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表面限域原子银中心催化甲醛氧化。

Surface-confined atomic silver centers catalyzing formaldehyde oxidation.

机构信息

Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science and Engineering, Fudan University , Shanghai 200433, China.

出版信息

Environ Sci Technol. 2015 Feb 17;49(4):2384-90. doi: 10.1021/es504570n. Epub 2015 Jan 29.

Abstract

Formaldehyde (HCHO) is a prior pollutant in both indoor and outdoor air, and catalytic oxidation proves the most promising technology for HCHO abatement. For this purpose, supported metal catalysts with single silver atoms confined at 4-fold O4-terminated surface hollow sites of a hollandite manganese oxide (HMO) as catalytic centers were synthesized and investigated in the complete oxidation of HCHO. Synchrotron X-ray diffraction patterns, X-ray absorption spectra, and electron diffraction tomography revealed that geometric structures and electronic states of the catalytic centers were tuned by the changes of HMO structures via controllable metal-support interactions. The catalytic tests demonstrated that the catalytically active centers with high electronic density of states and strong redox ability are favorable for enhancement of the catalytic efficiency in the HCHO oxidation. This work provides a strategy for designing efficient oxidation catalysts for controlling air pollution.

摘要

甲醛(HCHO)是室内和室外空气的首要污染物,催化氧化被证明是去除 HCHO 的最有前途的技术。为此,我们合成了负载型金属催化剂,其中单原子银被限制在锰钙钛矿型氧化物(HMO)的 4 配位 O4 终止表面中空位作为催化中心,并研究了其在 HCHO 完全氧化中的性能。同步辐射 X 射线衍射图谱、X 射线吸收谱和电子衍射断层扫描揭示了通过可控的金属-载体相互作用,HMO 结构的变化可以调节催化中心的几何结构和电子态。催化测试表明,具有高密度态电子和强氧化还原能力的催化活性中心有利于提高 HCHO 氧化的催化效率。这项工作为设计用于控制空气污染的高效氧化催化剂提供了一种策略。

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