Liu Lan-Ying, Liu Guo-Shuai, Niu Shi-Ming, Liu He, Cui Min-Hua, Wang Ai-Jie
Jiangsu Key Laboratory of Anaerobic Biotechnology, School of Environmental and Civil Engineering, Jiangnan University, Wuxi 214122, PR China.
Jiangsu Key Laboratory of Anaerobic Biotechnology, School of Environmental and Civil Engineering, Jiangnan University, Wuxi 214122, PR China; Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment, Suzhou University of Science and Technology, Suzhou 215009, PR China.
J Hazard Mater. 2023 Oct 5;459:132113. doi: 10.1016/j.jhazmat.2023.132113. Epub 2023 Jul 22.
In this study, a Pd@MXene catalyst was synthesized to enhance the electrocatalytic hydrodehalogenation (ECH) of emerging halogenated organic pollutants (HOPs) by improving the dispersibility, catalytic activity, and stability of palladium (Pd). The average size of Pd nanoparticles (NPs) was reduced to 3.62 ± 0.34 nm with a more intensive peak of Pd (111), which facilitated atomic hydrogen (H*) production. The Pd@MX/CC electrode demonstrated superior ECH activity for diclofenac (DCF) degradation, with a reaction rate constant (k) 2.48 times higher than that of Pd/CC (without MXene). The satisfactory ECH performance of Pd@MX/CC remained consistent within a wide range of initial DCF concentrations (5-100 mg/L), and no significant ECH attenuation was observed even after up to 10 batches. Furthermore, the high activity of Pd@MX/CC was also observed in the ECH of other halogenated organic pollutants (levofloxacin, tetrabromobisphenol A, and diatrizoate). Density functional theory (DFT) calculations revealed that electronic configuration modulation of the Pd@MXene catalyst optimized binging energies to H* , DCF, and dechlorinated products, thereby enhancing the ECH efficiency of DCF.
在本研究中，通过提高钯（Pd）的分散性、催化活性和稳定性，合成了一种Pd@MXene催化剂，以增强新型卤代有机污染物（HOPs）的电催化加氢脱卤（ECH）性能。Pd纳米颗粒（NPs）的平均尺寸减小到3.62±0.34 nm，且Pd（111）的峰更强，这有利于原子氢（H*）的产生。Pd@MX/CC电极对双氯芬酸（DCF）降解表现出优异的ECH活性，反应速率常数（k）比Pd/CC（无MXene）高2.48倍。在较宽的初始DCF浓度范围（5-100 mg/L）内，Pd@MX/CC的ECH性能令人满意，即使经过多达10批次的反应，也未观察到明显的ECH衰减。此外，在其他卤代有机污染物（左氧氟沙星、四溴双酚A和泛影酸盐）的ECH中也观察到了Pd@MX/CC的高活性。密度泛函理论（DFT）计算表明，Pd@MXene催化剂的电子构型调制优化了对H*、DCF和脱氯产物的结合能，从而提高了DCF的ECH效率。
