Sulfur Atomically Doped Bismuth Nanobelt Driven by Electrochemical Self-Reconstruction for Boosted Electrocatalysis

Abstract

Recent years have witnessed various in-depth research efforts on selfreconstruction behavior toward electrocatalysis. Tracking the phase transformation and evolution of true active sites is of great significance for the development of self-reconstructed electrocatalysts. Here, the optimized atomic sulfur-doped bismuth nanobelt (S−Bi) is fabricated via an electrochemical self-reconstruction evolved from Bi 2 S 3 . Advanced technologies have demonstrated that the nonmetallic S atoms have been doped into the lattice Bi frame, leading to the reconstruction of local electronic structure of Bi. The asprepared S−Bi nanobelt exhibits a remarkable NH 3 generation rate of 10.28 μg h −1 mg −1 and Faradaic efficiency of 10.48%. Density functional theory calculations prove that the S doping can significantly lower the energy barrier of the rate-determining step and enlarge the N≡N bond for further dissociation toward N 2 fixation. This work not only establishes insights into the evolution process of electrochemically derived self-reconstruction but also unravels the root of the N 2 reduction reaction mechanism associated with the atomic nonmetal dopants.

Tracking structural evolution: operando regenerative CeOx/Bi interface structure for high-performance CO2 electroreduction

“…44-1246: Bi; JCPDS No. 34-0394: CeO 2 ), respectively [ 6 , 23 , 24 ]. The results indicated that the BiOCl was converted into metallic Bi, and the CeO 2 was apparently unchanged.…”

“…2 g). It is noted that the Ce 3+ species were obviously enriched from 26.1% to 42.3% as a result of the increase of oxygen defects during the reduction process (Supplementary Table 1) [ 24 ]. And these oxygen defects were readily filled by the hydroxyl in aqueous solution [ 25 ].…”

“…Thus Ce 4+ species in the CeO 2 component were readily reduced to the Ce 3+ species, but were hardly converted to Ce 0 species. It has to be pointed out that nanostructured metallic Bi is air-sensitive, and is easily surface-oxidized [ 24 ]. And the CeO 2 has the high ability to capture and release oxygen [ 31 , 32 ].…”

Promoting Electrocatalytic Hydrogen Evolution Reaction and Oxygen Evolution Reaction by Fields: Effects of Electric Field, Magnetic Field, Strain, and Light

“…[ 297 ] Ammonia, an essential chemical for both agriculture and industry applications, can be synthesized by nitrogen reduction reaction (NRR) under room temperature. [ 298–300 ] Furthermore, ORR is a rate‐limiting step of fuel cells. [ 301–305 ] However, the effects of external fields on these electrocatalysis have by far been rarely investigated.…”

How to select effective electrocatalysts: Nano or single atom?

“…In particular, a great deal of research has been devoted to exploiting the effective regulation of the morphology, composition, nanostructure, and molecular structure of electrocatalysts, so as to improve their electrocatalytic performance. [ 13–17 ] Among them, the nanoparticle electrocatalysts (NPCs) and emerging single atom site electrocatalysts (SACs) are considered to be the most potential electrocatalysts for several electrochemical reactions mentioned above (Figure 1). [ 18–24 ]…”