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.
Research Center for Environmental Science & Technology, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, China.
J Hazard Mater. 2020 Jun 15;392:122357. doi: 10.1016/j.jhazmat.2020.122357. Epub 2020 Feb 19.
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 CN (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 (NO). 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 CN. Compared to bare CN, the synthesized PdCN exhibits highly enhanced purification of NO in air and strong inhibition of toxic NO 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.
理性设计高效且选择性的光催化剂用于去除 NO 对于光催化技术的商业应用具有重要意义，因为在非选择性的污染物氧化过程中，如果去除不充分，会产生二次副产物，这是一个主要的挑战。在这项工作中，首先通过密度泛函理论（DFT）设计了钯纳米粒子修饰的碳氮（PdCN）。PdCN 在动力学和热力学性能方面均优于 CN，具体表现在速率决定步骤的活化能垒更低，最终产物（硝酸盐）的选择性更高，而非有毒中间体（NO）。然后，通过一种简便的方法制备了具有超低含量 Pd 粒子负载的 CN 的高选择性和高效光催化剂。与纯 CN 相比，合成的 PdCN 表现出在空气中对 NO 的高度净化作用和对有毒 NO 副产物的强烈抑制作用，这与原位 DRIFTS 研究的结果一致，这也符合理论预测。这项工作是在理论和实验之间架起桥梁的典型范例，为先进光催化剂的理性设计和原子反应机制的理解提供了有前景的途径。
