Plasma-Enzyme Catalysis and Processing for Nitrogen Fixation from Artificial Urine in ‘Plasma Bubbles’

IF 7 2区 工程技术 Q1 ENERGY & FUELS
Changping Zhuang , Tianqi Zhang , Patrick Cullen , Nguyen Van Duc Long , Muhammad Yousaf Arshad , Marc Escribà-Gelonch , Nam Nghiep Tran , Volker Hessel
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Abstract

Artificial urine decomposition was studied in a gas–liquid microplasma reactor (‘plasma bubble reactor’) for nitrogen (N)-fixation, synthesising nitrate, nitrite, and ammonium in aqueous solution. The testing includes varying experimental parameters of non-catalytic and catalytic plasma operation. Longer reaction time and higher voltage, as expected, increased the N-fixation yield. At the highest input voltage (240 V) investigated, the N-fixation selectivity switches from nitrate to ammonium, which is the homologous N-product of urea. The nitrate yield almost doubles by isothermal operation at room temperature. Use of nitrogen plasma gives lower yield than for air plasma. Micro- and nano-scale refractory oxide catalysts were able to change the selectivity from nitrate towards ammonium, while maintaining the N-fixation yield. Enzyme catalysis by urease provides by far the highest ammonium yields (without nitrate or nitrite). Urease processing is most effective at 60 °C but has lower performance at 25 °C. In combination with plasma, the urease catalysis provides a mixture of ammonium, nitrate or nitrite, which demonstrates additive performance of both processes. Plasma processing of urea in the presence of organic N-compounds, typical for artificial urine, achieves much higher (up to a factor of four) nitrate and ammonium yields, seemingly boosting the urea conversion. The environmental impacts of the three process variants (enzyme, plasma-enzyme, plasma) are scoped, using circularity metrics, green chemistry metrics, and life cycle assessment, providing a holistic sustainability view. Main result is that combine plasma-enzyme operation is predicted to lower the environmental impact as compared to plasma-only operation via the practice in the AU system.
血浆酶催化及“血浆泡”中人工尿液固氮的处理
在气液微等离子体反应器(“等离子体气泡反应器”)中研究了人工尿液分解,用于固氮,在水溶液中合成硝酸盐,亚硝酸盐和铵。测试包括非催化和催化等离子体操作的不同实验参数。正如预期的那样,较长的反应时间和较高的电压提高了固氮收率。在最高输入电压(240 V)下,固氮选择性从硝态氮切换到氨态氮,后者是尿素的同源n产物。在室温下等温操作,硝酸盐产量几乎翻倍。氮等离子体的产量低于空气等离子体。微纳米级难降解氧化物催化剂能够改变硝态氮对铵态氮的选择性,同时保持固氮收率。脲酶催化的氨产量最高(不含硝酸盐或亚硝酸盐)。脲酶处理在60°C时最有效,但在25°C时性能较低。与血浆相结合,脲酶催化提供了铵、硝酸盐或亚硝酸盐的混合物,这表明了两种工艺的添加剂性能。在有机n化合物(典型的人造尿液)存在的情况下,血浆处理尿素可以获得更高的硝酸盐和铵的产量(高达四倍),似乎可以促进尿素的转化。使用循环度指标、绿色化学指标和生命周期评估,对三种工艺变体(酶、血浆酶、血浆)的环境影响进行了界定,提供了一个整体的可持续性观点。主要结果是,通过在AU系统中的实践,与仅等离子体操作相比,预计等离子体-酶联合操作可以降低对环境的影响。
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来源期刊
Sustainable Energy Technologies and Assessments
Sustainable Energy Technologies and Assessments Energy-Renewable Energy, Sustainability and the Environment
CiteScore
12.70
自引率
12.50%
发文量
1091
期刊介绍: Encouraging a transition to a sustainable energy future is imperative for our world. Technologies that enable this shift in various sectors like transportation, heating, and power systems are of utmost importance. Sustainable Energy Technologies and Assessments welcomes papers focusing on a range of aspects and levels of technological advancements in energy generation and utilization. The aim is to reduce the negative environmental impact associated with energy production and consumption, spanning from laboratory experiments to real-world applications in the commercial sector.
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