eg occupancy as an effective descriptor for the catalytic activity of perovskite oxide-based peroxidase mimics.,Nature Communications

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eg occupancy as an effective descriptor for the catalytic activity of perovskite oxide-based peroxidase mimics.
Nature Communications ( IF 14.7 ) Pub Date : 2019-02-11 , DOI: 10.1038/s41467-019-08657-5
Xiaoyu Wang ₁ , Xuejiao J Gao ₂ , Li Qin ₁ , Changda Wang ₃ , Li Song ₃ , Yong-Ning Zhou ₄ , Guoyin Zhu ₅ , Wen Cao ₁ , Shichao Lin ₁ , Liqi Zhou ₁ , Kang Wang ₆ , Huigang Zhang ₁ , Zhong Jin ₅ , Peng Wang ₁ , Xingfa Gao ₂ , Hui Wei _{1,

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Affiliation

A peroxidase catalyzes the oxidation of a substrate with a peroxide. The search for peroxidase-like and other enzyme-like nanomaterials (called nanozymes) mainly relies on trial-and-error strategies, due to the lack of predictive descriptors. To fill this gap, here we investigate the occupancy of eg orbitals as a possible descriptor for the peroxidase-like activity of transition metal oxide (including perovskite oxide) nanozymes. Both experimental measurements and density functional theory calculations reveal a volcano relationship between the eg occupancy and nanozymes' activity, with the highest peroxidase-like activities corresponding to eg occupancies of ~1.2. LaNiO3-δ, optimized based on the eg occupancy, exhibits an activity one to two orders of magnitude higher than that of other representative peroxidase-like nanozymes. This study shows that the eg occupancy is a predictive descriptor to guide the design of peroxidase-like nanozymes; in addition, it provides detailed insight into the catalytic mechanism of peroxidase-like nanozymes.

中文翻译：

例如，作为钙钛矿氧化物基过氧化物酶模拟物催化活性的有效描述指标。

过氧化物酶用过氧化物催化底物的氧化。由于缺乏预测性的描述，过氧化物酶类和其他酶类纳米材料（称为纳米酶）的搜索主要依靠反复试验的策略。为了填补这一空白，我们在这里调查了例如轨道的占用情况，以作为过渡金属氧化物（包括钙钛矿氧化物）纳米酶过氧化物酶样活性的一种可能的描述。实验测量和密度泛函理论计算均揭示了例如占有率与纳米酶活性之间的火山关系，其中最高的过氧化物酶样活性对应于例如约1.2的占有率。基于例如占用率优化的LaNiO3-δ表现出比其他代表性的过氧化物酶样纳米酶高一到两个数量级的活性。这项研究表明，例如占有率是指导过氧化物酶样纳米酶设计的预测指标。此外，它提供了过氧化物酶样纳米酶催化机理的详细见解。

更新日期：2019-02-11

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