Selective electrochemical synthesis of urea from nitrate and CO2 via relay catalysis on hybrid catalysts
Selective electrochemical synthesis of urea from nitrate and CO2 via relay catalysis on hybrid catalysts
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通过混合催化剂的中继催化从硝酸盐和二氧化碳选择性电化学合成尿素
DOI：
10.1038/s41929-023-01020-4
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发表时间：
2023
期刊：
影响因子：
37.8
通讯作者：
Grigioni, Ivan
中科院分区：
文献类型：
--
作者：
Luo, Yuting;Xie, Ke;Ou, Pengfei;Lavallais, Chayse;Peng, Tao;Chen, Zhu;Zhang, Zhiyuan;Wang, Ning;Li, Xiao-Yan;Grigioni, Ivan
规模农业所需的氮循环依赖于能源和碳密集型过程，并产生含硝酸盐的废水。本文重点研究了硝酸盐与CO2的电化学共电解合成尿素的方法。当将其应用于工业废水或农业径流时，该方法有可能实现低碳强度的尿素生产，同时提供废水脱氮。我们报告了一种使用混合催化剂提高尿素选择性的策略：两类位点通过接力催化机制独立稳定尿素形成所需的关键中间体 * CO2 NO2和 * COOHNH 2。在废水水平的硝酸盐浓度（1，000 ppm NO3−[N]）下，Zn/Cu催化剂的法拉第效率达到75%。所得到的催化剂显示出16 µmol h−1cm−2的尿素生产速率。生命周期评估表明，电化学途径每千克尿素的温室气体排放量为0.28千克CO2 e，而目前的途径为1.8千克CO2 e kg− 1。
The nitrogen cycle needed for scaled agriculture relies on energy- and carbon-intensive processes and generates nitrate-containing wastewater. Here we focus on an alternative approach—the electrified co-electrolysis of nitrate and CO2to synthesize urea. When this is applied to industrial wastewater or agricultural runoff, the approach has the potential to enable low-carbon-intensity urea production while simultaneously providing wastewater denitrification. We report a strategy that increases selectivity to urea using a hybrid catalyst: two classes of site independently stabilize the key intermediates needed in urea formation, *CO2NO2and *COOHNH2, via a relay catalysis mechanism. A Faradaic efficiency of 75% at wastewater-level nitrate concentrations (1,000 ppm NO3−[N]) is achieved on Zn/Cu catalysts. The resultant catalysts show a urea production rate of 16 µmol h−1cm−2. Life-cycle assessment indicates greenhouse gas emissions of 0.28 kg CO2e per kg urea for the electrochemical route, compared to 1.8 kg CO2e kg−1for the present-day route.