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硅酸盐通报 ›› 2021, Vol. 40 ›› Issue (11): 3762-3768.

• 陶瓷 • 上一篇    下一篇

SrFe0.6Co0.4O3催化降解孔雀石绿的研究

李家飞, 徐凯, 张永明, 潘莉莎   

  1. 海南大学,海南省精细化工工程技术研究中心,海口 570228
  • 收稿日期:2021-05-18 修回日期:2021-06-30 出版日期:2021-11-15 发布日期:2021-12-08
  • 通讯作者: 张永明,教授。E-mail:zh_yongming@163.com
  • 作者简介:李家飞(1992—),男,硕士研究生。主要从事无机非金属材料方面的研究。E-mail:jfei_li@163.com
  • 基金资助:
    海南大学横向项目(HD-KYH2014012)

Catalytic Degradation of Malachite Green by SrFe0.6Co0.4O3

LI Jiafei, XU Kai, ZHANG Yongming, PAN Lisha   

  1. Hainan Provincial Fine Chemical Engineering Research Center, Hainan University, Hainan 570228, China
  • Received:2021-05-18 Revised:2021-06-30 Online:2021-11-15 Published:2021-12-08

摘要: 具有复杂分子结构的三苯甲烷类染料孔雀石绿是一种典型的较难降解染料,是工业废水处理的难点之一。本文根据Goldschmidt半径容差规则法,设计了用于孔雀石绿降解的ABO3型SrFe(1-x)CoxO3催化剂,并选择出活性较高的SrFe0.6Co0.4O3催化剂。通过XRD、SEM、BET吸附及XPS分析表明:该催化剂是纯净钙钛矿结构,颗粒形貌为无规则堆叠的“蜂窝”片状;吸附等温线没有明显的回滞环,说明没有“墨水瓶”类孔结构;XPS谱中,B位离子同时存在Fe2+/Fe3+和Co2+/Co3+ 4种价态离子,且反应前后,4种离子的分布比例有较大变化。根据实验结果,推测该催化反应机理为:催化剂B位Co3+与溶解氧形成活性氧[O2]+和Co2+;活性氧[O2]+完成氧化反应后其正电荷转移到B位Fe2+上形成Fe3+,Fe3+的正电荷可再转移到Co2+形成Co3+,完成催化过程的电荷转移与循环。

关键词: SrFe0.6Co0.4O3催化剂, 孔雀石绿, 催化, 降解, 反应机理, 电荷转移

Abstract: Malachite green (MG) is a triphenylmethane dye with a complex molecular structure, which is difficult to be degraded, and it makes a difficulty in industrial wastewater treatment. In this paper,based on Goldschmidt radius tolerance rule, the ABO3 type catalysts with formula SrFe(1-x)CoxO3 (x=0~1) for degrading MG was designed. After experimental investigation, the SrFe0.6Co0.4O3 with highest catalytic activity was selected as target catalyst for MG degradation. The characteristics of this catalyst were analysed by XRD, SEM, BET and XPS methods. XRD pattern shows that the catalyst is pure perovskite crystal; the SEM image shows the morphology of catalyst particles is “honeycomb” flake with irregular stacking. In the BET adsorption isotherm of the catalyst, there is no obvious hysteresis loop, which means that there is no pore like “ink bottle”. Seeing from the XPS spectrum of the catalyst, the B-position has four ions (Fe2+/Fe3+ and Co2+/Co3+) at the same time, and the distribution ratio of above four ions vary greatly before and after the catalytic reaction. Based on these results, the mechanism of the catalytic reaction is speculated as follow: at first the Co3+ on B-site with the dissolved oxygen to form active oxygen [O2]+ and Co2+; then the [O2]+ oxidizes the MG, as well as the positive charge of [O2]+ is transferred to the Fe2+ on B-site to form Fe3+; at last, the positive charge of Fe3+ could be transferred to Co2+ on the B-site to form Co3+, and the transfer and circulation of the charge in catalytic process is completed.

Key words: SrFe0.6Co0.4O3 catalyst, malachite green, catalysis, degradation, reaction mechanism, charge transfer

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