Liu Nan, Zhang Jin, Cai Ya-Lan, Zhang Ji-Guo, Ouyang Du-Juan, Wang Shao-Bo, Xu Qi-Man, Hu Jia-Jun, Chen Di-Ming, Wang Guo-Wen, Li Ji-Xiang
Department of Material and Chemical Engineering, Zhengzhou University of Light Industry, Zhengzhou 450001, China.
Zhejiang Qiushi Environmental Monitoring Co., Ltd., Hangzhou 310000, China.
Toxics. 2025 Jun 14;13(6):503. doi: 10.3390/toxics13060503.
Recently, research has increasingly focused on the introduction of non-precious metals and developing highly stable carriers to enhance catalyst performance. In this study, we successfully synthesized copper (Cu)-modified biochar catalysts utilizing a sequential approach involving enzymatic treatment, liquid impregnation, and activation processes, which effectively enhanced the dispersion and introduction efficiency of Cu onto the biochar, thereby reducing the requisite Cu loading while maintaining high catalytic activity. The experimental results showed that the toluene degradation of 10%Cu@BCL was three times higher than that of unmodified activated carbon (AC) at 290 °C. A more uniform distribution of Cu was obtained by the enzymatic and activation treatments, optimizing the catalyst's structural properties and reducing the amount of Cu on the biochar. Moreover, the transformation between various oxidation states of Cu (from Cu/Cu(I) to Cu(II)) facilitated the electron transfer during the degradation of toluene. To further understand the catalytic mechanisms, density functional theory (DFT) calculations were employed to elucidate the interactions between toluene molecules and the Cu-modified biochar surface. These findings reveal that the strategic modification of biochar as a carrier not only enhances the dispersion and stability of active metal species but contributes to improved catalytic performance, thereby enhancing its degradation efficiency for VOCs in high-temperature conditions.
近年来,研究越来越多地集中在引入非贵金属和开发高度稳定的载体以提高催化剂性能。在本研究中,我们采用了一种包括酶处理、液体浸渍和活化过程的顺序方法,成功合成了铜(Cu)改性生物炭催化剂,该方法有效提高了Cu在生物炭上的分散性和引入效率,从而在保持高催化活性的同时降低了所需的Cu负载量。实验结果表明,在290℃下,10%Cu@BCL对甲苯的降解率是未改性活性炭(AC)的三倍。通过酶处理和活化处理获得了更均匀的Cu分布,优化了催化剂的结构性能并减少了生物炭上的Cu含量。此外,Cu的各种氧化态之间的转变(从Cu/Cu(I)到Cu(II))促进了甲苯降解过程中的电子转移。为了进一步了解催化机理,采用密度泛函理论(DFT)计算来阐明甲苯分子与Cu改性生物炭表面之间的相互作用。这些发现表明,作为载体对生物炭进行策略性改性不仅提高了活性金属物种的分散性和稳定性,而且有助于提高催化性能,从而提高其在高温条件下对挥发性有机化合物的降解效率。