Regulating Oriented Adsorption on Targeted Nickel Sites for Antibiotic Oxidation with Simultaneous Hydrogen Energy Recovery by a Direct Electrochemical Process
文献类型：期刊论文
| 作者 | Liu, Chunlei; Zhang, Gong; Zhou, Wei; Zhang, Kai ; Qu, Jiuhui; Liu, Huijuan
|
| 刊名 | ACS APPLIED MATERIALS & INTERFACES
 |
| 出版日期 | 2021-04-28 |
| 卷号 | 13期号:16页码:18673-18682 |
| 关键词 | adsorption orientation (NiOOH)-O-III in situ Raman spectra antibiotic oxidation hydrogen energy recovery |
| ISSN号 | 1944-8244 |
| 英文摘要 | The efficiency of antibiotic oxidation by direct electrochemical processes based on transition metal electrodes is largely restricted by the adsorption capacity for single molecules on targeted active sites. Inspired by density functional theory (DFT) calculations, we found that the adsorption energy of sulfanilamide molecules on Ni sites could be markedly changed by regulating the local atomic environment of the Ni atoms (for NiCo2O4 and NiCoP, Delta G(Ni) = -0.11 and +0.47 eV, respectively). The high electronegativity of oxygen changed the electron cloud density around the Ni atoms, leading to an oriented adsorption of SA on Ni sites. Moreover, the oriented adsorption on Ni sites occurs not only on NiCo2O4 but on the in situ-generated (NiOOH)-O-III (Delta G(Ni) = -0.09 eV). Consequently, utilizing NiCo2O4 as the anode resulted in superior removal performance (97% vs 55% efficiency) for SA oxidation, with a kinetic constant similar to 10 times higher than that of NiCoP (0.031 min(-1) vs 0.0029 min(-1)). Meanwhile, non-oriented adsorption reduced the competition between SA molecules and H+ for active sites, which benefitted the activity of the hydrogen evolution reaction at the NiCoP cathode (68 mV at j = 10 mA.cm(-2), 0.5 mmol.L-1 SA added in). Furthermore, the in situ Raman spectra and DFT calculations confirmed that (NiOOH)-O-III dominated the oxidation process and terminated it at the p-benzoquinone stage. These findings provide a feasible strategy to combine electrochemical antibiotic oxidation by Ni-based electrodes with hydrogen energy recovery. |
| WOS研究方向 | Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary |
| 源URL | [http://ir.rcees.ac.cn/handle/311016/46257]  |
| 专题 | 生态环境研究中心_中国科学院饮用水科学与技术重点实验室 |
| 作者单位 | 1.Chinese Acad Sci, Res Ctr Ecoenvironm Sci, Key Lab Drinking Water Sci & Technol, Beijing 100085, 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.Beihang Univ, Beijing Adv Innovat Ctr Biomed Engn, Sch Chem, Beijing 100191, Peoples R China |
| 推荐引用方式 GB/T 7714 | Liu, Chunlei,Zhang, Gong,Zhou, Wei,et al. Regulating Oriented Adsorption on Targeted Nickel Sites for Antibiotic Oxidation with Simultaneous Hydrogen Energy Recovery by a Direct Electrochemical Process[J]. ACS APPLIED MATERIALS & INTERFACES,2021,13(16):18673-18682. |
| APA | Liu, Chunlei,Zhang, Gong,Zhou, Wei,Zhang, Kai,Qu, Jiuhui,&Liu, Huijuan.(2021).Regulating Oriented Adsorption on Targeted Nickel Sites for Antibiotic Oxidation with Simultaneous Hydrogen Energy Recovery by a Direct Electrochemical Process.ACS APPLIED MATERIALS & INTERFACES,13(16),18673-18682. |
| MLA | Liu, Chunlei,et al."Regulating Oriented Adsorption on Targeted Nickel Sites for Antibiotic Oxidation with Simultaneous Hydrogen Energy Recovery by a Direct Electrochemical Process".ACS APPLIED MATERIALS & INTERFACES 13.16(2021):18673-18682. |
入库方式： OAI收割
来源：生态环境研究中心
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