在具有可调缺陷的 Ru 负载刻面工程 {201}-TiO2 催化剂上可持续、高效地催化氧化氯化挥发性有机化合物

Bohua Sun, Qianqian Li, Guijin Su, Maoyong Song, Chunyan Ma, Jiaxin Pang, Xu Zhao, Jing Meng, Bin Shi
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引用次数: 0

摘要

可持续、高效地催化氧化氯化挥发性有机化合物(CVOC)是一项长期挑战。这一瓶颈源于氧化还原反应和氯脱附的催化活性有限,导致催化剂失活和二次污染。在此,我们的合理策略是在 Ru 负载面工程{201}-TiO 中加入可调整的缺陷,从而提高其反应活性。全面的表征和 DFT 计算表明,Ru/{201}-TiO 具有丰富的氧空位、Ti 缺陷和强大的金属-支撑相互作用,可实现灵活的电子转移以激活 O 和 HO 的解离,从而促进活性氧(ROS)(如 -O 和羟基物种)的不断生成。这些活性氧能有效促进氯的解吸和氯苯的深度氧化。Ru/{201}-TiO 在氯苯降解方面表现出卓越的反应活性,表观活化能(Ea)为 31.0 KJ/mol,在 1000 分钟的稳定性测试中,即使引入 HO,氯苯的转化率也达到了 100%。Ru/{201}-TiO 产生的小分子氯化副产物比 Ru/{101}-TiO 少 2.2-3.1 倍,而且没有检测到多氯化苯。
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Sustainable and efficient catalytic oxidation of chlorinated volatile organic compounds over Ru-loaded facet-engineered {201}-TiO2 catalyst with tuned defects
Sustainable and efficient catalytic oxidation of chlorinated volatile organic compounds (CVOCs) poses an enduring challenge. This bottleneck arises from the limited catalytic activity of redox reactions and chlorine desorption, causing catalyst deactivation and secondary pollution. Herein, our sound strategy involves Ru-loaded facet-engineered {201}-TiO with tuned defects, thereby boosting its reactivity. Comprehensive characterizations and DFT calculation manifested that Ru/{201}-TiO, with abundant oxygen vacancies, Ti defects, and robust metal-support interaction, enabled flexible electron transfer to activate O and the dissociation of HO, thus facilitating the continuous generation of reactive oxygen species (ROS), such as •O and hydroxyl species. These ROS effectively enhance chlorine desorption and chlorobenzene deep oxidation. Ru/{201}-TiO exhibited superior reactivity for chlorobenzene degradation, with an apparent activation energy (Ea) of 31.0 KJ/mol and 100 % chlorobenzene conversion in a 1000-min stability test, even with HO introduction. Ru/{201}-TiO produced 2.2–3.1 times fewer small-molecule chlorinated byproducts than Ru/{101}-TiO, with no polychlorinated benzenes detected.
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