Wu Guangyu, Li Geng, Tang Yonggong, Tai Guoyu, Pan Yuwei, Han Jiangang, Xing Weinan
College of Ecology and the Environment, Co-Innovation Center for the Sustainable Forestry in Southern China, Nanjing Forestry University, Nanjing 210037, China.
Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology, School of Chemistry and Chemical Engineering, Guangxi University, Nanning 530004, China.
Langmuir. 2024 Dec 3;40(48):25657-25669. doi: 10.1021/acs.langmuir.4c03632. Epub 2024 Nov 19.
Constructing alternating donor-acceptor (D-A) units within g-CN represents an effective strategy for enhancing photocatalytic performance through improved charge carrier separation while concurrently addressing energy shortages and facilitating wastewater remediation. Here, a series of D-A-type conjugated photocatalysts (CNBTC-X) are prepared using g-CN as an acceptor unit and different masses of 5-bromo-2-thiophenecarboxaldehyde (BTC) as a donor unit by a one-step thermal polymerization. CNBTC-50 presents higher photocatalytic properties for CO reduction coupled with tetracycline (TC) removal than those of g-CN, CNBTC-10, CNBTC-30, and CNBTC-70. The introduction of the unique electron-donor-acceptor structure effectively drives the separation and transfer of photoinduced carriers while reducing the internal carrier transfer hindrance. Photocatalytic experiments reveal that the CNBTC-50 photocatalyst achieves up to 94.6% TC removal under visible light irradiation conditions. Compared with that of the pristine g-CN, the photocatalytic degradation reaction rate constant of CNBTC-50 is significantly increased by about 3.87 times. The study examines the influence of various reaction parameters on degradation activity, including catalyst concentration, pH, and TC concentration. Additionally, LC-MS is utilized to perform a comprehensive analysis of the intermediates and pathways involved in TC degradation. Furthermore, CNBTC-50 demonstrates remarkable photocatalytic CO reduction activity, achieving rates of 20.83 μmol g h (CO) and 9.36 μmol g h (CH), which are 10.68 and 5.98 times more efficient than those of g-CN, respectively. This work aims to offer valuable guidance for the rational design of nonmetal D-A-structured catalysts and effectively integrates reaction systems to couple CO reduction with antibiotic removal.
在石墨相氮化碳(g-CN)中构建交替的供体-受体(D-A)单元是一种有效的策略,可通过改善电荷载流子分离来提高光催化性能,同时解决能源短缺问题并促进废水处理。在此,以g-CN为受体单元,通过一步热聚合反应,使用不同质量的5-溴-2-噻吩甲醛(BTC)作为供体单元,制备了一系列D-A型共轭光催化剂(CNBTC-X)。与g-CN、CNBTC-10、CNBTC-30和CNBTC-70相比,CNBTC-50在光催化还原CO并去除四环素(TC)方面具有更高的光催化性能。独特的电子供体-受体结构的引入有效地驱动了光生载流子的分离和转移,同时降低了内部载流子转移的阻碍。光催化实验表明,在可见光照射条件下,CNBTC-50光催化剂对TC的去除率高达94.6%。与原始的g-CN相比,CNBTC-50的光催化降解反应速率常数显著提高了约3.87倍。该研究考察了各种反应参数对降解活性的影响,包括催化剂浓度、pH值和TC浓度。此外,利用液相色谱-质谱联用(LC-MS)对TC降解过程中涉及的中间体和途径进行了全面分析。此外,CNBTC-50表现出显著的光催化还原CO活性,CO生成速率为20.83 μmol g⁻¹ h⁻¹,CH生成速率为9.36 μmol g⁻¹ h⁻¹,分别是g-CN的10.68倍和5.98倍。这项工作旨在为非金属D-A结构催化剂的合理设计提供有价值的指导,并有效地整合反应体系,将CO还原与抗生素去除相结合。