硼
法拉第效率
电催化剂
可逆氢电极
电化学
产量(工程)
碳纤维
材料科学
催化作用
氨
化学工程
三键
氮气
循环伏安法
无机化学
纳米技术
电极
碳纳米管
碳化
X射线光电子能谱
作者
Nan Li,Yueyu Tong,Hao Li,Liqun Wang,Feng Hou,Shi Xue Dou,Ji Liang
出处
期刊:Carbon
[Elsevier]
日期:2021-09-01
卷期号:182: 233-241
被引量:5
标识
DOI:10.1016/j.carbon.2021.05.060
摘要
Electrochemical reduction of dinitrogen (N 2 ) to ammonia (NH 3 ) at the ambient condition is a promising alternative to the traditional Haber-Bosch process due its energy-saving and eco-friendly natures. However, the extremely stable N N triple-bonds in N 2 molecules and the competitive hydrogen evolution reaction (HER) have been regarded as the two essential issues in the electrocatalytic nitrogen reduction reaction (eNRR), making the simultaneous achievement of a high NH 3 yield rate and a satisfactory Faradaic efficiency (FE) very difficult. To address this issue, we herein report a metal-free electrocatalyst, the boron-doped carbon nanosphere, to effectively activate the N N triple-bonds and suppress the HER during the eNRR process. In this protocol, the B–C configurations can be easily tailored by simply changing the boron precursor amount, and the one that is ( i.e. , BC 3 ) beneficial to the enhancement of eNRR can achieve the maximum relative content of ∼43% in the optimum sample. Under this boron-doping amount, the material simultaneously delivers a high NH 3 yield of 33.8 μg h −1 mg −1 cat and a high FE of 39.2% at −0.7 V vs. reversible hydrogen electrode, accompanied with a superior stability for a continuous eNRR. This study thus offers an efficient, stable, and low-cost carbon-based catalyst for eNRR. Boron-doped carbon nanospheres were reported as electrocatalysts to activate the N N triple-bonds and suppress the HER during the eNRR process. Significantly, the B–C configurations can be easily regulated by changing the boron precursor adding amount during materials fabrication. The B–C configuration that is most desirable to improve the eNRR performance ( i.e. , BC 3 ) can achieve the maximum relative content of ∼43% in the material, resulting in a simultaneous and significant enhancement in both ammonian yield rate (33.8 μg h −1 mg −1 cat ) and Faradaic efficiency (39.2% at −0.7 V vs. reversible hydrogen electrode).
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