世界人口的快速增長與工業化的加快，不僅使自然資源枯竭、污染加劇，還產生了一個緊迫的全球性問題:水資源缺乏。薄膜技術是可以解決這些問題的一種永續且極具前景的方法。在許多添加於薄膜的材料中，氧化石墨烯 (graphene oxide, GO) 因為具有許多優勢而脫穎而出，例如: 高機械強度、高表面積以及可以促進協調性的眾多含氧官能基。

為了可以使用永續的方式解決水資源缺乏與污染的問題，並且回收有價值的資源，本研究有系統的探討GO在製備奈米過濾 (nanofiltration ,NF) 薄膜中的各種功能化和改質，用於不同廢水處理和海水淡化應用。透過調控不同GO薄膜的性質，例如:晶面間距 (d-spacing)、電性、親水性和自由體積，可以將欲處理物質:有毒離子和有害染料從廢水中分離。本研究的第一部分 (第4章)，探討在不同pH的環境下，對於GO分散性的影響；此外，也進一步探討這些條件對於GO薄膜交聯的影響。將所製備的薄膜用於重金屬離子的分離，可以對鉛金屬陽離子(Pb2+)有>95%的高截留率，這主要歸因於靜電的交互作用。

本研究的第二部分 (第 5 章)，進一步探討GO作為薄膜選擇層的功能，用來分離各種鹽類與染料，以取得乾淨的水。此部分使用含有不同官能基的各種交聯劑，用於奈米片的特定位置 (邊緣或基面)，得以調控GO薄膜的晶面間距(d-spacing)。由GO與二羧酸單體 (dicarboxylic acid monomer) 製備而成的薄膜，通量可以達到6.6 L m-2 h-1 bar-的PWP；對低分子量的染料，如:甲基橙和亞甲基藍，有高截留率（均達到>99.99%的選擇性）；對Na2SO4的選擇性約93%，可歸因於靜電的交互作用和尺寸篩分效應。

本研究的最後部分 (第6章)，深入探討GO作為thin-film nanocomposite (TFN) membranes的中間層，可以有效分離鹽類與染料的特質。此章節與前兩章節不同，不再探討GO同時對於鹽類與染料有顯著選擇性的優勢，而是設計了更寬鬆的薄膜結構，得以從紡織廢水中回收和再利用寶貴的資源。GO-TFN LNF membrane有約40 L m-2 h-1 bar-1的超高水滲透性；對低分子量的染料: Disperse Blue 1 (MW = 296.32 Da) 有傑出的截留率 (達到99.97%的選擇性)；對於氯化鈉鹽類的保留性極低(低至7.37%)。這種高分離效能顯示其用於處理紡織廢水的可行性。

總結，本博士論文對於 GO作為薄膜中主要選擇性層或中間層，進行了全面的探討，可以應用在廢水處理和海水淡化。而在各種奈米過濾製程中利用GO，也已驗證其可以永續地解決污染並同時回收資源。

The rapid growth of the world's population and the increasing pace of industrialization have not only depleted natural resources and escalated pollution but have also brought about a pressing global problem – water scarcity. Membrane technology distinguishes itself as a highly promising and sustainable approach to combat this series of problems, and among the numerous materials utilized as membrane materials, graphene oxide (GO) stands out due to its numerous favorable attributes such as its high mechanical strength, large surface area, and its abundant oxygen-containing functional groups that contribute to its tunability.

With the aim of addressing water scarcity and pollution in a sustainable manner, while simultaneously recovering valuable resources, this dissertation covers the systematic investigation of the functions and various modifications of GO in fabricating nanofiltration (NF) membranes for different wastewater treatment and desalination applications. Through controlled manipulation of the different properties of GO membranes such as the d-spacing, charge, hydrophilicity, and free volume, the regulated separation of target species such as toxic ions and harmful dyes from effluents can be achieved. The first part of this study (Chapter 4) deals with investigating the effects of dispersing GO in different pH environments on its fundamental properties, and explores the facilitation of crosslinking under such conditions. The resulting membranes were then employed to heavy metal ions separation application where a high Pb2+ rejection of >95% was achieved, which is mainly attributed to electrostatic interactions.

The second part (Chapter 5) of this study further examines GO's function as a membrane's selective layer in rejecting various salts and dyes to obtain clean water. This part proposes manipulation of GO's d-spacing by targeting specific locations of the nanosheets (edges or basal plane) using different crosslinkers that possess different functional groups. The membrane produced by crosslinking GO with a dicarboxylic acid monomer exhibited a PWP of 6.6 L m-2 h-1 bar-1, a high rejection of low-molecular-weight dyes, methyl orange and methylene blue (both reaching >99.99%), and an Na2SO4 rejection of around 93%, which could be ascribed to both electrostatic interaction and size sieving effects.

Lastly, the final part of this research (Chapter 6) delves into GO's role as an intermediate layer in thin-film nanocomposite (TFN) membranes that could efficiently fractionate dyes and salts. Unlike the two previous chapters that discussed impressive dyes and salts rejection simultaneously, a looser structure was engineered in this part in able to recover and reuse valuable resources from textile effluents. The resulting GO-TFN loose nanofiltration (LNF) membrane has an ultra-high water permeance of approximately 40 L m-2 h-1 bar-1, an excellent rejection of the low molecular weight dye, Disperse Blue 1 (MW = 296.32 Da), reaching 99.97%, and a very low retention of NaCl salt, as low as 7.37%. This high separation efficiency indicates its feasibility to be applied in textile wastewater treatment.

In conclusion, this dissertation presents a thorough analysis of the functions of GO (either as a main selective layer or an intermediate layer) in fabricating membranes for wastewater treatment and desalination applications. Herein, the practicality of utilizing GO in various NF processes for sustainably addressing pollution while recovering resources has been proven.

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