Hydrophilic and superhydrophilic surfaces are often used in various applications, such as biomedical surface modification, heat pipe design, lab-on-chip devices, microelectronic structure design, etc. Deposition of molecules on surfaces and chemical modification of the surface are two of the frequently adopted techniques to fabricate hydrophilic surfaces. However, achieving controlled and precise surface roughness is an expensive process, and the multiscale nature of liquid imbibition on rough surfaces complicates the system's physics. To address this challenge, we propose an alternative approach for creating controlled rough surfaces by electrodeposition of copper ions on copper electrodes, explore the influence of various length scales encountered in roughened surfaces, ranging from micrometers to angstroms, and examine the associated physics. The microscale roughnesses are controlled by adjusting the deposition time. A molecular level investigation is employed to probe the intriguing physics of liquid imbibition on the created rough surface. The molecular analysis of droplet contact line dynamics, including the contact angle and footprint radius, shows qualitative alignment with the real systems. Additionally, this study provides new insights into the flow velocities during imbibition within surface asperities at the molecular level. Directional velocities, such as axially downward and horizontally outward flows, which are otherwise challenging to measure experimentally, are also evaluated on a molecular scale. These findings provide a fundamental understanding of the intricate phenomena of liquid spreading and imbibition on metallic surfaces with randomly distributed rough textures, deepened by molecular-scale insights. The agreement, on a qualitative scale, between the experiments and simulations is successfully established, providing a fundamental understanding of the complex phenomena of water droplet imbibition dynamics on an electrodeposited surface.

Sodium diethyldithiocarbamate (DDTC), a common collector used to enhance the hydrophobicity of minerals in froth flotation, nevertheless weakens the hydrophobicity of the talc surface. To rationalize this anomaly, the interactions of a hydrophobic alkyl group and hydrophilic mineralophilic group (-NCS) of heteropolar surfactant DDTC, and a water molecule with the talc (001) surface, were investigated. Herein, DFT simulations found that the talc (001) surface features natural hydrophobicity determined by the competition between adhesion (surface water) and cohesion (water-water interactions). The interaction of the hydrophobic alkyl group of DDTC with the talc surface is more favorable compared to that of the -NCS group and HO, favoring the hydrophilic modification of the talc surface. Additionally, adsorption isotherms, time-of-flight secondary ion mass spectrometry (ToF-SIMS), microflotation tests, and contact angle measurements also indicate that the differences in adsorption orientation of the heteropolar surfactant DDTC on the talc surface enhance the hydrophilicity of the talc surface, leading to a decreased recovery of the talc. This study provides crucial surface chemistry evidence for the selective adsorption of heteropolar surfactants and contributes to the understanding of the mechanism for the efficient flotation separation of molybdenite from talc.

The potential application prospects of urea-assisted water electrolysis toward hydrogen production in renewable energy infrastructure can effectively alleviate energy shortages and environmental pollution caused by rich urea wastewater. It is of prominent significance that adjusting the CO desorption of nickel-based electrocatalysts can overcome the slow reaction kinetics for urea oxidation reaction (UOR) to achieve exceptional catalytic activity. In this work, cobalt (Co) metal doping is employed to boost the UOR performance of nitrogen-doped carbon nanotubes encapsulating nickel nanoparticle electrocatalysts (Ni@N-CNT). The influence of diverse Co doping concentrations on the performance of UOR and hydrogen evolution reaction (HER) catalytic activities associated with stability are systematically investigated. The Co dopant can effectively promote the dynamical conversion of Ni to Ni species; as a result, the UOR catalytic activity is improved by 1.8-fold at 1.6 V vs RHE. The DFT calculation results show that the CoNi bimetallic structure possesses a comparably lower binding energy for CO adsorption accelerating the rate-limiting step. Meanwhile, the Co dopant also boosts the HER performance, achieving a 57 mV reduction in overpotential at 100 mA cm due to the creation of more active sites. In addition, the assembled urea-assisted water electrolysis attains 10 mA cm at merely 1.51 V as well as excellent stability.

In this study, pyrite was used as the research object, and the behavior and mechanism of a copper-ion-enhanced organic depressant in depressing pyrite flotation were studied. Microflotation experiments showed that, after the addition of CuSO and ,-dimethyldithiocarbamate (,-DDS), the floating collection efficiency of pyrite declined from 82.37 to 21.03% at pH 8.5. Infrared spectroscopy studies indicated that the addition of CuSO caused a significant enhancement in the characteristic ,-DDS peaks on the pyrite surface. X-ray photoelectron spectroscopy (XPS) revealed that, following the addition of CuSO and ,-DDS, the relative atomic concentration of N 1s considerably enhanced on the surface of pyrite, with N 1s derived from ,-DDS. Time-of-flight secondary ion mass spectrometry showed that, before and after the addition of CuSO, the normalized peak values of CSN on the pyrite superficial layer were 0.0116 and 0.0032, respectively. All of the above-mentioned results indicate that the Cu ion promotes the adsorption of ,-DDS on pyrite and facilitates the formation of complex ((CH)NCSS)Cu. The N and S atoms in -NCS and metal ions formed chemical bonds, which were the primary mechanism of the interaction between ,-DDS and pyrite. This process reduces the floatability of pyrite and achieves the selective depression of pyrite.

The chitin hydrogel draws great attention in biomedical fields owing to its high similarity and good affinity for peptides. The conversion of raw chitin to the designed hydrogel through a sol-gel process prevails, while the modulus of the chitin hydrogel is significantly influenced by the factors of gelation technology (i.e., coagulation, involving polymer chain rearrangement and the reconstruction of multiple interactions). Water and several organic solvents such as ethanol, DMAc, and DMSO are effective coagulants for aqueous chitin/KOH/urea solutions. In particular, the concentration of aqueous ethanol solutions displays a high dependency on the modulus of chitin hydrogels. However, recent reports about chitin hydrogel fabrication seldom demonstrate the effect of coagulant factors on hydrogel performance. Our study found that the polarity of the coagulant and its diffusion index for entry into the chitin solution during the coagulation process had a direct influence on the hydrogel modulus. The influence of the two factors was investigated to find out their quantified relationship with the hydrogel modulus, which will inspire a practical method to develop new coagulants to prepare modulus-manipulable chitin hydrogels.

Ionic liquids (ILs) have promising applications in pharmaceuticals and green chemistry, but their use is limited by toxicity concerns, mainly due to their interactions with cell membranes. This study examines the effects of imidazolium-based ILs on the microscopic structure and phase behavior of a model cell membrane composed of zwitterionic dipalmitoylphosphatidylcholine (DPPC) lipids. Small-angle neutron scattering and dynamic light scattering reveal that the shorter-chain IL, 1-hexyl-3-methylimidazolium bromide (HMIM[Br]), induces the aggregation of DPPC unilamellar vesicles. In contrast, this aggregation is absent with the longer alkyl chain IL, 1-decyl-3-methylimidazolium bromide (DMIM[Br]). Instead, DMIM[Br] incorporation leads to the formation of distinct IL-poor and IL-rich nanodomains within the DPPC membrane, as evidenced by X-ray reflectivity, differential scanning calorimetry, and molecular dynamics simulations. The less evident nanodomain formation with HMIM[Br] underscores the role of hydrophobic interactions between lipid alkyl tails and ILs. Our findings demonstrate that longer alkyl chains in ILs significantly enhance their propensity to form membrane nanodomains, which is closely linked to enhanced membrane permeability, as shown by dye leakage measurements. This heightened permeability likely underlies the greater cytotoxicity of longer-chain ILs. This crucial link between nanodomains and toxicity provides valuable insights for designing safer, more environmentally friendly ILs, and promoting their use in biomedical applications and sustainable industrial processes.

This study involves the preparation of the precursor of magnesium aluminum layered double hydroxide (MgAl-LDH) through a hydrothermal synthesis method. Subsequently, altering the loading amount of the precursor to synthesize a series of nanomaterials (MgAl-LDH@ZIF-8, = 0.2, 0.5, and 0.8) composite with zeolitic imidazolate framework-8 (ZIF-8). The investigation delves into the electrocatalytic performance of the material in the electrochemical reduction of CO (CORR) for the production of CO. The electrocatalyst is subjected to analysis through various techniques such as XRD, XPS, Raman, FTIR, SEM, EDS, TEM, BET, etc., to examine the elemental composition, microscopic morphology, and surface area with pore size. The electrochemical performance of the materials is tested and analyzed using an electrochemical workstation and gas chromatograph. The research findings reveal that the electrocatalyst with a loading amount of 0.5 g, denoted as 0.5MgAl-LDH@ZIF-8, exhibits a well-defined rhombic dodecahedral morphology with a surface-attached layered structure. This structure, characterized by relatively strong interactions, provides abundant active sites for the reaction, consequently demonstrating superior electrochemical performance. The Faradaic efficiency (CO FE) for CORR to produce CO reaches a maximum of 88.08% at -1.5 V vs. RHE. Maintaining a constant applied voltage at -1.4 V vs. RHE ensures stability for up to 4 h.

Coarsening is a very common phenomenon that has a crucial impact on the average grain size and properties of materials. However, our current understanding of coarsening is mainly based on the mean-field theories or ex situ observations, and the influence of transient process-related phenomena, such as grain rotation, inverse growth, etc., on coarsening was not considered. In this work, we simulated the coarsening process of supported nanograins by a phase-field crystal (PFC) model. Our simulations show that the inverse coarsening phenomenon might occur under the influence of the substrate, where small grains grow at the expense of the large ones. We found that the substrate-induced grain rotation has a significant effect on the appearance of inverse coarsening, and the average size growth velocity of inverse coarsening is far slower than that of normal coarsening. Furthermore, the influences of initial grain size, misorientations, pinning potential strength, and the lattice mismatch on the coarsening of biocrystal systems are discussed in detail.

With the large-scale applications of cryopreservation technology in the cell therapy fields, traditional permeable cryoprotectants (CPAs) have led to serious issues, such as cell cycle arrest, inhibition of cell proliferation and differentiation, apoptosis, altered gene expression, etc. Development of green, non-toxic cryoprotectants is critically needed. Amino acids could serve as substrates for protein and cellular metabolism and as cryoprotectants with non-toxicity, balancing the intracellular water osmotic pressure. Current research on amino acids as cryoprotectants is hindered by several limitations, including unclear protection mechanisms, cryopreservation methods, and poor efficacy of individual formulations. Therefore, three specific amino acids and derivatives, including l-proline, l-carnitine, and betaine, as cryoprotectants were used for two types of cell cryopreservation. Single-factor experiments were conducted to obtain the optimal concentration range for each of the three amino acid cryoprotectants. On the basis of the key thermophysical parameters, the ability to inhibit ice crystals, and the effect after cryopreservation, multivariate orthogonal experiments were carried out to evaluate the actual effect of the three-component mixed cryoprotectant on cell cryopreservation. In comparison to the gold standard of 10% dimethyl sulfoxide (DMSO) for cell cryopreservation, the mixed cryoprotectant derived from amino acids achieves comparable preservation efficacy at lower concentrations with a convenient application method, which offers guidance for DMSO-free cryoprotectants.

This work demonstrates the utility of microfluidic devices for characterizing diffusion mechanisms. We determined Henry's constant and characterized the diffusion process of gaseous CO in silicone oil. Using microfluidic techniques, we analyzed the evolution of the CO bubble size in a solvent flowing through a microchannel system. The reduction in bubble size due to the mass transfer of gaseous CO into the solvent fluid primarily affects their length. A microfluidic device was used to produce bubbles, consisting of a pressure-driven injection system for the gas and a flow-driven system for the liquid. Additionally, an optical device was coupled for tracking and studying the bubbles in the microchannels, enabling us to study their spatial and temporal evolution using image analysis. From this study, we found two diffusion regimes. The first is a superdiffusive process for short times. In this regime, due to the high concentration gradient values at the gas-liquid interface, we observed a higher rate of carbon dioxide transfer to the silicone oil. At longer times, we see that the gas transfer rate significantly decreases compared to the previous regime, leading to a subdiffusive process. In this latter regime, it was found that if we increase the gas pressure, the system approaches a normal diffusive process that coincides with previously conducted studies by other researchers. It is suggested that the subdiffusion could be due to the high degree of confinement of the bubbles within the microchannel, similar to what occurs in porous media, the high viscosity of the fluid, and the low gas pressure used in the tests. The microfluidic device proved to be a very efficient method for determining the diffusion process and Henry's constant in this case. Its easy fabrication and low cost make this type of device appropriate for substance characterization.

We report an instantaneous room-temperature phase separation of 1 mM bovine serum albumin solution in the presence of (20% acetic acid+0.2 M NaCl), a routinely used food preservative; an opaque liquid-like phase (L) coexists in equilibrium with a granular gel like phase (G). Interestingly, neither 20% acetic acid nor 0.2 M NaCl individually induces such a phase separation. Field emission scanning electron microscopy (FESEM) and high-resolution transmission electron microscopy (HRTEM) imaging show aggregated proteins to be dispersed in the upper phase, while the lower phase is composed of cross-linked fibrils (hydrogels). Mid-IR FTIR, Raman scattering, and circular dichroism (CD) experiments reveal a significant increase in the β-sheet content in BSA, which confirms the formation of amyloids in the presence of the excipient. Both L and G phases undergo distinct visual and microscopic changes upon incubation at 25 and 80 °C. It is evident that the added salt plays a pivotal role in bringing about this otherwise unique phase behavior. We divulge the explicit role of the ion associated hydration using THz-FTIR measurements in the 1.5-16.7 THz (50-550 cm) frequency window. Systematic alteration in the ion-induced THz-active mode of water envisions the key role of ions in shaping the various phases. Our study depicts an intriguing observation of severe amyloidosis of BSA upon the addition of a food preservative, even at room temperature, which is expected to add new insight into amyloid research. Considering the increasing number of individuals suffering from several neurodegenerative disorders (Alzheimer's, Parkinson's, type-2 diabetes, obesity, cancer, etc.), this study leads a caution toward critically revisiting the usage of known food preservatives.

In this study, various compositions of α-FeO, LiFeO, where = 0.1, 0.3, and 0.5, along with chitosan (CTS)-coated LiFeO nanomaterials (NMs), were synthesized using a sol-gel method. Rietveld refinement analysis indicated a predominance of the rhombohedral phase for lower Li-doped content ( = 0.1) and a transition to cubic crystal structures at higher Li-doped content ( = 0.3 and 0.5) within the host lattice. Field emission scanning electron microscopy (FE-SEM) images revealed irregular spherical morphologies, while transmission electron microscopy (TEM) images showed average particle sizes ranging from 19 to 40 nm across the various NMs. Superconducting quantum interference device (SQUID) analysis demonstrated a ferromagnetic nature with the highest saturation magnetization measured at 49.84 emu/g for LiFeO NMs. X-ray photoelectron spectra (XPS) exhibited Fe 2p and Fe 2p peaks at 712.60 and 726.13 eV, respectively, Li 1s at 57.58 eV, and O 1s at 533.44 eV for the representative samples; these characteristic XPS peaks shifted to a lower binding energy for CTS-coated LiFeO NMs. Hyperthermia studies demonstrated that the Li-doped samples reached a temperature range between 42 and 44 °C under an alternating current (AC) magnetic field applied at 167.6 to 335.2 Oe, with a constant frequency of 278 kHz. The specific absorption rate (SAR) was recorded as 265.11 W/g for LiFeO and 153.48 W/g for CTS-coated LiFeO NMs, both surpassing the SAR values of the other samples. Furthermore, various machine learning techniques were utilized to analyze how different synthesis conditions and material properties affected the heating efficiency and SAR values of the synthesized materials. The study also suggests an optimized set of guidelines and heuristics to enhance the heating performance and SAR values of these materials. Finally, magnetic CTS-coated LiFeO NMs exhibited a higher cell viability, as confirmed by MTT assays conducted on the NRK 52 E normal cell line.

The reasonable design of highly efficient NiFe-based bifunctional electrocatalysts is imperative for water splitting and alleviation of the energy crisis. Herein, the NiFe-based bifunctional electrocatalysts are designed and grown in situ on Ni foam by a simple hydrothermal method. The interfacial effect among NiFe-LDH, FeO(OH), and NiFeO exposes more catalytic active sites, modulated electronic structure, and optimization of the electrocatalytic performances. The overpotentials of NiFe-LDH/FeO(OH)/NiFeO/NF-15h (NFN/NF-15h) for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are 78 and 208 mV at 10 mA cm, respectively. Overall water splitting can drive 10 mA cm with a cell voltage of only 1.538 V. This work contributes a feasible idea for the design and synthesis of NiFe-based bifunctional electrocatalysts with outstanding water splitting performance.

Tetrabutylammonium bromide (TBAB) has been proven to improve the growth of hydrate via experimental methods, which may be attributed to its different concentrations. In this study, the molecular dynamics (MD) simulation is employed to investigate the concentration dependent promotion effect of TBAB on the growth of CO hydrate. The tetrahedral order parameter, number of cages, hydrate crystal growth trajectories, significant microconfigurations, and distribution of CO and TBAB are analyzed in detail. It is found that the promotion effect of TBAB is more prominent at low concentrations (5 and 10 wt %) than that at high concentrations (15 and 20 wt %). During the growth of hydrate crystal, tetrabutylammonium (TBA) ions adsorb on the hydrate crystal and serve as guest molecules to form TBA semiclathrate hydrate cages. Then, the TBA semiclathrate hydrate cages undergo a self-adjustment process and induce the generation of CO hydrate cages. At high concentrations, the great accumulation of TBA at the hydrate-liquid interface disturbs the effective adsorption and self-adjustment processes, and the tightly packed arrangement of TBA at the gas-liquid interface partially inhibits the mass transfer of CO. This study provides visible mechanisms of the concentration dependent promotion effect of TBAB from the microscopic level, which complements the vacancy in experimental studies.

The photocatalytic production of hydrogen using biopolymer-immobilized titanium dioxide (TiO) is an innovative and sustainable approach to renewable energy generation. TiO, a well-known photocatalyst, benefits from immobilization on biopolymers due to its environmental friendliness, abundance, and biodegradability. In another way, to boost the efficiency of TiO, its surface properties can be modified by incorporating co-catalysts like platinum (Pt) to improve charge separation. In this work, the surface of commercial TiO PC500 was modified with Pt nanoparticles (Pt1%@PC500) and then immobilized on glass surfaces using polyhydroxyalkanoate biopolymer poly(hydroxybutyrate--hydroxyhexanoate) (PHBH). The as-prepared immobilized Pt-modified TiO photocatalysts were fully characterized using various physicochemical techniques. The photocatalytic activity of the photocatalyst film was investigated for photocatalytic hydrogen production through water reduction using ethanol as a sacrificial donor. The impact of the film preparation conditions, e.g., PHBH concentration, PHBH:catalyst ratio, and temperature, on activity and stability was studied in detail. The application of biopolymer PHBH as a binder provides a green alternative to conventional immobilization methods, and with the application of PHBH, a stable and active photocatalyst film that showed lower activity compared to that of the suspended photocatalyst but good recyclability in six runs was prepared. A long-term photocatalytic hydrogen production experiment was carried out. In 98 h of operation, 12 mmol of hydrogen was produced in three consecutive runs with a PHBH/Pt1%@PC500 film having an area of ∼5.3 cm. A significantly lower hydrogen productivity was observed after the first run, possibly due to a change in film structure, but thereafter, the productivity remained almost constant for the second and third runs. Hydrogen was the main product in the gas phase (90%), but carbon dioxide (4-5%) and methane (4-5%) were obtained as important byproducts. The byproducts are a consequence of the use of the sacrificial reagent ethanol. The results of the film performance are very promising, with regard to large-scale continuous hydrogen production.

Water-soluble poly(vinyl alcohol) (PVA) has great potential for the preparation of environmentally friendly adhesives. However, the application of PVA adhesives in the wood industry has been limited by their poor water and mildew resistance. Herein, a polyester-type PVA adhesive (CPVA) with good bonding performance, water resistance, and antimildew performance was synthesized using PVA and citric acid (CA). The cross-linking reaction, including esterification between PVA and CA chains and etherification between PVA chains, was demonstrated by Fourier-transform infrared (FTIR) and X-ray photoelectron spectroscopy (XPS). Due to the cross-linked structure of the reaction, the CPVA1 (mass ratio of CA/PVA = 1:1) adhesive showed a low soluble content of 5% when it was soaked in water for 24 h. The dry strength, warm water (63 °C) strength, and hot water (93 °C) strength of the plywood hot-pressed from the CPVA1 adhesive at 200 °C were 1.06 1.52, and 1.45 MPa, respectively, which met the Chinese National Standard GB/T 9846-2015. The developed CPVA adhesive also adhered to glass and steel at room temperature. Therefore, the CPVA adhesive developed in this study can serve as a potential candidate for the production of nonformaldehyde wood-based composites with excellent bonding strength, water resistance, and mildew resistance.

The adhesion of tissues to external devices is fundamental to numerous critical applications in biomedical engineering, including tissue and organ repair, bioelectronic interfaces, adhesive robotics, wearable electronics, biomedical sensing and actuation, as well as medical monitoring, treatment, and healthcare. A key challenge in this context is that tissues are typically situated in aqueous and dynamic environments, which poses a bottleneck to further advancements in these fields. Wet adhesion technology (WAT) presents an effective solution to this issue. In this review, we summarize the three major design strategies and control methods of wet adhesion, comprehensively and systematically introducing the latest applications and advancements of WAT in the field of biomedical engineering. First, single adhesion mechanism under the frameworks of the three design strategies is systematically introduced. Second, control methods for adhesion are comprehensively summarized, including spatiotemporal control, detachment control, and reversible adhesion control. Third, a systematic summary and discussion of the latest applications of WAT in biomedical engineering research and education were presented, with a particular focus on innovative applications such as tissue-electronic interface devices, ingestible devices, end-effector components, in vivo medical microrobots, and medical instruments and equipment. Finally, opportunities and challenges encountered in the design and development of wet adhesives with advanced adhesive performance and application prospects are discussed.

Zwitterionic materials, known for their high hydrophilicity, are widely used to minimize the nonspecific adsorption of biomolecules in complex biological solutions. However, these materials can also reduce the capture efficiency between targets and peptide probes. To demonstrate how antifouling surfaces affect capture efficiency, we utilize a poly(3,4-ethylenedioxythiophene) (PEDOT)-based surface incorporating varying ratios of phosphorylcholine (PEDOT-PC) and maleimide functional groups to achieve both antifouling properties and peptide-protein binding. As a model system, the peptide YWDKIKDFIGGSSSSC, attached via maleimide groups, is used to capture the target protein, calmodulin (CaM). By systematically monitoring protein binding on both antifouling and peptide-immobilized PEDOT surfaces using a quartz crystal microbalance with dissipation, the results reveal that PEDOT-PC reduces both the specific binding between peptides and target proteins as well as the rate of protein fouling on the electrode surface. From these findings, we propose an equation for quantitative analysis. Furthermore, electrochemical impedance spectroscopy and differential pulse voltammetry are performed to measure the changes in the impedance in CaM solutions. The data indicate that impedance increases with protein adsorption, confirming the practical utility of the designed electrode surface.

This work explores the adsorption and permeation of chemical warfare agents on polymer coatings to assess their protective potential. Two highly cross-linked aliphatic polyurethanes (PUs) were synthesized from two diisocyanate trimers, and their adsorption and permeation of dimethyl methylphosphonate (DMMP) and 2-chloroethyl ethyl sulfide (CEES) were analyzed using quartz crystal microbalance with dissipation and gas chromatography. The study revealed distinct adsorption properties for each agent and the PU. CEES, with higher polarity, exhibited greater readsorption compared to DMMP. IPtri-PU (alicyclic structure) showed negligible desorption and resorption, resulting in minimal permeation, unlike Htri-PU (aliphatic structure). Thus, alicyclic PUs are more promising for reducing adsorption and permeation.

We have studied the interfacial properties of Zn vs selected transition metal cations such as Fe, Cu, and Cr in a water-ethanol mixture using field-induced droplet ionization. This was in particular inspired by the specific surface activity of Zn that has been observed on several occasions and a desire to clarify the root cause for this behavior. We have found that Zn, due to its unique electronic configuration and atomic size, is the only ion of those under study that gives rise to specific speciation at the air-liquid interface with three ethanol molecules attached to the central atom for optimal polarity.

Silicone sealants and adhesives are extensively used in construction, automotive, industrial, and electronic applications because they exhibit excellent mechanical properties, strong adhesion, and good weather resistance. Room-temperature vulcanized (RTV) silicones develop good adhesion to many substrates and do not require heat for curing, which leads to flexible use in many applications. Although it is known that various factors such as relative humidity and temperature affect the curing of the RTV silicone adhesives, the interfacial chemistry that occurs during the curing process is still poorly understood but critical for success in adhesive applications. To address this, sum frequency generation (SFG) vibrational spectroscopy was used to probe the molecular details of the buried interface of the RTV silicone adhesive in situ. Time-dependent SFG experiments were conducted on two polydimethylsiloxane (PDMS) matrices, at three humidity levels, and with two kinds of silica surfaces to investigate the behavior of the methoxy groups at the interface and the impact of environmental conditions on the adhesion mechanism. It was found that both the methoxy groups from methyltrimethoxysilane (MTMS) and methoxy-terminated PDMS could segregate to the interface. The diffusion of MTMS and bulk rearrangement of methoxy-terminated PDMS lead to the segregation and ordering of methoxy groups at the interface. After comparing eight samples cured under different environmental conditions, the reactions of the interfacial methoxy groups were found to be facilitated by both the surface water on silica and moisture from the environment. The silylation treatment on the silica slows the reactions of the interfacial methoxy groups, while the high environmental humidity accelerates the consumption of the interfacial methoxy groups. These findings provide insightful information about the adhesion mechanism of RTV silicone adhesives and accelerate new product development.