近年來透過環境友善方法以進行薄膜製備與膜表面改質引起廣泛之注意，特別是這類方法能有更優秀的防污性、表面潤濕性與重複使用性。利用生物高分子如多醣、多酚、多肽等得到不同表面改質之薄膜進而製備聚電解質複合物(PEC)，PEC因其多樣的表面官能基團而展現超親水及在水中的超疏油特性，使之預期能成為膜科學中極具潛力的技術。以生物高分子為基材的PEC塗佈膜在環境整治應用、廢水處理、油水分解、染料去除、蛋白質吸附、抗菌、太陽能海水淡化等面向皆能有優異的效用。本論文將聚焦在一些新穎生物高分子基礎之PEC塗佈膜的結構、特徵與應用，並針對不同環境汙染狀況整理並提出處置方案與材料。本文的第一章將有更詳盡之介紹；第二章則會闡述實驗之細節。
本文的第三章中，我們試著發展能處理油水乳液分離、染料廢水處理、太陽能水淨化之多功能光電PEC膜，此PEC膜由硫酸軟骨素(CS)作為陰離子型聚電解質材料並以二甲基二丙烯基氯化銨-丙烯醯胺共聚物(PAAm-DADMAc)作為陽離子處理，表面則透過PEC為顆粒自組裝成的花菜結構提供能達99.4%的油水乳液分離效率且在八個過濾循環後仍有2316 L m-2 h-1 bar-1的乳液滲透通量，此官能基團亦表現出超親水性及在水中對由高到低不同黏度的油皆表現的超疏油性(接觸角~150o)，由於PEC具充足的官能基團使其對陰離子型剛果紅染料、陽離子型亞甲藍染料及織物製程中產生之工業染料廢水皆能有效率的吸附並有99%的分離效率。除此之外，此PEC膜亦能用於太陽蒸氣淨水，在熱流密度 1 kW m–2下淨化含3.5%氯化鈉水，光熱轉換效率在經歷五個日照循環後亦能維持有2.31 kg m–2h–1之蒸氣效率。
第四章中則探討自組裝核-殼PEC用於蛋白質吸附和抗微生物性上。靜電吸附自組裝是最有機會可達成可調電荷及親水性之多層PEC，這種製備方法也用於製作防污薄膜，在此我們透過單寧酸(TA)交聯之微米顆粒以穩定尺寸而多層結構提供表面和孔洞之功能性，我們也對帶相反電荷之PEC進行蛋白質的置換吸附與蛋白質透過鹽析方式聚集做深入討論。透過將具有多孔性之聚電解質多層結構塗佈到醋酸纖維素(CS)上以達到蛋白質吸附，多層結構和PEC表面官能基團的協同作用使得抗微生物性、超親水性、滲透性、抗污性等皆有提升。
第五章討論使用合理化設計方法，以透過具有油/水乳液分離和能進行染料分離之PEC製備多功能性膜材料。在此多功能PEC膜中，嵌入混有奈米黏土鋰皂石(LP)之卡拉膠(CGN)，且其表面由單寧酸交聯而成。透過這種方法取得的多功能膜材料(TA@CGN-LP)塗佈到濾紙上以對亞甲藍基染料進行乳液分離。TA@CGN-LP塗佈膜具有超親水性，水中對原油的接觸角為150 o，在空氣下對水之接觸角為40 o，表面官能基團亦能提供優秀的乳液分離效率達99.8%及約1721 Lm-2h−1 bar-1之流速。
總的來說，我們設計的生物基PEC可作為膜表層鍍材，並能進行蛋白質分離、染料乳液分離、油水分離、廢水中之染料去除，此材料之優勢不僅在其能工業化製造，亦能對太陽能海水淡化與抗微生物性有更深入之學術與實務探討。

An ecofriendly synthetic approach to membrane preparation and membrane surface modification has received much attention due to its excellent antifouling, surface wettability, and reusability. Utilization of biopolymers to the membrane modification surface is highly desirable to the formation of polyelectrolyte complex (PEC) and is attributed to variable surface functional groups of the biopolymers such as polysaccharides, polyphenol, and polypeptides. Thus, PEC-based membranes materials preparation is anticipated as an appropriate candidate in separation science because of its superhydrophilic and underwater superoleophobic properties from the versatile surface functional groups. Particularly in environmental remedies applications, wastewater treatment oil-water separation, dye removal, protein adsorption, antibacterial properties, and solar desalination materials with excellent efficiency can be achieved when biopolymer-based PEC is coated on the surface of the membrane. Hence, this dissertation mainly focuses on the formation, characterization, and application of some novel biopolymers-based polyelectrolyte complex materials as membrane surface-modified materials to sort out the various environmental contamination as remedy materials are the main goal of this Ph.D. work. The content begins with a detailed introduction in the first chapter and described the experimental section in the second chapter.
Chapter 3 describes the development of multifunctional photothermal PEC membrane materials for oil/water emulsion separation, dye effluent removal, and solar water purification from chondroitin sulfate (CS) as anionic polyelectrolyte material, and treated with a cationic copolymer of poly (acrylamide-co-diallyl dimethylammonium chloride) (PAAm-DADMAc). The surfaces of the fabricated PEC cauliflower-like self-assembled microparticles exhibited good emulsion separation efficiency (99.4%) and emulsion permeation flux of 2316 L m-2 h-1 bar-1 after eight filtration cycles. The versatile functional groups were recognized for their superhydrophilicity and underwater superoleophobic nature (~150° of contact angle) for low-and high-viscosity oils. The abundance of functional groups of the PECs effectively absorbed anionic Congo red dye, cationic methylene blue dye, and textile dyeing industrial effluent with 99% separation efficiency. In addition, PEC modified membrane materials were successfully utilized as an effective solar steam generation to purify 3.5% NaCl contaminated water under 1 kW m–2. The efficient photo-thermal effects of PEC make a good evaporation rate and were retained with 2.31 kg m–2h–1 for five cycles.

Chapter 4 dealt with the fabrication of a self-assembled core-shell polyelectrolyte complex for protein adsorption and antimicrobial activity. Electrostatic assembly-based deposition of polyelectrolytes is a promising method for the preparation of multilayers with modified charge and hydrophilicity, as well as for the preparation of antifouling membranes. The Tannic acid (TA) crosslinked microparticle complex provides tight dimensional control and the multilayer provides functionalities on the surface and in the pores. Particularly, protein adsorption into polyelectrolyte microparticles via alternate adsorption of oppositely charged polyelectrolytes was investigated, and adsorbed protein aggregates generated by salting out proteins were used as a matrix. Polyelectrolyte multilayer systems are integrated into the pore structure of microporous, track-etched cellulose acetate membranes (CA) based on a convective transport of adsorbing species. The synergistic combination of the multilayer structure and surface functional groups of PEC enabled antimicrobial properties with superhydrophilicity, permeability, antifouling, and antibacterial properties.
Chapter 5 reported on a rational design for the fabrication of multifunctional membrane materials with a polyelectrolytic nature for oil/water emulsion separation, and dye mixed with emulsion separation. The multifunctional PEC membrane material was formed by intercalating through carrageenan (CGN) mixed with nanoclay laponite (LP), and its surface functionality was altered by the addition of Tannic acid (TA) for effective cross-link formation. The obtained multifunctional membrane (TA@CGN-LP) material was coated on filter paper for emulsion and methylene blue dye mixed with emulsion separation by filtration. The TA@CGN-LP coated membrane shows a superhydrophilic property with an underwater oil contact angle of 150° for crude oil and a water contact angle of 40° in air. Surface functional groups on the TA@CGN-LP membrane offer an excellent emulsion separation with high efficiency of 99.8% and a flux rate of approximately 1721 Lm-2h−1 bar-1.
Overall, the designed biopolymer-based PEC can offer a new route to treat protein separation, dye mixed emulsion separation, oil-in-water emulsions, and dye removal from wastewater as membrane surface modify materials at an industrial level with solar desalination and antimicrobial activity by providing essential insight into scientific and practical accessibility.

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