Climate Change Technology Research Division, Korea Institute of Energy Research, 102 Gajeong-ro, Yuseong-gu, Daejeon 305-343, Korea.
Chemistry. 2012 Sep 17;18(38):12028-34. doi: 10.1002/chem.201201112. Epub 2012 Aug 9.
Bovine carbonic anhydrase (BCA) was covalently immobilized onto OAPS (octa(aminophenyl)silsesquioxane)-functionalized Fe(3)O(4)/SiO(2) nanoparticles by using glutaraldehyde as a spacer. The Fe(3)O(4) nanoparticles were coated with SiO(2), onto which was grafted OAPS, and the product was characterized using SEM, TEM, XRD, IR, X-ray photoelectron spectroscopy (XPS), and magnetometer analysis. The enzymatic activities of the free and Fe(3)O(4)/SiO(2)/OAPS-conjugated BCA (Fe-CA) were investigated by hydrolyzing p-nitrophenylacetate (p-NPA), and hydration and sequestration of CO(2) to CaCO(3). The CO(2) conversion efficiency and reusability of the Fe-CA were studied before and after washing the recovered Fe-CA by applying a magnetic field and quantifying the unreacted Ca(2+) ions by using ion chromatography. After 30 cycles, the Fe-CA displayed strong activity, and the CO(2) capture efficiency was 26-fold higher than that of the free enzyme. Storage stability studies suggested that Fe-CA retained nearly 82 % of its activity after 30 days. Nucleation of the precipitated CaCO(3) was monitored by using polarized light microscopy, which revealed the formation of two phases, calcite and valerite, at pH 10 upon addition of serine. The magnetic nanobiocatalyst was shown to be an excellent reusable catalyst for the sequestration of CO(2).
牛碳酸酐酶(BCA)通过戊二醛作为间隔臂共价固定在八(氨基苯基)倍半硅氧烷(OAPS)功能化的 Fe3O4/SiO2 纳米粒子上。Fe3O4 纳米粒子被 SiO2 包覆,其上接枝有 OAPS,并用 SEM、TEM、XRD、IR、X 射线光电子能谱(XPS)和磁力计分析对产物进行了表征。通过水解对硝基苯乙酸酯(p-NPA)、水化和将 CO2 螯合为 CaCO3,研究了游离态和 Fe3O4/SiO2/OAPS 接枝 BCA(Fe-CA)的酶活性。通过施加磁场回收 Fe-CA 并使用离子色谱定量未反应的 Ca2+离子,研究了回收的 Fe-CA 在洗涤前后的 CO2 转化率和可重复使用性。经过 30 个循环后,Fe-CA 仍表现出很强的活性,CO2 捕获效率比游离酶高 26 倍。储存稳定性研究表明,Fe-CA 在 30 天后仍保留近 82%的活性。通过偏光显微镜监测沉淀 CaCO3 的成核,发现在添加丝氨酸时,在 pH 10 下形成两种相,方解石和缬草酸钙。该磁性纳米生物催化剂是一种用于 CO2 螯合的优良可重复使用的催化剂。