Journal
ADVANCED FUNCTIONAL MATERIALS
Volume 30, Issue 11, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.201907376
Keywords
electrocatalysis; nitrogen reduction reaction; rhenium disulfide; transition-metals
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Funding
- National Natural Science Foundation of China [51433001, 21674019, 21604010, 51671003, 21802003]
- China Postdoctoral Science Foundation [2016M600268, 2017T100255, 2017M620494, 2018M631239]
- Program of Shanghai Academic Research Leader [17XD1400100]
- National Key Research and Development Program of China [2016YFB0100201]
- Chenguang Program - Shanghai Education Development Foundation
- Shanghai Municipal Education Commission
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Electrocatalytic nitrogen reduction reaction (NRR) and hydrogen evolution reaction (HER) are intriguing approaches to nitrogen fixation and hydrogen production under ambient conditions, given the need to discover efficient and stable catalysts to light up the green chemistry future. However, bottlenecks are often found during N-2/H2O activation, the very first step of NRR/HER, due to energetic electron injection from the surface of electrocatalysts. It is reported that the bottlenecks for both NRR and HER can be tackled by engineering the energy level via low-valent transition-metal doping, simultaneously, where rhenium disulfide (ReS2) is employed as a model platform to prove the concept. The doped low-valent transition-metal domains (e.g., Fe, Co, Ni, Cu, Zn) in ReS2 provide more active sites for N-2/H2O chemisorption and electron transfer, not only weakening the N(sic)N/O-H bonds for easier dissociation through proton coupling, but also elevating d-band center toward the Fermi level with more electron energy for N-2/H2O reduction. As a result, it is found that iron-doped ReS2 nanosheets wrapped nitrogen-doped carbon nanofiber (Fe-ReS2@N-CNF) catalyst exhibits superior electrochemical activity with eightfold higher ammonia production yield of 80.4 mu g h(-1) mg(cat.)(-1), and lower onset overpotential of 146 mV and Tafel slope of 63 mV dec(-1), when comparing with the pristine ReS2.
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