|
|||||
|
|
Atomically Dispersed Nickel(I) on an Alloy-Encapsulated Nitrogen-Doped Carbon Nanotube Array for High-Performance Electrochemical CO2 Reduction Reaction |
|
| Authors: | Tianyu Zhang Xu Han Hongbin Yang Prof Aijuan Han Enyuan Hu Prof Yaping Li Prof Xiao-qing Yang Prof Lei Wang Prof Junfeng Liu Prof Bin Liu |
| Institution: | 1. State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029 P. R. China
School of Chemical and Biomedical Engineering, Nanyang Technological University, Singapore, Singapore;2. State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029 P. R. China;3. School of Chemical and Biomedical Engineering, Nanyang Technological University, Singapore, Singapore;4. Chemistry Division, Brookhaven National Laboratory, Upton, NY, USA;5. College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao, 266042 P. R. China |
| Abstract: | Single-atom catalysts (SACs) show great promise for electrochemical CO2 reduction reaction (CRR), but the low density of active sites and the poor electrical conduction and mass transport of the single-atom electrode greatly limit their performance. Herein, we prepared a nickel single-atom electrode consisting of isolated, high-density and low-valent nickel(I) sites anchored on a self-standing N-doped carbon nanotube array with nickel–copper alloy encapsulation on a carbon-fiber paper. The combination of single-atom nickel(I) sites and self-standing array structure gives rise to an excellent electrocatalytic CO2 reduction performance. The introduction of copper tunes the d-band electron configuration and enhances the adsorption of hydrogen, which impedes the hydrogen evolution reaction. The single-nickel-atom electrode exhibits a specific current density of −32.87 mA cm−2 and turnover frequency of 1962 h−1 at a mild overpotential of 620 mV for CO formation with 97 % Faradic efficiency. |
| Keywords: | carbon dioxide reduction reaction electrocatalysis nanoarrays single-atom catalysts |