Journal
ADVANCED FUNCTIONAL MATERIALS
Volume 31, Issue 50, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202104243
Keywords
accelerating proton transfer; CO; (2) electroreduction; high current density; single atom catalysts; Zn-CO; (2) batteries
Categories
Funding
- National Natural Science Foundation of China [21922811, 21878270, 21961160742]
- Zhejiang Provincial Natural Science Foundation of China [LR19B060002]
- Fundamental Research Funds for the Central Universities [2020XZZX002-09]
- Startup Foundation for Hundred-Talent Program of Zhejiang University, Zhejiang Key Laboratory of Marine Materials and Protective Technologies [2020K10]
- Key Laboratory of Marine Materials and Related Technologies, CAS
- Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang [2019R01006]
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This study reports a porous Ni-N-C catalyst, ZrO2@Ni-NC, synthesized using a post-synthetic coordination coupling carbonization strategy, which shows high activity and selectivity in CO2RR. The isolated Ni-N-4 species are identified as the real active sites, while the nanostructured ZrO2 accelerates the protonation process, reducing the energy barrier and enhancing catalytic performance.
Developing single-atom electrocatalysts with high activity and superior selectivity at a wide potential window for CO2 reduction reaction (CO2RR) still remains a great challenge. Herein, a porous Ni-N-C catalyst containing atomically dispersed Ni-N-4 sites and nanostructured zirconium oxide (ZrO2@Ni-NC) synthesized via a post-synthetic coordination coupling carbonization strategy is reported. The as-prepared ZrO2@Ni-NC exhibits an initial potential of -0.3 V, maximum CO Faradaic efficiency (F.E.) of 98.6% +/- 1.3, and a low Tafel slope of 71.7 mV dec(-1) in electrochemical CO2RR. In particular, a wide potential window from -0.7 to -1.4 V with CO F.E. of above 90% on ZrO2@Ni-NC far exceeds those of recently developed state-of-the-art CO2RR electrocatalysts based on Ni-N moieties anchored carbon. In a flow cell, ZrO2@Ni-NC delivers a current density of 200 mA cm(-2) with a superior CO selectivity of 96.8% at -1.58 V in a practical scale. A series of designed experiments and structural analyses identify that the isolated Ni-N-4 species act as real active sites to drive the CO2RR reaction and that the nanostructured ZrO2 largely accelerates the protonation process of *CO2- to *COOH intermediate, thus significantly reducing the energy barrier of this rate-determining step and boosting whole catalytic performance.
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