N/B/Fe共掺杂生物质炭阴极制备及电芬顿降解对硝基酚

doi:10.16085/j.issn.1000-6613.2020-1646

化工进展 ›› 2021, Vol. 40 ›› Issue (7): 4064-4073.DOI: 10.16085/j.issn.1000-6613.2020-1646

N/B/Fe共掺杂生物质炭阴极制备及电芬顿降解对硝基酚

汤茜¹^,²(), 范艺馨², 苏欣², 黄成思¹^,², 孙玉伟¹^,², 高永慧¹, 王栋³

^1.吉林省高校环境材料与污染控制重点实验室，吉林四平 136000
^2.吉林师范大学环境科学与工程学院，吉林四平 136000
^3.大连理工大学环境学院，辽宁大连 116024

收稿日期:2020-08-17 修回日期:2020-09-10 出版日期:2021-07-06 发布日期:2021-07-19
通讯作者: 汤茜
作者简介:汤茜（1980—），女，副教授，硕士生导师，研究方向为有机废水高级氧化处理。E-mail：tangqian327@jlnu.edu.cn。
基金资助:
国家自然科学基金青年科学基金(51708250);国家级大学生创新创业训练计划支持项目(202010203001)

Preparation of N/B/Fe co-doped biochar cathode for degradation of p-nitrophenol

TANG Qian¹^,²(), FAN Yixin², SU Xin², HUANG Chengsi¹^,², SUN Yuwei¹^,², GAO Yonghui¹, WANG Dong³

^1.Key Laboratory of Environmental Materials and Pollution Control, the Education Department of Jilin Province, Jilin Normal University, Siping 136000, Jilin, China
^2.College of Environmental Science and Engineering, Jilin Normal University, Siping 136000, Jilin, China
^3.School of Environmental Science and Technology, Dalian University of Technology, Dalian 116024, Liaoning, China

Received:2020-08-17 Revised:2020-09-10 Online:2021-07-06 Published:2021-07-19
Contact: TANG Qian

摘要/Abstract

摘要：

以玉米芯为主要原料，采用热沉积、高温焙烧法，制备N/B/Fe共掺杂生物质炭（N/B/Fe@BC），通过X射线衍射（XRD）、扫描电子显微镜（SEM）、高分辨透射电子显微镜（HRTEM）和X射线光电子能谱仪（XPS）等手段对样品的晶格结构、形貌特征和组成等进行表征，并以对硝基酚为对象，探究N/B/Fe@BC电极的电芬顿催化性能。结果表明，N/B/Fe@BC为纳米薄片交错堆积的三维多孔结构，表面缺陷较未掺杂生物质炭显著增加，催化氧还原以两电子产H₂O₂为主。在电流强度50mA、初始pH为3的电芬顿体系中，120min时对硝基酚的去除率为97.93%±1.62%，60min内反应速率常数k为0.040min^-1，是未掺杂生物质炭电极的2.7倍。N/B/Fe@BC电极的pH适用范围较宽，受水质的影响较小，循环使用10次后120min对硝基酚的去除率仍可达到85%以上。

关键词: N/B/Fe共掺杂, 生物质炭, 玉米芯, 电芬顿, 对硝基酚

Abstract:

N/B/Fe co-doped biochar (N/B/Fe@BC) was synthesized from corncob by thermal deposition and calcination. The crystal lattice structure, morphology, composition and other properties of the sample were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), high resolution transmission electron microscopy (HRTEM) and X-ray photoelectron spectroscopy (XPS) and so on. The catalytic performance in electro-Fenton system with N/B/Fe co-doped cathode was investigated using p-nitrophenol as the model pollutant. The results showed that N/B/Fe@BC had a three-dimensional porous structure with staggered accumulation of nanosheets, and its surface defects were significantly increased compared with the undoped biochar. The catalytic oxygen reduction on the N/B/Fe@BC was dominated by the production of H₂O₂via two electrons reduction. The degradation rate of p-nitrophenol could reach 97.93%±1.62% in 120min with the current intensity of 50mA and initial pH of 3, and the apparent rate constant within 60min was 0.040min^-1, which was 2.7 times higher than that of the undoped biochar cathode. The N/B/Fe@BC cathode expressed high activity in a wide pH range of 3—9 and feasibility in different water matrix including tap water, river water and municipal sewage. In addition, after ten times cycle, the degradation rate of p-nitrophenol could still reach more than 85% in 120min with the N/B/Fe@BC cathode.

Key words: N/B/Fe co-doped, biochar, corncob, electro-Fenton, p-nitrophenol

中图分类号:

X703.1

汤茜, 范艺馨, 苏欣, 黄成思, 孙玉伟, 高永慧, 王栋. N/B/Fe共掺杂生物质炭阴极制备及电芬顿降解对硝基酚[J]. 化工进展, 2021, 40(7): 4064-4073.

TANG Qian, FAN Yixin, SU Xin, HUANG Chengsi, SUN Yuwei, GAO Yonghui, WANG Dong. Preparation of N/B/Fe co-doped biochar cathode for degradation of p-nitrophenol[J]. Chemical Industry and Engineering Progress, 2021, 40(7): 4064-4073.

图/表 12

图1 样品的SEM、HRTEM和元素分布图

图2 样品的XRD图谱

图3 样品的FTIR图谱

图4 样品的XPS图谱

图5 N/B/Fe@BC的旋转圆盘电极测试图

表1 样品的电催化氧还原电子转移数

样品	电子转移数n
样品	-0.60V	-0.70V	-0.80V	-0.90V	-1.00V
N/B/Fe@BC	1.88	1.87	1.87	1.96	2.23
Fe@BC	2.26	2.35	2.53	2.85	3.72
N/B@BC	2.23	2.12	2.10	2.26	2.95
BC	2.10	2.13	2.22	2.49	3.38

图6 不同电极体系中对硝基酚降解效果图

图7 不同初始pH下对硝基酚降解效果

图8 不同水质中对硝基酚降解效果图

图9 N/B/Fe@BC电极的循环次数对降解效果的影响

图10 反应体系中·OH与H2O2浓度分析

图11 不同捕获剂对对硝基酚降解率的影响

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N/B/Fe共掺杂生物质炭阴极制备及电芬顿降解对硝基酚

Preparation of N/B/Fe co-doped biochar cathode for degradation of p-nitrophenol

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