过电位
电化学
法拉第效率
氨
电解
氧化还原
密度泛函理论
空位缺陷
化学
材料科学
纳米技术
化学工程
无机化学
结晶学
电极
物理化学
计算化学
有机化学
工程类
电解质
作者
Zhenqing Zhao,Jongseo Park,Changhyeok Choi,Song Hong,Xiangchao Hui,Hao Zhang,Tsz Woon Benedict Lo,Alex W. Robertson,Zengxiang Lv,Yousung Jung,Zhenyu Sun
出处
期刊:The Innovation
[Elsevier]
日期:2022-01-01
卷期号:3 (1): 100190-100190
被引量:20
标识
DOI:10.1016/j.xinn.2021.100190
摘要
Demand for ammonia continues to increase to sustain the growing global population. The direct electrochemical N2 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 N2. 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 ∗ + N2 + (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.
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