电化学
法拉第效率
氨生产
氨
可逆氢电极
化学
无机化学
产量(工程)
氢
反应机理
材料科学
作者
Weizheng Cai,Ya-Fei Jiang,Jincheng Zhang,Hongbin Yang,Junming Zhang,Cong-Qiao Xu,Wei Liu,Jun Li,Bin Liu
出处
期刊:Chem catalysis
[Elsevier]
日期:2022-05-01
卷期号:2 (7): 1764-1774
被引量:1
标识
DOI:10.1016/j.checat.2022.05.009
摘要
The electrochemical nitrogen reduction reaction (eNRR) offers a promising strategy to synthesize ammonia at ambient conditions. However, the selectivity and yield of ammonia are greatly impeded by the slow kinetics of the eNRR and the competing hydrogen evolution reaction (HER). Herein, we find that by growing Ru nanoparticles on rutile TiO 2 , the intimate electronic coupling between Ru nanoparticles and TiO 2 support is able to greatly promote the first protonation of N 2 via an associative mechanism in the eNRR while suppressing the HER, resulting in a greatly improved ammonia Faradaic efficiency of 40.7% and yield of 10.4 μg NH3 h −1 cm −2 geometric area at −0.15 V versus the reversible hydrogen electrode (RHE) in 0.5 M K 2 SO 4 aqueous solution at room temperature and ambient pressure. Our work provides a general approach to achieve selective electrochemical reaction by controlling the binding strength of reactive intermediates via interface engineering. • Greatly improved ammonia Faradaic efficiency with suppressed HER • Interface engineering to control the binding strength of reactive intermediates • In situ spectroscopies to observe N–H-related intermediates during eNRR As a key process of ammonia-based energy prospective, ammonia synthesis via the electrochemical nitrogen reduction reaction (eNRR) at ambient conditions has been widely studied in recent years. However, the poor selectivity and low yield of ammonia are still the main challenges due to the slow kinetics of the eNRR and the competing hydrogen evolution reaction (HER). Herein, we present a simple method to prepare Ru/TiO 2 that exhibits high Faradaic efficiency for the eNRR toward producing ammonia. By a sophisticated design of the Ru/TiO 2 interface, the binding strength of H-related intermediates is weakened, while the binding strength of N 2 -related intermediates is strengthened, resulting in promoted reaction kinetics of the eNRR with suppressed HER. This work provides an effective and controllable method of interfacial engineering to boost the activity and selectivity of the electrochemical reaction by controlling the binding strength of reactive intermediates. To address the challenges of low activity and poor selectivity in the electrochemical nitrogen reduction reaction (eNRR), Ru/TiO 2 with a sophisticated interface is designed and synthesized. By constructing the Ru-TiO 2 interface, the valence states of Ru can be carefully modulated, resulting in promoted reaction kinetics of the eNRR with suppressed HER.
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