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一步法合成 N 掺杂金属/生物炭复合材料,采用 NH 气氛热解,高效降解和矿化亚甲基蓝。

One-step synthesis of N-doped metal/biochar composite using NH-ambiance pyrolysis for efficient degradation and mineralization of Methylene Blue.

机构信息

CAS Key Laboratory of Crust-Mantle Materials and the Environments, School of Earth and Space Sciences, University of Science and Technology of China, Hefei 230026, China; State Key Laboratory of Loess and Quaternary Geology, Institute of Earth Environment, Chinese Academy of Sciences, Shaanxi 710075, China.

CAS Key Laboratory of Crust-Mantle Materials and the Environments, School of Earth and Space Sciences, University of Science and Technology of China, Hefei 230026, China; State Key Laboratory of Loess and Quaternary Geology, Institute of Earth Environment, Chinese Academy of Sciences, Shaanxi 710075, China.

出版信息

J Environ Sci (China). 2019 Apr;78:29-41. doi: 10.1016/j.jes.2018.06.014. Epub 2018 Jun 28.

Abstract

A series of new biochar-supported composite based on the combination of biochar and metallic nanoparticles (NPs) were produced through single-step pyrolysis of FeCl-Ti(OBu) laden agar biomass under NH environment. The physiochemical properties of composites were characterized thoroughly. It has found that heating temperature and N-doping through NH-ambiance pyrolysis significantly influence the visible-light sensitivity and bandgap energy of composites. The catalytic activities of composites were measured by degradation of Methylene Blue (MB) in the presence or absence of HO and visible-light irradiation. Our best catalyst (N-TiO-FeO-biochar) exhibits rapid and high MB removal competency (99.99%) via synergism of adsorption, photodegradation, and Fenton-like reaction. Continuous production of O and OH radicles performs MB degradation and mineralization, confirmed by scavenging experiments and degradation product analysis. The local trap state Ti, FeO, and N-carbon of the catalyst acted as active sites. It has suggested that the Ti and N-doped dense carbon layer improve charge separation and shuttle that prolonged photo-Fenton like reaction. Moreover, the catalyst is highly stable, collectible, and recyclable up to 5 cycles with high MB degradation efficiency. This work provides a new insight into the synthesis of highly visible-light sensitized biochar-supported photocatalyst through NH-ambiance pyrolysis of NPs-laden biomass.

摘要

一系列新型的基于生物炭和金属纳米粒子(NPs)复合的材料是通过在 NH 环境下,一步热解负载有 FeCl-Ti(OBu)的琼脂生物质制备得到的。对复合材料的物理化学性质进行了全面的表征。研究发现,加热温度和 NH 气氛热解过程中的 N 掺杂显著影响了复合材料的可见光敏感性和带隙能。通过在有或没有 HO 和可见光照射的情况下,用复合材料降解亚甲基蓝(MB)来测量其催化活性。我们的最佳催化剂(N-TiO-FeO-生物炭)通过吸附、光降解和类 Fenton 反应的协同作用,表现出快速和高的 MB 去除能力(99.99%)。通过清除实验和降解产物分析证实,连续产生的 O 和 OH 自由基使 MB 降解和矿化。催化剂中的局部陷阱态 Ti、FeO 和 N-碳作为活性位点。研究表明,Ti 和 N 掺杂的致密碳层提高了电荷分离和穿梭效应,从而延长了类光 Fenton 反应的时间。此外,该催化剂具有高度的稳定性、可回收性,可在 5 次循环内保持高的 MB 降解效率。这项工作为通过 NPs 负载生物质的 NH 气氛热解合成高可见光敏化的生物炭负载光催化剂提供了新的思路。

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