Copper–iron catalyst supported on oxygen vacancy–containing titanium dioxide for deep ambient-temperature desulfurization

烟气脱硫 催化作用 煅烧 二氧化硫 化学 无机化学 氧气 热重分析 二氧化钛 硫黄 傅里叶变换红外光谱 氧化还原 X射线光电子能谱 氧气储存 硝酸盐 氯化物 极限氧浓度 催化氧化 核化学
作者
Min-Ju Kim,Sunjae Lee,Na Rae Lee,Waleed Ahmad,Hocheol Song,Youngtak Oh,Yongtae Ahn,Jaeyoung Choi
出处
期刊:Journal of environmental chemical engineering [Elsevier BV]
卷期号:13 (6): 120236-120236
标识
DOI:10.1016/j.jece.2025.120236
摘要

Efficient H 2 S removal from gas streams is essential for mitigating environmental pollution, preventing catalyst poisoning, and reducing equipment corrosion. Consequently, the corresponding catalysts, particularly those enabling room-temperature desulfurization, are highly sought after. To address this need, we herein prepared a copper (Cu)–iron (Fe) catalyst supported on titanium dioxide with oxygen vacancies (Cu-Fe/V o -TiO 2 ) via incipient wetness coimpregnation and evaluated its H 2 S removal ability under ambient conditions. The results of Brunauer–Emmett–Teller analysis, Fourier transform infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and thermogravimetric analyses revealed the presence of oxygen vacancies, Cu(NO 3 ) 2 , and FeOOH, which synergistically enhanced catalytic activity. Specifically, oxygen vacancies facilitated electron transfer and hydroxyl radical generation, nitrate groups promoted the oxidation of H 2 S to elemental sulfur and sulfate, and FeOOH enhanced the redox properties of the catalyst, promoted sulfur oxidation, and formed stable sulfur intermediates. Cu-Fe/V o -TiO 2 exhibited desulfurization capacities of 56.1 and 161.6 mg S g −1 at H 2 S concentrations of 10 and 100 mg L −1 , respectively, and achieved nearly quantitative removal within 10 min. Calcination and chloride precursor control experiments revealed that nitrate group removal decreased NO release and desulfurization efficiency, confirming the active role of these groups in the reaction mechanism. Thus, this work highlights the potential of Cu-Fe/V o -TiO 2 as a highly efficient and sustainable catalyst for H 2 S removal, eliminating the need for external energy inputs, addressing the limitations of conventional desulfurization methods, and facilitating the development of advanced multimetal catalysts for industrial desulfurization and air purification. • Cu-Fe/V o -TiO₂ showed the highest H₂S removal among all tested TiO₂ catalysts. • Cu and Fe improved oxygen vacancies, boosting H₂S conversion via electron transfer. • Nitrate species facilitated H₂S oxidation affecting desulfurization efficiency. • H₂S oxidation on Cu(OH)₂ and FeOOH primarily forms copper and iron sulfates.
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