Lu Minglei, Zheng Zhuoyu, Lu Weiwei, Zhu Haiping, Liao Junwei, Ge Yuxin, Huang Xueer, Zhang Qian, Li Jiajin, Zhou Yiyuan, Wu Xiaoping, Chen Baozhu, Yang Chunxiao, Qian Xitang, Shao Minhua, Wang Tiejun
School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou, Guangdong 510006, China.
Guangdong Provincial Key Laboratory of Plant Resources Biorefinery, Guangzhou, Guangdong 510006, China.
ACS Nano. 2024 Sep 17;18(37):25636-25646. doi: 10.1021/acsnano.4c07386. Epub 2024 Sep 5.
Aqueous-phase reforming of methanol represents a promising avenue for hydrogen (H) production. However, developing highly efficient and low-cost nonprecious catalysts remains challenging. Here, we report the synthesis of Cu-based catalysts with Cu, CuO, and CuN nanoparticles anchored on the nitrogen-doped carbon, forming Cu/Cu/Cu-N active sites. This catalyst achieves a H production rate of 140.1 μmol/g/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 site facilitates water dissociation into *OH and improves *CO and *OH conversion, leading to enhanced CO conversion and H production kinetics.
甲醇的水相重整是一种很有前景的制氢途径。然而，开发高效且低成本的非贵金属催化剂仍然具有挑战性。在此，我们报道了一种铜基催化剂的合成方法，该催化剂由锚定在氮掺杂碳上的铜、氧化铜和铜纳米颗粒组成，形成了Cu/Cu/Cu-N活性位点。这种催化剂在210℃时的产氢速率达到140.1μmol/g/s，比铜基、镍基甚至铂基催化剂高出几倍至两个数量级，在210℃下350小时内表现出优异的长期稳定性。机理研究表明，Cu-N位点促进水分解为OH，并提高CO和*OH的转化率，从而增强了CO转化率和产氢动力学。
