化工进展 ›› 2023, Vol. 42 ›› Issue (7): 3652-3663.DOI: 10.16085/j.issn.1000-6613.2022-1588

• 材料科学与技术 • 上一篇    下一篇

炭化与焙烧温度对植物基铁碳微电解材料去除As(Ⅲ)性能的影响

李海东1(), 杨远坤1,2, 郭姝姝1, 汪本金1, 岳婷婷1, 傅开彬1,2, 王哲1,2, 何守琴3, 姚俊4, 谌书1,2()   

  1. 1.西南科技大学环境与资源学院,四川 绵阳 621000
    2.固体废物处理与资源化教育部重点实验室,四川 绵阳 621000
    3.西南科技大学经济管理学院,四川 绵阳 621000
    4.中国地质大学(北京)水资源与 环境学院,北京 100083
  • 收稿日期:2022-08-29 修回日期:2022-11-02 出版日期:2023-07-15 发布日期:2023-08-14
  • 通讯作者: 谌书
  • 作者简介:李海东(1997—),男,硕士研究生,研究方向为水污染治理。E-mail:3064651627@qq.com
  • 基金资助:
    国家重点研发计划(2019YFC1803500);国家自然科学基金青年基金(42107481);川省科技计划-重点研发项目(2021YFS0289);西南科技大学科研基金(20zx7150);四川循环经济研究中心科技项目(XHJJ-1417)

Effect of carbonization and calcination temperature on As(Ⅲ) removal performance of plant-based Fe-C microelectrolytic materials

LI Haidong1(), YANG Yuankun1,2, GUO Shushu1, WANG Benjin1, YUE Tingting1, FU Kaibin1,2, WANG Zhe1,2, HE Shouqin3, YAO Jun4, CHEN Shu1,2()   

  1. 1.School of Environment and Resource, Southwest University of Science and Technology, Mianyang 621010, Sichuan, China
    2.Key Laboratory of Solid Waste Treatment and Resource Recycle, Ministry of Education, Mianyang 621010, Sichuan, China
    3.School of Economics and Management, Southwest University of Science and Technology, Mianyang 621010, Sichuan, China
    4.China University of Geosciences in Beijing, Beijing 100083, China
  • Received:2022-08-29 Revised:2022-11-02 Online:2023-07-15 Published:2023-08-14
  • Contact: CHEN Shu

摘要:

以美人蕉、还原铁粉和膨润土为原材料制备植物基铁碳微电解材料,先通过单因素实验确定Fe/C物质的量比、炭化温度和焙烧温度3个影响因素,后采用Box-Behnken响应面法对“均质化-炭化-焙烧”制备工艺进行优化,以确定最优制备条件。并结合X射线衍射(XRD)、电子顺磁共振波谱仪(EPR)、傅里叶红外光谱仪(FTIR)等表征方法,探究烧制温度对植物基铁碳微电解材料固有性质及其去除As(Ⅲ)性能的影响。结果表明,最优制备条件为Fe/C=1.05、炭化温度502.87℃、焙烧温度760.92℃。烧制温度的升高,有利于增强碳基组分得电子能力,加速As(Ⅲ)氧化为As(Ⅴ),降低水体生物毒性的同时提高对As(Ⅲ)的去除率;当焙烧温度高于700℃时,膨润土晶体结构层瓦解,渗透性提高的同时加速Ca2+、Mg2+离子释放,并促进Fe3+的水解沉积物互斥作用减弱,提高对As(Ⅲ)的吸附容量;还原铁粉过量5%,在保证反应时微原电池数量的同时,表面氧化产生的Fe3O4、Fe2O3在酸性条件下易反应形成Fe2+、Fe3+,对As(Ⅲ)的吸附去除作用加强。

关键词: 铁碳微电解材料, As(Ⅲ), 响应面优化, 热解, 电化学, 造粒

Abstract:

Plant-based iron-carbon microelectrolysis materials were prepared by use of canna, reduced iron powder and bentonite as raw materials. Three main factors affected on As(Ⅲ) removal efficiency were firstly determined through single factor experiment, and the determined influencing factors were iron-carbon molar ratio, carbonization temperature and roasting temperature. In order to determine the optimal preparation conditions, box-Behnken response surface method was then used to optimize the preparation process of “homogenization, carbonization and roasting”. The effect of firing temperature on the intrinsic properties of plant-based iron-carbon microelectrolysis materials and their influence on As() removal performance were finally investigated in combination with X-ray diffraction (XRD), electron paramagnetic resonance spectroscopy (EPR), Fourier transform infrared spectrometer (FTIR) and other characterization methods. The results showed that the optimum preparation conditions of Fe/C, carbonization temperature and roasting temperature were 1.05℃, 502.87℃ and 760.92℃, respectively. As increase of firing temperature, the electron separation capacity of carbon base enhanced which further accelerated the oxidation of As() to As() and improved the removal rate of As(). When the calcination temperature was higher than 700℃, the crystal structure layer of bentonite collapsed and increased their permeability, which can accelerate the release of Ca2+ and Mg2+ ions, weaken the mutual exclusion of Fe3+ hydrolyzed sediments, and thus improved the adsorption capacity of As(). When utilized amount of reduced iron powder exceeds 5%, the Fe3O4 and Fe2O3 produced by surface oxidation can easily react to form Fe2+ and Fe3+ under acidic conditions while ensuring the number of microgalvanic cells in the reaction. All of these strengthened the adsorption removal effect of As(Ⅲ).

Key words: iron micro-electrolysis material, As(), response surface optimization, pyrolysis, electrochemistry, granulation

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