Smart Interfacing between Co-Fe Layered Double Hydroxide and Graphitic Carbon Nitride for High-efficiency Electrocatalytic Nitrogen Reduction

Energy & Environmental Materials

article

Xiaohui Wu¹  Lu Tang¹  Yang Si²  Chunlan Ma³  Peng Zhang⁴  Jianyong Yu²  Yitao Liu¹  Bin Ding¹ 

[1] Key Laboratory of High Performance Fibers & Products ,(Ministry of Education), College of Textiles, Donghua University;Innovation Center for Textile Science and Technology, Donghua University;Jiangsu Key Laboratory of Micro and Nano Heat Fluid Flow Technology and Energy Application, School of Physical Science and Technology, Suzhou University of Science and Technology;State Center for International Cooperation on Designer Low-carbon & Environmental Materials ,(CDLCEM), School of Materials Science and Engineering, Zhengzhou University

关键词: density functional theory;    electrocatalytic nitrogen reduction;    graphitic carbon nitride;    interface engineering;    layered double hydroxide;   

DOI  :  10.1002/eem2.12316

来源: Wiley

【 摘 要 】

Bimetallic compounds such as hydrotalcite-type layered double hydroxides (LDHs) are promising electrocatalysts owing to their unique electronic structures. However, their abilities toward nitrogen adsorption and reduction are undermined since the surface-mantled, electronegative –OH groups hinder the charge transfer between transition metal atoms and nitrogen molecules. Herein, a smart interfacing strategy is proposed to construct a coupled heterointerface between LDH and 2D g-C3N4, which is proven by density functional theory (DFT) investigations to be favorable for nitrogen adsorption and ammonia desorption compared with neat LDH surface. The interfaced LDH and g-C3N4 is further hybridized with a self-standing TiO2 nanofibrous membrane (NM) to maximize the interfacial effect owing to its high porosity and large surface area. Profited from the synergistic superiorities of the three components, the LDH@C3N4@TiO2 NM delivers superior ammonia yield (2.07 × 10−9 mol s−1 cm−2) and Faradaic efficiency (25.3%), making it a high-efficiency, noble-metal-free catalyst system toward electrocatalytic nitrogen reduction.

【 授权许可】

Unknown