期刊
INNOVATION
卷 3, 期 1, 页码 -出版社
CELL PRESS
DOI: 10.1016/j.xinn.2021.100190
关键词
-
资金
- National Natural Science Foundation of China [21972010]
- Beijing Natural Science Foundation [2192039]
- State Key Laboratory of Organic-Inorganic Composites [oic-201901001]
- Beijing University of Chemical Technology [XK180301]
- NRF Korea [NRF-2016M3D1A1021147]
- DCCEM, at the Materials Department, Oxford [EP/R010145/1]
This study successfully increased the efficiency of ambient NRR for ammonia production by tuning the Te vacancies and surface hydrophobicity of two-dimensional TaTe2 nanosheets. It achieved remarkable NH3 faradic efficiency and maintained high stability, with the edge plane of TaTe2 and VTe identified as the main active sites for NRR.
Demand for ammonia continues to increase to sustain the growing global population. The direct electrochemical N-2 reduction reaction (NRR) powered by renewable electricity offers a promising carbon-neutral and sustainable strategy for manufacturing NH3, yet achieving this remains a grand challenge. Here, we report a synergistic strategy to promote ambient NRR for ammonia production by tuning the Te vacancies (VTe) and surface hydrophobicity of two-dimensional TaTe2 nanosheets. Remarkable NH3 faradic efficiency of up to 32.2% is attained at a mild overpotential, which is largely maintained even after 100 h of consecutive electrolysis. Isotopic labeling validates that the N atoms of formed NH4+ originate from N-2. In situ X-ray diffraction indicates preservation of the crystalline structure of TaTe2 during NRR. Further density functional theory calculations reveal that the potential-determining step (PDS) is *NH2 + (H+ + e(-)) -> NH3 on VTe-TaTe2 compared with that of * + N-2 + (H+ + e-) -> *N-NH on TaTe2. We identify that the edge plane of TaTe2 and VTe serve as the main active sites for NRR. The free energy change at PDS on VTe-TaTe2 is comparable with the values at the top of the NRR volcano plots on various transition metal surfaces.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据