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Coupling N2 and CO2 in H2O to synthesize urea under ambient conditions.
Nature Chemistry ( IF 21.8 ) Pub Date : 2020-06-15 , DOI: 10.1038/s41557-020-0481-9
Chen Chen 1 , Xiaorong Zhu 2 , Xiaojian Wen 3 , Yangyang Zhou 1 , Ling Zhou 1 , Hao Li 1 , Li Tao 1 , Qiling Li 1 , Shiqian Du 1 , Tingting Liu 1 , Dafeng Yan 1 , Chao Xie 1 , Yuqin Zou 1 , Yanyong Wang 1 , Ru Chen 1 , Jia Huo 1 , Yafei Li 2 , Jun Cheng 3 , Hui Su 4 , Xu Zhao 4 , Weiren Cheng 4 , Qinghua Liu 4 , Hongzhen Lin 5 , Jun Luo 6 , Jun Chen 7 , Mingdong Dong 8 , Kai Cheng 9 , Conggang Li 9 , Shuangyin Wang 1
Affiliation  

The use of nitrogen fertilizers has been estimated to have supported 27% of the world’s population over the past century. Urea (CO(NH2)2) is conventionally synthesized through two consecutive industrial processes, N2 + H2 → NH3 followed by NH3 + CO2 → urea. Both reactions operate under harsh conditions and consume more than 2% of the world’s energy. Urea synthesis consumes approximately 80% of the NH3 produced globally. Here we directly coupled N2 and CO2 in H2O to produce urea under ambient conditions. The process was carried out using an electrocatalyst consisting of PdCu alloy nanoparticles on TiO2 nanosheets. This coupling reaction occurs through the formation of C–N bonds via the thermodynamically spontaneous reaction between *N=N* and CO. Products were identified and quantified using isotope labelling and the mechanism investigated using isotope-labelled operando synchrotron-radiation Fourier transform infrared spectroscopy. A high rate of urea formation of 3.36 mmol g–1 h–1 and corresponding Faradic efficiency of 8.92% were measured at –0.4 V versus reversible hydrogen electrode.



中文翻译:

在环境条件下,将H2O中的N2和CO2耦合以合成尿素。

据估计,在过去的一个世纪中,氮肥的使用已为世界27%的人口提供了支持。尿素(CO(NH 22)通常通过两个连续的工业过程合成:N 2  + H 2  →NH 3,然后是NH 3  + CO 2  →尿素。两种反应均在苛刻的条件下运行,消耗了世界2%以上的能量。尿素合成消耗了全球生产的NH 3约80%。在这里,我们直接将H 2中的N 2和CO 2耦合O在环境条件下产生尿素。该过程是使用由PdCu合金纳米颗粒组成的电催化剂在TiO 2纳米片上进行的。这种偶联反应是通过* N = N *和CO之间的热力学自发反应通过形成C–N键而发生的。使用同位素标记法鉴定和定量了产物,并使用同位素标记的同步辐射-傅立叶变换红外光谱研究了机理。与可逆氢电极相比,在–0.4 V时测得的尿素形成速率高,为3.36 mmol g –1  h –1,相应的法拉第效率为8.92%。

更新日期:2020-06-15
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