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原子层沉积技术沉积的FeOx包裹层显著提高Pd/C催化剂在甲酸分解放氢反应中的催化活性
李俊杰,路军岭*
作者单位E-mail
李俊杰 中国科学技术大学化学物理系, 合肥微尺度国家科学实验室, 能源材料化学协同创新中心, 中国科学院能量转换材料重点实验室, 合肥 230026  
路军岭* 中国科学技术大学化学物理系, 合肥微尺度国家科学实验室, 能源材料化学协同创新中心, 中国科学院能量转换材料重点实验室, 合肥 230026 junling@ustc.edu.cn 
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DOI:10.1063/1674-0068/30/cjcp1703032
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基金项目:This work was supported by the National Natural Science Foundation of China (No.51402283 and No.21473169),One Thousand Young Talents Program under the Recruitment Program of Global Experts,the Fundamental Research Funds for the Central Universities (No.WK2060030017),and the Startup Funds from University of Science and Technology of China.
FeOx Coating on Pd/C Catalyst by Atomic Layer Deposition Enhances the Catalytic Activity in Dehydrogenation of Formic Acid
Jun-jie Li,Jun-ling Lu*
Abstract:
Hydrogen generation from formic acid (FA) has received significant attention.The challenge is to obtain a highly active catalyst under mild conditions for practical applications.Here atomic layer deposition (ALD) of FeOx was performed to deposit an ultrathin oxide coating layer to a Pd/C catalyst,therein the FeOx coverage was precisely controlled by ALD cycles.Transmission electron microscopy and powder X-ray diffraction measurements suggest that the FeOx coating layer improved the thermal stability of Pd nanoparticles (NPs).X-ray photoelectron spectroscopy measurement showed that deposition of FeOx on the Pd NPs caused a positive shift of Pd3d binding energy.In the FA dehydrogenation reaction,the ultrathin FeOx layer on the Pd/C could considerably improve the catalytic activity,and Pd/C coated with 8 cycles of FeOx showed an optimized activity with turnover frequency being about 2 times higher than the uncoated one.The improved activities were in a volcanoshape as a function of the number of FeOx ALD cycles,indicating the coverage of FeOx is critical for the optimized activity.In summary,simultaneous improvements of activity and thermal stability of Pd/C catalyst by ultra-thin FeOx overlayer suggest to be an effective way to design active catalysts for the FA dehydrogenation reaction.
Key words:  Formic acid  Hydrogen generation  Atomic layer deposition  FeOx coating  Pd catalyst