Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2020-06-13 , DOI: 10.1016/j.cej.2020.125869 Jian Hu , Xiangkang Zeng , Gen Wang , Binbin Qian , Yue Liu , Xiaoyi Hu , Brandon He , Lian Zhang , Xiwang Zhang
The role of oxygen vacancy (VO) in catalyst is manifested to be positive in the Fenton-like process. However, rational modulation of VO with a simple strategy for the efficient Fenton-like catalysts remains desirable and challenging. Here a facile heat treatment method without any additives was demonstrated to introduce VO on mesoporous cobalt oxide (Co3O4) hollow nanospheres, which served as highly reactive and stable Fenton-like catalysts for recalcitrant organic pollutants (bisphenol A, BPA) degradation by activating peroxymonosulfate (PMS). The VO-rich Co3O4 nanospheres exhibited superior BPA removal efficiency with high BPA degradation rate (0.0232 min−1, 100 min). The concentration of VO in Co3O4 was proved to act as an important role for the PMS activating efficiency. A series of mechanism studies, including radical scavengers, chemical probes and electrochemical characterizations, were conducted to identify the active radicals generated by PMS activation. Singlet oxygen produced from the VO-based reaction pathway, rather than sulfate radical and hydroxyl radical, was unveiled to play a key role in the BPA degradation process. This work provided new insight into designing transition metal oxide-based Fenton-like catalysts with efficient and sustainable remediation of refractory organic contaminants in wastewater.
中文翻译:
调节氧空位介孔Co 3 O 4空心纳米球的高效过氧单硫酸盐活化
氧空位的作用(V ø在催化剂)则表现为在类芬顿处理阳性。然而,用简单的策略对V O进行合理的调制以制得高效的Fenton类催化剂仍然是人们所期望和挑战的。在这里,没有任何添加剂的简便热处理方法被证明可以在介孔氧化钴(Co 3 O 4)空心纳米球上引入V O,该空心球可作为高反应性和稳定的类Fenton催化剂,用于降解难降解的有机污染物(双酚A,BPA)通过激活过氧一硫酸盐(PMS)。在V ø富含共3 ö 4纳米球表现出优异的BPA去除效率高BPA降解率(0.0232分钟-1,100分钟)。事实证明,Co 3 O 4中的V O浓度对PMS活化效率起着重要作用。进行了一系列机理研究,包括自由基清除剂,化学探针和电化学表征,以鉴定由PMS活化产生的活性自由基。V O产生的单重态氧揭示了基于反应的途径,而不是硫酸根和羟基,在BPA降解过程中起关键作用。这项工作为设计基于过渡金属氧化物的Fenton类催化剂提供了新的见识,该催化剂可以高效,可持续地修复废水中的难降解有机污染物。