Intrinsic Electron Localization of Metastable MoS2 Boosts Electrocatalytic Nitrogen Reduction to Ammonia

• DOI: 10.1002/adma.202007509
• Publication Date: 2021-07-05T07:13:38Z
• Authors: Gaoxin Lin; Qiangjian Ju; Xiaowei Guo; Wei Zhao; Samira Adimi; Jinyu Ye; Qingyuan Bi; Jiacheng Wang; Minghui Yang; Fuqiang Huang
• Keywords: Metastability

Abstract The advancement of efficient electrocatalysts toward the nitrogen reduction reaction (NRR) is critical in sustainable ammonia synthesis under ambient pressure and temperature. Manipulating electronic configuration particularly vital to form metal–nitrogen (MN) bonds during NRR through regulating active states sites. Here, sharp contrast stable 2H MoS 2 without metal chains, MoMo bonding metastable polymorphs bulk (zigzag chain 1T′ phase diamond 1T″′ phase) discovered significantly increase intrinsic electron localization around chains. This can enhance charge transfer from adsorbed molecule allowing for boosted kinetics. electrochemical experiments show that NH 3 yield rate faradaic efficiency rich with abundant Mo–Mo are about 9 12 times above average than those , correspondingly. Theoretical simulations reveal high local density surrounding chains sites promote π back‐donation, which beneficial increasing adsorption, strengthening MN bonds, reducing cleavage barrier triple NN bond.