Stable Cu/Cu<sub>2</sub>O/CuN<sub>3</sub>@NC Catalysts for Aqueous Phase Reforming of Methanol.

Lu, Minglei; Zheng, Zhuoyu; Lu, Weiwei; Zhu, Haiping; Liao, Junwei; Ge, Yuxin; Huang, Xueer; Zhang, Qian et al. · ACS Nano · 2024

basic_science · Level V

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Abstract

Aqueous-phase reforming of methanol represents a promising avenue for hydrogen (H<sub>2</sub>) production. However, developing highly efficient and low-cost nonprecious catalysts remains challenging. Here, we report the synthesis of Cu-based catalysts with Cu, Cu<sub>2</sub>O, and CuN<sub>3</sub> nanoparticles anchored on the nitrogen-doped carbon, forming Cu<sup>0</sup>/Cu<sup>+</sup>/Cu-N<sub>3</sub> active sites. This catalyst achieves a H<sub>2</sub> production rate of 140.1 μmol/g<sub>cat</sub>/s at 210 °C, which is several times to 2 orders of magnitude higher than that of Cu-, Ni-, even Pt-based catalysts, demonstrating excellent long-term stability over 350 h at 210 °C. A mechanism investigation reveals that the Cu-N<sub>3</sub> site facilitates water dissociation into *OH and improves *CO and *OH conversion, leading to enhanced CO conversion and H<sub>2</sub> production kinetics.