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標題: | 電催化產氫之表面電荷效應 Surface-charging effect on electrocatalytic hydrogen evolution |
作者: | 陳彥妤 Yen-Yu Chen |
指導教授: | 陳浩銘 Hao Ming Chen |
關鍵字: | 單原子催化劑,電解水產氫反應,臨場光譜分析,X光吸收譜,中間體, single-atom catalysts,HER,in-situ spectroscopy,XAS,intermediates, |
出版年 : | 2023 |
學位: | 碩士 |
摘要: | 隨著化石燃料使用率的提升導致二氧化碳排放逐年上升,全球暖化的問題越來越嚴重,因此通過開發綠氫來取代化石燃料能源有助於減少二氧化碳的排放。其中,電解水產氫反應(HER)可以說是現今開發綠氫的一大主流,有許多研究已經開發多種不同電催化劑以提高產氫效率,並通過薩巴捷原理之火山圖呈現並解釋。在薩巴捷原理中,鍵結能是探討這個原理中最關鍵的因素,但是鍵結能的概念從理論預測或從實驗的角度來說都非常具有挑戰性,因此本研究將透過HER來深入探討其中。
本研究主要是通過簡單的HER機制了解關於反應中間體之鍵結能及電荷儲存在電催化劑表面之現象。對於反應中間體的探討,大多數的研究都是透過薩巴捷原理來解釋,然而實際上,真實反應過程中之環境複雜性及結構變動性造成與薩巴捷原理之火山圖形有所偏差。因此在本研究中,我們將通過探討5d單金屬原子模型在HER中的電荷儲存來了解中間體的鍵結性質,其中電荷儲存的情況會反應到氫電荷的覆蓋率,並透過固液界面中中間體之分子內相互作用決定,而這又與d電子的數量有直接的相關性。從臨場實驗結果中發現當動態d電子數為5時,可以達到一個最佳的分子內相互作用從而提供最佳的反應活性、最低的電荷轉移電阻及最少的電荷累積,也因此推敲出固液界面的結構及其對應之等效電路。通過這些發現我們可以將實驗和理論之間的關聯性連結起來,也能夠更準確的去設計出活性優異的催化劑材料,此外本研究提出之模型也可以被應用至其他電催化反應。 With the increasing use of fossil fuels leading to a rise in carbon dioxide emissions year by year, the issue of global warming is becoming increasingly severe. Therefore, developing green hydrogen as a substitute for fossil fuel energy helps reduce carbon dioxide emissions. Among various methods, the hydrogen evolution reaction (HER) through water electrolysis has become a major mainstream approach for green hydrogen production. Many studies have been conducted to develop different electrocatalysts to enhance hydrogen production efficiency and are explained using the Sabatier volcano plot. In the Sabatier principle, bond energy is a crucial factor, but the concept of bond energy is challenging from both theoretical predictions and experimental perspectives. Thus, this study aims to delve into the HER process to gain a deeper understanding. The primary focus of this research is to comprehend the bond energy of reaction intermediates and the charge storage phenomenon on the electrocatalyst surface during the HER mechanism. Previous studies have mostly explained the reaction intermediates through the Sabatier principle. However, due to the complexity of the actual reaction environment and structural variations, there are deviations from the volcano plot of the Sabatier principle. Therefore, in this study, we investigate the charge storage on 5d single-atom catalysts (SACs) models during HER to understand the bonding properties of intermediates. The charge storage affects the coverage of hydrogen charges, determined by the intramolecular interactions at the solid-liquid interface and directly related to the number of d-electrons. From in-situ experimental results, we find that when the dynamic d-electron count is 5, the optimal intramolecular interactions can be achieved, leading to the best reaction activity, lowest charge transfer resistance, and minimal charge accumulation. This insight helps deduce the structure of the solid-liquid interface and its corresponding equivalent circuit. By connecting these findings, we can establish a link between experiments and theories and design more accurate catalyst materials with excellent activity. Additionally, the proposed model in this study can be applied to other electrocatalytic reactions as well. |
URI: | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/90706 |
DOI: | 10.6342/NTU202303675 |
全文授權: | 同意授權(全球公開) |
顯示於系所單位: | 化學系 |
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