Abstract In this work, an acetylacetonate-modified equimolar SiO2–ZrO2 composite-derived membrane with molecular sieving properties was successfully fabricated. The sol-gel method was successfully employed to chemically modify zirconium tetrabutoxide prior to co-hydrolysis and -condensation with tetraethoxysilane, the resulting sol then used to fabricate a gas separation layer. An acetylacetonate-modified SiO2–ZrO2-derived membrane prepared at 300 °C showed H2 permeance of 9.9 × 10 −7 mol m−2 s−1 Pa−1 with a H2/SF6 permeance ratio of 7,600, which was a significant improvement over pure SiO2–ZrO2-derived membranes (H2 permeance: 1.4 × 10 −6 mol m−2 s−1 Pa−1, H2/SF6 permeance ratio: 11). Heat-treatment of an acac−-modified SiO2–ZrO2-derived membrane prepared at temperatures that ranged from 250 °C (H2 permeance: 4.5 × 10−8 mol m−2 s−1 Pa−1, H2/CH4: 100, CO2/CH4: 60, H2/SF6: >18,000 at 50 °C) to 550 °C resulted in an improved H2 permeance of 3.4 × 10−6 mol m−2 s−1 Pa−1 with reduced permeance ratios (H2/CH4: 3, H2/SF6: 9) at 50 °C. A membrane prepared by heat-treating a 250 °C-fired membrane at 300 °C showed the best trade-off with H2 permeance-H2/SF6 permeance ratios above the trade-off line compared with membranes prepared at other temperatures.

中文翻译：

---

适用于气体分离的乙酰丙酮改性二氧化硅-氧化锆复合膜的研制

摘要 在这项工作中，成功地制备了具有分子筛特性的乙酰丙酮改性等摩尔 SiO2-ZrO2 复合衍生膜。在与四乙氧基硅烷共水解和缩合之前，成功地采用溶胶-凝胶法对四丁氧基锆进行化学改性，然后将所得溶胶用于制造气体分离层。在 300 °C 下制备的乙酰丙酮改性 SiO2–ZrO2 衍生膜的 H2 渗透率为 9.9 × 10 -7 mol m-2 s-1 Pa-1，H2/SF6 渗透率为 7,600，与纯 SiO2–ZrO2 衍生膜（H2 渗透率：1.4 × 10 -6 mol m-2 s-1 Pa-1，H2/SF6 渗透率：11）。在 250 °C 范围内制备的 acac-改性 SiO2-ZrO2 衍生膜的热处理（H2 渗透率：4.5 × 10-8 mol m-2 s-1 Pa-1，H2/CH4：100, CO2/CH4: 60, H2/SF6: >18,000 at 50 °C) 到 550 °C 导致 H2 渗透率提高 3.4 × 10-6 mol m-2 s-1 Pa-1，同时渗透率降低（ H2/CH4: 3, H2/SF6: 9) 在 50 °C。与在其他温度下制备的膜相比，通过在 300°C 下对 250°C 烧制的膜进行热处理而制备的膜显示出在平衡线以上的 H2 渗透率-H2/SF6 渗透率比的最佳权衡。