Mineralize complex organic contaminants using only oxygen on dense copper atoms embedded in the walls of carbon nanotubes
Mineralize complex organic contaminants using only oxygen on dense copper atoms embedded in the walls of carbon nanotubes
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DOI：
10.1016/j.apsusc.2022.154760
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发表时间：
2022-09
影响因子：
6.7
通讯作者：
Jiabai Cai;Qi Jing;Huan Li;Lin Wang;Yingchao Cheng;M. Takaoka
中科院分区：
文献类型：
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作者：
Jiabai Cai;Qi Jing;Huan Li;Lin Wang;Yingchao Cheng;M. Takaoka
在这项研究中，提出了一种新的催化空气氧化（CAO）过程的基础上，一个简单的合成纳米复合催化剂。将Cu单原子（CuSA）嵌入到多壁碳纳米管（CNTs）上，制备了CNTs@CuSA催化剂，CuSA的质量分数为10.02%。以腐殖酸（HA）等典型难降解污染物为研究对象，考察了CNTs@ CuSA在CAO中的降解能力。催化剂在120 °C下预激发10 min以越过能垒，然后在90 °C下催化HA氧化50 min。当CuSA质量分数为8.39%时，CNTs@ CuSA具有上级的催化活性，溶液中99%的HA被降解，98%的有机碳被矿化.畸变校正透射电子显微镜，电子顺磁共振光谱，密度泛函理论计算被应用到检测的机制。结果表明，碳纳米管壁面上的Cu-N配位和碳纳米管的限制效应激活O2产生·OH自由基，具有较高的激活效率。此外，该催化剂在多次循环后仍保持活性。该结果为低温催化空气氧化法处理有机废水提供了一种新的催化剂。
In this study, a novel catalytic air oxidation (CAO) process is proposed based on a facilely synthesized nanocomposite catalyst. The catalyst was prepared using Cu single atoms (CuSA) embedded on multiwalled carbon nanotubes (CNTs), denoted as CNTs@CuSA, with mass ratio of CuSAup to 10.02 %. Humic acid (HA) and other typical refractory contaminents were used to investigate the ability of CNTs@CuSAin CAO. The catalysts were pre-excited to cross the energy barrier at 120 °C for 10 min, and then used to catalyze the oxidation of HA at 90 °C in 50 min. The CNTs@CuSAwith CuSAmass ratio 8.39 % showed a superior catalytic activity, and 99 % of HA in solution was degraded with 98 % of organic carbon mineralization. Aberration-corrected transmission electron microscopy, electron paramagnetic resonance spectroscopy, and density functional theory calculations were applied to detect the mechanism. The results showed that the Cu-N coordination sites on CNT walls and the confinement effect of CNTs activated O2to produce ·OH radicals, with a high activation efficiency. Moreover, this catalyst remained active after multiple cycles. This result provides a new catalyst to support low-temperature catalytic air oxidation for organic wastewater treatment.