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优化掺氮污泥焦的制备及室温下 NO 催化氧化的机理研究。

Optimization of nitrogen-doped sludge char preparation and mechanism study for catalytic oxidation of NO at room temperature.

机构信息

College of Environmental Science and Engineering, Donghua University, Shanghai 201620, China.

College of Environmental Science and Engineering, Donghua University, Shanghai 201620, China.

出版信息

J Environ Sci (China). 2025 Apr;150:503-514. doi: 10.1016/j.jes.2023.11.025. Epub 2023 Dec 1.

Abstract

Catalytic oxidation of NO at room temperature was carried out over nitrogen (N)-doped sludge char (SC) prepared from pyrolysis of municipal sewage sludge, and urea was adopted as nitrogen source. The effects of different N-doping methods (one-step and two-step method), dried sludge (DS)/urea mass ratios (5:1, 4:1, 3:1, 2:1, and 1:1), SC preparation procedures (pyrolysis only, pyrolysis with acid washing, and pyrolysis with KOH activation and acid washing), and different pyrolysis temperatures (500, 600, 700, and 800°C) on the catalytic oxidation of NO were compared to optimize the procedure for SC preparation. The results indicated that N-doping could obviously promote the catalytic performance of SC. The one-step method with simultaneous sludge pyrolysis (at 700°C), KOH activation, and N-doping (DS/urea of 3:1) was the optimal procedure for preparing the N-doped SC with the NO conversion rate of 54.7%, whereas the optimal NO conversion rate of SC without N-doping was only 47.3%. Urea worked both as carbon and nitrogen source, which could increase about 2.9%-16.5% of carbon and 24.8%-42.7% of nitrogen content in SC pyrolyzed at 700°C. N-doping significantly promoted microporosity of SC. The optimal N-doped SC showed specific surface areas of 571.38 m/g, much higher than 374.34 m/g of the optimal SC without N-doping. In addition, N-doping also increased amorphousness and surface basicity of SC through the formation of N-containing groups. Finally, three reaction paths, i.e. microporous reactor, active sites, and basic site control path, were proposed to explain the mechanism of N-doping on promoting the catalytic performance of NO.

摘要

在室温下,通过在氮气(N)掺杂污泥炭(SC)上进行催化氧化,完成了对 NO 的催化氧化,该 SC 由城市污水污泥热解制成,且尿素被用作氮源。采用不同的 N 掺杂方法(一步法和两步法)、干燥污泥(DS)/尿素质量比(5:1、4:1、3:1、2:1 和 1:1)、SC 制备程序(仅热解、热解与酸洗、热解与 KOH 活化和酸洗)和不同的热解温度(500、600、700 和 800°C),对 NO 的催化氧化效果进行了比较,以优化 SC 制备程序。结果表明,N 掺杂可以明显提高 SC 的催化性能。通过同步进行污泥热解(700°C)、KOH 活化和 N 掺杂(DS/尿素比为 3:1)的一步法,制备出的 N 掺杂 SC 的 NO 转化率最高,为 54.7%,而未进行 N 掺杂的 SC 的最佳 NO 转化率仅为 47.3%。尿素既作为碳源又作为氮源,可以使在 700°C 热解的 SC 中的碳含量增加约 2.9%-16.5%,氮含量增加 24.8%-42.7%。N 掺杂显著提高了 SC 的微孔率。最佳 N 掺杂 SC 的比表面积高达 571.38 m/g,远高于未进行 N 掺杂的最佳 SC 的比表面积 374.34 m/g。此外,N 掺杂还通过形成含 N 基团来提高 SC 的非晶度和表面碱性。最后,提出了三种反应途径,即微孔反应器、活性位和碱性位控制途径,来解释 N 掺杂对促进 NO 催化性能的作用机制。

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