期刊
NANO ENERGY
卷 78, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.nanoen.2020.105213
关键词
Ni single atoms; Ni-C-4; Coordination tuning; CO2 reduction reaction; Hydrophobicity; Electrolyzer; Ni-N-x
类别
资金
- Australian Research Council (ARC) Research Hub on Integrated Energy Storage Solutions [IH180100020]
- UNSW Digital Grid Futures Institute, UNSW Sydney
- Ministry of Science and Technology in Taiwan [MOST 107-2113-M-002-008-MY3]
Nitrogen-coordinated single-atom catalysts (SACs) catalyzed electrochemical reduction of CO2 (CO2RR) to CO has emerged as a promising strategy in the management of the global carbon cycle. Herein, we carried out density functional theory (DFT) calculations to investigate the role of possible Ni-N-x and Ni-C-4 coordinations in CO2RR catalysis. We discover that the free energy change for CO2RR is lowered with a decrease in Ni-N-x co-ordination number, with Ni-C-4 displaying the lowest overpotential for CO2RR. Using these findings, we develop an effective strategy to transform Ni-N-4 to Ni-C-4 active sites by removing N moieties within Ni embedded in a hollow nitrogen-doped carbon shell (Ni@NCH). We demonstrate an improvement in CO selectivity with this transformation of active sites and the optimized Ni@NCH-1000 catalyst is capable of converting CO2 to CO with high Faradaic efficiency for CO (FECO) of 96% and a current density (j) of -35 mA cm(-2) at an applied potential of -1 V vs Reversible Hydrogen Electrode (RHE). When adopted in a high-throughput gas diffusion electrolyzer, the newly-developed superhydrophobic catalyst is capable of maintaining CO selectivity >95% over a wide range of applied cell voltages from 2.4 V to 3 V with high current densities (similar to 100 mA cm(-2) at 3 V). Our insights and findings with active site transformation in Ni-N-C SACs can serve as guidelines for designing highly active SACs for large-scale CO2RR systems.
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