Breaking the Selectivity Barrier: Reactive Oxygen Species Control in Photocatalytic Nitric Oxide Conversion
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Published:2023-10-25
Issue:4
Volume:34
Page:
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ISSN:1616-301X
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Container-title:Advanced Functional Materials
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language:en
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Short-container-title:Adv Funct Materials
Author:
Dai Wenrui1,
Zhang Shao2,
Shang Huan1,
Xiao Shuning1,
Tian Zhangliu3,
Fan Wenbo2,
Chen Xiaolang2,
Wang Shike2,
Chen Wei3,
Zhang Dieqing2ORCID
Affiliation:
1. School of Materials and Chemistry University of Shanghai for Science and Technology Shanghai 200093 P. R. China
2. The Education Ministry Key Lab of Resource Chemistry Joint International Research Laboratory of Resource Chemistry Ministry of Education and Shanghai Key Laboratory of Rare Earth Functional Materials College of Chemistry and Materials Science Shanghai Normal University Shanghai 200234 P. R. China
3. Department of Chemistry National University of Singapore 3 Science Drive 3 Singapore 117543 Singapore
Abstract
AbstractSemiconductor photocatalytic technology holds promise in efficiently reducing low concentrations of gaseous nitric oxide (NO). However, the suboptimal selectivity in NO removal, leading to the undesired production of NO2 byproducts, poses a challenge. In this study, a defective CdS/Na2Ti3O7 heterostructure is rationally designed with strong electronic interaction and intimate interface contact for promoting charge transfer kinetics. This design refines reactive oxygen species (ROS) generation, resulting in an impressive 81% NO elimination and 99.7% selectivity toward nitrates. Detailed mechanistic studies reveal an intriguing catalysis scenario in which reactant molecules are selectively adsorbed and activated at different sites. Anionic vacancies on the CdS/Na2Ti3O7 surface render the activation of molecular O2 to reactive superoxide radicals (O2
−) species. Furthermore, intrinsic surface basicity and O vacancy sites of the Na2Ti3O7 cocatalyst facilitate the capture and activation of acidic nitrogen oxides (NOx) molecules as nitrate species, contributing to enhanced catalytic activity and selectivity. As a result, anionic vacancies and basic sites over CdS/Na2Ti3O7 heterostructure synergistically regulate the NOx oxidation pathway, refining the products toward nitrate with remarkable selectivity. These insights guide the development of advanced photocatalytic systems for environmental remediation, highlighting the importance of managing ROS production for efficient pollutant removal.
Funder
National Natural Science Foundation of China
National Key Research and Development Program of China
Agency for Science, Technology and Research
National Research Foundation Singapore
Subject
Electrochemistry,Condensed Matter Physics,Biomaterials,Electronic, Optical and Magnetic Materials
Cited by
1 articles.
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