ABSTRACT Ultra‐deep heavy oil is an important unconventional resource, but its extremely high viscosity, poor mobility, and the high energy demand for conventional recovery methods severely limit its efficient and sustainable production. To address these limitations, a triflate‐functionalized Ni–Ce/MOF superacid catalyst (Ni–Ce/MOF–OTf), based on a UiO‐66(Ce)–type (BTC‐based) framework, was developed to enable low‐temperature in situ upgrading under near‐reservoir conditions. The catalyst was synthesized through a two‐step post‐synthetic modification route using a Ni–Ce/MOF precursor, involving acid activation followed by grafting of triflate groups onto the framework. This design was intended to integrate strong Brønsted acidity, tunable Ni/Ce Lewis acid sites, and pore confinement within a single catalytic microenvironment, thereby promoting selective bond cleavage and suppressing secondary repolymerization. Under reservoir‐mimicking conditions (∼140°C), Ni–Ce/MOF–OTf achieved a viscosity reduction of 92.11% within 12 h, maintained viscosity rebound below 10% over 60 days, and retained about 80% of its activity after four cycles. Structural characterization and theoretical calculations showed that triflate functionalization enhanced acidity, increased oxygen vacancy density, and strengthened metal–ligand interactions, enabling efficient cleavage of C–C/‐C–C, C–S, and C–O bonds at a lower temperature. Core‐scale physical simulation further demonstrated a recovery factor of 90.25% through gas‐assisted catalytic upgrading. In addition, techno‐economic and cradle‐to‐wellhead assessments indicated improved economic competitiveness and the lowest cradle‐to‐wellhead carbon footprint among the evaluated heavy oil recovery routes. These results demonstrate an effective materials–reaction–engineering strategy for cleaner and more sustainable utilization of ultra‐deep heavy oil.
Wang et al. (Sat,) studied this question.