Impurity Tolerance of Unsaturated Ni-N-C Active Sites for Practical Electrochemical CO2 Reduction
Source abstract
Abstract
Demonstrating the potential of the electrochemical carbon dioxide reduction reaction (CO2RR) in industrially relevant conditions is a promising route for achieving net-zero emissions through decarbonization. This requires a catalyst system that displays not only high activity and stability but also the capacity to deliver a consistent performance in the presence of waste stream impurities. To explore these opportunities, we investigate the role that the Ni coordination structure plays on the impurity tolerance of highly active single-atom catalysts (SACs) during CO2RR. The as-synthesized materials are highly active for CO2RR to CO, achieving a current density of 470 mA cm–2 and a CO selectivity of 99% in a CO2 electrolyzer. We demonstrate, through high-temperature pyrolysis, that a higher concentration of “unsaturated” Ni-N4-x-Cx sites significantly improves the tolerance to NOx, SOx, volatile organic compounds, and SCN– impurities in aqueous electrolyte, paving the way for SACs capable of CO2RR in industrial conditions.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: CO2 Reduction Techniques and Catalysts · Electrocatalysts for Energy Conversion · Catalytic Processes in Materials Science
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
School of Chemical Engineering, University of New South Wales, Sydney, NSW 2052, Australia
College of Engineering and Computer Science, Australian National University, Canberra, ACT 2601, Australia
Nanotechnology Research Laboratory, College of Engineering and Computer Science, The Australian National University, Canberra, ACT 2601, Australia
Australian Centre for Microscopy and Microanalysis, The University of Sydney, Sydney, New South Wales 2006, Australia
School of Chemistry and the ARC Centre of Excellence for Electromaterials Science, Monash University, Victoria, VIC 3800, Australia
School of Science, Swinburne University of Technology, Melbourne, VIC 3122, Australia
Australian Synchrotron, Clayton, VIC 3168, Australia
Funding
Australian Research Council
References (52)
Show source-provided references
1. 10.1021/acsenergylett.0c0224910.1021/acsenergylett.0c02249 ↗
2. Friedman D. · 2012 · 21
3. 10.1016/j.nanoen.2020.10521310.1016/j.nanoen.2020.105213 ↗
4. 10.1039/C9TA02405K10.1039/C9TA02405K ↗
5. 10.1038/s41467-020-16119-610.1038/s41467-020-16119-6 ↗
6. 10.1002/smll.20190366810.1002/smll.201903668 ↗
7. 10.1021/acsnano.1c0329310.1021/acsnano.1c03293 ↗
8. 10.1038/s41929-020-00546-110.1038/s41929-020-00546-1 ↗
9. 10.1007/s41918-019-00050-610.1007/s41918-019-00050-6 ↗
10. 10.1007/s11356-016-6810-210.1007/s11356-016-6810-2 ↗
11. Schmick, M. T.; Last, G. V. Identification and Selection of Major Carbon Dioxide Stream Compositions, PNNL-20493; U.S. Department of Energy, June 2011.
12. 10.1016/j.ijggc.2013.08.02110.1016/j.ijggc.2013.08.021 ↗
13. 10.1021/jacs.9b0321510.1021/jacs.9b03215 ↗
14. 10.1016/j.jcou.2020.10131510.1016/j.jcou.2020.101315 ↗
15. 10.1038/s41467-020-19731-810.1038/s41467-020-19731-8 ↗
16. 10.1039/C9SE00024K10.1039/C9SE00024K ↗
17. 10.1149/1.322017510.1149/1.3220175 ↗
18. 10.1021/acsaem.9b0147010.1021/acsaem.9b01470 ↗
19. 10.1002/smll.20200189610.1002/smll.202001896 ↗
20. 10.1002/advs.20190308910.1002/advs.201903089 ↗
21. 10.1021/jacs.8b0983410.1021/jacs.8b09834 ↗
22. 10.1039/D0TA04943C10.1039/D0TA04943C ↗
23. 10.3389/fctls.2021.75416710.3389/fctls.2021.754167 ↗
24. 10.1021/acsnano.9b0924510.1021/acsnano.9b09245 ↗
25. 10.1039/C9SE00814D10.1039/C9SE00814D ↗
26. 10.1098/rsta.2010.021310.1098/rsta.2010.0213 ↗
27. 10.1209/epl/i2001-00105-410.1209/epl/i2001-00105-4 ↗
28. 10.3390/c703005110.3390/c7030051 ↗
29. 10.1016/j.carbon.2020.02.06510.1016/j.carbon.2020.02.065 ↗
30. 10.1016/S0039-6028(96)01179-X10.1016/S0039-6028(96)01179-X ↗
31. 10.1103/PhysRevLett.27.120410.1103/PhysRevLett.27.1204 ↗
32. 10.1002/aenm.20190210610.1002/aenm.201902106 ↗
33. 10.1039/C9SE00252A10.1039/C9SE00252A ↗
34. 10.1002/9781118684030.ch1410.1002/9781118684030.ch14 ↗
35. 10.1021/jacs.7b0907410.1021/jacs.7b09074 ↗
36. 10.1038/s41467-020-14402-010.1038/s41467-020-14402-0 ↗
37. 10.1039/C7EE03245E10.1039/C7EE03245E ↗
38. 10.1016/j.apcatb.2021.12033110.1016/j.apcatb.2021.120331 ↗
39. 10.1016/j.joule.2018.10.01510.1016/j.joule.2018.10.015 ↗
40. 10.1021/acsaem.0c0128310.1021/acsaem.0c01283 ↗
41. 10.1016/j.cej.2021.13106310.1016/j.cej.2021.131063 ↗
42. 10.1021/acsaem.9b0211210.1021/acsaem.9b02112 ↗
43. 10.1039/D1EE00594D10.1039/D1EE00594D ↗
44. 10.1002/smll.20200452610.1002/smll.202004526 ↗
45. 10.1038/s41467-021-23115-x10.1038/s41467-021-23115-x ↗
46. 10.1002/anie.20180838310.1002/anie.201808383 ↗
47. 10.1016/j.carbon.2020.03.03610.1016/j.carbon.2020.03.036 ↗
48. 10.1002/chem.20190423310.1002/chem.201904233 ↗
49. 10.1021/jp983752c10.1021/jp983752c ↗
50. 10.1021/jp058119n10.1021/jp058119n ↗
51. 10.31635/ccschem.019.2019001110.31635/ccschem.019.20190011 ↗
52. 10.1021/jz101628410.1021/jz1016284 ↗