Triggering surface oxygen vacancies on atomic layered molybdenum dioxide for a low energy consumption path toward nitrogen fixation | |
Zhang, Gong; Ji, Qinghua; Zhang, Kai; Chen, Yu; Li, Zhaohui; Liu, Huijuan; Li, Jinghong; Qu, Jiuhui | |
刊名 | NANO ENERGY |
2019-05 | |
卷号 | 59页码:2020-10-16 |
关键词 | Oxygen vacancies Molybdenum dioxide N-2 Fixation Low-energy-consumption Electrocatalyst Ammonia |
ISSN号 | 2211-2855 |
英文摘要 | Facilitating catalyst accessibility to cleavage of N=N bond and breakage of competition from hydrogen evolution reaction (HER) remain great challenges in catalytic nitrogen reduction reaction (NRR). By fine confining of oxygen vacancies (OVs) in atomic layered molybdenum oxide (MoO2), we herein reported a sustainable strategy to tackle the rigorous requirements, thereby figuring out the deep-seated mechanism underlying the increment mechanism. X-ray absorption near edge structure (XANES) and Electron Paramagnetic Resonance (EPR) results primarily indicated that vast majority of OVs with different concentrations distributed well on layered MoO2. Based on the combined results of chemical N-2 adsorption isotherm and DFT calculation, we revealed that OVs favoured chemical adsorption for N-2 molecular via electron donation on defective Mo, providing the prerequisite for following activation. Remarkably, the energy change calculation unveiled that suitable confined OVs on MoO2 NRR followed an novel distal/alternating hybrid path, whereby the energy barrier was effectively lowered after directly protonation of N2H2* to HN2H2* (Delta G = 0.36 eV), so that OVs-MoO2 catalyst exhibited a high activity and selectivity with NH3 yield rate of similar to 12.20 mu g h(-1) mg(-1) and a Faradaic efficiency of 8.2% at a low potential of - 0.15 V. |
内容类型 | 期刊论文 |
源URL | [http://ir.rcees.ac.cn/handle/311016/43286] |
专题 | 生态环境研究中心_水污染控制实验室 |
作者单位 | 1.Zhengzhou Univ, Coll Chem & Mol Engn, Zhengzhou 450001, Henan, Peoples R China 2.Tsinghua Univ, Ctr Water & Ecol, Beijing 100084, Peoples R China 3.Tsinghua Univ, Sch Environm, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100084, Peoples R China 4.Chinese Acad Sci, Res Ctr Ecoenvironm Sci, Key Lab Drinking Water Sci & Technol, Beijing 100085, Peoples R China 5.Tsinghua Univ, Beijing Key Lab Microanalyt Methods & Instrumenta, Key Lab Bioorgan Phosphorus Chem & Chem Biol, Dept Chem, Beijing 100084, Peoples R China |
推荐引用方式 GB/T 7714 | Zhang, Gong,Ji, Qinghua,Zhang, Kai,et al. Triggering surface oxygen vacancies on atomic layered molybdenum dioxide for a low energy consumption path toward nitrogen fixation[J]. NANO ENERGY,2019,59:2020-10-16. |
APA | Zhang, Gong.,Ji, Qinghua.,Zhang, Kai.,Chen, Yu.,Li, Zhaohui.,...&Qu, Jiuhui.(2019).Triggering surface oxygen vacancies on atomic layered molybdenum dioxide for a low energy consumption path toward nitrogen fixation.NANO ENERGY,59,2020-10-16. |
MLA | Zhang, Gong,et al."Triggering surface oxygen vacancies on atomic layered molybdenum dioxide for a low energy consumption path toward nitrogen fixation".NANO ENERGY 59(2019):2020-10-16. |
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