Guo Xiao-Tong, Zhang Juan, Chi Jian-Chao, Li Zhi-Hui, Liu Yu-Chen, Liu Xin-Ru, Zhang Shu-Yong
School of Chemistry and Chemical Engineering, Shandong University Jinan 250100 P. R. China
RSC Adv. 2019 Feb 18;9(11):5995-6002. doi: 10.1039/c8ra09534e.
A series of AuPd/C catalysts were prepared and tested for the first time for active and stable dehydrogenation of a formic acid-ammonium formate (FA-AF) mixture. The catalysts with different Au-to-Pd molar ratios were prepared using a facile simultaneous reduction method and characterized using transmission electron microscopy (TEM), high-resolution TEM, energy dispersive X-ray spectroscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. It was found that the catalytic activity and stability of the AuPd/C catalyst was the best. The initial turnover frequency for the dehydrogenation of the FA-AF mixture over the AuPd/C catalyst can reach 407.5 h at 365 K. The reaction order with respect to FA and AF is 0.25 and 0.55, respectively. The apparent activation energy of dehydrogenation is 23.3 ± 1.3 kJ mol. The catalytic activity of the AuPd/C catalyst remains 88.0% after 4 runs, which is much better than the single Pd/C catalyst. The mechanism for the dehydrogenation is also discussed.
首次制备并测试了一系列用于甲酸 - 甲酸铵（FA - AF）混合物活性和稳定脱氢反应的AuPd/C催化剂。采用简便的同步还原法制备了不同金钯摩尔比的催化剂，并通过透射电子显微镜（TEM）、高分辨率TEM、能量色散X射线光谱、X射线衍射和X射线光电子能谱对其进行了表征。结果发现，AuPd/C催化剂的催化活性和稳定性最佳。在365 K下，AuPd/C催化剂上FA - AF混合物脱氢反应的初始周转频率可达407.5 h⁻¹。FA和AF的反应级数分别为0.25和0.55。脱氢反应的表观活化能为23.3±1.3 kJ mol⁻¹。经过4次循环后，AuPd/C催化剂的催化活性仍保持88.0%，远优于单一的Pd/C催化剂。同时还讨论了脱氢反应的机理。
