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通过氮掺杂共修饰混合晶体TiO实现光催化直接将甲烷氧化为甲醛

Direct Photocatalytic Methane Oxidation to Formaldehyde by N Doping Co-Decorated Mixed Crystal TiO.

作者信息

Zhang Ruixue, Shi Jiale, Fu Lei, Liu Ya-Ge, Jia Yibing, Han Zhenyu, Yuan Kun, Jiang Hai-Ying

机构信息

Key Lab of Synthetic and Natural Functional Molecule Chemistry of Ministry of Education and the Energy and Catalysis Hub, College of Chemistry and Materials Science, Northwest University, Xi'an 710127, P.R. China.

College of Chemical Engineering and Technology, Tianshui Normal University, Tianshui 741001, P. R. China.

出版信息

ACS Nano. 2024 May 21;18(20):12994-13005. doi: 10.1021/acsnano.4c01318. Epub 2024 May 9.

Abstract

In this paper, N-doped TiO mixed crystals are prepared via direct calcination of TiN for highly selective oxidation of CH to HCHO at room temperature. The structures of the prepared TiO samples are characterized to be N-doped TiO of anatase and rutile mixed crystals. The crystal structures of TiO samples are determined by XRD spectra and Raman spectra, while N doping is demonstrated by TEM mapping, ONH inorganic element analysis, and high-resolution XPS results. Significantly, the production rate of HCHO is as high as 23.5 mmol·g·h with a selectivity over 90%. Mechanism studies reveal that HO is the main oxygen source and acts through the formation of ·OH. DFT calculations indicate that the construction of a mixed crystal structure and N-doping modification mainly act by increasing the adsorption capacity of HO. An efficient photocatalyst was prepared by us to convert CH to HCHO with high yield and selectivity, greatly promoting the development of the photocatalytic CH conversion study.

摘要

在本文中,通过直接煅烧TiN制备了N掺杂的TiO混合晶体,用于在室温下将CH高选择性氧化为HCHO。所制备的TiO样品的结构被表征为锐钛矿和金红石混合晶体的N掺杂TiO。TiO样品的晶体结构通过XRD光谱和拉曼光谱确定,而N掺杂通过TEM映射、ONH无机元素分析和高分辨率XPS结果得到证实。值得注意的是,HCHO的产率高达23.5 mmol·g·h,选择性超过90%。机理研究表明,HO是主要的氧源,并通过形成·OH起作用。DFT计算表明,混合晶体结构的构建和N掺杂改性主要通过提高HO的吸附能力起作用。我们制备了一种高效的光催化剂,以高产率和选择性将CH转化为HCHO,极大地推动了光催化CH转化研究的发展。

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