Nguyen Vinh Huu, Ha Hiep Quang, Nguyen Oanh T K, Thai Truc Thanh, Doan Que-Minh T, Hoang Lan-Anh T, Lee Taeyoon, Nguyen Trinh Duy
Center for High Technology Development, Nguyen Tat Thanh University, Ho Chi Minh City Hi-Tech Park, Ho Chi Minh City, Viet Nam; Institute of Applied Technology and Sustainable Development, Nguyen Tat Thanh University, Ho Chi Minh City, Viet Nam.
Center for High Technology Development, Nguyen Tat Thanh University, Ho Chi Minh City Hi-Tech Park, Ho Chi Minh City, Viet Nam; Faculty of Applied Science and Technology (FAST), Nguyen Tat Thanh University, Ho Chi Minh City, Viet Nam.
Environ Res. 2025 Sep 8;286(Pt 1):122805. doi: 10.1016/j.envres.2025.122805.
The development of novel multijunction heterostructure photocatalysts is critical for the efficient degradation of organic pollutants, attributed to their ability to enhance the separation of photogenerated electron-hole pairs. In our study, a ternary composite, melem/BiVO/g-CN (BVO/CNMH), was synthesized via an acid-soaking method followed by calcination, using g-CN as a sacrificial precursor in the presence of BiVO. This approach yielded a porous, interconnected architecture in BVO/CNMH. Detailed analyses revealed the retention of crystalline phases, enhanced light absorption, expanded photoactive surface sites, and improved charge separation kinetics. The heterostructure demonstrated exceptional photocatalytic performance in degrading tetracycline hydrochloride (TCH), achieving a removal efficiency of up to 99.68 % within 60 min of LED light irradiation, corresponding to rate constants 2.6 to 31.7 times higher than those of the individual semiconductors. Moreover, the heterostructure demonstrated excellent photocatalytic stability, retaining over 80 % of its TCH removal efficiency after five reuse cycles. The superior photocatalytic performance can be ascribed to the conjugated S-scheme charge transfer pathway, which collectively promoted the efficient preservation of highly active photogenerated charge carriers. Trapping experiments identified the reactive species, including O, photogenerated electrons, OH, and photogenerated holes, as the main contributors to TCH degradation. Based on experimental data, a degradation mechanism and pathway for TCH were proposed. The final degradation products exhibited significantly reduced acute and chronic toxicity compared to the parent compound. This study provides a novel strategy for constructing advanced g-CN-based multijunction heterostructure photocatalysts with strong potential for antibiotic wastewater remediation.
新型多结异质结构光催化剂的开发对于有机污染物的高效降解至关重要，这归因于它们能够增强光生电子 - 空穴对的分离。在我们的研究中，通过酸浸法然后煅烧合成了一种三元复合材料，三聚氰胺/钒酸铋/石墨相氮化碳（BVO/CNMH），在钒酸铋存在的情况下使用石墨相氮化碳作为牺牲前驱体。这种方法在BVO/CNMH中产生了一种多孔的、相互连接的结构。详细分析表明保留了晶相，增强了光吸收，扩大了光活性表面位点，并改善了电荷分离动力学。该异质结构在降解盐酸四环素（TCH）方面表现出优异的光催化性能，在LED光照射60分钟内实现了高达99.68%的去除效率，其速率常数比单个半导体高2.6至31.7倍。此外，该异质结构表现出优异的光催化稳定性，在五个重复使用循环后仍保留超过80%的TCH去除效率。优异的光催化性能可归因于共轭S型电荷转移途径，该途径共同促进了高活性光生电荷载流子的有效保存。捕获实验确定了活性物种，包括O、光生电子、OH和光生空穴，是TCH降解的主要贡献者。基于实验数据，提出了TCH的降解机理和途径。与母体化合物相比，最终降解产物的急性和慢性毒性显著降低。本研究为构建具有强大抗生素废水修复潜力的先进石墨相氮化碳基多结异质结构光催化剂提供了一种新策略。
