期刊
NANO LETTERS
卷 21, 期 24, 页码 10284-10291出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.1c03381
关键词
single-atom Cu; nitrostyrene; chemoselective hydrogenation reaction; hydrogenation mechanism
类别
资金
- National Natural Science Foundation of China [11772257, 21871221]
- Shaanxi Science Foundation [2020JM-356, 2021JM-103]
- National Science Fund for Distinguished Young Scholars [52025133]
- Tencent Foundation
The researchers have developed a new strategy to incorporate single atom Cu sites into melem ring, resulting in Cu-1/CN catalyst with high selectivity, activity, and stability for selective hydrogenation of 4-nitrostyrene. The presence of hydroxymethyl from trimethylolmelamine is found to be beneficial for atomically dispersing Cu atoms in CN, contributing to the optimal chemical environment for efficient hydrogenation reaction. X-ray absorption fine structure tests indicate that the Cu atom of Cu-1/CN is dominated by quaternary coordination way in the melem ring of CN.
The Cu-based nanocatalysts have shown a high selectivity toward selective hydrogenation reaction, but the underlying catalytic mechanism is still murky. Herein, we report a new gram-scale strategy for realizing the single atom Cu site incorporated into the melem ring of graphitic carbon nitride (Cu-1/CN) for understanding the catalytic mechanism of a hydrogenation reaction. The as-synthesized Cu-1/CN exhibits unprecedented selectivity (100%), high activity (TOF = 2.9 x 10(3) h(-1)), and outstanding stability for selective hydrogenation of 4-nitrostyrene. We reveal that the presence of hydroxymethyl from trimethylolmelamine is beneficial to atomically disperse Cu atoms in the CN. X-ray absorption fine structure tests reveal that the Cu atom of Cu-1/CN is dominated by the quaternary coordination way (Cu-N-4) in the melem ring of CN. Density functional theory calculations confirm that the high reactivity and selectivity originate from the anchored Cu sites creating the optimal chemical environment for the highly efficient hydrogenation reaction.
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