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Single-layer HNb3O8 with strong and nearby Lewis and Brønsted acid sites boosts amide bond hydrolysis for urease mimicking

尿素酶 催化作用 水解 尿素 化学 酰胺 热稳定性 路易斯酸 环境污染 三聚氰酸 有机化学 三聚氰胺 环境保护 环境科学
作者
Guohan Sun,Bo Yuan,Xinyu Wu,Shun Ying Lau,Linyuan Tian,Jung‐Hoon Lee,Keizo Nakagawa,Yung‐Kang Peng
出处
期刊:Nanoscale [Royal Society of Chemistry]
卷期号:15 (22): 9752-9758 被引量:1
标识
DOI:10.1039/d3nr01262j
摘要

Urea pollution is a growing environmental concern, and its removal via catalytic hydrolysis is challenging due to the resonance-stabilized amide bonds. In nature, this reaction is catalyzed by ureases in many soil bacteria. However, the remedy of this problem with natural enzymes is not feasible as they are easily denatured and require high costs for both preparation and storage. Given this, the development of nanomaterials bearing enzyme-like activity (nanozymes) with advantages such as low production cost, simple storage, and pH/thermal stability has attracted much attention over the past decade. As inspired by the mechanism of urease-catalyzed urea hydrolysis, the co-presence of Lewis acid (LA) and Brønsted acid (BA) sites is imperative to proceed with this reaction. Herein, layered HNb3O8 samples with intrinsic BA sites were adopted for investigation. The layer reduction of this material to few-/single layers can expose Nb sites with various LA strengths depending on the degree of NbO6 distortion. Among the catalysts examined, single-layer HNb3O8 bearing strong LA and BA sites displays the best hydrolytic activity towards acetamide and urea. This sample with high thermal stability was found to outperform urease at temperatures higher than 50 °C. The acidity-activity correlation established in this study is believed to guide the future design of industrial catalysts to remediate urea pollution.
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