Lu Jialin, Shen Bing, Qu Wenwen, Zhao Li, Yang Shu, Liu Qi, Liu Yihui
Faculty of Science, Kunming University of Science and Technology, Kunming 650500, PR China.
Faculty of Science, Kunming University of Science and Technology, Kunming 650500, PR China; Key Laboratory of Unconventional Metallurgy, Ministry of Education, Kunming University of Science and Technology, Kunming 650093, PR China; National Local Joint Laboratory of Engineering Application of Microwave Energy and Equipment Technology, Kunming University of Science and Technology, Kunming 650093, PR China.
Bioresour Technol. 2025 Nov;435:132837. doi: 10.1016/j.biortech.2025.132837. Epub 2025 Jun 20.
Photo-Fenton-like catalytic reactions exhibit remarkable effectiveness in environmental remediation owing to the synergistic interaction between photocatalysis and peroxide activation. Herein, biomass carbon quantum dots (BCDs) derived from pomelo peels were used to modulate BCDs/WO (BW) composites with dual reaction centers via a microwave-induced solvothermal approach, forming an iron-free photo-Fenton-like system (PFLS). Driven by the built-in electric field across the BW heterointerface, a Z-scheme charge transfer route was elucidated, which endows rapid photoexcited electron transfer from the WO to the BCDs. Notably, the dual reaction centers on BCDs and electron-rich oxygen vacancies of WO acted as both electron transmission "channel" and electron "reservoir", thereby accelerating the redox cycle of W/W to phenomenally enhanced production of O and ·O species involving interfacial reactions. Simulated adsorption and cleavage behaviors of HO on BW revealed a lower Gibbs free energy difference (ΔG) for O evolution (1.90 eV) compared to ‧OH (4.10 eV) evolution. The optimal BW-10 PFLS is efficient in various pollutants removal, with the maximum degradation rate constant (k) for RhB being 25.9 and 6.4 times higher than that of conventional Fenton-like and photocatalytic systems, respectively. It also exhibited outstanding synergistic degradation performance with 83.2 % TC-HCl and 98.6 % RhB removal in their mixed solution. Meanwhile, the BW-10 PFLS had excellent recyclability and anti-interference capability in complex real water matrices. Additionally, the bean sprout growth experiments demonstrated the negligible toxicity of the degradation products in the BW-10 PFLS. This work provides a fresh insight into the design of WO-based photo-Fenton-like photocatalysts for environmental remediation.
类光芬顿催化反应由于光催化与过氧化物活化之间的协同作用,在环境修复方面表现出显著的效果。在此,通过微波诱导溶剂热法,利用柚子皮衍生的生物质碳量子点(BCD)来调控具有双反应中心的BCD/WO(BW)复合材料,形成无铁类光芬顿体系(PFLS)。在BW异质界面处内置电场的驱动下,阐明了一种Z型电荷转移途径,该途径使光激发电子从WO快速转移至BCD。值得注意的是,BCD上的双反应中心和WO富含电子的氧空位既作为电子传输“通道”又作为电子“储存库”,从而加速W/W的氧化还原循环,显著增强涉及界面反应的O和·O物种的生成。HO在BW上的模拟吸附和裂解行为表明,与·OH生成(4.10 eV)相比,O生成的吉布斯自由能差(ΔG)更低(1.90 eV)。最佳的BW-10 PFLS对各种污染物的去除效率很高,RhB的最大降解速率常数(k)分别比传统类芬顿和光催化体系高25.9倍和6.4倍。在混合溶液中,它还表现出出色的协同降解性能,对TC-HCl的去除率为83.2%,对RhB的去除率为98.6%。同时,BW-10 PFLS在复杂的实际水基质中具有出色的可回收性和抗干扰能力。此外,豆芽生长实验表明BW-10 PFLS中降解产物的毒性可忽略不计。这项工作为基于WO的类光芬顿光催化剂用于环境修复的设计提供了新的见解。