Catalytic Dephosphorylation Using Ceria Nanocrystals

Catalytic Dephosphorylation Using Ceria Nanocrystals
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DOI:
10.1021/acscatal.6b03472
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发表时间:
2017-03-01
期刊:
影响因子:
12.9
通讯作者:
Wang, Chao
Wang, Chao
中科院分区:
化学1区
文献类型:
--
作者:
Manto, Michael J.;Xie, Pengfei;Wang, Chao

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磷是生命系统的重要元素,在植物生长中起着重要作用。然而,当今世界的磷供应依赖于耗尽的原料,如磷酸盐岩,而对磷肥的需求随着人口的持续增长而升级。因此,迫切需要开发磷的可持续来源和生产方法。在这里,我们报告了从有机和生物分子中回收磷的催化去磷酸化。通过形貌控制合成了CeO2纳米晶,并将其作为人工磷酸酶,在水溶液中裂解对硝基苯基磷酸酯中的磷酸酯键,释放出游离的磷酸根阴离子。在不同温度下的CeO2纳米晶体上的脱磷酸化反应进行了研究,以评估速率常数,活化能和可回收性对颗粒形状的依赖性。在这些研究中建立的结构性质关系表明,CeO2表面的氧空位是脱磷酸化的活性位点。
Phosphorus is a crucial element for living systems and plays significant roles in plant growth. The world's supply of phosphorus today, however, relies on depleting feedstocks such as phosphate rocks, while the demand for phosphorus fertilizers escalates as the population continues to grow. It is thus urgent to develop sustainable sources and production methods for phosphorus. Here, we report on catalytic dephosphorylation for phosphorus recovery from organic and biological molecules. Ceria (CeO2) nanocrystals were synthesized with shape control and applied as artificial phosphatases to cleave the phosphate ester bond in paranitrophenyl phosphate and release free phosphate anions in aqueous solutions. The dephosphorylation reaction was studied on the CeO2 nanocrystals at various temperatures to evaluate the dependences of rate constant, activation energy, and recyclability on the particle shape. The structure property relationships established in these studies suggest that the oxygen vacancies on the surface of CeO2 are the active sites for dephosphorylation.