博碩士論文 107324068 完整後設資料紀錄

DC 欄位 語言
DC.contributor化學工程與材料工程學系zh_TW
DC.creator趙冠傑zh_TW
DC.creatorGuan-Jie Zhaoen_US
dc.date.accessioned2020-8-18T07:39:07Z
dc.date.available2020-8-18T07:39:07Z
dc.date.issued2020
dc.identifier.urihttp://ir.lib.ncu.edu.tw:88/thesis/view_etd.asp?URN=107324068
dc.contributor.department化學工程與材料工程學系zh_TW
DC.description國立中央大學zh_TW
DC.descriptionNational Central Universityen_US
dc.description.abstract光電化學系統(PEC)可以像自然界通過光合作用一樣直接利用半導體 電極中的光生電子-電動對來催化反應,若使用生物質當反應物進行選擇性氧化來生成高經濟價值的產物,將是一道對環境友善且節省能源的製程。我們 究 嘗 試 開 發 吸 收 可 見 光 的 光 陽 極 , 並 應 用 在 5- 羥甲基糠醛 (5-hydroxymethylfurfural, HMF)的選擇性氧化上。本研究首先用旋轉塗佈法製備 BiVO4 薄膜光電極,並經由塗佈緩衝層、保護層和裝載共觸媒來提升光電極之性能。緩衝層改善了 BiVO4 表面的性質,使晶粒更為均一完整,在1.2 V vs. RHE 下,光電流密度提升 33%,且 IPCE 在波段 400 nm 時從 16%提升至 34%;NiOx 共觸媒的裝載提升了氧化動力,讓水解反應之起始電位往還原方向 0.2 V vs. RHE,但在高偏壓區的電流卻出現被抑制的情形,代表也存在界面與表面的問題需要克服;保護層 TiO2 的性質有類似透明導電氧化物(Transparent conductive oxide)的作用,能有效降低半導體與電解液界面之電子-電洞對再結合。而後我們選用光電流密度最高的 BiVO4/SnO2光電極在不同離子電解液與 pH 值環境下測試穩定性,發現在 pH=10 的硼酸鈉緩衝溶液有最好的表現性,並在此進行 HMF 之選擇性氧化反應。我們藉由 TEMPO 當反應媒介,成功轉化出產物 FDCA,在反應總載子數為 78 庫倫後,HMF 有 74%的轉化率,FFCA 與 FDCA 分別有 29%、30%的產率,40%、41%的選擇率,法拉第效率為 91%。而由濃度變化的計算,我們得出 HMF 為一級反應。zh_TW
dc.description.abstractThe photoelectrochemical (PEC) can directly utilize the photo-generatedelectron-hole pair in semiconductor electrode to catalyze the reaction like nature through photosynthesis. If the biomass is used as the reactant for selectiveoxidation to generate a product of high economic value, it will be anenvironmentally friendly and energy-saving process. We tried to develop a photoanode that absorbs visible light and applies it to the selective oxidation of 5-hydroxymethylfurfural (HMF). In this study, the BiVO4 thin film photoelectrode was first prepared by spin coating, and the performance of the photoelectrode was improved by coating a buffer layer, a protective layer, and a co-catalyst. The buffer layer improves the properties of the BiVO4 structure, making the grain moreuniform and complete. At 1.2 V vs. RHE, the photocurrent is increased by 33%,and the IPCE is increased from 16% to 34% at 400 nm. Loading of the NiOx cocatalyst improves the oxidation kinetics, shifting the oneset potential to thenegative side by 0.2 V vs. RHE of the water splitting reaction, but the current in the high-bias region is suppressed, indicating that there are also problems with theinterface and surface. The property of the protective layer TiO2 is similar to that of a transparent conductive oxide (TCO), which can effectively reduce the recombination of electron-hole pairs at the interface between the semiconductorand the electrolyte. After that, we selected the BiVO4/SnO2 photoelectrode with the highestphotocurrent properties to test the stability under different electrolytes and pH environments, and found that the borate buffer solution at pH=10 showed the best performance. By using TEMPO as the mediator, we have demonstrated a electrochemicaloxidation of HMF into FDCA. When 78 C was passed, HMF had a conversion rate of 74%, FFCA and FDCA had 29%, 30% yield, and 40%, 41% selectivity,Faraday efficiency is 91%. From the calculation of the concentration change, we conclude that HMF is a first order reaction.en_US
DC.subject光陽極zh_TW
DC.subject選擇性氧化zh_TW
DC.subject5-羥甲基糠醛zh_TW
DC.subjectBiVO4en_US
DC.subjectselectove oxidationen_US
DC.subjectHMFen_US
DC.titleBiVO4為基底的光陽極應用在選擇性氧化HMF及其衍生物zh_TW
dc.language.isozh-TWzh-TW
DC.titlePhotoelectrochemical selective oxidation of HMF derivatives on BiVO4-based photoanodeen_US
DC.type博碩士論文zh_TW
DC.typethesisen_US
DC.publisherNational Central Universityen_US

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