Electronic Regulation of Nickel Single Atoms by Confined Nickel Nanoparticles for Energy-Efficient CO2 Electroreduction

Wenhao Ren; Xin Tan; Chen Jia; Anna Krammer; Qian Sun; Jiangtao Qu; Sean C Smith; Andreas Schueler; Xile Hu; Chuan Zhao

doi:10.1002/anie.202203335

Electronic Regulation of Nickel Single Atoms by Confined Nickel Nanoparticles for Energy-Efficient CO₂ Electroreduction

Angew Chem Int Ed Engl. 2022 Jun 27;61(26):e202203335. doi: 10.1002/anie.202203335. Epub 2022 Apr 27.

Authors

Wenhao Ren^{1

2}, Xin Tan³, Chen Jia¹, Anna Krammer⁴, Qian Sun¹, Jiangtao Qu⁵, Sean C Smith³, Andreas Schueler⁴, Xile Hu², Chuan Zhao¹

Affiliations

¹ School of Chemistry, University of New South Wales, Sydney, New South Wales 2052, Australia.
² Laboratory of Inorganic Synthesis and Catalysis, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Fédérale de Lausanne (EPFL), ISIC-LSCI, 1015, Lausanne, Switzerland.
³ Department of Materials Physics, Research School of Physics, Australian National University, Canberra, ACT 2601, Australia.
⁴ Solar Energy and Building Physics Laboratory, Ecole Polytechnique Fédérale de Lausanne, EPFL LESO-PB, 1015, Lausanne, Switzerland.
⁵ Australian Centre for Microscopy and Microanalysis, University of Sydney, 2006, NSW, Sydney, Australia.

PMID: 35315559
DOI: 10.1002/anie.202203335

Abstract

Modulating the electronic structure of atomically dispersed active sites is promising to boost catalytic activity but is challenging to achieve. Here we show a cooperative Ni single-atom-on-nanoparticle catalyst (NiSA/NP) prepared via direct solid-state pyrolysis, where Ni nanoparticles donate electrons to Ni(i)-N-C sites via a network of carbon nanotubes, achieving a high CO current density of 346 mA cm^-2 at -0.5 V vs RHE in an alkaline flow cell. When coupled with a NiFe-based anode in a zero-gap membrane electrolyzer, the catalyst delivers an industrially relevant CO current density of 310 mA cm^-2 at a low cell voltage of -2.3 V, corresponding to an overall energy efficiency of 57 %. The superior CO₂ electroreduction performance is attributed to the enhanced adsorption of key intermediate COOH* on the electron-rich Ni single atoms, as well as a high density of active sites.

Keywords: CO2 Reduction; Cooperative Single-Atom Catalyst; Electrocatalyst; Electronic Regulation; Metal-Nitrogen-Carbon.

Abstract

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