Partially Nitrided Ni Nanoclusters Achieve Energy-Efficient Electrocatalytic CO 2 Reduction to CO at Ultralow Overpotential.
Runyao ZhaoYiding WangGuipeng JiJiajun ZhongFengtao ZhangMeifang ChenShengrui TongPeng WangZhonghua WuBuxing HanZhimin LiuPublished in: Advanced materials (Deerfield Beach, Fla.) (2022)
Electrocatalytic CO 2 reduction reaction (CO 2 RR) offers a promising strategy to lower CO 2 emission while producing value-added chemicals. A great challenge facing CO 2 RR is how to improve energy efficiency by reducing overpotentials. Herein, we report partially nitrided Ni nanoclusters (NiN x ) immobilized on N-doped carbon nanotubes (NCNT) for CO 2 RR, which achieves the lowest onset overpotential of 16 mV for CO 2 -to-CO and the highest cathode energy efficiency of 86.9% with CO Faraday efficiency >99.0% to date. Interestingly, NiN x /NCNT affords a CO generation rate of 43.0 mol⋅g -1 ⋅h -1 at a low potential of -0.572 V (versus RHE). DFT calculations reveal that the NiN x nanoclusters favour *COOH formation with lower Gibbs free energy than isolated Ni single-atom, hence lowering CO 2 RR overpotential. As NiN x /NCNT is applied to a membrane electrode assembly system coupled with oxygen evolution reaction, a cell voltage of only 2.13 V is required to reach 100 mA cm -2 , with total energy efficiency of 62.2%. This article is protected by copyright. All rights reserved.
Keyphrases
- carbon nanotubes
- metal organic framework
- sensitive detection
- reduced graphene oxide
- single cell
- fluorescent probe
- molecular dynamics
- density functional theory
- quantum dots
- energy transfer
- molecular dynamics simulations
- dna methylation
- molecular docking
- risk assessment
- stem cells
- gold nanoparticles
- electron transfer