Journal of Catalysis ( IF 6.5 ) Pub Date : 2024-01-23 , DOI: 10.1016/j.jcat.2024.115316 Jianxian Li , Wenting Lin , Minglei Lu , Junwei Liao , Changsong Hu , Tiejun Wang
Efficient release of H2 with negligible CO impurities from sustainable MeOH/H2O has become a promising goal for on-board hydrogen generator. However, hydrogen release kinetics still face challenges. In this work, the Cu/ZnO/CeO2 catalyst with high density ultra-small Cu nanoparticles and abundant oxygen vacancies were prepared for intensifying hydrogen evolution in aqueous phase reforming of methanol (APRM). The optimized 55% Cu/ZnO/CeO2 catalyst (Cu NPs of 3.8 nm, Cu loading of 55.89 wt%, oxygen vacancies of 2.316 × 1015 spins g−1) exhibited an excellent H2 evolution rate of 58.39 μmolgcat−1 s−1 even at low temperature of 210 °C, which was 2.1-fold enhancement than that of commercial Cu/ZnO/Al2O3 catalyst. Characterizations and experiments revealed that ZnO/CeO2 intensified the strong metal-support interaction (SMSI), which anchored the Cu NPs, generated abundant oxygen vacancies and adjusted electronic structure to form Cu0-Cu+-Ov active sites for facilitating the kinetics of APRM.
中文翻译:
高密度超小铜纳米粒子,具有丰富的氧空位,可从 MeOH/H2O 中高效析氢
从可持续的MeOH/H 2 O中高效释放H 2且CO杂质可忽略不计已成为机载氢气发生器的一个有前景的目标。然而,氢释放动力学仍然面临挑战。本工作制备了具有高密度超小Cu纳米粒子和丰富氧空位的Cu/ZnO/CeO 2催化剂,用于强化甲醇水相重整(APRM)中的析氢。优化的55% Cu/ZnO/CeO 2催化剂(Cu NPs为3.8 nm,Cu负载量为55.89 wt%,氧空位为2.316 × 10 15 spins g -1)表现出优异的H 2析出速率,为58.39 μmolg cat -1即使在210℃的低温下也能实现 s -1 ,这比商业Cu/ZnO/Al 2 O 3催化剂提高了2.1倍。表征和实验表明,ZnO/CeO 2增强了强金属-载体相互作用(SMSI),锚定了Cu NPs,产生丰富的氧空位并调整电子结构,形成Cu 0 -Cu + -O v活性位点,以促进动力学的APRM。