Journal
ACS NANO
Volume 15, Issue 7, Pages 12109-12118Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.1c03465
Keywords
electrochemical nitrogen reduction reaction; synergistic effect; Mo-N-C active sites; nitrogen configuration; in situ FTIR
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Funding
- National Natural Science Foundation of China [21573115, 21875118]
- Natural Science Foundation of Tianjin [19JCZDJC37700]
- Tianjin Research Innovation Project for Postgraduate Students [2020YJSB143]
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The hybridization of MoS2 and N-doped carbon can synergistically enhance the efficiency of electrochemical nitrogen reduction reaction (NRR). In this study, the decisive role of pyridinic-N-Mo bonding in enhancing NRR electrocatalysis was revealed, providing deep insights into the underlying mechanisms at a molecular level.
For electrochemical nitrogen reduction reaction (NRR), hybridizing transition metal (TM) compounds with nitrogen-doped carbonaceous materials has been recognized as a promising strategy to improve the activity and stability of electrocatalysts due to the synergistic interaction from the TM-N-C active sites. Nevertheless, up to date, the fundamental mechanism of this so-called synergistic electrocatalysis for NRR is still unclear. Particularly, it remains ambiguous which configuration of N dopants, either pyridinic N or pyrrolic N, when coordinated with the TM, predominately contributes to this synergy. Herein, a self-assembled three-dimensional 1T-phase MoS2 microsphere coupled with N-doped carbon was developed (termed MoS2/NC), showing an impressive NRR performance in neutral medium. The hybridization of MoS2 and N-doped carbon can synergistically enhance the NRR efficiency by optimizing the electron transfer of catalyst. Acidification/blocking/poisoning experiments reveal the decisive role of pyridinic-N-Mo bonding, rather than pyrrolic-N-Mo bonding, in synergistically enhancing NRR electrocatalysis. The electrochemical-based in situ Fourier transform infrared spectroscopy (in situ FTIR) technology provides deep insights into the substantial contribution of pyridinic-N-MoS2 sites to NRR electrocatalysis and further uncover the underlying mechanism (associative pathway) at a molecular level.
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