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Low-coordinated Ni-N1-C3 sites atomically dispersed on hollow carbon nanotubes for efficient CO2 reduction.
- Source :
- Nano Research; Jan2023, Vol. 16 Issue 1, p146-154, 9p
- Publication Year :
- 2023
-
Abstract
- Low-coordinated single atom catalysts compared to M-N<subscript>4</subscript> are appealing in optimized electronic structure for CO<subscript>2</subscript> electro-reduction, but the preparation is still very challenging. Herein, a novel single Ni atom catalyst with Ni-N<subscript>1</subscript>-C<subscript>3</subscript> configuration is in-situ evolved on curved carbon nanotubes. The obtained Ni-N<subscript>1</subscript>-C<subscript>3</subscript> catalyst exhibits a superior CO Faradaic efficiency of 97% and turnover frequency of 2,890 h<superscript>−1</superscript> at −0.9 V versus the reversible hydrogen electrode, as well as long-term stability over 45 h. High current densities exceeding 200 mA·cm<superscript>−2</superscript> and CO Faradaic efficiency of 99% are achieved in flow-cell. Moreover, in-situ potential-and time-dependent Raman spectra identify the key intermediates of *COOH and *CO during CO<subscript>2</subscript>-to-CO conversion. Theoretical calculations reveal that the upward-shifted d-band center and charge-rich Ni sites of Ni-N<subscript>1</subscript>-C<subscript>3</subscript> facilitate the electron transfer to *COOH and thus reduce the *COOH formation energy barrier. This work demonstrates a strategy for modulating the coordination environment for efficient CO<subscript>2</subscript> reduction. [ABSTRACT FROM AUTHOR]
Details
- Language :
- English
- ISSN :
- 19980124
- Volume :
- 16
- Issue :
- 1
- Database :
- Complementary Index
- Journal :
- Nano Research
- Publication Type :
- Academic Journal
- Accession number :
- 161304591
- Full Text :
- https://doi.org/10.1007/s12274-022-4623-9