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Trace FeCu@PC Derived from MOFs for Ultraefficient Heterogeneous Electro-Fenton Process: Enhanced Electron Transfer and Bimetallic Synergy
ACS ES&T Engineering Pub Date : 2021-07-28 , DOI: 10.1021/acsestengg.1c00131
Xuedong Du , Wenyang Fu , Pei Su , Linlan Su , Qizhan Zhang , Jingju Cai , Minghua Zhou

A Fe0/Cu0-based bimetallic submicro-particle core with porous carbon (PC) shell hybrid rods, i.e., core–shell structured FeCu@PC-800/6, was successfully fabricated from the mixture of MIL-88B(Fe) and Cu-BDC through pyrolysis at 800 °C for 6 h and employed as novel heterogeneous electro-Fenton (Hetero-EF) catalysts to remove sulfamethazine (SMT). A trace dose catalyst (25.0 mg L–1) could achieve efficient catalytic activity (turnover frequency (TOFd), 3.92 L g–1 min–1) due to the synergy of catalytic reactivity among iron, copper, and PC, possessing the pseudo-first-order rate for SMT removal that was 3.27-foldsand 4.08-fold of the Fe@PC-800/6/Hetero-EF and Cu@PC-800/6/Hetero-EF process, respectively. According to experiments and density functional theory (DFT) calculations, Hetero-EF reactions enhanced by internal-microelectrolysis (IME) were proposed, in which Cu0 promoted the electrons transfer of Fe0 to PC while the introduced Cu+ could promote the decomposition of H2O2 and the cycle of Fe3+/Fe2+. A possible mechanism and SMT degradation pathway were suggested for this Hetero-EF process, confirming that the surface-bound hydroxyl radical played a major role. This FeCu@PC-800/6 catalyst was cost-effective and could be reused after thermal treatment in H2, demonstrating super efficiency for organic contaminants degradation by EF process.

中文翻译:

源自 MOF 的痕量 FeCu@PC 用于超高效多相电芬顿工艺:增强的电子转移和双金属协同作用

由MIL-88B(Fe)的混合物成功制备了具有多孔碳(PC)壳杂化棒的Fe 0 /Cu 0基双金属亚微粒核,即核壳结构的FeCu@PC-800/6和 Cu-BDC 通过在 800°C 下热解 6 小时,并用作新型多相电芬顿 (Hetero-EF) 催化剂以去除磺胺二甲嘧啶 (SMT)。痕量催化剂 (25.0 mg L –1 ) 可以实现高效的催化活性(周转频率 (TOF d ),3.92 L g –1 min –1) 由于铁、铜和 PC 之间催化反应性的协同作用,SMT 去除的伪一级速率是 Fe@PC-800/6/Hetero-EF 和 Cu 的 3.27 倍和 4.08 倍@PC-800/6/Hetero-EF 过程,分别。根据实验和密度泛函理论(DFT)计算,提出了内微电解(IME)增强的杂-EF反应,其中Cu 0促进了Fe 0向PC的电子转移,而引入的Cu +可以促进Fe 0的分解。 H 2 O 2与Fe 3+ /Fe 2+循环. 提出了这种 Hetero-EF 过程的可能机制和 SMT 降解途径,证实了表面结合的羟基自由基发挥了主要作用。这种 FeCu@PC-800/6 催化剂具有成本效益,可在 H 2 中热处理后重复使用,证明了通过 EF 工艺降解有机污染物的超高效。
更新日期:2021-09-10
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