Study on the construction of nitrogen-doped porous biochar via dual template synergistic regulation and its non-radical dominated PMS activation mechanism

IF 3.9 3区 工程技术 Q2 ENGINEERING, CHEMICAL
Yuye Liu , Haozhan Zheng , Yintao Shi , Chuangyi Chi , Hao Zhang , Dongsheng Xia , Bin Zhang
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引用次数: 0

Abstract

A high-efficiency material with uniform pores (2.1–2.4 nm) was successfully prepared via a "doping-volatilization" dual-template strategy using ZnCl2 and urea as dual-template reagents for walnut shell biochar modification. The influence of this material on peroxymonosulfate (PMS) activation was systematically investigated. Experimental results demonstrated that uniform pores played a critical role in regulating morphology and enhancing mass transfer rates. Under identical experimental conditions (i.e., catalyst dosage: 40 mg; PMS concentration: 200 mg·L⁻¹), the catalyst prepared via the dual-template method exhibited significantly higher catalytic activity compared to those derived from single-template methods (NBC and ZBC). Specifically, it demonstrated a 6.5-fold enhancement in activity relative to NBC and a 1.8-fold improvement over ZBC. Significant performance differences were observed among catalysts in PMS activation for tetracycline (TC) degradation, where non-radical pathways (e.g., 1O2) dominated the reaction, and pore/defect structures served as primary active sites. This study further revealed that the dual-template synergy originated from the coupling of ZnCl2 volatilization-induced pore formation and urea-mediated nitrogen doping. During pyrolysis, urea acted as an exogenous nitrogen source to stabilize nitrogen content whereas ZnCl2 volatilized but removed endogenous nitrogen from biomass. This work provides insights into the structure-property relationships of carbon materials and advances.
双模板协同调控构建氮掺杂多孔生物炭及其非自由基主导的PMS活化机制研究
以ZnCl2和尿素为双模板剂,采用掺杂-挥发双模板策略,成功制备了具有均匀孔隙(2.1 ~ 2.4 nm)的高效改性核桃壳生物炭材料。系统地研究了该材料对过氧单硫酸盐(PMS)活化的影响。实验结果表明,均匀孔隙在调节形态和提高传质速率方面起着至关重要的作用。在相同的实验条件下(即催化剂用量为40 mg; PMS浓度为200 mg·L⁻¹),双模板法制备的催化剂比单模板法(NBC和ZBC)制备的催化剂表现出更高的催化活性。具体来说,它比NBC的活性提高了6.5倍,比ZBC的活性提高了1.8倍。不同催化剂在PMS降解四环素(TC)过程中表现出显著的性能差异,其中非自由基途径(如1O2)主导了反应,孔/缺陷结构是主要的活性位点。本研究进一步揭示了双模板协同作用源于ZnCl2挥发诱导的孔形成和尿素介导的氮掺杂的耦合。在热解过程中,尿素作为外源氮源稳定氮含量,而ZnCl2挥发但去除生物质中的内源氮。这项工作提供了对碳材料结构-性能关系的见解和进展。
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来源期刊
Chemical Engineering Research & Design
Chemical Engineering Research & Design 工程技术-工程:化工
CiteScore
6.10
自引率
7.70%
发文量
623
审稿时长
42 days
期刊介绍: ChERD aims to be the principal international journal for publication of high quality, original papers in chemical engineering. Papers showing how research results can be used in chemical engineering design, and accounts of experimental or theoretical research work bringing new perspectives to established principles, highlighting unsolved problems or indicating directions for future research, are particularly welcome. Contributions that deal with new developments in plant or processes and that can be given quantitative expression are encouraged. The journal is especially interested in papers that extend the boundaries of traditional chemical engineering.
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