Cu–Ni alloy decorating N-doped carbon nanosheets toward high-performance electrocatalysis of mildly acidic CO<sub>2</sub> reduction

Wen, Zhenhai; Pan, Weifan; Wang, Peng; Fan, Linfeng; Chen, Kai; Yi, Lijun; Huang, Jianfeng; Cai, Pingwei; Liu, Xi; Chen, Qingsong; Wang, Genxiang

doi:10.1039/d3qi00207a

“…Transition metal-nitrogen-doped carbon (MÀ NÀ C) with optimal binding strength for chemical species is emerging as a promising class of SAC for the acidic CO 2 RR. [12,[52][53][54][55] For instance, NiÀ NÀ C electrocatalysts synthesized by high-temperature pyrolysis treatment exhibited nearly 100 % FE CO at industry-relevant current densities exceeding 250 mA/cm 2 under acidic conditions. [8,49] This excellent electrocatalytic performance is attributed to the electrode structure design or electrolyte engineering, which will be discussed in the relevant sections.…”

Section: Electrocatalyst Designmentioning

confidence: 99%

“… [8,49–51] The electrocatalytic performance relies on the central metal atoms, coordination environment, and support. Transition metal‐nitrogen‐doped carbon (M−N−C) with optimal binding strength for chemical species is emerging as a promising class of SAC for the acidic CO 2 RR [12,52–55] . For instance, Ni−N−C electrocatalysts synthesized by high‐temperature pyrolysis treatment exhibited nearly 100 % FE CO at industry‐relevant current densities exceeding 250 mA/cm 2 under acidic conditions [8,49] .…”

Section: Electrocatalyst Designmentioning

confidence: 99%

Reaction Environment Regulation for Electrocatalytic CO₂ Reduction in Acids

Zeng,

Fang,

Cen

et al. 2024

Angew Chem Int Ed

22

0

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The electrocatalytic CO2 reduction reaction (CO2RR) is a sustainable route for converting CO2 into value‐added fuels and feedstocks, advancing a carbon‐neutral economy. The electrolyte critically influences CO2 utilization, reaction rate and product selectivity. While typically conducted in neutral/alkaline aqueous electrolytes, the CO2RR faces challenges due to (bi)carbonate formation and its crossover to the anolyte, reducing efficiency and stability. Acidic media offer promise by suppressing these processes, but the low Faradaic efficiency, especially for multicarbon (C2+) products, and poor electrocatalyst stability persist. The effective regulation of the reaction environment at the cathode is essential to favor the CO2RR over the competitive hydrogen evolution reaction (HER) and improve long‐term stability. This review examines progress in the acidic CO2RR, focusing on reaction environment regulation strategies such as electrocatalyst design, electrode modification and electrolyte engineering to promote the CO2RR. Insights into the reaction mechanisms via in situ/operando techniques and theoretical calculations are discussed, along with critical challenges and future directions in acidic CO2RR technology, offering guidance for developing practical systems for the carbon‐neutral community.

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“… [8,49–51] The electrocatalytic performance relies on the central metal atoms, coordination environment, and support. Transition metal‐nitrogen‐doped carbon (M−N−C) with optimal binding strength for chemical species is emerging as a promising class of SAC for the acidic CO 2 RR [12,52–55] . For instance, Ni−N−C electrocatalysts synthesized by high‐temperature pyrolysis treatment exhibited nearly 100 % FE CO at industry‐relevant current densities exceeding 250 mA/cm 2 under acidic conditions [8,49] .…”

Section: Electrocatalyst Designmentioning

confidence: 99%

Reaction Environment Regulation for Electrocatalytic CO₂ Reduction in Acids

Zeng,

Fang,

Cen

et al. 2024

Angewandte Chemie

3

0

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The electrocatalytic CO2 reduction reaction (CO2RR) is a sustainable route for converting CO2 into value‐added fuels and feedstocks, advancing a carbon‐neutral economy. The electrolyte critically influences CO2 utilization, reaction rate and product selectivity. While typically conducted in neutral/alkaline aqueous electrolytes, the CO2RR faces challenges due to (bi)carbonate formation and its crossover to the anolyte, reducing efficiency and stability. Acidic media offer promise by suppressing these processes, but the low Faradaic efficiency, especially for multicarbon (C2+) products, and poor electrocatalyst stability persist. The effective regulation of the reaction environment at the cathode is essential to favor the CO2RR over the competitive hydrogen evolution reaction (HER) and improve long‐term stability. This review examines progress in the acidic CO2RR, focusing on reaction environment regulation strategies such as electrocatalyst design, electrode modification and electrolyte engineering to promote the CO2RR. Insights into the reaction mechanisms via in situ/operando techniques and theoretical calculations are discussed, along with critical challenges and future directions in acidic CO2RR technology, offering guidance for developing practical systems for the carbon‐neutral community.

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“…27 Recently, Ni−Cu dual atom catalyst and Cu−Ni alloy have been designed for CO 2 RR toward CO with high selectivity. 28,29 Although carbon-based bimetallic catalysts provide a promising strategy for the CO 2 RR, there is still room for further optimizing their electrochemical performance. In addition, water can participate in the reaction in the drainage electrolyte, which leads to HER competition with CO 2 RR and affects the selectivity of CO products.…”

Section: ■ Introductionmentioning

confidence: 99%

Hydrophobic Nitrogen-Doped Nanocarbon with Cu–Ni Alloy Sites as a Catalyst for CO₂ Electroreduction

Cao,

Hu,

Hui

et al. 2024

ACS Appl. Nano Mater.

0

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The electrochemical reduction of CO 2 to value-added fuels or chemicals is considered one of the most appealing routes to establish an artificial carbon cycle. In this regard, the design of catalysts with high activity and selectivity in a wide potential window is pursued. Herein, the Cu−Ni alloy/nitrogen-doped nanocarbon (Cu−Ni/NC) with hydrophobicity is synthesized for the electrochemical CO 2 reduction reaction (CO 2 RR) through the thermal decomposition of metal−organic frameworks. In the H-cell, the Cu−Ni/NC displays superior selectivity toward CO with a Faradaic efficiency (FE) over 90% in a wide potential window from −0.7 to −1.2 V versus the reversible hydrogen electrode (RHE). Further, a high FE CO of 98.8% and an impressive CO partial current density (j CO ) of 27.6 mA cm −2 were achieved at −1.1 V, superior to those of their single metal counterparts. The enhanced CO selectivity may be related to the hydrophobicity, which can suppress the competitive hydrogen evolution reaction. Moreover, in situ ATR-SEIRAS and density functional theory (DFT) calculations reveal that the synergistic effects via intermetal interaction on Cu−Ni(111) surface can facilitate the proton-coupled electron transfer process, and then well balance the formation of COOH* and the CO* desorption.

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Cu–Ni alloy decorating N-doped carbon nanosheets toward high-performance electrocatalysis of mildly acidic CO₂ reduction

Abstract: Electrochemical CO2 reduction to value-added chemicals or fuels is a prospective strategy for facilitating closing carbon loop. However, there still exist challenges in developing efficient catalysts and optimizing the electrolyzer...

Cited by 10 publications

References 48 publications

Reaction Environment Regulation for Electrocatalytic CO₂ Reduction in Acids

Reaction Environment Regulation for Electrocatalytic CO₂ Reduction in Acids

Reaction Environment Regulation for Electrocatalytic CO₂ Reduction in Acids

Hydrophobic Nitrogen-Doped Nanocarbon with Cu–Ni Alloy Sites as a Catalyst for CO₂ Electroreduction

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Cu–Ni alloy decorating N-doped carbon nanosheets toward high-performance electrocatalysis of mildly acidic CO2 reduction

Abstract: Electrochemical CO2 reduction to value-added chemicals or fuels is a prospective strategy for facilitating closing carbon loop. However, there still exist challenges in developing efficient catalysts and optimizing the electrolyzer...

Cited by 10 publications

References 48 publications

Reaction Environment Regulation for Electrocatalytic CO2 Reduction in Acids

Reaction Environment Regulation for Electrocatalytic CO2 Reduction in Acids

Reaction Environment Regulation for Electrocatalytic CO2 Reduction in Acids

Hydrophobic Nitrogen-Doped Nanocarbon with Cu–Ni Alloy Sites as a Catalyst for CO2 Electroreduction

Contact Info

Product

Resources

About

Cu–Ni alloy decorating N-doped carbon nanosheets toward high-performance electrocatalysis of mildly acidic CO₂ reduction

Reaction Environment Regulation for Electrocatalytic CO₂ Reduction in Acids

Reaction Environment Regulation for Electrocatalytic CO₂ Reduction in Acids

Reaction Environment Regulation for Electrocatalytic CO₂ Reduction in Acids

Hydrophobic Nitrogen-Doped Nanocarbon with Cu–Ni Alloy Sites as a Catalyst for CO₂ Electroreduction