N-, P-co-doped hierarchically porous carbon fiber derived from bamboo pulp as efficient carbocatalyst for reduction of 4-nitrophenol

IF 5.5 3区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Liyun Zhang, Weihai Zhou, Yongle Cao, Heng Zhang, Wancheng Zhu
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Abstract

For metal-free carbocatalysts, heteroatom doping and hierarchically porous structure are the significant factors to improve their catalytic performances. Herein, N-, P-co-doped hierarchically porous carbon fiber (NPC–2–800) was prepared by pyrolyzing bamboo pulp in combination with (NH4)2HPO4 and activator K2CO3. It was found that (NH4)2HPO4 not only provides N and P atoms, but also significantly affect the morphology and pore structure of the porous carbon. An appropriate dosage of (NH4)2HPO4 facilitates the formation of hierarchically porous carbon fiber in NPC-2–800. Whereas, the carbon fragments with only micropores were obtained in absence of (NH4)2HPO4. The hierarchical porosity and the co-doping of N and P atoms in the NPC-2–800 contribute to its outstanding catalytic performances in the 4-Nitrophenol (4-NP) reduction assisted by NaBH4. The NPC-2–800 exhibits an attractive turnover frequency (TOF) value of 4.29 × 10–4 mmol mg−1 min−1, a low activation energy (Ea) of 24.76 kJ/mol, and an acceptable recyclability for 7 cycles without obvious decrease in activity. Kinetics analyses suggest that the 4-NP reduction proceeds through the Langmuir–Hinshelwood model. In addition, the NPC-2–800 can also efficiently catalyze the 2-NP and 3-NP reduction. Moreover, in the real water body, the NPC-2–800 also showed superior catalytic activity to catalyze 4-NP reduction. This study provides an efficient catalyst for pollutant conversion and elimination as well as guidelines for designing versatile carbon-based catalysts.

Graphical abstract

Abstract Image

竹浆衍生的掺杂 N、P 的分层多孔碳纤维作为还原 4-硝基苯酚的高效碳催化剂
对于无金属碳催化剂而言,杂原子掺杂和分层多孔结构是提高其催化性能的重要因素。本文通过热解竹浆,结合(NH4)2HPO4 和活化剂 K2CO3,制备了掺杂 N、P 的分层多孔碳纤维(NPC-2-800)。研究发现,(NH4)2HPO4 不仅能提供 N 原子和 P 原子,还能显著影响多孔碳的形态和孔隙结构。适当剂量的 (NH4)2HPO4 有助于在 NPC-2-800 中形成分层多孔碳纤维。而在不添加 (NH4)2HPO4 的情况下,得到的碳碎片只有微孔。NPC-2-800 中的分层多孔性以及 N 原子和 P 原子的共掺杂使其在 NaBH4 辅助的 4-硝基苯酚(4-NP)还原反应中具有出色的催化性能。NPC-2-800 的翻转频率 (TOF) 值为 4.29 × 10-4 mmol mg-1 min-1,活化能 (Ea) 低至 24.76 kJ/mol,可循环使用 7 次而活性不会明显降低。动力学分析表明,4-NP 的还原是通过 Langmuir-Hinshelwood 模型进行的。此外,NPC-2-800 还能有效催化 2-NP 和 3-NP 还原。此外,在实际水体中,NPC-2-800 在催化 4-NP 还原方面也表现出了卓越的催化活性。这项研究为污染物的转化和消除提供了一种高效催化剂,也为设计多功能碳基催化剂提供了指导。
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来源期刊
Carbon Letters
Carbon Letters CHEMISTRY, MULTIDISCIPLINARY-MATERIALS SCIENCE, MULTIDISCIPLINARY
CiteScore
7.30
自引率
20.00%
发文量
118
期刊介绍: Carbon Letters aims to be a comprehensive journal with complete coverage of carbon materials and carbon-rich molecules. These materials range from, but are not limited to, diamond and graphite through chars, semicokes, mesophase substances, carbon fibers, carbon nanotubes, graphenes, carbon blacks, activated carbons, pyrolytic carbons, glass-like carbons, etc. Papers on the secondary production of new carbon and composite materials from the above mentioned various carbons are within the scope of the journal. Papers on organic substances, including coals, will be considered only if the research has close relation to the resulting carbon materials. Carbon Letters also seeks to keep abreast of new developments in their specialist fields and to unite in finding alternative energy solutions to current issues such as the greenhouse effect and the depletion of the ozone layer. The renewable energy basics, energy storage and conversion, solar energy, wind energy, water energy, nuclear energy, biomass energy, hydrogen production technology, and other clean energy technologies are also within the scope of the journal. Carbon Letters invites original reports of fundamental research in all branches of the theory and practice of carbon science and technology.
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