Reversible Ni exsolution for syngas production via self-regeneration without additional hydrogen: From mechanism to economic/environmental viability

Dry reforming of methane (DRM) is hindered by catalyst deactivation and the high costs of conventional hydrogen-reduction-based regeneration. In this study, we propose a novel Ni-substituted SrTiO 3 (STN) catalyst system enabling full activity recovery via a simplified self-regeneration without the need for additional H 2 reduction DRM (SR-DRM) scenario. This study employs a multidisciplinary approach to bridge atomic-level catalyst dynamics and industrial-scale sustainability through a multi-scale evaluation. At the atomic scale, spectroscopic analysis and CO 2 pulse tests reveal a structural memory effect where lattice-confined Ni 3+ and high oxygen mobility drive reversible Ni exsolution and self-regeneration. This microscopic resilience facilitates process-level innovation by eliminating external hydrogen and minimizing downtime. To evaluate systemic impact, techno-economic and life-cycle assessments (TEA/LCA) were integrated. Based on the scenario-based process simulation under identical operating conditions, SR-DRM showed an additional 328.4 ton/year of syngas production (1.9% increase) and approximately 22.19 ton H 2 /year of hydrogen savings (2.0% increase) under identical operating conditions, together with 6.2% reduction of levelized cost of hydrogen and a 18.6% reduction in global warming potential. The economic and environmental benefits are mainly caused by SR-DRM operation. By reconciling fundamental materials science with rigorous process evaluation, this framework demonstrates how atomic-scale lattice design dictates macroscopic economic and environmental viability, offering a new paradigm for sustainable carbon capture and utilization.