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In Situ Hydrochar Regulates Cu Fate and Speciation: Insights into Transformation Mechanism
Journal of Hazardous Materials ( IF 12.2 ) Pub Date : 2020-11-20 , DOI: 10.1016/j.jhazmat.2020.124616
Hugang Li , Maojiong Cao , Jamison Watson , Yuanhui Zhang , Zhidan Liu

Cu is one of the dominant heavy metals toxic to human health and environmental ecosystems. Understanding its fate and chemical speciation is of great importance for hydrothermal liquefaction (HTL) of Cu-rich hazardous streams. Herein, we investigated its evolution during the HTL of wastewater algae through ICP-MS, XRD, XANES, and EXAFS. Cu-cysteine complexes (51.5%) and Cu2S (40.4%) were the main components of Cu in algae, whereas the predominant form was CuS (70.9%) in 220oC-hydrochar. Model compound experiments indicated that Cu-cysteine could be converted into CuS, while Cu2S was stable during HTL. However, Cu2S was partially converted into CuS in the hydrochar. Subsequently, the positive Gibbs free energy (36.8KJ/mol) indicates that the oxidation from Cu+ to Cu2+ can’t occur spontaneously. Furthermore, cyclic voltammograms demonstrated that hydrochar facilitated the oxidation of Cu2S due to its higher capability of electron acceptance. All these results prove that hydrochar serves as a catalyst for the conversion of Cu2S to CuS during HTL. This study firstly elucidated that Cu2S was oxidized into CuS in the presence of hydrochar, and Cu-cysteine was converted into CuS under HTL. This study provides a critical insight into the transformation mechanism of Cu during the HTL of hazardous streams.



中文翻译:

原位水焦调节铜的命运和形态:转化机制的见解。

铜是对人体健康和环境生态系统有毒的主要重金属之一。了解其命运和化学形态对于富含铜的危险物流的水热液化(HTL)至关重要。在这里,我们通过ICP-MS,XRD,XANES和EXAFS研究了废水藻类HTL期间其演变。铜-半胱氨酸配合物(51.5%)和铜2 S(40.4%)是藻类中铜的主要成分,而主要形式是在220 o C的碳氢盐中的铜(CuS)(70.9%)。模型化合物实验表明,Cu半胱氨酸可转化为CuS,而HTL期间Cu 2 S稳定。但是,Cu 2S在水焦中部分转化为CuS。随后,正吉布斯自由能(36.8KJ / mol)表明不能自发发生从Cu +到Cu 2+的氧化。此外,循环伏安图表明,水煤由于其较高的电子接受能力而促进了Cu 2 S的氧化。所有这些结果证明,在HTL期间,水焦炭可作为Cu 2 S转化为CuS的催化剂。该研究首先阐明了在水煤油存在下Cu 2 S被氧化为CuS,而HTL催化下Cu-半胱氨酸被转化为CuS。这项研究提供了对有害流HTL过程中Cu转化机理的重要见解。

更新日期:2020-11-21
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