Stable Cu/Cu2O/CuN3@NC Catalysts for Aqueous Phase Reforming of Methanol

Minglei Lu; Zhuoyu Zheng; Weiwei Lu; Haiping Zhu; Junwei Liao; Yuxin Ge; Xueer Huang; Qian Zhang; Jiajin Li; Yiyuan Zhou; Xiaoping Wu; Baozhu Chen; Chunxiao Yang; Xitang Qian; Minhua Shao; Tiejun Wang

doi:10.1021/acsnano.4c07386

Stable Cu/Cu₂O/CuN₃@NC Catalysts for Aqueous Phase Reforming of Methanol

ACS Nano. 2024 Sep 17;18(37):25636-25646. doi: 10.1021/acsnano.4c07386. Epub 2024 Sep 5.

Authors

Minglei Lu^{1

2

3}, Zhuoyu Zheng^{1

2}, Weiwei Lu^{1

2}, Haiping Zhu^{1

2}, Junwei Liao^{1

2}, Yuxin Ge^{1

2}, Xueer Huang^{1

2}, Qian Zhang^{1

2}, Jiajin Li^{1

2}, Yiyuan Zhou^{1

2}, Xiaoping Wu^{1

2}, Baozhu Chen^{1

2}, Chunxiao Yang⁴, Xitang Qian³, Minhua Shao^{3

5

6

7}, Tiejun Wang^{1

2}

Affiliations

¹ School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou, Guangdong 510006, China.
² Guangdong Provincial Key Laboratory of Plant Resources Biorefinery, Guangzhou, Guangdong 510006, China.
³ Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong 999077, China.
⁴ School of Analysis and Test Center, Guangdong University of Technology, Guangzhou 510006, China.
⁵ CIAC-HKUST Joint Laboratory for Hydrogen Energy, The Hong Kong University of Science and Technology, Clear Watery Bay, Kowloon, Hong Kong 999077, China.
⁶ Guangzhou Key Laboratory of Electrochemical Energy Storage Technologies, Fok Ying Tung Research Institute, The Hong Kong University of Science and Technology, Guangzhou 511458, China.
⁷ Energy Institute, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong 999077, China.

PMID: 39235312
DOI: 10.1021/acsnano.4c07386

Abstract

Aqueous-phase reforming of methanol represents a promising avenue for hydrogen (H₂) production. However, developing highly efficient and low-cost nonprecious catalysts remains challenging. Here, we report the synthesis of Cu-based catalysts with Cu, Cu₂O, and CuN₃ nanoparticles anchored on the nitrogen-doped carbon, forming Cu⁰/Cu⁺/Cu-N₃ active sites. This catalyst achieves a H₂ production rate of 140.1 μmol/g_cat/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-N₃ site facilitates water dissociation into *OH and improves *CO and *OH conversion, leading to enhanced CO conversion and H₂ production kinetics.

Keywords: Cu-based catalysts; H2 production; Nonprecious metal; hydrothermal stability; methanol reforming.