碱改性铜锰尖晶石室温催化氧化空气中甲醛

doi:10.1016/S1872-2067(24)60022-7

催化学报 ›› 2024, Vol. 60: 337-350.DOI: 10.1016/S1872-2067(24)60022-7

碱改性铜锰尖晶石室温催化氧化空气中甲醛

Yongbiao Hua^a, Kumar Vikrant^a, Ki-Hyun Kim^a^,^*(), Philippe M. Heynderickx^b^,^c, Danil W. Boukhvalov^d^,^e

^a汉阳大学土木与环境工程系, 首尔, 韩国
^b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
^c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
^d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
^e乌拉尔联邦大学物理与技术研究所, 叶卡捷琳堡, 俄罗斯

收稿日期:2024-02-02 接受日期:2024-03-08 出版日期:2024-05-18 发布日期:2024-05-20
通讯作者: *电子信箱: kkim61@hanyang.ac.kr (K.-H. Kim).

Alkali-modified copper manganite spinel for room temperature catalytic oxidation of formaldehyde in air

Yongbiao Hua^a, Kumar Vikrant^a, Ki-Hyun Kim^a^,^*(), Philippe M. Heynderickx^b^,^c, Danil W. Boukhvalov^d^,^e

^aDepartment of Civil and Environmental Engineering, Hanyang University, 222 Wangsimni-Ro, Seoul 04763, Korea
^bCenter for Environmental and Energy Research (CEER), Engineering of Materials via Catalysis and Characterization, Ghent University Global Campus, 119-5 Songdo Munhwa-ro, Yeonsu-gu, Incheon 406-840, Korea
^cDepartment of Green Chemistry and Technology, Faculty of Bioscience Engineering, Ghent University, Coupure Links 653, B-9000 Ghent, Belgium
^dCollege of Science, Institute of Materials Physics and Chemistry, Nanjing Forestry University, Nanjing 210037, Jiangsu, China
^eInstitute of Physics and Technology, Ural Federal University, 620002 Yekaterinburg, Russia

Received:2024-02-02 Accepted:2024-03-08 Online:2024-05-18 Published:2024-05-20
Contact: *E-mail: kkim61@hanyang.ac.kr (K.-H. Kim).

摘要/Abstract

摘要：

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4777 h^‒1时, 甲醛转化率(X_FA)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, 1-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.

关键词: 甲醛, 碱修饰, 锰酸铜尖晶石, 催化氧化, 室内空气

Abstract:

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 requirement (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 (X_FA) at RT. The steady-state reaction rate of 1-CuMn₂O₄ at 10% X_FA is 8.18 × 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 functional theory simulation, the higher catalytic performance of 1-CuMn₂O₄ 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.

Key words: Formaldehyde, Alkali modification, Copper manganite spinel, Catalytic oxidation, Indoor air

Yongbiao Hua, Kumar Vikrant, Ki-Hyun Kim, Philippe M. Heynderickx, Danil W. Boukhvalov. 碱改性铜锰尖晶石室温催化氧化空气中甲醛[J]. 催化学报, 2024, 60: 337-350.

Yongbiao Hua, Kumar Vikrant, Ki-Hyun Kim, Philippe M. Heynderickx, Danil W. Boukhvalov. Alkali-modified copper manganite spinel for room temperature catalytic oxidation of formaldehyde in air[J]. Chinese Journal of Catalysis, 2024, 60: 337-350.

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Order	Material	BET surface area (m² g^‒1)	Pore volume (cm³ g^‒1)	Actual content^a (wt%)			XPS
Order	Material	BET surface area (m² g^‒1)	Pore volume (cm³ g^‒1)	K	Cu	Mn	Cu⁺/Cu²⁺	Mn³⁺/Mn⁴⁺	(O_β+O_γ)/O_α
1	CuMn₂O₄	11.54±0.04	0.008	—	31.73	47.88	0.40	1.58	0.59
2	0.2-CuMn₂O₄	31.55±0.16	0.046	0.56	28.67	49.30	0.36	2.08	0.89
3	1-CuMn₂O₄	38.96±0.17	0.067	0.65	28.52	50.15	0.42	2.18	1.08
4	10-CuMn₂O₄	33.42±0.15	0.050	1.90	22.55	50.66	0.40	2.66	1.34

Order	Material	BET surface area (m² g^‒1)	Pore volume (cm³ g^‒1)	Actual content^a (wt%)			XPS
Order	Material	BET surface area (m² g^‒1)	Pore volume (cm³ g^‒1)	K	Cu	Mn	Cu⁺/Cu²⁺	Mn³⁺/Mn⁴⁺	(O_β+O_γ)/O_α
1	CuMn₂O₄	11.54±0.04	0.008	—	31.73	47.88	0.40	1.58	0.59
2	0.2-CuMn₂O₄	31.55±0.16	0.046	0.56	28.67	49.30	0.36	2.08	0.89
3	1-CuMn₂O₄	38.96±0.17	0.067	0.65	28.52	50.15	0.42	2.18	1.08
4	10-CuMn₂O₄	33.42±0.15	0.050	1.90	22.55	50.66	0.40	2.66	1.34

Order	Catalyst	Catalyst mass (mg)	Reactant mixture	Pollutant concentration (ppm)	Flow rate (mL min^‒1)	Flow rate (mol s^‒1)	Space velocity (h^‒1)	Maximum X_FA(%) at 30 °C	r (mmol g_cat^‒1 h^‒1) at 30 °C
1	CuMn₂O₄	120	FA + Air (balance)	50	50	1.70 × 10^‒9	4777	27.5	1.41 × 10^‒2
2	0.2-CuMn₂O₄	120	FA + Air (balance)	50	50	1.70 × 10^‒9	4777	56.1	2.87 × 10^‒2
3	1-CuMn₂O₄	120	FA + Air (balance)	50	50	1.70 × 10^‒9	4777	100	5.11 × 10^‒2
4	10-CuMn₂O₄	120	FA + Air (balance)	50	50	1.70 × 10^‒9	4777	100	5.11 × 10^‒2

Order	Catalyst	Catalyst mass (mg)	Reactant mixture	Pollutant concentration (ppm)	Flow rate (mL min^‒1)	Flow rate (mol s^‒1)	Space velocity (h^‒1)	Maximum X_FA(%) at 30 °C	r (mmol g_cat^‒1 h^‒1) at 30 °C
1	CuMn₂O₄	120	FA + Air (balance)	50	50	1.70 × 10^‒9	4777	27.5	1.41 × 10^‒2
2	0.2-CuMn₂O₄	120	FA + Air (balance)	50	50	1.70 × 10^‒9	4777	56.1	2.87 × 10^‒2
3	1-CuMn₂O₄	120	FA + Air (balance)	50	50	1.70 × 10^‒9	4777	100	5.11 × 10^‒2
4	10-CuMn₂O₄	120	FA + Air (balance)	50	50	1.70 × 10^‒9	4777	100	5.11 × 10^‒2

Catalyst	Catalyst activation	m_cat (mg)	Reactant mixture	FA concentration (ppm)	Flow rate (mL min^‒1)	F_FA (mol s^‒1)	Space velocity	r (mmol g_cat^‒1 h^‒1)^a			T (10% X_FA)	Maximum X_FA (%)	Ref.
Catalyst	Catalyst activation	m_cat (mg)	Reactant mixture	FA concentration (ppm)	Flow rate (mL min^‒1)	F_FA (mol s^‒1)	Space velocity	10% X_FA	maximum X_FA		T (10% X_FA)	Maximum X_FA (%)	Ref.
Graphene oxide/MnO₂	NA	100	FA + air ^c	100	50	3.41 × 10^‒9	30000 mL g^‒1 h^‒1	NA		2.45 × 10^‒2	NA	20	[89]
Partially crystallized MnO_x	NA	2000	FA + air^c	1	52000	3.54 × 10^‒8	48000 h^‒1	NA		1.34 × 10^‒2	NA	21	[90]
K-MnO₂	NA	75	FA + O₂(20 vol%) + N₂^c +RH50%	200	100	1.36 × 10^‒8	80000 mL g^‒1 h^‒1	6.54 × 10^‒2		1.96 × 10^‒2	50	3	[81]
Pd-CeO₂ octahedrons	200 °C using H₂ gas for 1 h	100	FA + N₂^c +O₂ (20%)	600	45	1.84 × 10^‒8	10000 h^‒1	6.63 × 10^‒2		2.65 × 10^‒2	11	4	[82]
Pd-TS-1(EG)	NA	100	FA +O₂ (20%) +N₂^c	110	100	7.50 × 10^‒9	60000 mL g^‒1 h^‒1	2.70 × 10^‒2		2.16 × 10^‒2	35	8	[83]
Pd-TS-1(CO)	NA	100	FA +O₂ (20%) + N₂^c	110	100	7.50 × 10^‒9	36000 mL h^‒1 g^‒1	2.70 × 10^‒2		8.10 × 10^‒3	64	3	[83]
0.1Pd-Layered double hydroxides	NA	200	FA +air/N₂ mixture	50	80	2.73 × 10^‒9	24,000 mL h^‒1 g^‒1	NA		1.87 × 10^‒2	NA	38	[91]
0.5%-Pt-4%-CeO₂/Activated carbon	400 °C using 20 vol% H₂ gas (mixed with N₂ gas) for 5 h	2800	FA + air^c	61	800	3.32652 × 10^‒8	8000 h^‒1	NA		4.28× 10^‒2	NA	100	[92]
0.5%-Pt-3%-La/TiO₂	NA	100	FA + O₂ (21%) + RH50% + N₂ ^c	0.5	100	3.40832 × 10^‒11	60000 mL. g^‒1 h^‒1	NA		1.20 × 10^‒3	NA	98	[93]
0.2%-Pt/MnO₂/TiO₂ nanotube	at 300 °C using H₂ gas for 3 h	200	FA+ RH35%+ air^c	50	100	3.41 × 10^‒9	30000 mL h^‒1 g^‒1	NA		5.83 × 10^‒2	NA	95	[84]
0.1%-Pt-Ni/ZSM-5	during synthesis using FA solution	200	FA + O₂(20 vol%) + N₂^c	50	80	2.73 × 10^‒9	30000 mL h^‒1 g^‒1	NA		4.91 × 10^‒2	NA	100	[94]
1%-Pt-K-MnO₂	during synthesis using NaBH₄	60	FA + O₂ (20 vol%) + N₂^c	20	50	6.82 × 10^‒10	50000 mL. g^‒1 h^‒1	NA		4.09 × 10^‒2	NA	100	[95]
3%-Pt-MnO_x-CeO₂	at 200 °C using H₂ for 1 h	200	FA + O₂ (20 vol%) + He^c	30	100	2.04 × 10^‒9	30000 mL g^‒1 h^‒1	NA		3.68 × 10^‒2	NA	100	[96]
0.8%Pt-FeOOH long rod	NA	200	FA + air^c	50	80	2.73 × 10^‒9	24000 mL g^‒1 h^‒1	NA		4.91 × 10^‒2	NA	100	[85]
Pt/siliceous beta zeolite	NA	100	FA + O₂ (20 vol%) + He^c + 50% RH	80	100	5.45 × 10^‒9	60000 mL g^‒1 h^‒1	NA		1.96 × 10^‒1	NA	100	[88]
Ag/manganese oxides with octahedral molecular sieve	NA	100	FA + O₂ (20 vol%) + He^c + 50% RH	80	100	5.45 × 10^‒9	60000 mL g^‒1 h^‒1	NA		1.96 × 10^‒1	NA	100	[87]
1-CuMn₂O₄	NA	60	FA + air^c	50	50	1.70 × 10^‒9	4777 h^‒1	8.18 × 10^‒2b		1.02 × 10^‒1	38	100	This work

碱改性铜锰尖晶石室温催化氧化空气中甲醛

Alkali-modified copper manganite spinel for room temperature catalytic oxidation of formaldehyde in air

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