Graphite supported zero-valent iron-copper bimetallic catalysts (ZVI-Cu/C) were successfully prepared from mill scale (MS) waste and spent lithium-ion battery (LIB) anode using carbothermic reduction as a new approach for the recycling and revalorization of these waste. Cu and graphite were obtained from the LIB anodes, while ZVI was provided by MS waste. ZVI-Cu/C were synthesized with different MS to LIB anode powers mass ratios (1 to 4) and used as catalysts for the degradation of 4-chlorophenol (4-CP) in water by both reduction and heterogeneous Fenton reactions. ZVI-Cu/C-2 showed the highest removal percentage of 4-CP in both reactions. The degradation rates fitted well to a pseudo first-order model for both reactions. Moreover, ZVI-Cu/C-2 catalyst showed a relatively low lixiviation of iron and copper ions and a high activity in the 4-CP removal even in the fourth reuse cycle, which supports the high stability of the synthesized catalyst. Hydroquinone and 4-chlorocatechol were identified as the main intermediate by-products of 4-CP degradation. The results of this study support the possibility of synthesizing high active and stable ZVI-Cu/C catalysts using graphite and copper from spent LIB anode and iron oxide from MS waste. These catalysts show promising prospective for the removal of 4-CP in water, with comparable activities to others previously reported. This study reports, for the first time, the combined recycling of MS waste and spent LIB anodes to synthesize ZVI-Cu/C catalysts for water treatment by both oxidation and reduction reactions.

石墨负载零价铁铜双金属催化剂 (ZVI-Cu/C) 采用碳热还原作为回收和再利用的新方法，成功地从氧化皮 (MS) 废料和废锂离子电池 (LIB) 阳极制备这些废物。铜和石墨从 LIB 阳极获得，而 ZVI 由 MS 废料提供。以不同的 MS 与 LIB 阳极功率质量比（1 比 4）合成 ZVI-Cu/C，并用作通过还原和非均相 Fenton 反应降解水中 4-氯苯酚 (4-CP) 的催化剂。ZVI-Cu/C-2 在两个反应中均显示出最高的 4-CP 去除率。降解速率很好地拟合了两种反应的伪一级模型。而且，ZVI-Cu/C-2催化剂即使在第四次重复使用循环中也表现出相对较低的铁和铜离子浸出和4-CP去除的高活性，这支持了合成​​催化剂的高稳定性。对苯二酚和 4-氯儿茶酚被确定为 4-CP 降解的主要中间副产物。这项研究的结果支持使用来自废 LIB 阳极的石墨和铜以及来自 MS 废物的氧化铁合成高活性和稳定的 ZVI-Cu/C 催化剂的可能性。这些催化剂显示出去除水中 4-CP 的前景，其活性与之前报道的其他催化剂相当。本研究首次报道了 MS 废物和废 LIB 阳极的联合回收利用，通过氧化和还原反应合成用于水处理的 ZVI-Cu/C 催化剂。