脱氢
纳米材料基催化剂
甲酸
柠檬酸
催化作用
氢
制氢
材料科学
氮化物
纳米颗粒
X射线光电子能谱
无机化学
贵金属
化学工程
金属
氢燃料
化学
透射电子显微镜
硝酸
粒子(生态学)
选择性
作者
Hongli Wang (172969),Zelong Wang (8905355),Xue Liu (420033),Nan Gao (196665),Xiaolei Song (551850),Zhankui Zhao (14671728)
出处
期刊:University of Illinois at Chicago - INDIGO
[University of Illinois Chicago]
日期:2023-02-23
标识
DOI:10.1021/acsanm.2c05062.s001
摘要
Formic\nacid (FA) dehydrogenation is a potential technology for\nsustainable hydrogen production, while the tardy nature of FA dehydrogenation\ninhibits its development. To optimize the catalytic activity of hydrogen\ngeneration from formic acid dehydrogenation, citric acid-modified\nboron nitride with abundant −NH<sub>2</sub> (CA–BN-NH<sub>2</sub>) is employed as a support to control the particle distribution,\nparticle size, and electronic structure of AuPd nanoparticles. The\nobtained Au<sub>0.3</sub>Pd<sub>0.7</sub>/CA–BN-NH<sub>2</sub> exhibits extraordinary catalytic activity for hydrogen production\nfrom FA dehydrogenation, possessing 100% hydrogen selectivity and\nan unprecedented initial turnover frequency (TOF) of 7046 mol H<sub>2</sub> mol catalyst<sup>–1</sup> h<sup>–1</sup> without\nany additive, outperforming most of the reported noble metal catalysts\nunder similar conditions. Transmission electron microscopy (TEM) images,\nX-ray photoelectron spectroscopy (XPS) analysis, and density functional\ntheory (DFT) calculations demonstrate that the extraordinary catalytic\nactivities are mainly due to the geometric effect and electronic effect\nof AuPd nanoparticles derived from the modification of h-BN with citric\nacid and the accompanying −NH<sub>2</sub>. This work provides\nmore flexibility for designing highly efficient nanocatalysts for\nhydrogen generation from FA dehydrogenation.
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