超臨界流體萃取是從環境基質中分離化合物最有效的綠色化學技術之一。此外，藉由超臨界流體反應沉積可以快速產生形狀和大小受控的單金屬或雙金屬奈米粒子。本研究中，利用超臨界氫氣（scH2）將Pd或PdCu修飾在石墨烯奈米複合材料上。與氧化石墨烯（GO）和還原氧化石墨烯（rGO）相比，石墨烯薄片（GF）是更適合在用於合成出均勻且分散性良好之石墨烯基材（即Pd/GF和PdCu/GF）。在超臨界氫氣和超臨界二氧化碳（scH2/scCO2）流體系統中，作為非均相催化劑的Pd/GF和PdCu/GF分別對4-PBDE和4,4-PBDE這兩種含溴二苯醚催化降解。在最佳條件下，這兩種含溴環境污染物成功進行了脫溴和氫解反應，在反應中僅一個小時或更短的時間就產生了無毒性之降解產物。該技術除了具有成本效益，高效性和環境友好性的優勢，還能夠有效降解摻入模擬真實海沙中的4-PBDE，進一步證明了其未來巨大的潛力。

Supercritical fluid extraction is one of the most potent green chemistry techniques to separate chemical compounds from the environmental matrix. Besides, supercritical fluid reactive deposition can quickly produce the shape- and size-controlled mono- or bimetallic nanoparticles. In this study, Pd or PdCu nanoparticle decorated graphene nanocomposites were synthesized by a simple chemical reduction process using supercritical hydrogen fluid （scH2）. Compared to graphene oxide （GO） and reduced graphene oxide （rGO）, the graphene flake sheet （GF） is a suitable substrate for the preparation of well-dispersed Pd and PdCu nanoparticles on graphene-based heterostructures （i.e. Pd/GF and PdCu/GF, respectively）. Catalytic degradation of poly-brominated diphenyl ethers, including 4-PBDE and 4,4-PBDE, were individually performed over the Pd/GF and PdCu/GF as a heterogeneous catalyst in supercritical hydrogen and supercritical carbon dioxide （scH2/scCO2） fluid system. Under the optimized condition, successful debromination and hydrogenolysis reaction happened on those two bromine-containing environmental pollutants, to generate down-stream degraded products only in an hour or less. Owing to the advantages of cost-effectiveness, high potency, and environmentally friendliness, this technique was further demonstrated its great potential by effectively degradation of 4-PBDE spiked in sea sand.

第一章 緒論
第二章 文獻討論
第三章 研究方法
第四章 結果與討論
第五章 結論
第六章 參考資料

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