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Metallic Powder Promotes Nitridation Kinetics for Facile Synthesis of (Oxy)Nitride Photocatalysts
Advanced Materials ( IF 27.4 ) Pub Date : 2023-05-03 , DOI: 10.1002/adma.202302276 Yunfeng Bao 1 , Hai Zou 1, 2 , Shiwen Du 1 , Xueshang Xin 1, 2 , Shuowen Wang 1 , Guosheng Shao 3 , Fuxiang Zhang 1
Advanced Materials ( IF 27.4 ) Pub Date : 2023-05-03 , DOI: 10.1002/adma.202302276 Yunfeng Bao 1 , Hai Zou 1, 2 , Shiwen Du 1 , Xueshang Xin 1, 2 , Shuowen Wang 1 , Guosheng Shao 3 , Fuxiang Zhang 1
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Nitrogen-containing semiconductors (including metal nitrides, metal oxynitrides, and nitrogen-doped metal oxides) have been widely researched for their application in energy conversion and environmental purification because of their unique characteristics; however, their synthesis generally encounters significant challenges owing to sluggish nitridation kinetics. Herein, a metallic-powder-assisted nitridation method is developed that effectively promotes the kinetics of nitrogen insertion into oxide precursors and exhibits good generality. By employing metallic powders with low work functions as electronic modulators, a series of oxynitrides (i.e., LnTaON2 (Ln = La, Pr, Nd, Sm, and Gd), Zr2ON2, and LaTiO2N) can be prepared at lower nitridation temperatures and shorter nitridation periods to obtain comparable or even lower defect concentrations compared to those of the conventional thermal nitridation method, leading to superior photocatalytic performance. Moreover, some novel nitrogen-doped oxides (i.e., SrTiO3−xNy and Y2Zr2O7−xNy) with visible-light responses can be exploited. As revealed by density functional theory (DFT) calculations, the nitridation kinetics are enhanced via the effective electron transfer from the metallic powder to the oxide precursors, reducing the activation energy of nitrogen insertion. The modified nitridation route developed in this work is an alternative method for preparing (oxy)nitride-based materials for energy/environment-related heterogeneous catalysis.
中文翻译：
金属粉末促进氮化动力学，轻松合成（氧）氮化物光催化剂
含氮半导体（包括金属氮化物、金属氮氧化物和氮掺杂金属氧化物）因其独特的特性，在能量转换和环境净化方面的应用得到了广泛的研究；然而，由于氮化动力学缓慢，它们的合成通常会遇到重大挑战。本文开发了一种金属粉末辅助氮化方法，该方法有效促进了氮插入氧化物前驱体的动力学，并具有良好的通用性。通过采用低逸出功金属粉末作为电子调制剂，可以在以下条件下制备一系列氮氧化物（即LnTaON 2 (Ln = La、Pr、Nd、Sm和Gd)、Zr 2 ON 2和LaTiO 2 N）。与传统热氮化方法相比，更低的氮化温度和更短的氮化时间可以获得相当甚至更低的缺陷浓度，从而获得优异的光催化性能。此外，可以利用一些具有可见光响应的新型氮掺杂氧化物（即SrTiO 3− x N y和Y 2 Zr 2 O 7− x N y ）。密度泛函理论（DFT）计算表明，氮化动力学通过从金属粉末到氧化物前体的有效电子转移而增强，从而降低了氮插入的活化能。这项工作中开发的改进氮化路线是制备用于能源/环境相关多相催化的（氧）氮化物基材料的替代方法。
更新日期：2023-05-03
中文翻译：
金属粉末促进氮化动力学，轻松合成（氧）氮化物光催化剂
含氮半导体（包括金属氮化物、金属氮氧化物和氮掺杂金属氧化物）因其独特的特性，在能量转换和环境净化方面的应用得到了广泛的研究；然而，由于氮化动力学缓慢，它们的合成通常会遇到重大挑战。本文开发了一种金属粉末辅助氮化方法，该方法有效促进了氮插入氧化物前驱体的动力学，并具有良好的通用性。通过采用低逸出功金属粉末作为电子调制剂，可以在以下条件下制备一系列氮氧化物（即LnTaON 2 (Ln = La、Pr、Nd、Sm和Gd)、Zr 2 ON 2和LaTiO 2 N）。与传统热氮化方法相比，更低的氮化温度和更短的氮化时间可以获得相当甚至更低的缺陷浓度，从而获得优异的光催化性能。此外，可以利用一些具有可见光响应的新型氮掺杂氧化物（即SrTiO 3− x N y和Y 2 Zr 2 O 7− x N y ）。密度泛函理论（DFT）计算表明，氮化动力学通过从金属粉末到氧化物前体的有效电子转移而增强，从而降低了氮插入的活化能。这项工作中开发的改进氮化路线是制备用于能源/环境相关多相催化的（氧）氮化物基材料的替代方法。
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