Metal-free catalytic reduction of 4-nitrophenol to 4-aminophenol by N-doped graphene
Metal-free catalytic reduction of 4-nitrophenol to 4-aminophenol by N-doped graphene
复制标题
N掺杂石墨烯无金属催化还原4-硝基苯酚为4-氨基苯酚
DOI：
10.1039/c3ee40918j
复制
发表时间：
2013-11-01
影响因子：
32.5
通讯作者：
Chen, Qian-wang
中科院分区：
文献类型：
--
作者：
Kong, Xiang-kai;Sun, Zhi-yuan;Chen, Qian-wang
报道了氮掺杂石墨烯（NG）介导的4-硝基苯酚（Nip）无金属催化还原为4-氨基苯酚（NEP）的反应。Nip可完全还原为N2，无任何副产物产生。NG的活性与先前报道的一些金属催化剂相当。有趣的是，NG片催化反应遵循伪零级动力学，而所有的金属催化剂遵循伪一级动力学。原位FTIR实验表明，Nip离子通过其羟基上的O原子与NG发生联合收割机结合。理论计算验证了该吸附模型，并证实了吸附的Nip离子是关键步骤，导致伪零级动力学。此外，只有在NG表面上的掺杂N原子旁边的碳原子可以被活化，作为活性位点。正如预期的那样，四种掺杂的N原子都有利于Nip的吸附和活化，有助于催化还原反应。
The metal-free catalytic reduction of 4-nitrophenol (Nip) to 4-aminophenol (Amp) mediated by N-doped graphene (NG) was reported. Nip could be reduced to Amp completely without any by-product generation. The activity of the NG is comparable with some of the previously reported metallic catalysts. Interestingly, the NG sheet catalyzed reaction follows pseudo-zero-order kinetics, while all the metallic catalysts follow pseudo-first-order kinetics. The in situ FTIR experiment demonstrated that Nip ions will combine with NG via the O atoms of their hydroxyl groups. Theoretical calculations verified this adsorption model, and confirmed that the adsorption of Nip ions is the critical step, leading to the pseudo-zero-order kinetics. Moreover, only the carbon atoms next to the doped N atoms on NG surface can be activated, serving as the active sites. As expected, all four kinds of the doped N atoms are beneficial to the adsorption and activation of Nip, contributing to the catalytic reduction reaction.