Mild and scalable synthesis of a high performance CrFeCoNiRu0.05 high entropy nano-alloy/carbon electrocatalyst for efficient urea production with a chelate-based ionic liquid

• Published in: New journal of chemistry Vol. 48; no. 21; pp. 9738 - 9747
• Main Authors: Zhang, Qingqing, Li, Ruiyi, Li, Zaijun, Yang, Yongqiang, Liu, Xiaohao
• Format: Journal Article
• Language: English
• Published: Cambridge Royal Society of Chemistry 2024
• Subjects: Alloys; Carbon; Carbon dioxide; Catalysis; Catalytic activity; Chelates; Chemical reactions; Chromium; Cobalt; Electrocatalysts; Electron conductivity; Electronegativity; Energy storage; Entropy; High entropy alloys; High temperature; Homogeneity; Ionic liquids; Iron; Low temperature; Nanoalloys; Nanocrystals; Nickel; Nitrogen atoms; Salicylic acid; Structural stability; Synthesis; Ureas
• ISSN: 1144-0546; 1369-9261
• DOI: 10.1039/d4nj00835a

High-entropy alloys show broad application prospects in electrocatalysis due to their high catalytic activity, conductivity and structural stability. However, achieving their mild and scalable synthesis still remains a great challenge. This paper reports a strategy for the synthesis of CrFeCoNiRu0.5 high entropy nano-alloy/carbon (termed as CrFeCoNiRu0.5–HENA/C) using a chelate-based ionic liquid. Cr(iii), Fe(iii), Co(ii), Ni(ii) and Ru(iii) were coordinated with salicylic acid ionic liquid to form a viscous metal complex solution, followed by low temperature carbonization and subsequent high temperature annealing. The resulting CrFeCoNiRu0.5–HENA/C consists of a three-dimensional carbon framework and CrFeCoNiRu0.5–HENA nanocrystal. The carbon framework offers high ion/electron conductivity and good affinity with NO3− and CO2 due to the presence of hydrophilic oxygen-containing groups and highly electronegative nitrogen atoms. The CrFeCoNiRu0.5–HENA nanocrystal has a small size of 52.5 ± 1.2 nm, good element homogeneity and high crystallinity. Such a unique structure improves the adsorption capacity towards NO3− and CO2 and the electrocatalytic activity towards the C–N coupling reaction. The CrFeCoNiRu0.5–HENA/C electrocatalyst exhibits a high urea yield of 35.57 ± 0.81 mmol gcatalyst−1 h−1 with a high faradaic efficiency of 21.02 ± 0.77%, which is much better than that of multi-component nano-alloys from Cr, Fe, Co, Ni and Ru. This study also provides an approach for the construction of high-entropy nano-alloys in catalysis, sensing and energy storage and conversion.