• Holistic “gas-catalytic reactor” strategy enables efficient photothermal rWGS. • 2D Pt-TiO 2 nanosheets broaden solar absorption via strong LSPR effect. • Hot-electron injection lowers activation energy from 24.0 to 20.0 kJ/mol. • 8.94 mmol g -1 h −1 CO rate with ∼ 100% selectivity at 350 °C. • Continuous gas-lift reactor triples space–time yield in comparison with batch systems. Integrating atomic-level catalyst design with macroscopic reactor engineering is pivotal for sustainable solar-to-fuel conversion. This study presents a comprehensive photothermal strategy for the reverse water-gas shift (rWGS) reaction utilizing 2D TiO 2 nanosheets decorated with Pt nanoparticles. By leveraging the Localized Surface Plasmon Resonance (LSPR) effect, the Pt-TiO 2 system extends solar absorption into the near-infrared region, achieving a CO production rate of 8.94 mmol/(g h) at a moderate bulk temperature of 350 °C. Kinetic analysis reveals a significant reduction in the apparent activation energy from 24.0 to 20.0 kJ/mol, providing the quantitative evidence of a non-thermal “kinetic overdrive” induced by hot-electron injection. While thermodynamic equilibrium predicts a parasitic methanation floor at 99%), demonstrating a remarkable improvement from thermal equilibrium limits. To bridge the endothermic enthalpy gap, a continuous gas-lift reactor featuring a spectrally selective Ti-Cr-Al coating was developed, delivering a threefold enhancement in space–time yield compared to traditional batch configurations. This work highlights the synergy between plasmonic kinetic steering and spectral-selective thermal management, providing a scalable and energy-efficient framework for the valorization of anthropogenic CO 2 .
Deng et al. (Sun,) studied this question.