Engineering Steam Induced Surface Oxygen Vacancy onto Ni–Fe Bimetallic Nanocomposite for CO2 Electroreduction. Issue 15 (27th February 2022)

• Record Type: Journal Article
• Authors: He, Qiang; Zhang, Yanxing; Li, Haijing; Yang, Yang; Chen, Shuai; Yan, Wenjun; Dong, Juncai; Zhang, Xian‐Ming; Fan, Xiujun
• Is Part Of: Small. Volume 18:Issue 15(2022)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-02-27
• Subjects: bimetallic nanocomposites -- chemical vapor deposition -- CO 2 reduction reaction -- oxygen vacancies -- steam treatment; Nanotechnology -- Periodicals; Nanoparticles -- Periodicals; Microtechnology -- Periodicals; 620.5
• DOI: 10.1002/smll.202108034
• Languages: English
• ISSNs: 1613-6810

Abstract

Abstract: Surface oxygen vacancies (Vo ) regulation is an effective strategy to improve the electrochemical CO2 reduction reaction (CO2 RR) performance by lowering the activation energy barrier of CO2 ; however, the lack of precise control over the local atomic structures severely hinders the large‐scale application of Vo ‐activated electrocatalyst for CO2 RR. Herein, an efficient strategy to facilitate CO2 activation is developed by introducing Vo into transition metal nanoparticles (NPs) with a steam‐assisted chemical vapor deposition method. With the steam process, abundant surface Vo are introduced into the assembled Ni–Fe bimetallic NPs composite (H‐NiFe/NG), which adjust surface Ni/Fe atoms to low‐valent coordinatively unsaturated Ni (+1)/Fe (+2) sites, serving as electron‐rich centers to adsorb and activate inert CO2 molecules. The as‐prepared H‐NiFe/NG composite exhibits excellent catalytic performance with a maximum Faradaic efficiency of 94% at −0.80 V (vs RHE) for CO production with remarkable stability. The density function theory calculations corroborate that the Ni atoms around surface Vo significantly lower the energy barrier for COOH* intermediate formation, which gives a low overpotential for reducing CO2 to CO, exhibiting superior CO2 RR performance. This general synthetic strategy provides a new insight to introduce surface Vo on transition metal for efficient CO2 reduction. Abstract : A steam‐assisted chemical vapor deposition method is reported to facilitate the CO2 reduction reaction on iron‐group metal. With the steam process, abundant surface oxygen vacancies are introduced into the assembled Ni–Fe bimetallic nanoparticle composites, which effectively activate the basal plane metal active sites, serving as electron‐rich centers to adsorb and activate inert CO2 molecules.