This study investigates the use of fly ash to mitigate the long-term performance degradation of Portland cement-based sealing materials in high-salinity environments, such as those found in gas storage reservoirs. We systematically evaluated the evolution of material properties under different temperatures and curing periods. Our integrated methodology combining mechanical tests, microstructural analysis, and chloride migration assessment, reveals a multi-faceted mechanism by which fly ash enhances chloride resistance. The key findings demonstrate that reactive Al₂O₃ in fly ash promotes the formation of Friedel’s salt, increasing chemical chloride binding and reducing the chloride ingress rate in the Portland cement–Fly ash system (PFS) to only 26.6% of that in the Portland Cement system (PCS). Concurrently, the pozzolanic reaction consumes portlandite (Ca(OH)₂), forming stable C-A-S-H gel and refining the pore structure by filling interconnected channels. This nanoscale pore refinement decreased permeability by nearly an order of magnitude. After 90 days of curing in 90 °C saline solution, PFS achieved a compressive strength of 28.2 MPa and maintained an exceptionally low internal chloride content of 0.08 wt.%, demonstrating superior long-term durability. This work clarifies the synergistic mechanisms of fly ash modification and temperature effects, providing a theoretical basis for optimizing sealing materials for deep geological reservoirs and experimental support for the application of fly ash in high-temperature, high-salinity engineering environments.

This study investigates the protective performance of a triazole-based Mannich base corrosion inhibitor, 4-((1,2,4-triazolyl)methyl) dibutylamine (TZMBA), on P110 carbon steel in dissolved oxygen environments. TZMBA was synthesized via a Mannich reaction, and its molecular structure was confirmed by Fourier transform infrared spectroscopy (FT-IR). The corrosion inhibition behavior and underlying mechanisms were systematically explored through weight loss measurements, surface characterization, and multiscale molecular simulations. Weight loss results indicated that TZMBA significantly mitigates the corrosion of P110 steel, with inhibition efficiency reaching 81.5% at 1.67 mmol/L and 82.0% at 2.14 mmol/L. Adsorption thermodynamic analysis revealed that the process follows the Langmuir isotherm model. The calculated standard Gibbs free energy ${∆G}_{ads}^0$ of −38.69 kJ/mol suggests a spontaneous, mixed-type adsorption mechanism involving both physisorption and chemisorption. Scanning electron microscopy (SEM) observations confirmed a marked reduction in surface degradation, characterized by suppressed corrosion products and minimized localized attack. X-ray photoelectron spectroscopy (XPS) further verified that TZMBA anchors to the metal surface through chemical coordination, forming a robust organic-inorganic composite film. From a theoretical perspective, frontier molecular orbital (FMO) analysis showed that TZMBA’s high E_HOMO and narrow energy gap facilitate efficient electron transfer. Combined Fukui function and molecular electrostatic potential (MEP) maps identified the nitrogen atoms in the triazole ring and amine group as the primary active sites. Furthermore, molecular dynamics (MD) simulations demonstrated that TZMBA molecules adopt a nearly parallel configuration on the Fe surface. The high negative interaction energy obtained from MD simulations confirms a strong binding affinity and a potent inherent driving force for the formation of a stable protective layer. Overall, the integration of experimental data and theoretical calculations establishes TZMBA as an effective inhibitor that provides superior protection by forming a stable, compact adsorption film on P110 carbon steel.