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用于4-氯苯酚电催化加氢脱氯的碳纳米管掺杂Pd-Ni双金属三维电极:增强的活性和稳定性

Carbon-nanotube-doped Pd-Ni bimetallic three-dimensional electrode for electrocatalytic hydrodechlorination of 4-chlorophenol: Enhanced activity and stability.

作者信息

Wu Yifan, Gan Ling, Zhang Shupeng, Song Haiou, Lu Chang, Li Wentao, Wang Zheng, Jiang Bicun, Li Aimin

机构信息

State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, PR China.

State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing 210023, PR China; School of Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, PR China.

出版信息

J Hazard Mater. 2018 Aug 15;356:17-25. doi: 10.1016/j.jhazmat.2018.05.034. Epub 2018 May 16.

Abstract

A novel composite bimetallic electrode, palladium-nickel/multi-walled carbon nanotubes/graphite felt (Pd-Ni/MWCNTs/GF), was synthesized for the electrocatalytic hydrodechlorination of 4-chlorophenol (4-CP). GF with a three-dimensional structure was used as the electrode substrate, and doped with MWCNTs, which can improve the GF conductivity and serve as a skeleton for metal loading. Ni and Pd were deposited on the electrode surface stepwise to obtain a well-aligned, highly active and stable Pd-Ni/MWCNTs/GF electrode. The Pd-Ni/MWCNTs/GF cathode showed a high reactivity for the electrocatalytic hydrodechlorination of 4-CP; up to 100% removal of 4-CP was achieved within 30 min, and followed pseudo-first-order kinetics with a rate constant of 0.162 min. Compared with other cathodes, the Pd-Ni/MWCNTs/GF electrode showed superior performance in 4-CP reduction. Excessive current will lower the reaction efficiency and current efficiency because of hydrogen evolution, and acidic solution conditions are more conducive to electrocatalytic reactions. Experiments confirmed that the Ni had a small amount of loss under acidic conditions but remained stable under neutral and alkaline conditions, whereas the loss of Pd for different pH values was constantly low. In cycle tests, the bimetallic electrode exhibits a better reactivity and stability than the single-metal Pd electrode in the long-term.

摘要

合成了一种新型复合双金属电极,即钯 - 镍/多壁碳纳米管/石墨毡(Pd - Ni/MWCNTs/GF),用于4 - 氯苯酚(4 - CP)的电催化加氢脱氯反应。具有三维结构的石墨毡用作电极基底,并掺杂多壁碳纳米管,这可以提高石墨毡的导电性并作为金属负载的骨架。镍和钯逐步沉积在电极表面,以获得排列良好、高活性且稳定的Pd - Ni/MWCNTs/GF电极。Pd - Ni/MWCNTs/GF阴极对4 - CP的电催化加氢脱氯反应表现出高反应活性;在30分钟内实现了高达100%的4 - CP去除率,并且遵循准一级动力学,速率常数为0.162 min⁻¹。与其他阴极相比,Pd - Ni/MWCNTs/GF电极在4 - CP还原方面表现出优异的性能。由于析氢,过大的电流会降低反应效率和电流效率,并且酸性溶液条件更有利于电催化反应。实验证实,镍在酸性条件下有少量损失,但在中性和碱性条件下保持稳定,而钯在不同pH值下的损失一直很低。在循环测试中,双金属电极在长期内比单金属钯电极表现出更好的反应活性和稳定性。

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