Dung Nguyen Trung, Khiem Ta Cong, Thao Nguyen Phuong, Phu Nguyen Anh, Son Nguyen Truong, Dat Tran Quang, Phuong Nguyen Thu, Trang Tran Thi, Nhi Bui Dinh, Thuy Nguyen Thi, Lin Kun-Yi Adrew, Huy Nguyen Nhat
Faculty of Physics and Chemical Engineering, Le Quy Don Technical University, 236 Hoang Quoc Viet St., Bac Tu Liem District, Hanoi, Viet Nam.
Innovation and Development Center of Sustainable Agriculture and Department of Environmental Engineering, National Chung Hsing University, 250 Kuo-Kuang Road, Taichung, Taiwan.
Chemosphere. 2024 Aug;361:142452. doi: 10.1016/j.chemosphere.2024.142452. Epub 2024 May 27.
CuCoFe-LDO/BCD was successfully synthesized from CuCoFe-LDH and biochar derived from durian shell (BCD). Ciprofloxacin (CFX) degraded more than 95% mainly by O and O in CuCoFe-LDO/BCD(2/1)/PMS system within 10 min with a rate constant of 0.255 min, which was 14.35 and 2.66 times higher than those in BCD/PMS and CuCoFe-LDO/PMS systems, respectively. The catalytic system exhibited good performance over a wide pH range (3-9) and high degradation efficiency of other antibiotics. Built-in electric field (BIEF) driven by large difference in the work function/Fermi level ratio between CuCoFe-LDO and BCD accelerated continuous electron transfer from CuCoFe-LDO to BCD to result in two different microenvironments with opposite charges at the interface, which enhanced PMS adsorption and activation via different directions. As a non-radical, O was mainly generated via PMS activation by C=O in BCD. The presence of C=O in BCD resulted in an increase in atomic charge of C in C=O and redistributed the charge density of other C atoms. As a result, strong adsorption of PMS at C atom in C=O and other C with a high positive charge was favorable for O generation, whereas an enhanced adsorption of PMS at negatively charged C accounted for the generation of OH and SO. After adsorption, electrons in C of BCD became deficient and were fulfilled with those transferred from CuCoFe-LDO driven by BIEF, which ensured the high catalytic activity of CuCoFe-LDO/BCD. O, on the other hand, was generated via several pathways that involved in the transformation of OH and SO originated from PMS activation by the transition of metal species in CuCoFe-LDO and negatively charged C in BCD. This study proposed a new idea of fabricating a low-cost metal-LDH and biomass-derived catalyst with a strong synergistic effect induced by BIEF for enhancing PMS activation and antibiotic degradation.
通过CuCoFe-LDH和榴莲壳衍生的生物炭(BCD)成功合成了CuCoFe-LDO/BCD。在CuCoFe-LDO/BCD(2/1)/PMS体系中,环丙沙星(CFX)在10分钟内主要通过O和O降解率超过95%,速率常数为0.255 min,分别比BCD/PMS和CuCoFe-LDO/PMS体系高14.35倍和2.66倍。该催化体系在较宽的pH范围(3-9)内表现出良好的性能,对其他抗生素也具有较高的降解效率。CuCoFe-LDO和BCD之间功函数/费米能级比的巨大差异驱动的内建电场(BIEF)加速了电子从CuCoFe-LDO向BCD的连续转移,导致界面处形成两个带相反电荷的不同微环境,通过不同方向增强了PMS的吸附和活化。作为一种非自由基,O主要通过BCD中C=O对PMS的活化产生。BCD中C=O的存在导致C=O中C的原子电荷增加,并重新分布了其他C原子的电荷密度。结果,PMS在C=O中的C原子和其他带高正电荷的C上的强吸附有利于O的生成,而PMS在带负电荷的C上的增强吸附则导致了OH和SO的生成。吸附后,BCD中C的电子变得不足,并由BIEF驱动从CuCoFe-LDO转移来的电子填充,这确保了CuCoFe-LDO/BCD的高催化活性。另一方面,O通过多种途径生成,这些途径涉及由CuCoFe-LDO中的金属物种转变和BCD中带负电荷的C对PMS活化产生的OH和SO的转化。本研究提出了一种制备低成本金属-LDH和生物质衍生催化剂的新思路,该催化剂具有由BIEF诱导的强协同效应,可增强PMS活化和抗生素降解。