State Key Laboratory of Chem/Bio-Sensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University, Changsha, P. R. China.
College of Chemistry and Materials Science, Nanjing Normal University, Nanjing, P. R. China.
Nat Chem. 2020 Aug;12(8):717-724. doi: 10.1038/s41557-020-0481-9. Epub 2020 Jun 15.
The use of nitrogen fertilizers has been estimated to have supported 27% of the world's population over the past century. Urea (CO(NH)) is conventionally synthesized through two consecutive industrial processes, N + H → NH followed by NH + CO → urea. Both reactions operate under harsh conditions and consume more than 2% of the world's energy. Urea synthesis consumes approximately 80% of the NH produced globally. Here we directly coupled N and CO in HO to produce urea under ambient conditions. The process was carried out using an electrocatalyst consisting of PdCu alloy nanoparticles on TiO 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 h and corresponding Faradic efficiency of 8.92% were measured at -0.4 V versus reversible hydrogen electrode.
据估计,在过去一个世纪里,氮肥的使用养活了全世界 27%的人口。传统上,尿素(CO(NH))是通过两个连续的工业过程合成的,即 N+H→NH,然后 NH+CO→urea。这两个反应都在苛刻的条件下进行,消耗了全球超过 2%的能源。尿素合成消耗了全球生产的 NH 的大约 80%。在这里,我们在 HO 中直接将 N 和 CO 耦合,在环境条件下生成尿素。该过程使用由 PdCu 合金纳米粒子负载在 TiO 纳米片上的电催化剂进行。这种偶联反应是通过 N=N 和 CO 之间的热力学自发反应形成 C-N 键来实现的。通过使用同位素标记来鉴定和定量产物,并使用同位素标记的原位同步辐射傅里叶变换红外光谱来研究反应机制。在相对于可逆氢电极的-0.4 V 下,测量到 3.36 mmol g h 的高尿素形成速率和相应的法拉第效率 8.92%。