Asymmetric dinitrogen-coordinated nickel single-atomic sites for efficient CO2 electroreduction

Abstract

Developing highly efficient, selective and low-overpotential electrocatalysts for carbon dioxide (CO2) reduction is crucial. This study reports an efficient Ni single-atom catalyst coordinated with pyrrolic nitrogen and pyridinic nitrogen for CO2 reduction to carbon monoxide (CO). In flow cell experiments, the catalyst achieves a CO partial current density of 20.1 mA cmgeo−2 at −0.15 V vs. reversible hydrogen electrode (VRHE). It exhibits a high turnover frequency of over 274,000 site−1 h−1 at −1.0 VRHE and maintains high Faradaic efficiency of CO (FECO) exceeding 90% within −0.15 to −0.9 VRHE. Operando synchrotron-based infrared and X-ray absorption spectra, and theoretical calculations reveal that mono CO-adsorbed Ni single sites formed during electrochemical processes contribute to the balance between key intermediates formation and CO desorption, providing insights into the catalyst’s origin of catalytic activity. Overall, this work presents a Ni single-atom catalyst with good selectivity and activity for CO2 reduction while shedding light on its underlying mechanism.

Stabilizing Undercoordinated Zn Active Sites through Confinement in CeO2 Nanotubes for Efficient Electrochemical CO2 Reduction

“…Electrocatalytic carbon dioxide reduction reaction (CO 2 RR) to CO is widely recognized as the most economically viable reaction when considering the market princes of CO 2 RR products and the cost of electricity [1–3] . Recently, various studies have delivered excellent performances achieving high CO faradaic efficiency (FE) of nearly 100 % and partial current density over 100 mA ⋅ cm −2 [4–5] .…”

Phase Engineering and Synchrotron-Based Study on Two-Dimensional Energy Nanomaterials

“…The effectiveness of energy storage and conversion activities resulting from local dynamic reconstruction has been widely acknowledged, necessitating the identification of the true active phases formed to reveal the underlying reaction mechanisms. , A high level of understanding of the electronic and coordinate evolution of materials under working conditions can be provided through synchrotron-based in situ XAS . For instance, Chen et al researched a Ru-CuNW, which is an outstandingly dispersed Ru-embedded Cu nanowire matrix that demonstrates the industrial-relevant current density for nitrate reduction .…”

“…282,283 To better understand these changes, in situ SR-XRD has been implemented to track the structural reconstruction of electrode materials. 284 286,287 A high level of understanding of the electronic and coordinate evolution of materials under working conditions can be provided through synchrotron-based in situ XAS. 288 For instance, Chen et al researched a Ru-CuNW, which is an outstandingly dispersed Ru-embedded Cu nanowire matrix that demonstrates the industrial-relevant current density for nitrate reduction.…”

Stabilizing Undercoordinated Zn Active Sites through Confinement in CeO2 Nanotubes for Efficient Electrochemical CO2 Reduction

“…Electrocatalytic carbon dioxide reduction reaction (CO 2 RR) to CO is widely recognized as the most economically viable reaction when considering the market princes of CO 2 RR products and the cost of electricity. [1][2][3] Recently, various studies have delivered excellent performances achieving high CO faradaic efficiency (FE) of nearly 100 % and partial current density over 100 mA • cm À 2 . [4][5] Nonetheless, the outperformance of CO production is largely dependent on noble metals Au or Ag, which is far from the target of cost saving.…”