Abstract
A highly efficient piezocatalyst of oxygen-incorporated MoS2 (O-MoS2) was designed and successfully synthesized via facile modulation of hydrothermal process temperature method. Remarkably, a superior piezocatalytic H2 evolution rate of 46.1 μmol·g−1·h−1 in pure water and 921.0 μmol·g−1·h−1 in methanol solution is obtained on optimal O-MoS2-180 (with a hydrothermal process temperature of 180 °C), outperforming pristine MoS2 and most of the reported other catalysts. Moreover, piezocatalytic activity of O-MoS2 toward the degradation of organic pollutants depends on hydrothermal temperatures. The suitable temperature of O-MoS2-180 presents dramatically excellent piezocatalytic capacity compared with the pristine MoS2 for degradation of methylene blue (MB) dye. The reaction rate constant of O-MoS2-180 reaches to 54.6 × 10−3 min−1, which is nearly 18 and 4-folds in contrast with pristine MoS2 and O-MoS2-140 (with a hydrothermal process temperature of 140 °C), respectively. Simultaneously, it also manifests that O-MoS2-180 endows relatively high degradation efficiency (84.6% within 30 min) and excellent stability. Moreover, it is also demonstrated that optimal O-MoS2 can dramatically promote charge carriers transport and separation. Furthermore, our theoretical calculation results suggest that the oxygen-incorporated can modulate the surface electronic state, enhance active sites as well as optimize the hydrogen adsorption Gibbs free energy of MoS2, thus extremely boosting piezocatalytic efficiency. Ultimately, an innovative piezocatalytic mechanism is proposed to reveal and expound the relationship between piezocatalytic property and oxygen-incorporated role.
Graphical abstract
摘要
本文采用简单调控水热温度的方法成功制备了高效的氧掺入二硫化钼(O-MoS2)压电催化剂。明显地,最优压电催化剂(O-MoS2-180)在纯水和甲醇溶液中分别表现出46.1 μmol·g−1·h−1 和921.0 μmol·g−1·h−1 优异的压电催化裂解水产氢速率,优于纯的MoS2和大多数已报道的其他体系催化剂。此外,O-MoS2降解有机污染物的压电催化活性取决于水热温度。与纯的MoS2相比,合适水热温度下的压电催化剂(O-MoS2-180)呈现出优异的压电催化降解亚甲基蓝(MB)染料能力,其动力学反应速率常数达到54.6 × 10−3 min−1,分别是原始MoS2和O-MoS2-140压电催化剂的18倍和4倍。同时,O-MoS2-180具有相对较高的压电催化降解效率(30分钟内达到84.6%)以及优异的稳定性。我们进一步证明了优化的O-MoS2可以显著地促进电荷载流子的输运和分离。此外,理论计算结果表明,氧的掺入可以调节MoS2的表面电子态、增强活性位点以及优化氢吸附吉布斯自由能,从而极大地提升其压电催化效率。最后,我们提出了一种新颖的压电催化机制并阐明了其压电催化性能与氧掺入作用之间的关系。
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This work was financially supported by the Talent Program of Tianshan Youth of Xinjiang Autonomous Region (No. 2020Q070) and the National Natural Science Foundation of China (No. 12064042).
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Ning, XE., Jia, DZ., Li, SH. et al. Oxygen-incorporated MoS2 catalyst for remarkable enhancing piezocatalytic H2 evolution and degradation of organic pollutant. Rare Met. 42, 3034–3045 (2023). https://doi.org/10.1007/s12598-023-02363-4
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DOI: https://doi.org/10.1007/s12598-023-02363-4