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Accelerated Dinitrogen Electroreduction to Ammonia via Interfacial Polarization Triggered by Single-Atom Protrusions

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成果类型:
期刊论文
作者:
Li, Jie;Chen, Shang;Quan, Fengjiao;Zhan, Guangming;Jia, Falong;...
通讯作者:
Zhang, Lizhi
作者机构:
[Quan, Fengjiao; Zhang, Lizhi; Chen, Shang; Li, Jie; Zhan, Guangming; Jia, Falong; Ai, Zhihui] Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ,Inst Environm & Appl Chem, 152 Luoyu Rd, Wuhan 430079, Peoples R China.
通讯机构:
[Zhang, Lizhi] C
Cent China Normal Univ, Coll Chem, Key Lab Pesticide & Chem Biol, Minist Educ,Inst Environm & Appl Chem, 152 Luoyu Rd, Wuhan 430079, Peoples R China.
语种:
英文
关键词:
electric field;electrocatalytic ammonia synthesis;interfacial polarization;SDG7: Affordable and clean energy;single atom catalysis
期刊:
Chem
ISSN:
2451-9294
年:
2020
卷:
6
期:
4
页码:
885-901
基金类别:
Provoked by SAC-mediated decline in NRR interfacial energy barrier, we therefore pursued whether SACs expedite NRR via interfacial polarization. The theoretical feasibility is supported by the vast electrostatic potential difference between SACs and N2 when a sufficient EF was applied (Figures 3A, S45, S46, and S47). Quantitative analysis of this polarization field gives a magnitude of 17.92 eV (Figure 3B), outcompeting N2 ionization potential (15.84 eV). Electrons from SAC protrusions are driven by this field, 36% to N≡N and 60% to the zone between SACs and N2 (Figure 3C). Efficient N2 scission occurs as a consequence of electrons encompassing and thus attacking N2 cadre. As comparison, for pure and nanocluster-interspersed MoS2, rare electrons reach N2 owing to their respective curvature-free and curvature-marginal features that generate insufficient polarization.This work was financially supported by National Natural Science Funds for Distinguished Young Scholars of China (21425728), National Science Foundation of China (51472100), and the 111 Project (B17019). This work has also benefited from National Synchrotron Radiation Laboratory in Beijing and Shanghai for the characterization. We thank the National Supercomputer Center in Jinan for providing high performance computation. We thank Y. Pang for the help during the course of study. We thank L. Cai and J. Shang for the help during the DFT simulation. J.L. and L.Z. supervised the project. J.L. S.C. and F.Q. designed and carried out the experiments. G.Z. carried out the DFT simulations. F.J. and Z.A. contributed to data analysis. J.L. and L.Z. wrote the paper. All the authors discussed results and provided comments during the manuscript preparation. The authors declare no competing interests.
机构署名:
本校为第一且通讯机构
院系归属:
化学学院
摘要:
Electrocatalytic N2 reduction reaction (NRR) offers a promising low-energy, sustainable ammonia-synthesizing alternative to Haber-Bosch reaction. One roadblock lying in access to high-performance ammonia electrosynthesis emanates from the unsatisfied ability of electrocatalysts to wreck N≡N bond. Here, we report that interfacial polarization is an efficient scenario to enhance N≡N fracture to boost electrocatalytic ammonia synthesis. As a proof-of-concept demonstration, protrusion-shaped Fe single-atom catalysts immobilized onto MoS2 nanoshee...

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