三维分层多孔 Co-Cu 纳米复合材料在低温高空间速度下催化消除挥发性有机化合物的非凡协同作用

IF 5.9 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Journal of Environmental Sciences-china Pub Date : 2024-04-27 DOI:10.1016/j.jes.2024.04.025
Jinyan Xiao, Chi Zhang, Lei Yang, Shengwei Tang, Wenxiang Tang
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引用次数: 0

摘要

用简单的方法开发分层纳米结构催化剂以提高低温催化活性仍是一项挑战。本文在不使用任何模板和表面活性剂的情况下,通过碳酸氢铵沉淀法成功制备了一组不同形态的介孔Co-Cu二元金属氧化物,并将其进一步应用于致癌物甲苯的催化脱除。在不同配比的催化剂中,CoCu0.2 复合氧化物的性能最佳,在 240,000 mL/(gcat-hr) 的高重量时空速度(WHSV)条件下,甲苯 90% 转化所需的温度仅为 237°C。同时,与使用不同沉淀剂(NaOH 和 H2C2O4)制备的相关 Co-Cu 复合氧化物相比,NH4HCO3 衍生的 CoCu0.2 样品在甲苯氧化中表现出更好的催化效率,而 T90 分别比使用 NaOH 和 H2C2O4 方法制备的样品低 22°C 和 28°C。根据各种表征,可以推断出其优异的性能与晶体尺寸小(6.7 nm)、比表面积大(77.0 m2/g)、具有丰富的高价钴离子和吸附氧物种的中空分层纳米结构有关。原位 DRIFTS 进一步揭示了 CoCu0.2 催化剂氧化甲苯的可能反应路径,即吸收甲苯→苯甲醇→苯甲醛→苯甲酸→碳酸盐→CO2 和 H2O。此外,CoCu0.2 样品可保持长期稳定运行,在潮湿条件下(5 vol.% 水)几乎不会失活,这表明 NH4HCO3 衍生的 CoCu0.2 纳米催化剂在工业应用中去除 VOCs 方面具有巨大潜力。
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Extraordinary synergy on 3D hierarchical porous Co-Cu nanocomposite for catalytic elimination of VOCs at low temperature and high space velocity

It is still a challenge to develop hierarchically nanostructured catalysts with simple approaches to enhance the low-temperature catalytic activity. Herein, a set of mesoporous Co-Cu binary metal oxides with different morphologies were successfully prepared via a facile ammonium bicarbonate precipitation method without any templates or surfactants, which were further applied for catalytic removal of carcinogenic toluene. Among the catalysts with different ratios, the CoCu0.2 composite oxide presented the best performance, where the temperature required for 90% conversion of toluene was only 237°C at the high weight hour space velocity (WHSV) of 240,000 mL/(gcat·hr). Meanwhile, compared to the related Co-Cu composite oxides prepared by using different precipitants (NaOH and H2C2O4), the NH4HCO3-derived CoCu0.2 sample exhibited better catalytic efficiency in toluene oxidation, while the T90 were 22 and 28°C lower than those samples prepared by NaOH and H2C2O4 routes, respectively. Based on various characterizations, it could be deduced that the excellent performance was related to the small crystal size (6.7 nm), large specific surface area (77.0 m2/g), hollow hierarchical nanostructure with abundant high valence Co ions and adsorbed oxygen species. In situ DRIFTS further revealed that the possible reaction pathway for the toluene oxidation over CoCu0.2 catalyst followed the route of absorbed toluene → benzyl alcohol → benzaldehyde → benzoic acid → carbonate → CO2 and H2O. In addition, CoCu0.2 sample could keep stable with long-time operation and occur little inactivation under humid condition (5 vol.% water), which revealed that the NH4HCO3-derived CoCu0.2 nanocatalyst possessed great potential in industrial applications for VOCs abatement.

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来源期刊
Journal of Environmental Sciences-china
Journal of Environmental Sciences-china 环境科学-环境科学
CiteScore
13.70
自引率
0.00%
发文量
6354
审稿时长
2.6 months
期刊介绍: The Journal of Environmental Sciences is an international journal started in 1989. The journal is devoted to publish original, peer-reviewed research papers on main aspects of environmental sciences, such as environmental chemistry, environmental biology, ecology, geosciences and environmental physics. Appropriate subjects include basic and applied research on atmospheric, terrestrial and aquatic environments, pollution control and abatement technology, conservation of natural resources, environmental health and toxicology. Announcements of international environmental science meetings and other recent information are also included.
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