Boosting light harvesting and charge separation over hollow double-shelled Ag@SrTiO3-TiO2 with Z-scheme heterostructure for highly efficient photocatalytic reduction of nitrate to N2

IF 12.5 1区 工程技术 Q1 ENGINEERING, CHEMICAL
Chemical Engineering Journal Pub Date : 2023-02-01 Epub Date: 2022-12-24 DOI:10.1016/j.cej.2022.140992
Yixuan Zhang , Cong Liu , Ye Zhou , Jinnan Wang , Aimin Li , Philippe François-Xavier Corvini
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引用次数: 11

Abstract

Hollow double-shelled Ag@SrTiO3-TiO2 with Z-scheme heterostructure was constructed for highly efficient photocatalytic reduction of nitrate to N2. The 3D finite-difference-time-domain analysis indicated that hollow double-shelled structure improved light harvesting due to multiple reflections. Photo-generated electrons transfer from SrTiO3 to Ag0 caused by electron sink effect were utilized to reduce nitrate, while photo-generated electrons of TiO2 migrated to SrTiO3 via transport bridge of Ti3+ defects for electron–hole recombination. Such charge carriers migration pathway facilitated the construction of Z-scheme heterostructure, which enhanced charge separation yet still retained high redox powers. Both photogenerated electrons and CO2− played important role in photocatalytic denitrification. Furthermore, Ag0 acted as co-catalyst which not only promoted photogenerated electrons transfer to nitrate but also enhanced nitrate conversion selectivity to N2. Combining the above advantages, nitrate removal rate and the nitrogen selectivity reached 97.2 % and 98.8 % within 60 min, respectively. Even after five cycles, it still remained satisfied photocatalytic activity and stability. In summary, this work proposed a feasible strategy to construct Z-scheme hollow double-shelled photocatalyst for efficient photocatalytic denitrification.

Abstract Image

中空双层壳上的光收集和电荷分离Ag@SrTiO3-TiO2具有Z-scheme异质结构的硝酸盐高效光催化还原为N2
构建了具有z型异质结构的中空双壳Ag@SrTiO3-TiO2,用于光催化硝酸还原成N2。三维时域有限差分分析表明,空心双壳结构由于多次反射而提高了光捕获能力。利用电子汇效应引起的光生电子从SrTiO3转移到Ag0来还原硝酸盐,而TiO2的光生电子通过Ti3+缺陷的输运桥迁移到SrTiO3进行电子-空穴复合。这种载流子迁移途径有利于z型异质结构的构建,在增强电荷分离的同时仍保持较高的氧化还原能力。光生电子和CO2−在光催化脱氮过程中都起着重要的作用。此外,Ag0作为助催化剂,不仅促进了光生电子向硝酸盐的转移,而且提高了硝酸盐对N2的转化选择性。综合以上优点,60 min内硝酸盐去除率和氮选择性分别达到97.2%和98.8%。经过5次循环后,其光催化活性和稳定性仍保持良好。综上所述,本工作提出了构建z型中空双壳光催化剂进行高效光催化脱氮的可行策略。
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来源期刊
Chemical Engineering Journal
Chemical Engineering Journal 工程技术-工程:化工
CiteScore
21.70
自引率
9.30%
发文量
6781
审稿时长
2.4 months
期刊介绍: The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.
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