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Relative Humidity Facilitated Urea Particle Reaction with Salicylic Acid: A Combined In Situ Spectroscopy and DFT Study
ACS Earth and Space Chemistry ( IF 2.9 ) Pub Date : 2020-06-01 , DOI: 10.1021/acsearthspacechem.0c00051 Manoj Silva 1 , Karolina Barcauskaite 1, 2 , Donata Drapanauskaite 1, 2 , Huijie Tian 1 , Tomáš Bučko 3, 4 , Jonas Baltrusaitis 1
ACS Earth and Space Chemistry ( IF 2.9 ) Pub Date : 2020-06-01 , DOI: 10.1021/acsearthspacechem.0c00051 Manoj Silva 1 , Karolina Barcauskaite 1, 2 , Donata Drapanauskaite 1, 2 , Huijie Tian 1 , Tomáš Bučko 3, 4 , Jonas Baltrusaitis 1
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Population growth is necessitating a significant increase in crop production, while regulations require less use of nitrogen (N) (as fertilizers, such as urea) to minimize its environmental influx. A large fraction of applied N fertilizers is currently lost with significant negative environmental effects. The urea decomposition pathways explored in the literature chiefly concern the gas emissions but provide less mechanistic insights into the urea particle/soil interface after deposition and during their environmental processing (aging). The present work investigated the mechanistic role of relative humidity (RH) at the model humic material (salicylic acid)–urea interface and the resulting surface reactions using dynamic vapor sorption and in situ spatially resolved Raman spectroscopy, combined with ab initio thermodynamic calculations. The formation of a reaction product between urea and salicylic acid, used as a model compound of humic substances, was observed, resulting in the profoundly different response to RH, with the hysteresis due to the bulk urea no longer apparent. Ab initio and resulting NH3 emission measurement experiments suggest a decreased propensity of such reaction products to hydrolyze due to the formation of strong molecular bonds between urea and salicylic acid at the interface. The reaction was facilitated by the formation of a supersaturated layer of aqueous urea on the surface, which is likely the driving force behind the new product formation due to its higher vapor pressure. The results suggest that RH-driven reactions of urea and humic substances of soil could profoundly influence gas-phase emissions and thus affect the global nitrogen cycle. The impact of the stabilizing structure and the properties of the resulting urea reaction products on organic moieties needs to be further studied in the future to better understand the implications toward global N cycle.
中文翻译：
相对湿度促进尿素颗粒与水杨酸的反应：结合原位光谱和DFT研究
人口增长使得必须大幅提高农作物的产量，而法规要求减少对氮（N）（作为肥料，如尿素）的使用，以最大程度地减少其对环境的影响。目前，大量的氮肥流失，对环境造成了严重的负面影响。文献中探讨的尿素分解途径主要涉及气体排放，但在沉积后以及环境处理（老化）过程中对尿素颗粒/土壤界面的机理了解较少。本工作调查了模型腐殖质材料（水杨酸）-尿素界面处的相对湿度（RH）的机械作用，以及利用动态蒸气吸附和原位空间分辨拉曼光谱结合表面活性产生的表面反应。从头算热力学计算。观察到尿素和水杨酸之间的反应产物的形成（用作腐殖质的模型化合物），导致对RH的反应截然不同，由于大量尿素引起的滞后现象不再明显。从头算和所得NH 3发射测量实验表明，由于在界面上尿素和水杨酸之间形成了牢固的分子键，因此这种反应产物水解的倾向降低。通过在表面上形成尿素水过饱和层来促进反应，这可能是由于较高的蒸气压而形成新产物的驱动力。结果表明，尿素和腐殖质在土壤中的相对湿度驱动反应可深刻影响气相排放，进而影响全球氮循环。将来需要进一步研究稳定结构和所得尿素反应产物的性质对有机部分的影响，以更好地了解其对全球氮循环的影响。
更新日期：2020-07-16
中文翻译：
相对湿度促进尿素颗粒与水杨酸的反应：结合原位光谱和DFT研究
人口增长使得必须大幅提高农作物的产量，而法规要求减少对氮（N）（作为肥料，如尿素）的使用，以最大程度地减少其对环境的影响。目前，大量的氮肥流失，对环境造成了严重的负面影响。文献中探讨的尿素分解途径主要涉及气体排放，但在沉积后以及环境处理（老化）过程中对尿素颗粒/土壤界面的机理了解较少。本工作调查了模型腐殖质材料（水杨酸）-尿素界面处的相对湿度（RH）的机械作用，以及利用动态蒸气吸附和原位空间分辨拉曼光谱结合表面活性产生的表面反应。从头算热力学计算。观察到尿素和水杨酸之间的反应产物的形成（用作腐殖质的模型化合物），导致对RH的反应截然不同，由于大量尿素引起的滞后现象不再明显。从头算和所得NH 3发射测量实验表明，由于在界面上尿素和水杨酸之间形成了牢固的分子键，因此这种反应产物水解的倾向降低。通过在表面上形成尿素水过饱和层来促进反应，这可能是由于较高的蒸气压而形成新产物的驱动力。结果表明，尿素和腐殖质在土壤中的相对湿度驱动反应可深刻影响气相排放，进而影响全球氮循环。将来需要进一步研究稳定结构和所得尿素反应产物的性质对有机部分的影响，以更好地了解其对全球氮循环的影响。
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