustard simulant (2-chloroethyl ethyl sulfide, CEES) degradation efficiency achieved half lifetime (t1/2) 1.5 min with 100%...

Pt nanocatalysts play a critical role in direct methanol fuel cells (DMFCs) due to their appropriate adsorption/desorption energy, yet suffer from an unbalanced relationship between size-dependent activity and stability. Herein, mixed-dimensional Pt-Ni alloy polyhedral nanochains (Pt-Ni PNCs) with ordered assembly of nanopolyhedra-nanowire-nanopolyhedra architecture are fabricated as bifunctional electrocatalysts for DMFCs, effectively alleviating the size effect. The PNCs exhibit 7.23 times...

Deciphering the precise physical mechanism of interaction between an adsorbed species and a reactive site in heterogeneous catalysis is crucial for predictive design highly efficient catalysts. Here, using first-principles calculations we identify that two-dimensional ferromagnetic metal organic framework Mn2C18H12 can serve as single-atom catalyst spin-triplet O2 activation CO oxidation. The underlying via "concerted charge-spin catalysis", involving delicate synergetic process charge...

Abstract Physical unclonable functions (PUFs) have emerged as a promising encryption technology, utilizing intrinsic physical identifiers that offer enhanced security and tamper resistance. Multi‐level PUFs boost system complexity, thereby improving reliability fault tolerance. However, crosstalk‐free multi‐level remain persistent challenge. In this study, hierarchical PUF harnesses the spontaneous phase separation of silk fibroin /PVA blend random distribution silicon‐vacancy diamonds...

Self-assembled monolayers (SAMs) with excellent hole conduction capabilities significantly improve the performance of inverted perovskite solar cells (PSCs). However, amphiphilic nature SAMs causes spontaneous formation spherical micelles in solution, limiting their surface coverage and uniformity on indium tin oxide (ITO) substrates. Furthermore, distribution directly affects morphology films charges transfer properties at buried interface. This study employs a cosolvent strategy combining...

Motivated by recent experimental developments of graphitic-CN (g-CN) sheets, we investigate the suitability hydrogen storage on Li decorated g-CN via first-principles calculations. We find that binding energies atoms are very large, ranging from 2.70 to 4.73 eV, which significantly higher than cohesive energy bulk Li. Lithium therefore tend form 2D rather 3D patterns g-CN, promoting reversible adsorption and desorption. Remarkably, average H2 molecules falls in 0.14-0.23 eV range, CN shows a...

Abstract Lead‐free halide double perovskites (HDPs) are promising candidates for high‐performance solar cells because of their environmentally‐friendly property and chemical stability in air. The power conversion efficiency HDPs‐based needs to be further improved before commercialization the market. It requires a thoughtful understanding correlation between specific structure property. Here, structural optical properties an important HDP‐based (NH 4 ) 2 SeBr 6 investigated under high...

Efficient oxygen reduction reactions (ORRs) rely on the appropriate chemical adsorption of triplet (O2) surface catalyst and rapid conversion to doublet intermediate species, accelerating ORR process. However, overcoming energy barrier this spin-forbidden transition via spin coupling with a remains major challenge. Herein, iron phthalocyanine (FePc) was attached intrinsic atomic step sites semiconductor TiO2 nanotubes (FePc@TiO2). The inherent magnetic field these induced flip within Fe 3d...

Construction of two-dimensional van der Waals (vdW) heterostructure has been well recognized to provide an avenue towards designing functional optoelectronic and photovoltaic devices. Here, a type-II vdW consisting anisotropic black phosphorus (BP) ${\mathrm{TiS}}_{3}$ possessing ultrafast interlayer charge transfer for photoconversion is established using ab initio nonadiabatic molecular dynamics with HSE06 hybrid functional. The present results demonstrate that the electron hole occur...

Chemical reactions of burning Poly(methyl methacrylate) (PMMA) are reviewed in this paper although kinetics thermal decomposition believed to be fairly simple. Basically, there three stages the combustion PMMA. Firstly, PMMA decomposes produce monomer methyl methacrylate (MMA). Secondly, MMA generate small gaseous molecules that usually combustible. Finally, these undergo combustion. Recent studies on and stability also introduced. Results useful for understanding heat released per unit mass...

Nanoclusters with extra stability at certain cluster sizes are known as magic clusters exotic properties. The classic Wulff construction principle, which stipulates that the preferred structure of a should minimize its total surface energy, is often invoked in determining magicity, resulting close-shelled Mackay icosahedronal odd-numbered 13, 55, 147, etc. Here we use transition metal around size 55 prototypical examples to demonstrate that, nanometer regime, principle needs be generalized...

Catalysis using gold nanoparticles supported on oxides has been under extensive investigation for many important application processes.

Understanding hot carrier dynamics between plasmonic nanomaterials and its adsorbate is of great importance for plasmon-enhanced photoelectronic processes such as photocatalysis, optical sensing spectroscopic analysis. However, it often challenging to identify specific dominant mechanisms a given process because the complex pathways ultrafast interactive photoelectrons. Here, using CO2 reduction an example, underlying plasmon-driven catalysis at single-molecule level time-dependent density...

Abstract Constructing high‐performance‐2D heterostructures and deciphering the underlying microscopic mechanism of carrier dynamics are crucial in optoelectronic photovoltaic applications. Here, taking black phosphorus (BP)/MoS 2 heterostructure with type‐II band alignment as a prototypical example, ab initio nonadiabatic molecular simulations demonstrate that interlayer thickness dependent. Specifically, electron transfer from monolayer (1L)‐BP to MoS occurs quickly within 54 fs. In...

Magnetic single-atom catalysts (MSAC), due to the intrinsic spin degree of freedom, are particular importance relative other conventional SAC for applications in various catalytic processes, especially those cases that involve spin-triplet O2. However, bottleneck issue this field is clustering during processes. Here using first-principles calculations we predict Mn atoms can be readily confined interface porous g-C3N4/CeO2(111) heterostructure, forming high-performance MSAC O2 activation via...

Abstract Diamond, with ultrahigh hardness, high wear resistance, thermal conductivity, and so forth, has attracted worldwide attention. However, researchers found emergent reactions at the interfaces between diamond ferrous materials, which significantly affects performance of diamond‐based devices. Herein, combing experiments theoretical calculations, taking diamond–iron (Fe) interface as a prototype, counter‐diffusion mechanism Fe/carbon atoms been established. Surprisingly, it is...

The burning behavior and combustion mechanism of polymethylmethacrylate (PMMA) were studied by using cone calorimeter, mass spectrograph gas chromatograph. Main mechanisms PMMA reviewed. Results indicated that would burn steadily under low radiative heat flux; or with thicker samples. yields carbon dioxide monoxide not be changed. Under high heating rate, there are three broad stages. Firstly, upon external sources, decompose to generate monomer MMA a small amount other products. Secondly,...

The usage of ZnO as active layers to fabricate hybrid heterojunction light-emitting diodes is expected be an effective approach for ultraviolet light sources. Individual microwires with controlled gallium (Ga) incorporation (ZnO/Ga MWs) have been fabricated via a chemical vapor deposition method. It found that the increasing Ga-incorporated concentration, near-band-edge (NBE) photoluminescence MWs blue-shifted gradually from 390 370 nm. Heterojunction comprising single ZnO/Ga and p-GaN...

Single-atom catalysts (SACs) are of great scientific and technical importance due to their low cost, high site density, specificity enhance chemical reactions. Nevertheless, a major issue that severely limits the practical exploration SACs is instability, i.e., preference sintering clustering over defect-free substrate during operation. Here, we employ first-principles calculations investigate how engineering can stabilize by strain-tuning electronic interactions between metal using two Pd...

Selective hydrogenation of carbon dioxide (CO2) into value-added chemicals via highly efficient catalysts is great significance in CO2 conversion and utilization. Here, taking CuN/MoS2/Ag(111) heterostructures (N = 1–8) as prototypical examples, we theoretically establish a concept dynamically magic single-cluster catalyst (DMSCC) for high-efficient selective to CH3OH. It found that, though Cu2 Cu8 the gas phase are well recognized clusters due closed-shell electronic structures, Cu3 Cu7...

With the introduction of single atoms in photocatalysis, a small change electronic and geometric structure substrate can result higher energy conversion efficiency, whereas underlying microscopic dynamics are rarely illustrated. Here, employing real-time time-dependent density functional theory, we explore ultrafast structural single-atom photocatalysts (SAPCs) water splitting at scale. The results demonstrate that Pt loaded on graphitic carbon nitride greatly promotes photogenerated...