Synthesis of ethylene urea using carbon-dioxide-adsorbed titanium–zirconium mixed oxides

Q2 Environmental Science Environmental Challenges Pub Date : 2024-06-27 DOI:10.1016/j.envc.2024.100970
Fiona Motswaiso , Ukyo Suzuki , Kyosuke Sawaguchi , Farzana Rahman , Tomohito Kameda , Shogo Kumagai , Yuko Saito , Toshiaki Yoshioka
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Abstract

To address the increasing global levels of CO2 emissions, it is necessary to develop efficient strategies that can convert CO2 into useful chemicals such as carbonates, ureas, and carbamates. Hybrid systems that combine direct capture and subsequent utilization of CO2 offer a unique emission-controlling pathway for achieving a carbon-neutral society. Ti-Zr mixed oxides could be ideal candidates for CO2 adsorption owing to the high specific surface areas pore sizes. Therefore, in this study, metal oxides with desirable acid-base sites that is, TixZr(1−x)O2 with different Ti/Zr ratios were synthesized using combined sol-gel and solvothermal methods and then utilized to adsorb and synthesize ethylene urea (EU), an important precursor of pharmaceuticals and agricultural products. The results indicated that the CO2 adsorption capacity of TiO2-ZrO2 mixed oxides were higher than that of TiO2 alone at 100 kPa and 25 °C, corresponding to their higher specific surface areas and pore volumes compared to their individual oxide counterparts. CO2-adsorbed TixZr(1−x)O2 was subsequently used as a CO2 source to generate EU through a reaction with ethylenediamine (EDA) and 2-propanol. Notably, samples containing higher proportions of Zr-Ti0.3Zr0.7O2 and ZrO2 produced EU in significant amounts, owing to their acid-base bifunctionality. Overall, EU was synthesized using CO2-adsorbed TixZr(1−x)O2 as a CO2 source and as an accelerator for reacting with EDA, without requiring high-pressure or high-purity CO2.

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利用二氧化碳吸附钛锆混合氧化物合成乙烯脲
为了解决全球二氧化碳排放量不断增加的问题,有必要制定高效的战略,将二氧化碳转化为有用的化学物质,如碳酸盐、脲和氨基甲酸酯。将二氧化碳的直接捕获和后续利用相结合的混合系统为实现碳中和社会提供了一种独特的排放控制途径。由于 Ti-Zr 混合氧化物具有高比表面积孔径,因此可以成为吸附二氧化碳的理想候选材料。因此,本研究采用溶胶-凝胶法和溶剂热法合成了具有理想酸碱位点的金属氧化物,即具有不同 Ti/Zr 比率的 TixZr(1-x)O2 ,然后利用其吸附和合成乙烯脲(EU),乙烯脲是一种重要的医药和农产品前体。结果表明,在 100 kPa 和 25 °C条件下,TiO2-ZrO2 混合氧化物的二氧化碳吸附能力高于单独的 TiO2,这与其比表面积和孔隙率高于单独的氧化物是相对应的。吸附了二氧化碳的 TixZr(1-x)O2 随后被用作二氧化碳源,通过与乙二胺(EDA)和 2-丙醇反应生成 EU。值得注意的是,Zr-Ti0.3Zr0.7O2 和 ZrO2 含量较高的样品由于具有酸碱双官能度而产生了大量的 EU。总之,使用二氧化碳吸附的 TixZr(1-x)O2 作为二氧化碳源和与 EDA 反应的促进剂合成了 EU,而不需要高压或高纯度的二氧化碳。
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来源期刊
Environmental Challenges
Environmental Challenges Environmental Science-Environmental Engineering
CiteScore
8.00
自引率
0.00%
发文量
249
审稿时长
8 weeks
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