Faculty of Geosciences and Environmental Engineering, Southwest Jiaotong University, Chengdu 610031, China; State Key Joint Laboratory of Environment Simulation and Pollution Control, School of Environment, Tsinghua University, Beijing 100084, China.
School of Life Sciences, Jinggangshan University, Ji'an 343009, China.
J Environ Sci (China). 2025 Mar;149:35-45. doi: 10.1016/j.jes.2023.10.019. Epub 2023 Oct 28.
Post-etching method using dilute acid solutions is an effective technology to modulate the surface compositions of metal-oxide catalysts. Here the α-MnO catalyst treated with 0.1 mol/L nitric acid exhibits higher ozone decomposition activity at high relative humidity than the counterpart treated with acetic acid. Besides the increases in surface area and lattice dislocation, the improved activity can be due to relatively higher Mn valence on the surface and newly-formed Brønsted acid sites adjacent to oxygen vacancies. The remnant nitro species deposited on the catalyst by nitric acid treatment is ideal hydrophobic groups at ambient conditions. The decomposition route is also proposed based on the DRIFTS and DFT calculations: ozone is facile to adsorb on the oxygen vacancy, and the protonic H of Brønsted acid sites bonds to the terminal oxygen of ozone to accelerate its cleavage to O, reducing the reaction energy barrier of O desorption.
后蚀刻法使用稀酸溶液是一种有效调节金属氧化物催化剂表面成分的技术。在此,用 0.1mol/L 硝酸处理的α-MnO 催化剂在高相对湿度下表现出比用乙酸处理的对应物更高的臭氧分解活性。除了表面积和晶格位错的增加外,活性的提高可能是由于表面上相对较高的 Mn 价态和邻近氧空位的新形成的 Brønsted 酸位。用硝酸处理在催化剂上沉积的残留硝化物是环境条件下理想的疏水分子。还根据 DRIFTS 和 DFT 计算提出了分解途径:臭氧易于在氧空位上吸附,Brønsted 酸位的质子 H 与臭氧的末端氧键合,以加速其裂解为 O,降低 O 脱附的反应能垒。