Fang Liping, Xu Ling, Li Ji, Huang Li-Zhi
Guangdong Key Laboratory of Integrated Agro-environmental Pollution Control and Management, Guangdong Institute of Eco-Environmental Science & Technology, No. 808, Tianyuan Road, Guangzhou 510650, China.
Faculty of Material Science and Chemistry, China University of Geosciences, No. 388, Lumo Road, Wuhan 430074, China.
Sci Total Environ. 2019 Sep 15;683:275-283. doi: 10.1016/j.scitotenv.2019.05.273. Epub 2019 May 20.
The combined effect of copper nanoparticles (Cu NPs) and reduced graphene oxide (RGO) on the reactivity of green rust (GR) towards reductive debromination of tetrabromobisphenol (TBBPA) has been systematically investigated. The removal efficiency of TBBPA increased from 28.78% to 44.70% and the pseudo first-order rate constant (k) increased from 0.002 min to 0.004 min when the content of Cu NPs in GR-Cu NPs increased from 0% to 0.5%. Cu NPs enhanced the reductive reactivity of GR via formation of a galvanic cell and Cu/Cu redox cycle. The adsorption capacity of RGO towards TBBPA was 13.75 mg/g. The pseudo first-order rate constant for TBBPA removal increased from 0.0341 min to 0.0866 min when the RGO content increased from 0 to 2% in GR-Cu NPs-RGO. RGO enhanced the debromination efficiency via enhancing the adsorption of TBBPA and accelerating electron transfer amongst GR, Cu NPs and TBBPA. The increased corrosion current demonstrates the enhanced electron transfer by RGO in GR-Cu NPs galvanic cell. Six-electron transfer process of TBBPA reduction was revealed by rotating disk electrode analysis, which was in line with the final debromination products (Mono-BPA) determined by ion chromatography and liquid chromatography-mass spectrometry.
系统研究了铜纳米颗粒（Cu NPs）和还原氧化石墨烯（RGO）对绿锈（GR）对四溴双酚（TBBPA）还原脱溴反应活性的联合影响。当GR-Cu NPs中Cu NPs的含量从0%增加到0.5%时，TBBPA的去除效率从28.78%提高到44.70%，伪一级反应速率常数（k）从0.002 min增加到0.004 min。Cu NPs通过形成原电池和Cu/Cu氧化还原循环增强了GR的还原反应活性。RGO对TBBPA的吸附容量为13.75 mg/g。当GR-Cu NPs-RGO中RGO的含量从0增加到2%时，TBBPA去除的伪一级反应速率常数从0.0341 min增加到0.0866 min。RGO通过增强TBBPA的吸附以及加速GR、Cu NPs和TBBPA之间的电子转移提高了脱溴效率。腐蚀电流的增加表明RGO在GR-Cu NPs原电池中增强了电子转移。旋转圆盘电极分析揭示了TBBPA还原的六电子转移过程，这与离子色谱和液相色谱-质谱法测定的最终脱溴产物（单溴双酚A）一致。
