镍负载对镍(Ni)/铁(Fe)双金属纳米颗粒对三氯乙烯和四氯化碳反应活性的影响

IF 5.8 2区 环境科学与生态学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Caijie WEI, Weizhong Wu, xufei zhao, Cheng Sun, Zehan Shi, jun Yang, Ming-Hong Wu
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引用次数: 0

摘要

为了提高纳米级零价铁的除氯反应活性,我们开发了双金属镍/铁纳米粒子。镍/铁-纳米粒子的物理结构(镍含量在 0.5wt% 到 20wt% 之间)以及对三氯乙烯(TCE)和四氯化碳(CT)的反应活性随结构的变化进行了全面研究。在镍含量较高(20 wt.%)的镍/锗氮氧化物中可以观察到镍堆积表面,其他镍/锗氮氧化物的结构被确定为类似镍/锗合金的结构,其中 5wt% 镍/锗氮氧化物的比表面积和 Fe0 含量最高。镍负载量为 5wt% 时,B-nZVI 的 CT 脱氯率最好,为 2.5 倍;而镍负载量为中等(3wt%-5wt%)时,B-nZVI 的 TCE 还原率最好,为 12 倍。由于 TCE 的主要降解机制是通过原子氢(H*),而 CT 的降解是通过直接电子转移进行的,因此 Ni/Fe NP 系统更有效的还原机制最好是 H* 还原。对于 TCE 而言,中等负载量(3wt%-5wt%)和低/高负载量(0.5wt%,20wt%)之间的还原速率和副产物产率差异比 CT 更为显著。研究发现,镍的中等负载量(3wt%- 5wt%)明显促进了 TCE 对 VC 的 β-消除,这是由于 H* 在镍催化剂中的良好储存。H* 的产生和电子迁移率的提高分别通过 CV 曲线和 Tafel 曲线得到了很好的证明。进一步讨论了直接电子转移和 H* 催化剂在 Ni/Fe 双金属体系中的出现位置。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Influence of nickel loading on reactivity of Ni/Fe bimetallic nanoparticles toward trichloroethene and carbon tetrachloride
Bimetallic Ni/Fe-nanoparticles has been developed to enhance the dechlorination reactivity of nano-sized zero-valent iron. The physical structures of Ni/Fe-NPs with Ni loading ranged from 0.5wt% to 20wt% and the structure dependent reactivity variation towards to trichloroethene (TCE) and carbon tetrachloride (CT) have been fully investigated. A Ni-accumulated surface can be observed for the Ni/Fe-NPs with high Ni loading (20 wt.%), and the structure of other Ni/Fe NPs were identified as a Ni/Fe alloy-like structure with 5wt% Ni/Fe NPs owning the highest surface area and Fe0 content. While the best CT dechlorination rate was 2.5-fold of B-nZVI at 5wt% Ni loading, the best TCE reduction was 12-fold of B-nZVI at medium Ni loading (3wt%-5wt%). Since the primary TCE degradation mechanism is via atomic hydrogen (H*) whereas degradation of CT proceeds via direct electron transfer, the more efficient reduction mechanism for the Ni/Fe NP system was preferably H* reduction. The reduction-rate and the by-products yield variation between medium loading((3wt%-5wt%) and low/high (0.5wt%,20wt%) loading was more significant for TCE than CT. It has been found that Medium Ni loading (3wt%- 5wt%) obviously boosted the β-elimination of TCE to VC due to good storage of H* in Ni catalyst. The production of H* and enhanced electron migration rate were well demonstrated by CV curve and Tafel curve, respectively. The occurrence location of direct electron transfer and H* catalyst in bimetallic Ni/Fe system was further discussed.
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来源期刊
Environmental Science: Nano
Environmental Science: Nano CHEMISTRY, MULTIDISCIPLINARY-ENVIRONMENTAL SCIENCES
CiteScore
12.20
自引率
5.50%
发文量
290
审稿时长
2.1 months
期刊介绍: Environmental Science: Nano serves as a comprehensive and high-impact peer-reviewed source of information on the design and demonstration of engineered nanomaterials for environment-based applications. It also covers the interactions between engineered, natural, and incidental nanomaterials with biological and environmental systems. This scope includes, but is not limited to, the following topic areas: Novel nanomaterial-based applications for water, air, soil, food, and energy sustainability Nanomaterial interactions with biological systems and nanotoxicology Environmental fate, reactivity, and transformations of nanoscale materials Nanoscale processes in the environment Sustainable nanotechnology including rational nanomaterial design, life cycle assessment, risk/benefit analysis
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