Efficient degradation of typical pharmaceuticals in water using a novel TiO2/ONLH nano-photocatalyst under natural sunlight
Efficient degradation of typical pharmaceuticals in water using a novel TiO2/ONLH nano-photocatalyst under natural sunlight
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在自然阳光下使用新型 TiO2/ONLH 纳米光催化剂有效降解水中的典型药物
DOI：
10.1016/j.jhazmat.2020.123582
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发表时间：
2021
影响因子：
13.6
通讯作者：
Deng Shubo
中科院分区：
文献类型：
--
作者：
Zhang Qianxin;Du Roujia;Tan Cuiwen;Chen Ping;Yu Gang;Deng Shubo
在自然光和实际水体中光催化降解典型药物具有重要意义。在本研究中，氧或氮连接的庚嗪基聚合物（ONLH）成功地纳入到纳米TiO 2，并形成了TiO 2/ONLH纳米复合材料，这是响应于自然光。在自然光照射下，TiO 2/ONLH可有效降解10种药物。特别是含N-哌嗪基的氟喹诺酮类药物和含长芳香侧链的心血管药物更容易被降解。普萘洛尔的最佳降解性能的半衰期小于5分钟。普萘洛尔使用的TiO 2/ONLH的速率常数分别约为原始TiO 2和ONLH的6倍和8倍。两种活性物质（自由基dotOH和Oradical dot 2 −）促进了普萘洛尔的快速降解，主要通过羟基自由基加成、开环和ipso取代反应发生。使用发光细菌的急性毒性试验表明，随着总有机碳（TOC）的降低，普萘洛尔反应液的毒性逐渐降低。单体产物毒性评价表明，TiO 2/ONLH也减少了有毒转化产物的生成。实际水/废水的处理效果进一步表明TiO 2/ONLH可用于废水中药物的去除。
Photocatalytic degradation of typical pharmaceuticals in natural sunlight and in actual water is of great significance. In this study, the oxygen or nitrogen linked heptazine-base polymer (ONLH) was successfully incorporated with TiO2nanoparticles and formed a TiO2/ONLH nanocomposite which was responded to the natural sunlight. Under natural sunlight, the TiO2/ONLH can effectively degrade ten types of pharmaceuticals. In particular, fluoroquinolone containing N-piperazinyl, and cardiovascular drugs containing long aromatic side chains were easily degraded. The half-life of the best degradation performance of propranolol was less than 5 min. The rate constants of propranolol using the TiO2/ONLH were approximately six- and eight-fold higher than those of pristine TiO2and ONLH, respectively. Two reactive species (radical dotOH and Oradical dot2−) facilitated the rapid degradation of propranolol, which occurred primarily through the hydroxyl radical addition, ring-opening, and ipso substitution reactions. An acute toxicity test using luminescent bacteria indicated that the toxicity of the propranolol reaction solution gradually decreased with lower total organic carbon (TOC). According to the toxicity evaluation of monomer products, the TiO2/ONLH also reduced the generation of toxic transformation products. The effects of actual water/wastewater have further shown the TiO2/ONLH might be applied for the removal of pharmaceuticals in wastewater.