釋氫用金屬奈米觸媒的探討(I)
學年 97
學期 1
出版(發表)日期 2009-01-01
作品名稱 釋氫用金屬奈米觸媒的探討(I)
作品名稱(其他語言) A Study of Metal Nanocatalysts for Hydrogen Evolution (I)
著者 鄧金培
單位 淡江大學化學學系
描述 計畫編號:NSC98-2113-M032-006 研究期間:200908~201007 研究經費:1,684,000
委託單位 行政院國家科學委員會
摘要 藉由未附著在載體的雙和參金屬奈米粒子,建立金屬奈米粒子對NaBH4 在 鹼性水溶液NaOH 水解反應中釋放氫氣與其粒子大小本質有關的催化活性,包 括:AgX、CuX、AuX、AgAuX、CuAuX 奈米粒子,X = Ru 或Pt。保護劑分子 可用在製備金和銀奈米粒子並控制其粒徑。同時,將製備不同金屬比例的雙和參 金屬合金奈米粒子和不同厚度比例的核-殻奈米粒子。同時,藉由調整金-銀合金 中(1)兩金屬的比例和(2)核-殻的厚度比例可以找到奈米合金最佳的催化活性; 這些結果是反應出合金中金屬在結構中混合的程度與Fermi level 平衡移動的位 置。最後,以單股DNA 修飾所有合成金屬奈米粒子的表面,並進一步與互補單 股DNA 修飾後的磁性奈米粒子自然結合而形成聚集;此奈米粒子聚集可被外加 磁鐵吸引並收集。藉由調整DNA 的長度便可以控制此聚集的分離溫度和金屬奈 米粒子的回收。這些研究結果將有助於雙和參金屬奈米觸媒的開發。 The intrinsic size-dependent catalytic activities of the bi- and tri-metallic nanoparticles (NPs) on H2 release by the hydrolysis of NaBH4 in aqueous NaOH solutions will be established with eliminating the support effect, including AgX, CuX, AuX, AgAuX, and CuAuX NPs, X = Ru or Pt. The preparation of all the metallic NPs may be size-controlled by the capping molecules. Moreover, the molar ratios of the two or three metals in the alloy NPs and the core/shell ratios in the core-shell NPs could be fine-tuned to exhibit their optimal activities. These results are taken as an indication for the structural change for the mixture of these atoms in the core-shell and alloy NPs, relating to the equilibration of Fermi level between them. Finally, the surface functionality of all the metallic NPs could be modified by the single-stranded DNA. After adding the complementary single-stranded DNA-derivatized magnetic NPs, the two DNA-derivatized NPs spontaneously aggregate and gathered by using an external magnet. The optimal dissociation temperature for recovering the metallic NPs will be established by adjusting the length of the DNA. They provide the useful information for developing the bi- and tri-metallic nanocatalysts.
關鍵字 釕奈米粒子; 鉑奈米粒子; 金-銀-釕合金和核-?奈米粒子; 磁性奈粒子; 氫氣; Ruthenium nanoparticles; Platinum nanoparticles; Au-Ag-Ru alloy andcore-shell nanoparticles; magnetic nanoparticles; Hydorgen
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