Bimetal-organic frameworks with coordinatively unsaturated metal sites for highly efficient Fenton-like catalysis
文献类型：期刊论文
| 作者 | Liang, He; Liu, Ruiping; An, Xiaoqiang; Hu, Chengzhi; Zhang, Xiwang; Liu, Huijuan |
| 刊名 | CHEMICAL ENGINEERING JOURNAL
 |
| 出版日期 | 2021-06-15 |
| 卷号 | 414页码:- |
| ISSN号 | 1385-8947 |
| 关键词 | Fenton-like catalysis Coordinatively unsaturated metal sites CUMSs/MIL-101(Fe,Cu) H2O2 activation Ciprofloxacin Density functional theory |
| 英文摘要 | Recently, Fe-based metal-organic frameworks (Fe-MOFs) have been widely investigated as Fenton-like catalysts for environmental applications. However, their catalytic performance is limited by the insufficient number of Lewis acid sites for hydrogen peroxide (H2O2) activation and the slow Fe(III)-Fe(II) conversion. To overcome these limitations, coordinatively unsaturated iron-copper bimetallic sites may serve as Lewis acid sites, thus enhancing Fenton-like catalytic activity. Herein, we successfully synthesized a new Fenton-like catalyst of CUMSs/MIL-101(Fe,Cu), i.e., MIL-101 (MIL, Mat ' erial Institute Lavoisier) with mixed valence of Fe(II)/Fe(III) and Cu(I)/Cu(II) as coordinatively unsaturated metal sites (CUMSs). Further, we evaluated the performance of catalytically activating H2O2 for ciprofloxacin (CIP) degradation. The results indicate a rapid CIP degradation by dosing CUMSs/MIL-101(Fe,Cu) (0.1 g.L-1) and H2O2 (3 mM) in the neutral pH range, with a 20-fold higher apparent rate constant than in a MIL-101(Fe)/H2O2 system. Various conditions of initial pH, catalyst amount, H2O2 concentration, and coexisting anions on the CIP degradation were systematically investigated for optimizing CIP degradation. Furthermore, we identified the intermediates during the CIP degradation and proposed the possible degradation pathways. We concluded that the thermodynamically favorable reaction between Cu(I) and Fe(III) and p-cation interactions accelerate the redox cycles of Fe(II)/Fe(III) and Cu(I)/Cu(II) CUMSs and this effect improves the Fenton-like performance over a broad pH range. Density functional theory calculations further clarified the dissociation process and the corresponding energy barriers of H2O2 at the atomic level. This work offers a new way for designing highly efficient, stable and harmless Fenton-like catalysts for achieving excellent environmental remediation efficiency over a wide pH range. |
| WOS研究方向 | Engineering, Environmental ; Engineering, Chemical |
| 源URL | [http://ir.rcees.ac.cn/handle/311016/45914]  |
| 专题 | 生态环境研究中心_环境水质学国家重点实验室 |
| 作者单位 | 1.Northeast Normal Univ, Sch Environm, Changchun 130117, Jilin, Peoples R China 2.Tsinghua Univ, Ctr Water & Ecol, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100084, Peoples R China 3.Monash Univ, Dept Chem Engn, Clayton, Vic 3800, Australia 4.Univ Chinese Acad Sci, Beijing 100039, Peoples R China 5.Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Lab Environm Aquat Chem, Beijing 100085, Peoples R China |
| 推荐引用方式 GB/T 7714 | Liang, He,Liu, Ruiping,An, Xiaoqiang,et al. Bimetal-organic frameworks with coordinatively unsaturated metal sites for highly efficient Fenton-like catalysis[J]. CHEMICAL ENGINEERING JOURNAL,2021,414:-. |
| APA | Liang, He,Liu, Ruiping,An, Xiaoqiang,Hu, Chengzhi,Zhang, Xiwang,&Liu, Huijuan.(2021).Bimetal-organic frameworks with coordinatively unsaturated metal sites for highly efficient Fenton-like catalysis.CHEMICAL ENGINEERING JOURNAL,414,-. |
| MLA | Liang, He,et al."Bimetal-organic frameworks with coordinatively unsaturated metal sites for highly efficient Fenton-like catalysis".CHEMICAL ENGINEERING JOURNAL 414(2021):-. |
入库方式： OAI收割
来源：生态环境研究中心
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