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Pure phase Ni12P5 anchored on N, P-codoped carbon nanosheet: A stable and highly efficient catalyst to reduce toxic organic compounds for continuous-flow application

Journal 2023 · IF 6.7 · 发表于 2023 年 4 月 6 日
作者: Bi-Xian Chen,Jing Tan,Yong-Jie Yie,Su-Ru Tang,Xin Deng,Hao-Yuan Xie,Wen-Ting Liu,Xiaojun Liu,Wei-Qin Xu,Chun-Cheng Lin,Sheng-Run Zheng
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摘要

The removal of toxic organic compounds from aqueous media through reduction reactions using nonnoble catalysts has attracted much attention in recent years. In this study, a simple method for the synthesis of pure-phase Ni 12 P 5 nanoparticles supported on N, P-codoped carbon (NPC) sheets was developed, in which a nickel phosphine complex was selected as the precursor due to its high Ni/P ratio, air stability and easy preparation. By controlling the pyrolysis temperature, Ni x P y @NPC 700 with a high dispersity and exposed active sites can be obtained, which was characterized by XRD, HRTEM, EDS, XPS, Raman and NH 3 -TPD. The catalytic performance of the composite in the reaction of 4-nitrophenol (4-NP) was assessed under mild conditions, exhibiting excellent catalytic activity with a low apparent activation energy E a (29.87 KJ·mol −1 ). In addition, the catalyst can be recycled without obvious loss of activity for up to ten successive cycles. The outstanding hydrogenation activity is ascribed to the exposed Ni 12 P 5 (3   1   2) crystal plane of Ni x P y @NPC 700 , which is attributed to the lower energy barrier required to form a hydrogen splitting state according to DFT calculations. Moreover, Ni x P y @NPC 700 was creatively coated in a Teflon tube with Nafion as the adhesive and constructed as a fixed-bed device. The continuous-flow catalytic reaction shows that the catalyst can maintain a satisfactory efficiency for approximately 6 h in the reduction of 4-NP and methyl orange (MO). These findings suggest that Ni x P y @NPC 700 is an ideal catalyst for industrial applications for the chemical reduction of toxic compounds from wastewater.

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