甲酸
氧烷
催化作用
X射线光电子能谱
三嗪
氢
扫描透射电子显微镜
扩展X射线吸收精细结构
化学
钯
制氢
选择性
无机化学
核化学
材料科学
吸收光谱法
光谱学
透射电子显微镜
化学工程
高分子化学
纳米技术
有机化学
工程类
物理
量子力学
作者
Dmitri A. Bulushev,Fedor S. Golub,С. В. Трубина,В. П. Зверева,L. G. Bulusheva,Evgeny Yu. Gerasimov,Miriam Navlani‐García,Anna Krot,Himanshu Sekhar Jena
出处
期刊:ACS applied nano materials
[American Chemical Society]
日期:2022-08-22
卷期号:5 (9): 12887-12896
被引量:13
标识
DOI:10.1021/acsanm.2c02746
摘要
According to our knowledge, single-atom Pd catalysts supported on covalent triazine frameworks (CTF) have not been studied in the production of hydrogen from formic acid. Therefore, we synthesized 1 wt % Pd single-atom catalysts based on CTF-1, pyCTF, and bipyCTF supports and tested them in the gas-phase decomposition of formic acid. The results were compared with those obtained for a Pd catalyst supported on mesoporous graphitic-type carbon (Pd/C) with nanoparticles (∼2.3 nm). The catalysts were characterized by high-angle annular dark-field/scanning transmission electron microscopy (HAADF/STEM), extended X-ray absorption fine structure/X-ray absorption near-edge structure (EXAFS/XANES), and X-ray photoelectron spectroscopy (XPS) methods. The following order of catalytic activity was obtained: Pd/CTF-1 > Pd/C > Pd/pyCTF ≥ Pd/bipyCTF. The best performance of the Pd/CTF-1 catalyst was associated with Pd2+–C2N2 sites. Pd2+–N4 sites formed on pyCTF and bipyCTF supports showed lower catalytic activity. The selectivity trend at temperatures above 500 K was as follows: Pd/bipyCTF > Pd/pyCTF > Pd/CTF-1 > Pd/C. For the Pd/bipyCTF catalyst, the selectivity reached 99.8%, which is very high for this temperature range. These results may be important for the development of CTF-based catalysts for hydrogen production reactions.
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