Theoretical design and experimental investigation on highly selective Pd particles decorated C3N4 for safe photocatalytic NO purification

Kanglu Li; Ye He; Peng Chen; Hong Wang; Jianping Sheng; Wen Cui; Geng Leng; Yinghao Chu; Zhiming Wang; Fan Dong

doi:10.1016/j.jhazmat.2020.122357

Theoretical design and experimental investigation on highly selective Pd particles decorated C₃N₄ for safe photocatalytic NO purification

J Hazard Mater. 2020 Jun 15:392:122357. doi: 10.1016/j.jhazmat.2020.122357. Epub 2020 Feb 19.

Authors

Kanglu Li¹, Ye He², Peng Chen³, Hong Wang², Jianping Sheng², Wen Cui³, Geng Leng⁴, Yinghao Chu⁵, Zhiming Wang², Fan Dong⁶

Affiliations

¹ Research Center for Environmental Science & Technology, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, China; College of Architecture and Environment, Sichuan University, Chengdu 610065, China.
² Research Center for Environmental Science & Technology, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, China.
³ Research Center for Environmental Science & Technology, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, China; The Center of New Energy Materials and Technology, School of Materials Science and Engineering, Southwest Petroleum University, Chengdu 610500, China.
⁴ Research Center for Environmental Science & Technology, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, China; School of Resources and Environment, University of Electronic Science and Technology of China, Chengdu 611731, China.
⁵ College of Architecture and Environment, Sichuan University, Chengdu 610065, China.
⁶ Research Center for Environmental Science & Technology, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, China. Electronic address: dfctbu@126.com.

PMID: 32097850
DOI: 10.1016/j.jhazmat.2020.122357

Abstract

Rational design of highly active and selective photocatalyst for NO removal is significant for the commercial application of photocatalytic technology because the secondary byproduct caused by insufficient and non-selective pollutant oxidation process is a major challenge. In this work, Pd nanoparticles decorated C₃N₄ (PdCN) is designed by density functional theory (DFT) at first. The PdCN exhibits superiority to CN in terms of both kinetics and thermodynamics performances, as reflected in the lower activation barrier of rate-determining step and higher selectivity for the final product (nitrate) instead of toxic intermediate (NO₂). The as-designed highly selective and efficient photocatalyst is then fabricated by a facile method with an extremely low content of Pd particles supported on C₃N₄. Compared to bare CN, the synthesized PdCN exhibits highly enhanced purification of NO in air and strong inhibition of toxic NO₂ by-product as supported by in-situ DRIFTS investigation, which is consistent with the theoretical prediction. This work is a typical demonstration of setting up a bridge between theory and experiment to give a promising way to the rational design of advanced photocatalysts and atomic understanding of the reaction mechanism.

Keywords: Band structure; Photocatalysis; Reaction mechanism; Theoretical design; Toxic intermediate.

Publication types

Research Support, Non-U.S. Gov't