Details

Autor(en) / Beteiligte

• Yu, Weikang
• Shu, Fenghao
• Huang, Yifeng
• Yang, Fangqi
• Meng, Qiangguo
• Zou, Zhi
• Wang, Jun
• Zeng, Zheling
• Zou, Guifu
• Deng, Shuguang

Titel

Enhanced electrocatalytic nitrogen reduction activity by incorporation of a carbon layer on SnS microflowers

Ist Teil von

• Journal of materials chemistry. A, Materials for energy and sustainability, 2020-10, Vol.8 (39), p.2677-2686

Ort / Verlag

Cambridge: Royal Society of Chemistry

Erscheinungsjahr

2020

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• Earth-abundant elements are highly desirable electrocatalysts for artificial N 2 fixation (NRR). However, most earth-abundant elements are inactive for the NRR, and the competitive hydrogen evolution reaction (HER) causes inferior faradaic efficiency. Thus, facile modification methods to transform an NRR-unfavorable electrocatalyst into its NRR-favorable counterpart are highly demanded. Herein, we present an efficient hydrophobic carbon layer incorporation strategy on tin monosulfide (SnS@C) to greatly boost the NRR activity of SnS. The hydrophobic carbon layer can limit proton availability at the electrode surface while integrating the advantages of strong N 2 adsorption and better conductivity that synergistically improve the NRR performance. Specifically, SnS@C delivers a high faradaic efficiency of 14.56% and NH 3 yield of 7.95 × 10 −11 mol s −1 cm −2 (24.33 μg NH 3 h −1 mg cat −1 ) at −0.5 V versus the reversible hydrogen electrode. It also exhibits durable stability for consecutive electrolysis over 18 h. Adequate control and 15 N isotopic labeling experiments confirm the reliability of N sources. Density functional theory calculations reveal that the superior activity is attributed to the redistribution and bias of electrons between the SnS and carbon-layer interface. This work highlights that the simple hydrophobic carbon layer incorporation strategy could guide the design and modification of advanced NRR catalysts. We report that incorporating a hydrophobic carbon layer can greatly boost the NRR activity of SnS. The C layer limits proton availability at the electrode surface while integrating the advantages of strong N 2 adsorption, better conductivity, and improved NRR performance.