Facet-selective response of trigger molecule to CeO2 {110} for up-regulating oxidase-like activity
Facet-selective response of trigger molecule to CeO2 {110} for up-regulating oxidase-like activity
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DOI：
10.1016/j.cej.2017.08.026
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发表时间：
2017-12-15
影响因子：
15.1
通讯作者：
Wang, Jianlong
中科院分区：
文献类型：
--
作者：
Huang, Lunjie;Zhang, Wentao;Wang, Jianlong
纳米酶作为天然酶的强有力的替代物，通常遭受不令人满意的催化效率和有限的调节灵活性。在此，我们提出了一种新的策略来克服这些缺点，依赖于面选择性响应的外部触发分子，这增强了氧化酶样催化的纳米氧化铈。结果表明触发分子（即，硫酸根离子）优选结合到棒状纳米氧化铈（在其独特的{110}面上）而不是纳米多面体或纳米立方体。硫酸根离子处理的CeO 2纳米棒（SO 42- /CeO 2 NRs）成为可调控的高效氧化酶模拟物，其对3，3 '，5，5'-四甲基联苯胺（TMB）氧化的催化效率（k（cat）/K-m）比裸CeO 2 NRs提高了近20倍。这种调制策略，连同背后的机制，最终应用于开发比色生物传感器，这为嵌入系统在生物和环境网络铺平了道路。
Nanozymes, as a robust alternative to natural enzyme, usually suffer from unsatisfactory catalytic efficiency and limited modulating flexibility. Herein, we proposed a novel strategy to conquer these disadvantages relying on the facet-selective response of external trigger molecule which boosts the oxidase-like catalysis of nanoceria. Results indicate that the trigger molecule (i.e., sulfate ion) prefers to bind to the rod-like nanoceria (on its unique {1 1 0} facets) rather than nanopolyhedra or nanocubes. Sulfate ion-treated CeO2 nanorods (SO42- /CeO2 NRs) became modulatable oxidase mimetics of high efficiency, and the catalytic efficiency (k(cat)/K-m) of SO42- /CeO2 NRs improved by nearly 20-fold (versus that of the naked CeO2 NRs) for 3,3 ',5,5 '-tetramethylbenzidine (TMB) oxidation. This modulating strategy, together with the mechanism behind, is finally applied to develop colorimetric biosensors, which paves the way for embedding the system in biological and environmental networks.