Lost circulation in oil-based drilling fluids (OBDFs) remains difficult to mitigate because particulate lost circulation materials depend on bridging/packing and gel systems for aqueous media often lack OBDF compatibility and controllable in situ sealing. A dual-precursor oil–water biphasic metal–organic supramolecular gel enables rapid in situ sealing in OBDF loss zones. The optimized formulation uses an oil-phase to aqueous gelling-solution volume ratio of 10:3, with 2.0 wt% Span 85, 12.5 wt% TXP-4, and 5.0 wt% NaAlO₂. Apparent-viscosity measurements and ATR–FTIR analysis were used to evaluate the effects of temperature, time, pH, and shear on MOSG gelation. Furthermore, the structural characteristics and performances of MOSGs were systematically investigated by combining microstructural characterization, thermogravimetric analysis, rheological tests, simulated fracture-plugging experiments, and anti-shear evaluations. The results indicate that elevated temperatures (30–70 °C) and mildly alkaline conditions in the aqueous gelling solution (pH ≈ 8.10–8.30) promote P–O–Al coordination and strengthen hydrogen bonding, thereby facilitating the formation of a three-dimensional network. In contrast, strong shear disrupts the nascent network and delays gelation. The optimized MOSGs rapidly exhibit pronounced viscoelasticity and thermal resistance (~193 °C); under high shear (380 rpm), the viscosity retention exceeds 60% and the viscosity recovery exceeds 70%. In plugging tests, MOSG forms a dense sealing layer, achieving a pressure-bearing gradient of 2.27 MPa/m in simulated permeable formations and markedly improving the fracture pressure-bearing capacity in simulated fractured formations.

This study focuses on hierarchical structure regulation and mechanical property enhancement in electrocatalytic composite materials, systematically elucidating strategies for achieving “structure-function-mechanics” synergistic optimization through multi-scale structural design. By integrating theoretical models with controllable synthesis methods, the research constructs composite systems featuring multi-level pores and interlocked networks. Multi-mode characterization techniques reveal the intrinsic mechanisms by which hierarchical structures improve electrocatalytic activity, mass transfer efficiency, and mechanical strength. Experimental results demonstrate that the optimized hierarchical composite materials maintain high specific surface area and abundant active interfaces while significantly enhancing fracture toughness, fatigue resistance, and long-term operational stability. These findings provide crucial theoretical and technical references for designing electrode materials for high-performance, long-life energy storage devices.