原子缺陷工程可以合理地修饰反应中间体的化学行为,以调节催化性能。在这里,我们在In(OH)3纳米带的表面上产生了氧空位,用于高效的尿素电合成。当在In(OH)3纳米带的表面上构建氧空位时,尿素的法拉第效率达到80.1%,比原始In(OH)3纳米带(20.7%)高2.9倍。在-0.8V对可逆氢电极,在具有丰富氧空位的(OH)3纳米带中,尿素的部分电流密度为-18.8mAcm-2。在最近的报道中,这样的值代表尿素电合成的最高活性。密度泛函理论计算表明,与氧缺陷相邻的不饱和In位点有助于优化关键中间体的吸附构型,促进C-N偶联和吸附的CO2NH2中间体的活化。原位光谱测量进一步验证了氧空位对尿素电合成的促进作用。
The atomic defect engineering could feasibly decorate the chemical behaviors of reaction intermediates to regulate catalytic performance. Herein, we created oxygen vacancies on the surface of In(OH)3 nanobelts for efficient urea electrosynthesis. When the oxygen vacancies were constructed on the surface of the In(OH)3 nanobelts, the faradaic efficiency for urea reached 80.1%, which is 2.9 times higher than that (20.7%) of the pristine In(OH)3 nanobelts. At -0.8 V versus reversible hydrogen electrode, In(OH)3 nanobelts with abundant oxygen vacancies exhibited partial current density for urea of -18.8 mA cm-2. Such a value represents the highest activity for urea electrosynthesis among recent reports. Density functional theory calculations suggested that the unsaturated In sites adjacent to oxygen defects helped to optimize the adsorbed configurations of key intermediates, promoting both the C-N coupling and the activation of the adsorbed CO2NH2 intermediate. In-situ spectroscopy measurements further validated the promotional effect of the oxygen vacancies on urea electrosynthesis.