Photothermal Dry Reforming of Methane Over Supported Bimetal Dual-Atom Pairs
Bin Liu, Bin Liu, Yuan Wang, Xiaonan Hu, Jiang Deng, Zhenyuan Teng, Wenqiang Qu, Zhenggang Xue, Haiyan Duan, Lupeng Han, Yongjie Shen, Jun Liu, Bin Liu, B. H. LIU, Dengsong Zhang
Abstract
Dry reforming of methane (DRM, CH 4 + CO 2 → 2H 2 + 2CO) offers a promising route for converting two greenhouse gases into valuable syngas. However, conventional thermal catalysis requires extreme temperatures (>800 °C) to overcome high energy barrier, leading to significant energy consumption and catalyst deactivation. Herein, we develop a Pt 1 –Ni 1 /CeO 2 photothermal catalyst with atomically dispersed Pt 1 –Ni 1 paired active sites for DRM under mild conditions. At 450 °C under light illumination, the catalyst exhibits high H 2 and CO production rates of 4.62 and 4.65 mmol g catalyst –1 min –1, respectively, with a H 2 /CO ratio close to unity (0.99). Mechanistic investigations reveal that light irradiation induces photogeneration of electrons and holes in CeO 2, which directionally transfer to atomic Ni and Pt sites, respectively, inducing asymmetric charge polarization that promotes the activation of reactants. Steady-state isotope transient kinetic analysis combined with diffuse reflectance infrared Fourier transform spectroscopy (SSITKA-DRIFTS) measurement identifies the critical *CH x O intermediate formed via *CH x + *O → *CH x O, a key step that suppresses deep dehydrogenation and carbon deposition. This work elucidates the regulation of parallel reactions over asymmetric dual-atom pairs in the transformation of CH 4 + CO 2 via photothermal synergy, paving the way for the targeted conversion of C1 molecules under mild conditions.