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硒氮共掺杂生物炭作为一种用于苯酚吸附和过一硫酸盐活化的新型无金属催化剂:阐明其增强的催化性能和稳定性

Selenium and nitrogen co-doped biochar as a new metal-free catalyst for adsorption of phenol and activation of peroxymonosulfate: Elucidating the enhanced catalytic performance and stability.

作者信息

Zhang Kejing, Min Xiaoye, Zhang Tingzheng, Xie Mingbo, Si Mengying, Chai Liyuan, Shi Yan

机构信息

School of Metallurgy and Environment, Central South University, Changsha 410083, PR China.

School of Metallurgy and Environment, Central South University, Changsha 410083, PR China; Chinese National Engineering Research Centre for Control & Treatment of Heavy Metal Pollution, Changsha 410083, PR China.

出版信息

J Hazard Mater. 2021 Jul 5;413:125294. doi: 10.1016/j.jhazmat.2021.125294. Epub 2021 Feb 3.

Abstract

Coupling of adsorption and advanced oxidation processes triggered by metal-free carbocatalysts is an appealing wastewater purification scheme. However, its practical application is challenging due to the unsatisfactory stability of conventional heteroatom-doped systems. Herein, we innovatively developed a simple and scalable biochemical strategy to synthesize selenium and nitrogen co-doped biochar (Se/N-BC) as a bifunctional catalyst of adsorption-oxidation. The Se/N-BC displays the highest efficiency of phenol (PE) degradation (99.2% of PE was removed within 5 min) with the lowest dosage of catalyst (0.1 g L) and peroxymonosulfate (PMS, 0.4 g L). More importantly, the Se/N-BC is not only universal in a wide pH range of 3.0-11.0 and complex ionic environment, but also possesses an excellent cycling stability. The Se/N co-doping induces a rapid cycle of adsorption-degradation for PE. The Se/N-BC acts as an "electron transfer bridge", guiding rapid electron transfer from PE to PMS to achieve high-efficient degradation. The Se/N co-doping facilitates the formation of graphitic N and unlocks the potential of adjacent C sites for PMS activation, consequently boost oxidation efficiency. In addition, the oxidation of catalyst is prevented due to the antioxidant properties of Se, which has been a primary concern either to regenerate adsorbate or to enhance degradation performance.

摘要

由无金属碳催化剂引发的吸附与高级氧化过程的耦合是一种颇具吸引力的废水净化方案。然而,由于传统杂原子掺杂体系稳定性不尽人意,其实际应用面临挑战。在此,我们创新性地开发了一种简单且可扩展的生化策略,合成了硒氮共掺杂生物炭(Se/N-BC)作为吸附-氧化双功能催化剂。Se/N-BC在最低催化剂用量(0.1 g/L)和过一硫酸盐(PMS,0.4 g/L)条件下,展现出最高的苯酚(PE)降解效率(5分钟内去除99.2%的PE)。更重要的是,Se/N-BC不仅在3.0 - 11.0的宽pH范围和复杂离子环境中具有通用性,还具备出色的循环稳定性。Se/N共掺杂引发了PE的快速吸附-降解循环。Se/N-BC充当“电子转移桥”,引导电子从PE快速转移至PMS以实现高效降解。Se/N共掺杂促进了石墨态氮的形成,并释放了相邻C位点用于PMS活化的潜力,从而提高氧化效率。此外,由于Se的抗氧化性能,防止了催化剂的氧化,这一直是再生吸附质或提高降解性能的主要关注点。

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