摘要
Catalytic decomposition of NH3 to high purity hydrogen offers a promising strategy for fuel cells,but presents challenges for high hydrogen yields at comparatively low temperatures due to the lack of efficient catalysts.Here,we report the facile preparation of ultra-fine ruthenium(Ru)species dispersed on MgO,which show excellent activity and high temperature stability for NH3 decomposition reaction.The hydrogen yield of the prepared Ru/MgO catalysts reaches ca.2,092 mmol H2 gRu^-1 min^-1 at 450℃,far exceeding that of the previously reported most reactive Ru・based catalysts and the same chemical composition samples prepared by other approaches.Various characterization techniques containing X-ray absorption fine structure(XAFS),in-situ diffuse reflectance infrared Fourier transform spectroscopy(in-situ DRTFTS)and temperature-programmed reduction/desorption(TPR/TPD)were carried out to explore the structure-function relation of the prepared Ru/MgO catalysts.We found that the Ru species interact strongly with the MgO support,which can efficiently protect the Ru species and MgO support from agglomerating during NH3 decomposition test,maintaining the stability of the catalysts.
Catalytic decomposition of NH3 to high purity hydrogen offers a promising strategy for fuel cells, but presents challenges for high hydrogen yields at comparatively low temperatures due to the lack of efficient catalysts. Here, we report the facile preparation of ultra-fine ruthenium(Ru) species dispersed on Mg O, which show excellent activity and high temperature stability for NH3 decomposition reaction. The hydrogen yield of the prepared Ru/Mg O catalysts reaches ca. 2,092 mmol H2 g–1 Ru min–1 at450 °C, far exceeding that of the previously reported most reactive Ru-based catalysts and the same chemical composition samples prepared by other approaches. Various characterization techniques containing X-ray absorption fine structure(XAFS),in-situ diffuse reflectance infrared Fourier transform spectroscopy(in-situ DRTFTS) and temperature-programmed reduction/desorption(TPR/TPD) were carried out to explore the structure-function relation of the prepared Ru/Mg O catalysts. We found that the Ru species interact strongly with the Mg O support, which can efficiently protect the Ru species and Mg O support from agglomerating during NH3 decomposition test, maintaining the stability of the catalysts.
基金
supported by the Excellent Young Scientists Fund from National Natural Science Foundation of China (21622106)
other projects from the National Natural Science Foundation of China (21773288, 21805167, 11574281, 21771117)
the Outstanding Scholar Fund (JQ201703)
the Doctoral Fund (ZR2018BB010)
the Science Foundation of Shandong Province of China
the Taishan Scholar Project of Shandong Province of China
the National Key Basic Research Program of China (2017YFA0403402)
the Future Program for Young Scholar of Shandong University