Confinement Effect Research Articles

Effect of electrostatic confinement on the dome-shaped superconducting phase diagram at the LaAlO3/SrTiO3 interface

The two-dimensional electron gas (2DEG) at the LaAlO\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$_3$$\\end{document}/SrTiO\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$_3$$\\end{document} (LAO/STO) interface exhibits gate-tunable superconductivity with a dome-like shape of critical temperature as a function of electron concentration. This behavior has not been unambiguously explained yet. Here, we develop a microscopic model based on the Schrödinger–Poisson approach to determine the electronic structure of the LAO/STO 2DEG, which we then apply to study the principal characteristics of the superconducting phase within the real-space pairing mean-field approach. For the electron concentrations reported in the experiment, we successfully reproduce the dome-like shape of the superconducting gap. According to our analysis such behavior results from the interplay between the Fermi surface topology and the gap symmetry, with the dominant extended s-wave contribution. Similarly as in the experimental report, we observe a bifurcation effect in the superconducting gap dependence on the electron density when the 2DEG is electrostatically doped either with the top gate or the bottom gate. Our findings explains the dome-shaped phase diagram of the considered heterostucture with good agreement with the experimental data which, in turn, strongly suggest the appearance of the extended s-wave symmetry of the gap in 2DEG at the LAO/STO interface.

Reduction and Quantum Confinement Effects in Graphene Oxide: Relevance for Electro-optical Applications

Reduction and Quantum Confinement Effects in Graphene Oxide: Relevance for Electro-optical Applications

CVD‐Synthesized CsAg2I3 Single Crystals toward Polarization UV Photodetection and Anti‐Counterfeiting Identification

AbstractLow‐dimensional ternary silver halide (CsAg2I3), an emerging inorganic lead‐free perovskite, has garnered significant scientific attention due to its strong quantum confinement effects, wide bandgaps, non‐toxicity, and others. However, the photophysical properties and optoelectronic performance of CsAg2I3 materials and devices are significantly compromised by crystal quality and defects arising from liquid‐phase preparation. Herein, 1D CsAg2I3 single crystals newly grown by the chemical vapor deposition method are reported. These crystals display exceptional quality and stability over a 3‐month period despite exposure to air and moisture. The high in‐plane anisotropic structure, phonon vibrations, and refractive index of CsAg2I3 crystals are also experimentally elucidated. Polarization‐sensitive ultraviolet photodetector based on the CsAg2I3 monocrystal features a responsivity of 139 mA W−1, a specific detectivity of 1.05 × 1011 cm Hz1/2 W−1, an ultra‐fast photoresponse speed of 48.2/69.1 µs, and a dichroic ratio of 2.66 upon 360 nm irradiation at −5.0 V bias. The photodetector excels amongst its competitors, moving toward the potential application of rapid optical anti‐counterfeiting identification. This work, which leverages grown high‐crystalline and highly stable CsAg2I3 monocrystals, holds promises for advancing this functional material into a robust next‐generation optoelectronic devices capable of probing sensitive optical sensing and specific azimuth recognition.

Structural Insight into Ionogels: A Case Study of 1-Methyl-3-octyl-imidazolium Tetrafluoroborate Confined in Aerosil.

Ionogels were obtained by impregnating Aerosil A380 with 1-methyl-3-octyl-imidazolium tetrafluoroborate (OMIM BF4) ionic liquid (IL). The IL content of the ionogels varied from 16.3 to 79.9 mol %. There was evidence of the confinement of the IL in silica in the shift and broadening of the BF4- 19F NMR signal and in the noticeable (∼50 °C) decrease in the temperature of IL decomposition. For both the ionogels and the pure IL, the frequencies of IR vibrations were different, providing further evidence of the confinement effect. An analysis of textural characteristics revealed that, upon its addition to Aerosil, the IL sequentially adsorbed in the micropores, mesopores and interparticle space. SAXS measurements showed that, in the confined IL, the size of nonpolar correlations substantially increased, from 21.5 Å in the bare IL to 25.6 Å in the ionogel containing 28.1 mol % IL. Unexpectedly, for the ionogel with the lowest IL content (16.3 mol %), no nonpolar correlations were observed, indicating the strong distortion of the structure of the confined ionic liquid. To the best of the authors' knowledge, this is the first report on regular changes in nonpolar correlations in ionic liquids upon confinement in a porous solid. These structural correlations can easily be tuned by simply changing the IL content in the ionogel material.

Investigation of structural frustration in symmetric diblock copolymers confined in polar discs through cell dynamic simulation

Nanotechnology has opened new avenues for advanced research in various fields of soft materials. Materials scientists, chemists, physicists, and computational mathematicians have begun to take a keen interest in soft materials due to their potential applications in nanopatterning, membrane separation, drug delivery, nanolithography, advanced storage media, and nanorobotics. The unique properties of soft materials, particularly self-assembly, have made them useful in fields ranging from nanotechnology to biomedicine. The discovery of new morphologies in the diblock copolymer system in curved geometries is a challenging problem for mathematicians and theoretical scientists. Structural frustration under the effects of confinement in the system helps predict new structures. This mathematical study evaluates the effects of confinement and curvature on symmetric diblock copolymer melt using a cell dynamic simulation model. New patterns in lamella morphologies are predicted. The Laplacian involved in the cell dynamic simulation model is approximated by generating a 17-point stencil discretized to a polar grid by the finite difference method. Codes are programmed in FORTRAN to run the simulation, and IBM open DX is used to visualize the results. Comparison of computational results with existing studies validates this study and identifies defects and new patterns.

Controllable multilevel quantized conduction states in vertical CBRAM using Cu-nanodot ion source

Restricting the injection of cations is crucial for implementing precise quantized conduction (QC) during the multi-level operation of conductive-bridge random-access memory (CBRAM). This study proposes a method that controls ion supply by confining the Cu ion source to 0D in a vertical structure. This confinement enables sophisticated filament control for multilevel operation. Cu nanodots are formed between the W electrodes, with W and Cu serving as the electron and ion sources for the conducting filament, respectively. When the Cu filament is confined to 0D, the controllability of the QC implementation is better than that in cases where the filament is restricted to 1D or bulk Cu. The highest number of quantized levels was observed for 0D Cu, which can be attributed to the synergistic effects of filament confinement and the decrease in the Cu electrochemical reaction rate. Furthermore, we analyzed the switching mechanism of the Cu nanodots by employing the activation energy extracted by the slope of the voltage-time dilemma. Our results demonstrate the effectiveness of confining the ion source to 0D for achieving precise filament control in CBRAM and enabling its applicability to vertical structures.

Incorporation of Multiple Binding Sites into an Adaptive MOF for Sieving Butane Isomers

AbstractEfficient separation of liner alkanes from branched alkanes is of prime importance in the petrochemical industry. Herein an adaptive metal‐organic framework FJI‐H38 is reported with 1D channel which can vary delicately ≈4.0 Å. The activated FJI‐H38 displays extremely large butane (n‐C4H10) capacity, especially at low pressure (44.15 cm3 g−1 at 298 K and 0.1 bar), but barely adsorbs isobutane (iso‐C4H10). Remarkably, FJI‐H38 possesses a high n‐C4H10/iso‐C4H10 selectivity of 246.75. Gas‐loaded single crystal X‐ray analysis and modeling calculation reveal that the synergetic effect of pore confinement and surfaces decorated with uncoordinated carboxyl group plays a critical role in the capture of the relatively smaller n‐C4H10 while the exclusion of the larger iso‐C4H10. In addition, dynamic breakthrough tests explicitly prove FJI‐H38 displays prominent separation performance for n/iso‐C4H10 under various conditions with ultra‐high productivity of high‐purity n‐C4H10 (42.48 L/kg, ≥99.0%) and iso‐C4H10 (42.35 L/kg, ≥99.95%).

Ultralong Room Temperature Phosphorescence Emission From Gels Induced by Multiple Confinement Effects

AbstractThe construction of ultra‐long room temperature phosphorescence (RTP) gels has always been a serious challenge because the dispersing medium would significantly deteriorate their rigidity, resulting in triplet excitons consumption by non‐radiative transitions. In this paper, eutectogel with ultra‐long RTP emission is successfully constructed by rebuilding the damaged rigid system with solvent exchange. Specifically, the formation of cyclic borate via the B─O click reaction between 1,3,5‐tris(4‐phenylboronic acid)benzene (TPPB) and poly(vinyl alcohol) (PVA) matrix is demonstrated to be favorable for RTP emission, with the resulting films possessing an afterglow duration of 26 s and a lifetime of up to 2.92 s. Based on this, deep eutectic solvents (DES)‐based RTP gel is successfully prepared by cyclic freezing‐thawing and solvent exchange of aqueous solution of TPPB functionalized PVA obtained by click reaction. The obtained gel exhibited an afterglow of up to 8 s and RTP lifetime of 902 ms under ambient conditions. Further analyses showed that the introduction of DES reconstructed interactions between polymer chains damaged by water and enhanced the rigidity of the system, thus promoting RTP emission.

Flexural performance of UHPC two-way slab reinforced with FRP bars

The flexural behaviors of ultra-high-performance concrete (UHPC) two-way square slabs reinforced with fiber-reinforced polymer (FRP) bars were studied experimentally. Flexural tests were conducted on eight specimens, varying in reinforcement type, reinforcement ratio and confinement condition in compressive zone. Test results showed that the bridging effects of steel fibers in UHPC can mitigate the brittle characteristics of slab experiencing punching shear failure. The failure modes of slabs shifted from tensile failure to compressive failure by increasing the tensile strength of bar, leading to an improvement on the flexural capacity and ductility. The ultimate capacity of the slab with a reinforcement ratio of 1.06 % was 15.8 % greater than that of the slab with a reinforcement ratio of 0.67 %. By incorporating a layer of basalt fiber-reinforced polymer (BFRP) grid in the compressive zone to confine UHPC, the bearing capacity and ductility index of the slab increased by 17.8 % and 56.7 %, respectively. Introducing an enhancement coefficient to account for the confinement effect induced by the BFRP grid, a method was developed for predicting the flexural capacity of FRP reinforced UHPC two-way slab subjected to a local load at the mid-span, and its prediction accuracy was well verified.

Saturation Mobility of 100 cm2 V-1 s-1 in ZnO Thin-Film Transistors through Quantum Confinement by a Nanoscale In2O3 Interlayer Using Spray Pyrolysis.

In this study, we present a comprehensive study on the fabrication and characterization of heterojunction In2O3/ZnO thin-film transistors (TFTs) aimed at exploiting the quantum confinement effect to enhance device performance. By systematically optimizing the thickness of the crystalline In2O3 (c-In2O3) layer to create a narrow quantum well, we observed a significant increase in saturation mobility (μSAT) from 12.76 to 97.37 cm2 V-1 s-1. This enhancement, attributed to quantum confinement, was achieved through the deposition of a 3 nm c-In2O3 semiconductor via spray pyrolysis. Various In2O3 layer thicknesses (2-5 nm) were obtained by adjusting precursor solution concentration, flow rate, and number of spray cycles. Post annealing treatments were employed to reduce the defects at the interface and within the oxide film, enhancing device stability and performance. Transmission electron microscopy (TEM) confirmed the uniformity of the c-In2O3 film thickness, while variations in thickness significantly influenced TFT performance, particularly the turn-on voltage (VGS) due to changes in the carrier concentration. Ultraviolet photoelectron spectroscopy (UPS) and X-ray photoelectron spectroscopy (XPS) supported the formation of a potential well with a two-dimensional electron gas (2DEG). The study of single and multiple superlattice structures of consecutive c-In2O3 and c-ZnO layers provided insights into the effects of multiple quantum wells on the TFT performance. This research presents an advanced approach to TFT optimization, highlighting high reliability, and environmental and bias stabilities. These lead to enhanced mobility and performance uniformity through the precise control of c-In2O3 layer thickness for the quantum confinement effect.

Mesoscale Reorganization of the Depolymerized Aluminosilicate into Single-Crystalline Hierarchical Zeolite.

Controllable synthesis of hierarchical zeolites from natural aluminosilicate minerals is considered an efficient and eco-friendly approach for the production of high-performance zeolites, but its synthesis mechanism is still obscure. Herein, we take the synthesis of a single-crystalline hierarchical NaA zeolite using submolten salt depolymerized kaolin (SMS-K) as the sole source of silicon and aluminum via a mesoscale reorganization strategy as an example to elucidate the reorganization process. Comprehensive morphological and structural analyses reveal that sodium-rich voids in SMS-K facilitate concurrent assembly both within the interior and at the interface of the amorphous gel, leading to the formation of numerous nanoparticles with short-range order which assemble into single-crystal nanocube NaA zeolites with intracrystalline mesopores. By harnessing confinement effects, SMS-K modulates the growth of nanoparticle sizes and enhances the intimate interconnection of nanocubes, thereby yielding NaA zeolite aggregates that exhibit hierarchical porosity, encompassing micro-, meso-, and macropores. This study offers the potential for designing and precisely controlling the fabrication of hierarchical zeolites derived from natural minerals.

Contrasting behavior of urea in strengthening and weakening confinement effects on polymer collapse.

Biomolecules inhabit a crowded living cell that is packed with high concentrations of cosolutes and macromolecules that result in restricted, confined volumes for biomolecular dynamics. To understand the impact of crowding on the biomolecular structure, the combined effects of the cosolutes (such as urea) and confinement need to be accounted for. This study involves examining these effects on the collapse equilibria of three model 32-mer polymers, which are simplified models of hydrophobic, charge-neutral, and uncharged hydrophilic polymers, using molecular dynamics simulations. The introduction of confinement promotes the collapse of all three polymers. Interestingly, addition of urea weakens the collapse of the confined hydrophobic polymer, leading to non-additive effects, whereas for the hydrophilic polymers, urea enhances the confinement effects by enhancing polymer collapse (or decreasing the polymer unfolding), thereby exhibiting an additive effect. The unfavorable dehydration energy opposes collapse in the confined hydrophobic and charge-neutral polymers under the influence of urea. However, the collapse is driven mainly by the favorable change in polymer-solvent entropy. The confined hydrophilic polymer, which tends to unfold in bulk water, is seen to have reduced unfolding in the presence of urea due to the stabilizing of the collapsed state by urea via cohesive bridging interactions. Therefore, there is a complex balance of competing factors, such as polymer chemistry and polymer-water and polymer-cosolute interactions, beyond volume exclusion effects, which determine the collapse equilibria under confinement. The results have implications to understand the altering of the free energy landscape of proteins in the confined living cell environment.

Helium roaming in excess electrons in C60F60 as dynamic quasi-Matryoshka dolls.

Multi-guest clathrates exhibit lots of functional characteristics owing to their unique structures, which herald beautiful application prospects, but their fundamental information is still scarce. Herein, we explore a type of (helium, excess electrons/EEs)-C60F60 co-clathrates with quasi-Matryoshka-doll structures using abinitio molecular dynamics simulation and reveal the EEs-entangled He roaming dynamics in C60F60 and its effect on the characteristics of clathrates. Perfluorination ensures that C60F60 possesses an extremely electropositive interior cavity. Its unique confinement effect can stabilize He as an extremely inert entity by noticeably enlarging the 1s-2s orbital gap and can also trap 1-2 EEs in its s-type interior orbital with extremely large binding energies. Co-inclusion of He and EEs in C60F60 exhibits inter-repulsive He⋯EEs entangling dynamics featuring quasi-Matryoshka-doll structures (He@EEs@C60F60). In this structure, EEs screen the attraction of cage-shell Cδ+ to He 1s2 electrons, thus inhibiting their stabilization and orbital expansion, while He conversely decreases the stability of EEs and redshifts their transition absorption. He can roam in the cavity, but its trajectory is impacted by EEs serving as a medium, and thus, the structures exhibit anormal dynamic variation of internuclear He⋯C spin coupling JHeC, which is manipulated by the EEs-entangled He roaming dynamics. JHeC and JHeC' present opposite distance dependences for the colinearly aligned C⋅⋅⋅He⋅⋅⊗⋅⋅⋅⋅⋅C' (⊗, the cage center). This work provides insights into the Matryoshka-doll structured He@EEs@C60F60 with He-EEs entangling dynamics and its modulation on EEs absorption and reveals the dynamic role of EEs in manipulating He-roaming and JHeC coupling properties for promising applications.

Selectivity Descriptors of Methanol-to-Aromatics Process over 3-Dimensional Zeolites.

The zeolite-catalyzed methanol-to-aromatics (MTA) process is a promising avenue for industrial decarbonization. This process predominantly utilizes 3-dimensional 10-member ring (10-MR) zeolites like ZSM-5 and ZSM-11, chosen for their confinement effect essential for aromatization. Current research mainly focuses on enhancing selectivity and mitigating catalyst deactivation by modulating zeolites' physicochemical properties. Despite the potential, the MTA technology is at a low Technology Readiness Level, hindered by mechanistic complexities in achieving the desired selectivity towards liquid aromatics. To bridge this knowledge gap, this study proposes a roadmap for MTA catalysis by strategically combining controlled catalytic experiments with advanced characterization methods (including operando conditions and "mobility-dependent" solid-state NMR spectroscopy). It identifies the descriptor-role of Koch-carbonylated intermediates, longer-chain hydrocarbons, and the zeolites' intersectional cavities in yielding preferential liquid aromatics selectivity. Understanding these selectivity descriptors and architectural impacts is vital, potentially advancing other zeolite-catalyzed emerging technologies.

Reducing Dielectric Confinement Effect Enhances Carrier Separation in Two-Dimensional Hybrid Perovskite Photocatalysts.

Two-dimensional organic-inorganic hybrid perovskites (OIHPs) with alternating structure of the organic and inorganic layers have a natural quantum well structure. The difference of dielectric constants between organic and inorganic layers in this structure results in the enhancement of dielectric confinement effect, which exhibits a large exciton binding energy and hinders the separation of electron-hole pairs. Herein, a strategy to reduce the dielectric confinement effect by narrowing the dielectric difference between organic amine molecule and [PbBr6]4- octahedron is put forward. The Ethanolamine (EOA) contains hydroxyl groups, resulting in the positive and negative charge centers of O and H non-overlapping, which generated a larger polarity and dielectric constant. The reduced dielectric constant produces a smaller exciton binding energy (71.03 meV) of (C2H7NO)2PbBr4 ((EOA)2PbBr4) than (C8H11N)2PbBr4 ((PEA)2PbBr4 (156.07 meV), and promotes the dissociation of electrons and holes. The increasing of lifetime of photogenerated carrier in (EOA)2PbBr4 are proved by femtosecond transient absorption spectra. Density functional theory (DFT) calculations have also indicated that the small energy shift of the total density of states (DOS) between the C/H/N and the Pb/Br in (EOA)2PbBr4 favors the separation of electrons and holes. In addition, this work demonstrates the application of (PEA)2PbBr4 and (EOA)2PbBr4 in the field of photocatalytic CO2 reduction.

Taylor-Aris Dispersion in Nanotubes: Analytical Solution, Effects of Slip and Surface Potential Landscape, and Measurement of the Slip Length.

Taylor-Aris (T-A) dispersion of a solute in a flowing solvent is a fundamental phenomenon in most mass-transfer processes. Despite its significance and numerous applications in microreactors, colloidal transport in confined media, chromatographic separation, and transport in biological tissues, the effect of the slip length and the topology of surface potential landscapes on T-A dispersion in nanostructured channels has not been studied in detail. We propose a novel methodology for molecular dynamics (MD) simulation of T-A dispersion in such systems, derive an analytical expression for the dispersion coefficient in them, and report on the results of extensive MD simulations of the phenomenon in carbon nanotubes and hexagonal carbon nanochannels. By broadening the topology of the surface energy landscape, we vary the slip lengths, making it possible to distinguish between the effects of confinement, the topology of the energy landscape, and the slip length on the T-A dispersion coefficient. It is demonstrated that measuring the T-A dispersion coefficient in laminar flow is a straightforward and reliable approach for estimating the slip length in nanotubes and other nanostructured materials.

Epitaxial Growth of a Three-Dimensional Hollow and Chestnut Shell Photothermal p-n Junction Photoanode.

The p-n junction, a widely studied semiconductor material structure, offers only limited improvements in photoelectrochemical (PEC) efficiency. Herein, a three-dimensional (3D) p-n junction h-Ta3N5@CoN featuring a stable chestnut shell hollow sphere structure and photothermal effect was synthesized by using an epitaxial growth strategy. The fine fibers within the sphere induce Rayleigh scattering, which scatters unabsorbed light, thereby enabling secondary absorption and enhancing light utilization. The quantum confinement effects generated by CoN fine fibers, which are sized in a few nanometers, inhibit the recombination of electron-hole pairs. Moreover, the lattice matching between Ta3N5 and CoN allows for smoother movement of carriers and nonradiative relaxation phonons along the lattice, thereby enhancing the transport of both carriers and heat. The obtained h-Ta3N5@CoN/FTO p-n junction photoanode, under near-infrared (NIR) auxiliary irradiation, demonstrates a photocurrent of 8.71 mA cm-2 at 1.23 VRHE. Moreover, the h-Ta3N5@CoN+NIR/FTO photoanode can sustain operation for 168 h, which, to my knowledge, surpasses the operational durations of all other Ta3N5-based photoanodes. This study synthesizes three-dimensional hollow chestnut shell photothermal p-n heterojunctions through an epitaxial growth strategy, endowing the material with a more efficient carrier separation and photothermal transfer efficiency.

Nitrogen-doped carbon nanosheet confined PtNi alloy for efficient acidic electrocatalytic hydrogen evolution reaction

Low intrinsic electrocatalytic activity and inferior conductivity limit the application of Ni/NC in acidic electrocatalytic hydrogen evolution reaction (HER). Herein, we prepared nitrogen-doped carbon nanosheet confined PtNi alloy electrocatalysts (PtNi/NC-10) using PtCl62− electrostatic adsorption coupling melamine pyrolysis nitriding strategy. PtNi alloying was confirmed by the crystallinity decrease and lattice expansion of Ni/NC. The alloying and confinement effect of Metal-Organic Frameworks (MOFs) suppresses the oxidation and agglomeration of metal nanoparticles during pyrolysis, thus significantly reducing particle size, increasing specific surface area, and promoting the exposure of active sites. The strong electronic interaction between Pt and Ni optimizeds the surface charge distribution, enhancing the adsorption of H species on electron-rich Pt sites, thereby improving reaction kinetics. In addition, PtNi alloying improves the conductivity of the material, accelerating charge transfer and proton transport. Consequently, the prepared PtNi/NC-10 exhibits superior HER performance than Ni/NC in 0.5 M H2SO4 solution, even comparable to commercial 20 wt% Pt/C, with the overpotentials of 35 mV at 0.01 A cm−2. Furthermore, the electrocatalysts assembled PtNi/NC-10-CP‖RuO2-TFF proton exchange membrane (PEM) electrolyzer only requires 2.32 V cell voltage to achieve 1 A cm−2, presenting practical application prospects. Our work provides a novel idea for designing efficient and stable MOFs confined to alloy-based HER electrocatalysts.

Entropy in catalyst dynamics under confinement.

Entropy during the dynamic structural evolution of catalysts has a non-trivial influence on chemical reactions. Confinement significantly affects the catalyst dynamics and thus impacts the reactivity. However, a full understanding has not been clearly established. To investigate catalyst dynamics under confinement, we utilize the active learning scheme to effectively train machine learning potentials for computing free energies of catalytic reactions. The scheme enables us to compute the reaction free energies and entropies of O2 dissociation on Pt clusters with different sizes confined inside a carbon nanotube (CNT) at the timescale of tens of nanoseconds while keeping ab initio accuracy. We observe an entropic effect owing to liquid-to-solid phase transitions of clusters at finite temperatures. More importantly, the confinement effect enhances the structural dynamics of the cluster and leads to a lower melting temperature than those of the bare cluster and cluster outside the CNT, consequently facilitating the reaction to occur at lower temperatures and preventing the catalyst from forming unfavorable oxides. Our work reveals the important influence of confinement on structural dynamics, providing useful insight into entropy in dynamic catalysis.

Dynamically Confined Active Silver Nanoclusters with Ultrawide Operating Temperature Window in CO oxidation.

Supported metal nanoclusters are often highly active in many catalytic reactions but less stable particularly under harsh reaction conditions. Here, we demonstrate that this activity-stability trade-off can be efficiently broken through rational design of surrounding microenvironment of the supported nanocatalyst including gas adsorbate overlayer and underneath support surface chemistry. Our studies reveal that chemisorbed oxygen species on Ag surface and surface hydroxyl groups on oxide support, which are dynamically consumed during reaction but sustained by reaction environment (O2 and H2O vapor), drive spontaneous redispersion of Ag particles and stabilization of highly active Ag nanoclusters. Such a dynamic confinement effect from gas-catalyst-support interaction enables the Ag nanoclusters to exhibit complete catalytic oxidation of CO over a wide temperature window of 25 - 500 °C under dry conditions and 200 - 800 °C under wet conditions as well as remarkable stability at 300 °C over 1000 h.