A boron-interstitial doped C2N layer as a metal-free electrocatalyst for N2 fixation: a computational study. Issue 5 (16th January 2019)

• Record Type: Journal Article
• Authors: Ji, Shuang; Wang, Zhongxu; Zhao, Jingxiang
• Is Part Of: Journal of materials chemistry. Volume 7:Issue 5(2019)
• Page Start: 2392
• Page End: 2399
• Publication Date: 2019-01-16
• Subjects: Materials -- Research -- Periodicals; Chemistry, Analytic -- Periodicals; Environmental sciences -- Research -- Periodicals; 543.0284
• DOI: 10.1039/c8ta10497b
• Languages: English
• ISSNs: 2050-7488

Abstract

Abstract : The B-interstitial C2 N layer can be utilized as a novel metal-free electrocatalyst with high efficiency and selectivity for the NRR due to its low limiting potential and significant suppressing effect on the HER. Abstract : Electrochemical reduction of the naturally abundant nitrogen (N2 ) in aqueous solutions under ambient conditions is a quite promising way for ammonia (NH3 ) synthesis, in which the development of highly efficient electrocatalysts is a key scientific issue. Herein, by means of extensive density functional theory (DFT) computations, we proposed that a boron-interstitial (Bint )-doped C2 N layer can act as a metal-free electrocatalyst for N2 fixation and reduction to NH3 . Our computations revealed that the Bint -doped C2 N layer can sufficiently activate the N2 molecule through the "acceptance-donation" process due to its significant positive charge and magnetic moment on the B dopant. In particular, the subsequent N2 reduction reaction prefers to proceed via the enzymatic mechanism with a rather low limiting potential (−0.15 V), suggesting its superior catalytic performance for N2 reduction. Importantly, the Bint -doped C2 N layer possesses comparable stability to the experimentally available S-doped one and thus holds great promise for experimental synthesis. Thus, by carefully controlling the doping sites, the B-doped C2 N layer can be utilized as a quite promising metal-free catalyst with high-efficiency for N2 reduction, which may provide useful guidance for further facilitating sustainable NH3 synthesis.