可见光驱动RGO/g-C3N4活化过硫酸盐降解水中双酚A

doi:10.15541/jim20190334

无机材料学报 ›› 2020, Vol. 35 ›› Issue (3): 329-336.DOI: 10.15541/jim20190334 CSTR: 32189.14.10.15541/jim20190334

所属专题： 2020年环境材料论文精选(三)有机小分子去除

可见光驱动RGO/g-C₃N₄活化过硫酸盐降解水中双酚A

张塞,邹英桐,陈中山,李冰峰,顾鹏程,文涛()

华北电力大学环境科学与工程学院, 资源环境系统优化教育部重点实验室, 北京 102206

收稿日期:2019-07-03 修回日期:2019-08-22 出版日期:2020-03-20 网络出版日期:2019-09-04
作者简介:张塞(1992-), 男, 博士研究生. E-mail: saizhang0910@gmail.com
基金资助:
科技部纳米专项重点研发计划(2017YFA0207002);科技部纳米专项重点研发计划(2018YFC1900105);国家自然科学基金(21607042);国家自然科学基金(21876048);国家自然科学基金(21836001);中央高校基本科研业务费专项资金(2019QN080);中央高校基本科研业务费专项资金(2018ZD11);中央高校基本科研业务费专项资金(2018MS114)

Visible-light-driven Activation of Persulfate by RGO/g-C₃N₄ Composites for Degradation of BPA in Wastewater

ZHANG Sai,ZOU Yingtong,CHEN Zhongshen,LI Bingfeng,GU Pengcheng,WEN Tao()

MOE Key Laboratory of Resources and Environmental Systems Optimization, College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, China

Received:2019-07-03 Revised:2019-08-22 Published:2020-03-20 Online:2019-09-04
About author:ZHANG Sai, male, PhD candidate. E-mail: saizhang0910@gmail.com
Supported by:
National Key Research and Development Program of China(2017YFA0207002);National Key Research and Development Program of China(2018YFC1900105);National Natural Science Foundation of China(21607042);National Natural Science Foundation of China(21876048);National Natural Science Foundation of China(21836001);Fundamental Research Funds for the Central Universities(2019QN080);Fundamental Research Funds for the Central Universities(2018ZD11);Fundamental Research Funds for the Central Universities(2018MS114)

摘要/Abstract

摘要：

光催化氧化法能够高效去除水体中的持久性有机污染物, 在污水净化领域展现出广阔的应用前景。本研究分别以尿素和双氰胺为原料, 采用冷干辅助热聚合法制备了还原性氧化物石墨烯/氮化碳(RGO/g-C₃N₄)二元可见光催化剂, 并对样品的形貌结构和光学性能进行了分析表征。结果表明, 二维层状g-C₃N₄与RGO在异质结界面上紧密的结合在一起。同时以内分泌干扰物双酚A (BPA)为降解污染物, 研究了不同催化剂在可见光下活化过硫酸盐去除BPA的活性。光催化实验结果显示, 在可见光(λ>420 nm)照射下, 加入氧化剂过硫酸盐(PS)作为电子受体, 有效地增强了光催化剂可见光降解BPA的活性。以尿素为原料制备的RGO/g-C₃N₄催化剂在40 min内几乎完全去除溶液中的BPA。经过5次循环反应后, 可见光照射40 min, 该催化剂对BPA的去除率仍能达到80%以上, 表现出良好的稳定性。

关键词: 氮化碳, 还原性氧化物石墨烯, 可见光光催化, 过硫酸盐

Abstract:

Persistent organic pollutants can be effectively removed by photocatalytic oxidation, which reveals potential application prospects in the field of wastewater purification. Binary reduced graphene oxide and graphitic carbon nitride (RGO/g-C₃N₄) visible-light photocatalyst was successfully fabricated by the freeze drying assisted thermal polymerization method with urea and dicyandiamide as raw materials, respectively. The morphologies, structures and optical properties were characterized by various techniques. It was found that g-C₃N₄ and RGO nanostructures formed an intimate contact across the heterojunction interface. The photodegradation performances of catalysts were evaluated by removing bisphenol A (BPA) with the activation of persulfate (PS). The results indicated that the photocatalytic activities of photocatalysts were enhanced with the addition of PS as an oxidant and electron acceptor under visible light irradiation (λ>420 nm). Moreover, BPA was almost completely removed by RGO/g-C₃N₄ prepared with urea as raw material in 40 min. After five recovery tests, the removal efficiency of BPA for the catalyst was up to 80% within 40 min under visible light irradiation, which exhibited superior stability.

Key words: g-C₃N₄, reduced graphene oxide, visible-light photocatalysis, persulfate

中图分类号:

TQ174

张塞, 邹英桐, 陈中山, 李冰峰, 顾鹏程, 文涛. 可见光驱动RGO/g-C₃N₄活化过硫酸盐降解水中双酚A[J]. 无机材料学报, 2020, 35(3): 329-336.

ZHANG Sai, ZOU Yingtong, CHEN Zhongshen, LI Bingfeng, GU Pengcheng, WEN Tao. Visible-light-driven Activation of Persulfate by RGO/g-C₃N₄ Composites for Degradation of BPA in Wastewater[J]. Journal of Inorganic Materials, 2020, 35(3): 329-336.

图/表 10

图1 GO、CND、G-CND、CNU和G-CNU样品的XRD谱图

Fig. 1 XRD patterns of GO, CNU, G-CNU, CND, and G-CND samples

图2 GO、CND、G-CND、CNU和G-CNU样品的红外光谱图

Fig. 2 FT-IR spectra of GO, CNU, G-CNU, CND, and G-CND samples

图3 (a) CND、(b) G-CND、(c) CNU和(d) G-CNU催化剂的透射电镜照片

Fig. 3 TEM images of (a) CND, (b) G-CND, (c) CNU, and (d) G-CNU photocatalysts

图4 CND、G-CND、CNU和G-CNU样品的N2吸附-脱附等温线

Fig. 4 N2 adsorption-desorption isotherms of CND, G-CND, CNU and G-CNU samples

图5 CND、G-CND、CNU和G-CNU样品的(a) C1s、(b) N1s和(c) O1s XPS谱图

Fig. 5 (a) C1s, (b) N1s and (c) O1s XPS spectra of CND, G-CND, CNU and G-CNU samples

图6 CND、G-CND、CNU和G-CNU催化剂的(a)紫外-可见漫反射光谱和(b) (αhν)1/2随hν的变化曲线

Fig. 6 (a) The UV-Vis DRS and (b) the (αhν)1/2-hν curves of CND, G-CND, CNU and G-CNU photocatalysts

图7 不同催化剂的荧光发射光谱

Fig. 7 PL spectra of different photocatalysts

图8 光催化剂在不同条件下对BPA的降解性能(a~c)和溶液pH对G-CNU在可见光下活化PS降解BPA的影响(d)

Fig. 8 (a-c) Catalytic activities of photocatalysts for BPA degradation under different conditions, and (d) effects of solutionpH on BPA removal over G-CNU catalysts by activating PS under visible light irradiation (λ>420 nm) (a) Visible light; (b) PS and (c) visible light/PS; Reaction conditions: C0(BPA) = 10 mg·L-1, C0(catalyst) = 0.5 g·L-1, C0(PS) = 1.0 g·L-1

图9 G-CNU在可见光(λ>420 nm)下活化PS循环降解BPA的曲线图

Fig. 9 Cycling tests in degradation of BPA over G-CNU by PS activation under visible light irradiation (λ>420 nm)

图10 不同捕获剂对G-CNU可见光活化PS降解BPA的影响(λ>420 nm) (a)及其光催化降解机理示意图(b)

Fig. 10 (a) Effect of different radical scavengers on BPA degradation in the G-CNU suspension under visible light irradiation (λ>420 nm) with the addition of PS, and (b) schematic diagram of photodegradation mechanism Reaction conditions: C0(BPA) = 10 mg·L-1, C0(catalyst) = 0.5 g·L-1, C0(PS) = 1.0 g·L-1

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可见光驱动RGO/g-C₃N₄活化过硫酸盐降解水中双酚A

Visible-light-driven Activation of Persulfate by RGO/g-C₃N₄ Composites for Degradation of BPA in Wastewater

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