Biomimetic FeMo(Se, Te) as Joint Electron Pool Promoting Nitrogen Electrofixation. (23rd February 2022)

• Record Type: Journal Article
• Authors: Sun, Yuntong; Ding, Shan; Xia, Baokai; Duan, Jingjing; Antonietti, Markus; Chen, Sheng
• Is Part Of: Angewandte Chemie. Volume 134:Number 16(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-02-23
• Subjects: Electrocatalysis -- Molybdenum Selenide -- Nanomaterials -- Nitrogen Fixation; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.202115198
• Languages: English
• ISSNs: 0044-8249

Abstract

Abstract: It has been long believed that the FeMoS structure, where Fe is bonded with S, plays a pivotal role as a biomimetic catalyst for electrochemical nitrogen (N2 ) fixation. Nevertheless, the structure of Fe bonded to heavier analogues (Se or Te) has never been explored for N2 electrofixation. Here, we theoretically predict the electronic structure of FeMo(Se, Te) composed of tri‐coordinated Fe species with open shells for binding with Se, which forms a joint electron pool for promoting N2 activation. Guided by this interesting prediction, we then demonstrate a two‐step procedure to synthesize such structures, which display remarkable N2 electrofixation activities with an ammonia yield of 72.54 μg h −1 mg −1 and a Faradic efficiency of 51.67 % that are more than three times of the FeMoS counterpart. Further mechanism studies have been conducted by density function theory (DFT) simulations. This work provides new clues for designing versatile electrocatalytic materials for large‐scale industrialization. Abstract : Nitrogenase‐inspired FeMo(Se, Te) catalysts have been theoretically predicted and experimentally synthesized. They exhibit remarkable structural features of joint electron pool for promoting N2 electrofixation.