Preparation of Sulfur and Nitrogen Co-doped Carbon-Based Porous Nanomaterials for Efficient Electrocatalytic N2 Reduction

• Published in: Journal of electronic materials Vol. 52; no. 3; pp. 2227 - 2235
• Main Authors: Wei, Bohui, Liang, Yaodong, Li, Lin, Yao, Chenzhong
• Format: Journal Article
• Language: English
• Published: New York Springer US 01.03.2023; Springer Nature B.V
• Subjects: Ammonia; Carbon; Catalysts; Characterization and Evaluation of Materials; Chemical reduction; Chemistry and Materials Science; Electrocatalysts; Electronics and Microelectronics; High temperature; Instrumentation; Materials Science; Nanomaterials; Nitrogen; Nitrogen oxides; Nitrogenation; Optical and Electronic Materials; Original Research Article; Photoelectrons; Raman spectroscopy; Solid State Physics; Spectrum analysis; Sulfur; electrocatalyst; Porous carbon; sulfur and nitrogen co-doping; ZIF-8; nitrogen reduction
• ISSN: 0361-5235; 1543-186X
• DOI: 10.1007/s11664-022-10189-6

Electrochemical nitrogen fixation represents a new strategy for low-cost fertilizer production because it can be carried out under mild conditions, but the selection of high-stability and high-activity electrocatalysts is a major challenge. In this work, nano-/mesoporous sulfur and nitrogen co-doped carbon as a nitrogen fixation catalyst was obtained by calcining sulfur-doped ZIF-8 at high temperature. The structures of the catalysts were characterized by transmission electron microscopy, x-ray diffraction, x-ray photoelectron spectroscopy, and Raman spectroscopy. The catalysts presented a highly disordered three-dimensional porous carbon structure. The formation of an appropriate amount of S 2− , S-O, nitrogen carbide, nitrogen oxide, and pyridinic nitrogen in the catalysts significantly promoted an electrochemical nitrogen reduction reaction (NRR). In 0.1 mol L −1 KOH, the S/N-C-11 catalyst showed a maximum ammonia production rate of 6.9396 μmol cm −2  h −1 and an optimal Faradaic efficiency of 22.74% at − 0.4 V versus a reversible hydrogen electrode under ambient conditions. These results suggest that porous carbon deliberately doped with select heteroatoms may serve as effective catalysts towards electrochemical NRR.