Pd nanoparticles supported on microflower NiMOF modified roughed nickel foam with the enhanced active site for electrochemical dechlorination of trichloroacetic acid

IF 9 1区 工程技术 Q1 ENGINEERING, CHEMICAL
Fangyuan Wang , Yuanyuan Li , Huanqing Xie , Chunyu Wu , Wen Gao , Jianping Qiu , Lexing You , Shuang Song
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引用次数: 2

Abstract

Electrocatalytic hydrodechlorination (ECH) has been considered as an effective method to convert refractory chlorinated organics into biodegradable chlorine-free organics under mild conditions. In this work, a composite electrode of Pd/NiMOF/roughed nickel foam (Pd/NiMOF/RNF) with excellent dechlorination performance was prepared by electrodeposition of Pd nanoparticles on the flower-shaped NiMOF interlayer grown in-situ. Benefiting from the high specific surface area of NiMOF structure and excellent dispersion of Pd facilitated, the Pd/NiMOF/RNF offered abundant active hydrogen and larger open channels for the easy diffusion of reactants and products in the electrochemical dechlorination process. 97% of 6 μmol/L trichloroacetic acid (TCAA) was dechlorinated at a cathodic potential of −1.2 V within 90 min. The corresponding palladium mass activity was calculated to be 0.39 μg min−1 cm−2 mg−1 Pd, which was approximately 3.5 times greater than other report on ECH cathode. Moreover, the Pd/NiMOF/RNF cathode remained stable even after five consecutive cycle tests. Toxic assessment results indicated that the dechlorination process was beneficial to the detoxification of TCAA at the end of reaction. The hydrodechlorination mechanism of TCAA was proposed by density functional theory (DFT) analysis and electrochemical characterization on the Pd/NiMOF/RNF electrode. The findings of this study have the potential to contribute to the development of electrocatalytic treatment methods for chlorinated organic compounds in drinking water.

微花纳米镍改性泡沫镍纳米粒子对三氯乙酸电化学脱氯活性的增强研究
电催化加氢脱氯(ECH)是在温和条件下将难降解的氯化有机物转化为可生物降解的无氯有机物的有效方法。在原位生长的花状NiMOF中间层上电沉积Pd纳米粒子,制备了具有优异脱氯性能的Pd/NiMOF/粗泡镍复合电极(Pd/NiMOF/RNF)。得益于NiMOF结构的高比表面积和优异的Pd分散性,Pd/NiMOF/RNF在电化学脱氯过程中提供了丰富的活性氢和较大的开放通道,便于反应物和产物的扩散。6 μmol/L的三氯乙酸(TCAA)在−1.2 V的阴极电位下,在90 min内脱氯97%,计算得到钯的质量活度为0.39 μg min−1 cm−2 mg−1 Pd,约为其他ECH阴极报道的3.5倍。此外,Pd/NiMOF/RNF阴极即使在连续五次循环测试后仍保持稳定。毒性评价结果表明,脱氯过程有利于反应结束时TCAA的解毒。通过密度泛函理论(DFT)分析和Pd/NiMOF/RNF电极的电化学表征,提出了TCAA的加氢脱氯机理。本研究结果对电催化处理饮用水中氯化有机化合物的方法的发展具有潜在的促进作用。
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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