Biomedical Multidisciplinary Innovation Research Institute, Shanghai East Hospital, State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, 1239 Siping Road, Shanghai, 200092, China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai, 200092, China.
Biomedical Multidisciplinary Innovation Research Institute, Shanghai East Hospital, State Key Laboratory of Pollution Control and Resource Reuse, College of Environmental Science and Engineering, Tongji University, 1239 Siping Road, Shanghai, 200092, China; Shanghai Institute of Pollution Control and Ecological Security, Shanghai, 200092, China.
Chemosphere. 2020 Mar;243:125423. doi: 10.1016/j.chemosphere.2019.125423. Epub 2019 Nov 22.
Transition metal and nanocarbon-based composites with high activity and stability draw great attention in electro-Fenton system for organic pollutants removal. In this study, HKUST-1-derived Cu@C nanoparticles embedded within three-dimensional reduced graphene oxide (rGO) network (denoted as 3DG/Cu@C) is synthesized through a simple strategy. The prepared catalyst shows ordered 3D porous carbon structure and Cu@C NPs are uniformly dispersed in the matrix. The 3DG/Cu@C is used as heterogeneous electro-Fenton (hetero-EF) catalyst and shows outstanding performance in various persistent organic pollutants removal. High concentration Rhodamine B (RhB) (40 mg L) can achieve a complete decolorization within 150 min with 25 mg L 3DG/Cu@C catalyst, which is one of the lowest catalyst dosages in hetero-EF for RhB removal. More importantly, the 3DG/Cu@C achieves high RhB mineralization efficiency of 81.5% and exhibits high catalytic performance in a wide pH window from 3 to 9. The 3DG/Cu@C also remains high efficiency after five successive reaction cycles. The working mechanism study shows that RhB is mainly oxidized by OH and O radicals through hetero-EF and anodic oxidation processes. The high stability and outstanding performance of 3DG/Cu@C provide new insights in organic pollutants removal by hetero-EF process with transition metal and nanocarbon-based catalysts.
具有高活性和稳定性的过渡金属和基于纳米碳的复合材料在用于有机污染物去除的电芬顿系统中引起了极大的关注。在本研究中，通过一种简单的策略合成了负载在三维还原氧化石墨烯（rGO）网络内的 HKUST-1 衍生的 Cu@C 纳米颗粒（记为 3DG/Cu@C）。所制备的催化剂具有有序的 3D 多孔碳结构，并且 Cu@C NPs 均匀分散在基质中。3DG/Cu@C 被用作非均相电芬顿（hetero-EF）催化剂，并在各种持久性有机污染物去除方面表现出优异的性能。高浓度的 Rhodamine B（RhB）（40 mg L）在 25 mg L 3DG/Cu@C 催化剂存在下，仅需 150 min 即可完全脱色，这是 RhB 去除的 hetero-EF 中所需催化剂用量最低的之一。更重要的是，3DG/Cu@C 实现了 81.5%的高 RhB 矿化效率，并在 3 至 9 的宽 pH 窗口内表现出高催化性能。3DG/Cu@C 在五个连续反应循环后仍保持高效率。工作机制研究表明，RhB 主要通过电芬顿和阳极氧化过程中通过 OH 和 O 自由基被氧化。3DG/Cu@C 的高稳定性和卓越性能为基于过渡金属和纳米碳的催化剂的电芬顿工艺去除有机污染物提供了新的见解。
