State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, 210023, China.
State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, Nanjing University, Nanjing, 210023, China.
Chemosphere. 2024 Jul;360:142359. doi: 10.1016/j.chemosphere.2024.142359. Epub 2024 May 21.
The excessive usage and emissions of triclosan (TCS) pose a serious threat to aquatic environments. Iron-based bimetallic particles (Pd/Fe, Ni/Fe, and Cu/Fe, etc.) were widely used for the degradation of chlorophenol pollutants. This study proposed a novel synthesis method for the preparation of Ni/Fe bimetallic particles (Ni-Fe) by ball milling microscale zero valent iron ZVI (mZVI) and NiSO. Ball-milling conditions such as ball-milling time, ball-milling speed and ball-to-powder ratio were optimized to prepare high activity Ni-Fe bimetallic particles. During the ball-milling process, Ni was reduced to Ni and formed a coupled structure with ZVI. The amount of Ni on ZVI significantly affected the activity of Ni-Fe bimetallic particles. The highest activity Ni-Fe bimetallic particles with Ni/Fe ratio of 0.03 were synthesized under optimized conditions, which could remove 86.56% of TCS (10 μM) in aerobic aqueous solution within 60 min. In addition, higher particle dosage, lower pH condition and higher reaction temperature were more conducive for TCS degradation. The higher corrosion current and lower electron transfer impedance of Ni-Fe bimetallic particles were the main reasons for its high activity. The hydrogen atom (•H) on the surface of Ni-Fe bimetallic particles was mainly contributed to the removal of TCS, as reductive transformation products of TCS were detected by LC-TOF-MS. Notably, a small amount of oxidation products were discovered. The total dechlorination rate of TCS was calculated to be 39.67%. After eight reaction cycles, the residual Ni-Fe bimetallic particles could still degrade 28.34% of TCS within 6 h. Low Ni leaching during reaction indicated that Ni-Fe bimetallic particles did not pose potential environmental risks. The prepared environmental-friendly Ni-Fe bimetallic particles with high activity have great potential in the degradation of other chlorinated organic compounds in wastewater.
三氯生(TCS)的过度使用和排放对水生环境构成了严重威胁。基于铁的双金属颗粒(Pd/Fe、Ni/Fe 和 Cu/Fe 等)被广泛用于降解氯酚污染物。本研究提出了一种通过球磨微尺度零价铁 ZVI(mZVI)和 NiSO4 制备 Ni/Fe 双金属颗粒(Ni-Fe)的新方法。优化了球磨时间、球磨速度和球料比等球磨条件,以制备高活性的 Ni-Fe 双金属颗粒。在球磨过程中,Ni 被还原为 Ni,并与 ZVI 形成耦合结构。ZVI 上 Ni 的含量显著影响 Ni-Fe 双金属颗粒的活性。在最佳条件下合成的 Ni/Fe 比为 0.03 的最高活性 Ni-Fe 双金属颗粒,可在有氧水溶液中 60 分钟内去除 86.56%的 TCS(10 μM)。此外,较高的颗粒用量、较低的 pH 值条件和较高的反应温度更有利于 TCS 的降解。Ni-Fe 双金属颗粒较高的腐蚀电流和较低的电子转移阻抗是其高活性的主要原因。Ni-Fe 双金属颗粒表面的氢原子(•H)主要有助于 TCS 的去除,因为通过 LC-TOF-MS 检测到了 TCS 的还原转化产物。值得注意的是,还发现了少量的氧化产物。TCS 的总脱氯率计算为 39.67%。经过 8 个反应循环后,剩余的 Ni-Fe 双金属颗粒仍可在 6 小时内降解 28.34%的 TCS。反应过程中 Ni 的浸出量低表明 Ni-Fe 双金属颗粒不会带来潜在的环境风险。制备的具有高活性的环保型 Ni-Fe 双金属颗粒在降解废水中其他氯化有机化合物方面具有巨大潜力。