綠色合成氧化亞銅修飾二氧化鈦光電化學降解布洛芬、雙氯芬酸和磺胺甲噁唑

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Title:	綠色合成氧化亞銅修飾二氧化鈦光電化學降解布洛芬、雙氯芬酸和磺胺甲噁唑
Other Titles:	Green Synthesized Cu2O Coated Titanium Nanotube Arrays for Photoelectrochemical Degradation of Ibuprofen, Diclofenac and Sulfamethoxazole
Authors:	林琬淳
Contributors:	彭彥彬 PENG, YEN-PING 環境科學與工程學系
Keywords:	二氧化鈦奈米管陣列;氧化亞銅;布洛芬;雙氯芬酸;磺胺甲噁唑 Titanium dioxide nanotube arrays;Cu2O;Ibuprofen;Diclofenac;Sulfamethoxazole
Date:	2019
Issue Date:	2019-03-21T09:13:20Z (UTC)
Abstract:	本研究利用氧化亞銅修飾二氧化鈦奈米管陣列(Cuprous Oxide Coated Titanium Dioxide Nanotube Array, Cu2O/TNAs)光電化學系統降解藥物和個人護理產品(Pharmaceuticals and Personal Care Products, PPCP）布洛芬(Ibuprofen, IBU)、雙氯芬酸(Diclofenac, DLC)和磺胺甲噁唑(Sulfamethoxazole, SMX)。藉由方法方波伏安電化學沉積法(Square Wave Voltammetry Electrochemical Deposition Method, SWVE)結合綠色方法合成Cu2O/TNAs。光電化學(Photoelectrochemical, PEC)系統中應用三電極(工作電極、參考電極及對電極)，它結合光能、電能和化學能，相較光催化和電化學較為優勢。Cu2O/TNAs為p-n型半導體，光照會產生氫氧自由基可有效降解污染物。SEM顯示，Cu2O/TNAs管徑及管長分別約為100 nm和1.4 μm。TNAs經過Cu2O修飾後，TNAs的吸收波長紅移至537 nm且光電流效率為3.87 mA/cm2，遠高於TNAs (1.73 mA/cm2)。XRD分析證明在430℃鍛燒後，Cu2O/TNAs以銳鈦礦相為主。XPS化學組成成分分析結果證明Cu2O成功地摻附在TNA上。EIS和Bode圖在外加電位1V 100W 汞燈照射下，TNAs和Cu2O/TNAs的電子壽命τt分別為579.962和921.57 ms，證明修飾過後TNAs可以增加電子壽命。布洛芬，雙氯芬酸和磺胺甲噁唑經四小時PEC降解實驗分別在0.5、0.25和0.25小時後完全被降解； TOC去除率分別為42、49和51％；此時，陰極槽產氫量為分別為1241.7、1159.68和1295.09 μM/cm2。Cu2O/TNAs作為電極光電化學降解布洛芬、雙氯芬酸和磺胺甲噁唑利用液相層析-質譜(liquid chromatography mass spectrometry, LC-MS)分析，並提出了布洛芬，雙氯芬酸和磺胺甲噁唑可能的降解途徑，同時提出了轉化產物的化學結構。 This study employed Cuprous Oxide Coated Titanium Nanotube Arrays (Cu2O/TNAs) for Photoelectrochemical degradation of the Pharmaceuticals and Personal Care Products(PPCPs) ibuprofen(IBU), diclofenac(DLC) and sulfamethoxazole(SMX). Cu2O/TNAs were green synthesized by square wave voltammetry electrochemical deposition method (SWVE). Cu2O/TNAs produced the OH radical, which could in turn oxidize pollutants effectively. Photoelectrochemical (PEC) system combined photocatalysis and electrochemical, could overcome the recombination electron-hole pair. SEM images illustrated that the diameter and the length of the Cu2O/TNAs was approximately 100 nm and 1.4 μm, respectively. The absorption wavelength of TNAs red shifted to 537 nm after Cu2O coating. The photocurrent of Cu2O/TNAs (3.87 mA/cm2) was higher than that of TNAs (1.73 mA/cm2). XRD analysis showed that the Cu2O/TNAs was dominated by anatase phase after sintering at 430℃. Results of XPS indicated that the Cu2O was successfully coated on TNAs. The EIS and Bode plot revealed that the estimated electron lifetimes, τt, of TNAs and Cu2O/TNAs were 57.6979 and 92.1596 ms, respectively. The complete removal of ibuprofen, diclofenac and sulfamethoxazole after 4 h reaction time was observed at 0.5, 0.25 and 0.25 h, respectively, under 100 W Hg light illumination at 1 V(v.s AgCl) bias potential. The TOC removal rated of ibuprofen, diclofenac and sulfamethoxazole were 42, 49 and 51％, respectively, by employed Cu2O/TNAs PEC system. The amount of hydrogen yield was 1241.7, 1159.68 and 1295.09 μM/cm2 for ibuprofen, diclofenac and sulfamethoxazole. LC/MS analysis the pathways by which Cu2O/TNAs removed ibuprofen, diclofenac and sulfamethoxazole. The chemical structures of transformation products were proposed based on using liquid chromatography mass spectrometry (LC/MS). By-products and possible degradation pathways of ibuprofen, diclofenac and sulfamethoxazole were proposed in this study.
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