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Refining Energy Levels in ReS₂ Nanosheets by Low‐Valent Transition‐Metal Doping for Dual‐Boosted Electrochemical Ammonia/Hydrogen Production

Lai, F; Chen, N; Ye, X; He, G; Zong, W; Holt, KB; Pan, B; ... Chen, R; + view all (2020) Refining Energy Levels in ReS₂ Nanosheets by Low‐Valent Transition‐Metal Doping for Dual‐Boosted Electrochemical Ammonia/Hydrogen Production. Advanced Functional Materials , 30 (11) , Article 1907376. 10.1002/adfm.201907376. Green open access

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Abstract

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 N2/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 N2/H2O chemisorption and electron transfer, not only weakening the N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 N2/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 µg h−1 mg−1cat., and lower onset overpotential of 146 mV and Tafel slope of 63 mV dec−1, when comparing with the pristine ReS2.

Type: Article
Title: Refining Energy Levels in ReS₂ Nanosheets by Low‐Valent Transition‐Metal Doping for Dual‐Boosted Electrochemical Ammonia/Hydrogen Production
Open access status: An open access version is available from UCL Discovery
DOI: 10.1002/adfm.201907376
Publisher version: https://doi.org/10.1002/adfm.201907376
Language: English
Additional information: This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions.
Keywords: electrocatalysis, nitrogen reduction reaction, rhenium disulfide, transition‐metals
UCL classification: UCL
UCL > Provost and Vice Provost Offices > UCL BEAMS
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences
UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry
URI: https://discovery.ucl.ac.uk/id/eprint/10091482
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