首页|碱改性铜锰尖晶石室温催化氧化空气中甲醛

碱改性铜锰尖晶石室温催化氧化空气中甲醛

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甲醛(FA)作为一种有致癌风险的有害污染物,在室内环境中普遍存在.为了高效去除甲醛,催化氧化技术成为了一种既经济又节能的选择,它不仅能降低材料成本(例如避免使用贵金属),也能在无光和室温的条件下进行.本文制备了一种成本效益高的碱改性锰酸铜尖晶石(CuMn2O4)催化剂,并用于甲醛催化氧化反应中.实验结果表明,采用碱(1 mol L-1氢氧化钾)改性的CuMn2O4(1-CuMn2O4)作为催化剂,在室温条件下,当甲醛浓度为50 ppm,气体空速为4777h-1时,甲醛转化率(XFA)达到100％;此外,在甲醛转化率为10％时,其稳态反应速率达到了8.18 × 10-2 mmol g-1 h-1.原位漫反射红外傅立叶变换光谱结果表明,在催化剂的作用下,甲醛分子经过二氧亚甲基和甲酸酯中间体的转化,最终被氧化为水和二氧化碳.进一步结合密度泛函理论模拟发现,l-CuMn2O4具有较高的催化氧化甲醛性能,可归因于甲醛分子更牢固地吸附在1-CuMn2O4表面,甲醛吸附所需的能量较低,以及最终产物从催化剂表面脱附所需的能量也较低的综合效应.本研究为在无光和室温条件下,高效去除空气中甲醛提供了新型高效、成本效益高且无需贵金属的催化剂,从而为室内空气净化提供了新的科学见解.
Alkali-modified copper manganite spinel for room temperature catalytic oxidation of formaldehyde in air
Formaldehyde(FA)is present ubiquitously in indoor environment as a hazardous pollutant with carcinogenic risks.For the efficient mitigation of FA,catalytic oxidation is a recommendable option to simultaneously satisfy both material cost(e.g.,avoiding noble metals)and low-energy require-ment(under dark and at room temperature(RT)).From this perspective,a cost-effective alkali modified copper manganite spinel(CuMn2O4)catalyst has firstly been prepared and employed for FA oxidation.Specifically,alkali(1 mol L-1 potassium hydroxide)-modified CuMn2O4(1-CuMn2O4)achieves 100％FA(50 ppm(gas hourly space velocity of 4777 h-1))conversion(XFA)at RT.The steady-state reaction rate of 1-CuMn2O4 at 10％XFA is 8.18 x 10-2 mmol g-1 h-1.According to in situ diffuse reflectance infrared Fourier transform spectroscopy,FA molecules are oxidized into water and carbon dioxide through dioxymethylene and formate intermediates.Based on density function-al theory simulation,the higher catalytic performance of 1-CuMn2C4 for FA oxidation is attributed to the combined effects of firmer attachment of FA molecules to 1-CuMn2O4 surface,lower energy cost of FA adsorption,and lower desorption energy for the final products from the substrate surface.The present work is expected to provide insights into high-performing non-noble metal catalysts for RT oxidative removal of FA from indoor air.

FormaldehydeAlkali modificationCopper manganite spinelCatalytic oxidationIndoor air

Yongbiao Hua、Kumar Vikrant、Ki-Hyun Kim、Philippe M.Heynderickx、Danil W.Boukhvalov

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汉阳大学土木与环境工程系,首尔,韩国

根特大学国际校区环境与能源研究中心,催化与表征材料工程,仁川,韩国

根特大学生物科学工程学院绿色化学与技术系,根特,比利时

南京林业大学理学院,材料物理与化学研究所,江苏南京 210037,中国

乌拉尔联邦大学物理与技术研究所,叶卡捷琳堡,俄罗斯

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甲醛 碱修饰 锰酸铜尖晶石 催化氧化 室内空气

National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(MSIT)of the Korean governmentResearch and Development Program of Ghent University Global Campus(GUGC),Korea

2021R1A3B1068304

2024

10.1016/S1872-2067(24)60022-7

催化学报
中国化学会 中国科学院大连化学物理研究所

催化学报

CSTPCD
影响因子：1.269
ISSN：0253-9837
年,卷(期)：2024.60(5)
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