BiOX(Cl,Br,I)/Bi2WO6异质结型复合光催化剂用于高浓度氮氧化物的脱除

doi:10.16085/j.issn.1000-6613.2020-2403

摘要/Abstract

摘要：

海中船舶排放的废气是大气污染的来源之一，其中的氮氧化物能使海洋酸化，不仅危害海洋生态系统，还会造成沿海城市空气污染，对人的身体健康也造成危害。光催化脱除大气中的氮氧化物被认为是可靠且有潜力的高级氧化脱除技术，但目前的研究大多针对低浓度（10^-9级）下氮氧化物脱除，针对船舶尾气中较高浓度（10^-6级）氮氧化物脱除的研究较少。本文采用超声辅助法制备了BiOX(Cl, Br, I)/Bi₂WO₆复合催化剂，紫外可见吸收光谱得到BiOX(Cl, Br, I)/Bi₂WO₆的带隙能分别为3.1eV、2.6eV和1.8eV，并且计算了其导带电位。光电流实验表明，BiOCl/Bi₂WO₆复合材料的光电流强度高于BiOBr/Bi₂WO₆和BiOI/Bi₂WO₆。模拟光催化脱硝实验表明，BiOCl/Bi₂WO₆在紫外线下NO的脱除率为37.5%，且BiOX/Bi₂WO₆复合光催化剂在5次循环后表现出良好的稳定性。通过原位红外吸收光谱分析，对BiOX/Bi₂WO₆催化剂上进行NO光催化氧化的中间产物进行了鉴定，提出了NO的氧化脱除途径。

关键词: 卤氧化铋, 钨酸铋, 异质结, 一氧化氮光催化氧化

Abstract:

The exhaust gas emitted by marine vessels is one of the air pollution sources, and the nitrogen oxides in the gas could cause ocean acidification, marine ecosystem damage, air pollution over coastal cities, and people’s health problems. Photocatalytic removal of nitrogen oxides from atmosphere is considered to be a reliable and potential advanced oxidation removal technology, but the current studies are mostly focused on the elimination of nitrogen oxides of low concentration(10^-9 level), and those on high concentration(10^-6 level)nitrogen oxides removal from ship exhausts are still rare. The heterojuncted BiOX(Cl, Br, I)/Bi₂WO₆ were prepared through a one-step ultrasonic-assisted method, and applied in the NO removal from exhaust gas. The band-gap energies of BiOX(Cl, Br, I)/Bi₂WO₆ were estimated to be 3.1eV, 2.6eV and 1.8eV, respectively. The conduction band potentials of pristine Bi₂WO₆ and BiOX/Bi₂WO₆ were calculated. The photocurrent density of BiOCl/Bi₂WO₆ composite electrode was higher than that of BiOBr/Bi₂WO₆ and BiOI/Bi₂WO₆, and BiOCl/Bi₂WO₆ showed the highest activity with the maximum NO removal rate of 37.5% under UV light. BiOX/Bi₂WO₆ revealed good stability after five cycles. In situ DRIFTS tests of NO photocatalytic oxidation on BiOX/Bi₂WO₆ were employed to identify the reaction intermediates and the NO oxidation pathway was proposed based on the electrochemical and photocurrent density measurements as well as in situ reaction study.

Key words: bismuth oxyhalide, dibismuth tris(tetraoxowolframate) (Bi₂WO₆), heterojunction, nitric oxide(NO) photocatalytic oxidation

中图分类号:

TQ09

卞俊杰, 王万圆, 满恒孝, 文成新. BiOX(Cl,Br,I)/Bi₂WO₆异质结型复合光催化剂用于高浓度氮氧化物的脱除[J]. 化工进展, 2021, 40(11): 6094-6101.

BIAN Junjie, WANG Wanyuan, MAN Hengxiao, WEN Chengxin. BiOX(Cl, Br, I)/Bi₂WO₆ heterojunction composites as photocatalysts for high concentration NO removal[J]. Chemical Industry and Engineering Progress, 2021, 40(11): 6094-6101.

图/表 8

参考文献 32

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催化剂	初始浓度/10^-9	脱除率/%	参考文献
BiOBr 微球	400	紫外线：45 可见光：30	［22］
Bi/OVs-BiOBr	600	可见光：65.3	［10］
（BiO）₂CO₃-CTAB	600	可见光：30.4	［23］
Bi/Bi₂O₃/Bi₂WO₆	550	可见光：55.4	［24］
Bi薄膜	550	紫外线：37.7	［25］
(BiO)₂CO₃/BiO_2-_x-石墨烯	430	模拟太阳光：53.6	［26］
Bi-BiOI/石墨烯	430	可见光：51.8	［27］
Bi₂WO₆-OVs	550	可见光：47	［11］
Bi/ZnWO₄	400	可见光：37	［28］
Bi₁₂O₁₇Br₂	600	可见光：28.3	［29］
Bi₄O₅Br₂	600	可见光：41.8	［29］
Fe(Ⅲ)-(BiO)₂CO₃	550	可见光：44.1	［30］
Bi₂WO₆/BiOI	300	可见光：40	［20］
BiOBr-OVs	600	可见光：38.7	［19］

催化剂	初始浓度/10^-9	脱除率/%	参考文献
BiOBr 微球	400	紫外线：45 可见光：30	［22］
Bi/OVs-BiOBr	600	可见光：65.3	［10］
（BiO）₂CO₃-CTAB	600	可见光：30.4	［23］
Bi/Bi₂O₃/Bi₂WO₆	550	可见光：55.4	［24］
Bi薄膜	550	紫外线：37.7	［25］
(BiO)₂CO₃/BiO_2-_x-石墨烯	430	模拟太阳光：53.6	［26］
Bi-BiOI/石墨烯	430	可见光：51.8	［27］
Bi₂WO₆-OVs	550	可见光：47	［11］
Bi/ZnWO₄	400	可见光：37	［28］
Bi₁₂O₁₇Br₂	600	可见光：28.3	［29］
Bi₄O₅Br₂	600	可见光：41.8	［29］
Fe(Ⅲ)-(BiO)₂CO₃	550	可见光：44.1	［30］
Bi₂WO₆/BiOI	300	可见光：40	［20］
BiOBr-OVs	600	可见光：38.7	［19］

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BiOX(Cl,Br,I)/Bi₂WO₆异质结型复合光催化剂用于高浓度氮氧化物的脱除

BiOX(Cl, Br, I)/Bi₂WO₆ heterojunction composites as photocatalysts for high concentration NO removal

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