Abstract
Electrochemical carbon monoxide reduction is a promising strategy for the production of value-added multicarbon compounds, albeit yielding diverse products with low selectivities and Faradaic efficiencies. Here, copper single atoms anchored to Ti3C2Tx MXene nanosheets are firstly demonstrated as effective and robust catalysts for electrochemical carbon monoxide reduction, achieving an ultrahigh selectivity of 98% for the formation of multicarbon products. Particularly, it exhibits a high Faradaic efficiency of 71% towards ethylene at −0.7 V versus the reversible hydrogen electrode, superior to the previously reported copper-based catalysts. Besides, it shows a stable activity during the 68-h electrolysis. Theoretical simulations reveal that atomically dispersed Cu–O3 sites favor the C–C coupling of carbon monoxide molecules to generate the key *CO-CHO species, and then induce the decreased free energy barrier of the potential-determining step, thus accounting for the high activity and selectivity of copper single atoms for carbon monoxide reduction.
| Original language | English |
|---|---|
| Article number | 238 |
| Journal | Nature Communications |
| Volume | 12 |
| Issue number | 1 |
| DOIs | |
| State | Published - Dec 1 2021 |
| Externally published | Yes |
Funding
This work was financially supported by the National Key R&D Program of China (2017YFA0700104), the National Natural Science Foundation of China (22075211, 51971157, 51808037, 21601136, and 51761165012), the Tianjin Science Fund for Distinguished Young Scholars (19JCJQJC61800), and the Science and Technology Development Fund of Tianjin Education Commission for Higher Education (No. 2018KJ126). The authors acknowledge Beijng PARATERA Tech CO., Ltd. for providing HPC resources that have contributed to the research results reported within this paper. The authors also thank Stanford Synchrotron Radiation Lightsource (SSRL) BL7-3 for providing the beam time. R.C. acknowledges support from DOE funded LDRD program and SSRL.