Plasma-etching enhanced titanium oxynitride active phase with high oxygen content for ambient electrosynthesis of ammonia
Plasma-etching enhanced titanium oxynitride active phase with high oxygen content for ambient electrosynthesis of ammonia
复制标题
用于常压电合成氨的高氧含量等离子蚀刻增强氮氧化钛活性相
DOI：
10.1016/j.elecom.2019.01.028
复制
发表时间：
2019-03-01
影响因子：
5.4
通讯作者：
Zhang, Haimin
中科院分区：
文献类型：
--
作者：
Kang, Shenghong;Wang, Jialu;Zhang, Haimin
Here we report that the plasma-etching processed commercial titanium nitride (TiN-PE, PE represents plasmaetching) that was first treated by ball-milling method (TiN-BM, BM represents ball-milling) is highly electrochemically active for the nitrogen (N-2) reduction reaction (NRR) to NH3. The results demonstrate that the TiN-PE as NRR electrocatalyst can deliver a yield rate of NH3 of 3.32 x 10(-)(10) mol s(-1) cm(-2) (4.1 mg h(-1) g(cat.)(-1)) with a Faradaic efficiency of 9.1% at - 0.6 V (vs. RHE) in 0.1 M Na2SO4 solution (pH = 3.2). The X-ray photoelectron spectroscopy (XPS) analysis indicates that the titanium oxynitride (TiOxNy) with high oxygen content on TiN surface was significantly enhanced by this plasma-etching approach, which is electrocatalytically active species for NRR. The N-15 isotopic labeling experimental results using N-15(2) as the feeding gas verify that the syntheized NH3 product during NRR is composed of N-15 in (NH4+)-N-15 (the enrichement of 64%) and N-14 in (NH4+)-N-14 (the enrichment of 36%), indicating that the NRR process follows the Mars-van Krevelen mechanism.
