Nickel-Nitrogen-Doped Ordered Macro-/Mesoporous Carbon Supported Ag Nanoparticles for Efficient Electrocatalytic CO2 Reduction

doi:10.6023/A21030104

Abstract

Electrocatalytic CO₂ reduction (ECR) into high value-added chemical products has been regarded as an effective strategy to release environmental crisis caused by high concentration of CO₂ in the atmosphere, because of its mild operation conditions and the ability to use renewable energy sources as power. Metal-nitrogen-doped carbon-based nanomaterials have been demonstrated as excellent catalysts for electrochemical reduction of CO₂ due to their high selectivity and low cost. However, it suffers from the problem of low Faradaic efficiency at high current density, which limits their further applications. In addition, the silver-based catalysts have good catalytic activity for the electrochemical reduction of CO₂ to CO, but they can only achieve high selectivity under high overpotentials. The synergistic effect in the multi-component system provides a new idea for the design of efficient electrocatalysts for carbon dioxide reduction. Herein, we first elaborately design and prepare an ordered macro-/mesoporous nickel-nitrogen-doped carbon (Ni-N-OMMC) supported silver nanoparticles composite (Ag/Ni-N-OMMC) by the use of silica colloidal crystal as the hard template and triblock copolymer Pluronic F127 as the mesoporous structure-directing agent, and study the electrocatalytic CO₂ reduction performance. Due to the confinement effect, the small silver nanoparticles are successfully loaded on the Ni-N-OMMC support by in-situ chemical reduction. Compared to Ni-N-OMMC, Ag/Ni-N-OMMC exhibits better electrocatalytic activity. The Faradaic efficiency of CO is as high as 98.7% when the potential is –0.7 V vs. reversible hydrogen electrode (RHE) in 0.1 mol•L^–1 KHCO₃ electrolyte. Moreover, Ag/Ni-N-OMMC has a wide operating voltage range with the Faradaic efficiency of CO over 90% at –0.7~ –1.0 V, and shows a high current density of CO (33.29 mA•cm^–2) at –1.0 V. The excellent ECR performance of Ag/Ni-N-OMMC may be attributed to the synergistic effect between Ag nanoparticles and the Ni-N-OMMC support with abundant Ni-N _x active sites, as well as the high specific surface area and efficient mass/charge transfer provided by the three-dimensional interconnected ordered macro-/mesoporous structure. This study provides an idea for future design and preparation of metal-carbon composite electrocatalysts with high activity and selectivity.

Key words: ordered macro-/mesoporous structure, Ni-N-doped carbon, dual-templating synthesis, Ag nanoparticle, electrocatalytic CO₂ reduction

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Chunhui Mu, Yixin Zhang, Wei Kou, Lianbin Xu. Nickel-Nitrogen-Doped Ordered Macro-/Mesoporous Carbon Supported Ag Nanoparticles for Efficient Electrocatalytic CO₂ Reduction[J]. Acta Chimica Sinica, 2021, 79(7): 925-931.

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Fig. & Tab. 5

Figure 1. Schematic of the synthesis of Ag/Ni-N-OMMC

Figure 2. SEM images of (a) SiO2 opal and (b) Ni-N-OMMC (inset: at a higher magnification); TEM images of (c) Ni-N-OMMC (inset: at a higher magnification) and (d) Ag/Ni-N-OMMC (inset: HR-TEM image of Ag nanoparticles); (e) EDS mapping images of C, N, Ni and Ag elements of Ag/Ni-N-OMMC

Figure 3. Wide-angle XRD patterns of Ni-N-OMMC, Ag/Ni-N-OMMC, Ag/OMMC and Ag/XC-72R

Figure 4. (a) XPS survey spectrum; high-resolution XPS spectra of (b) N 1s, (c) Ni 2p and (d) Ag 3d of Ag/Ni-N-OMMC

Figure 5. ECR performances for Ag/Ni-N-OMMC, Ni-N-OMMC, Ag/OMMC and Ag/XC-72R. (a) LSV curves in the CO2-saturated 0.1 mol•L–1 KHCO3 solution (inset: LSV curves for Ag/Ni-N-OMMC measured in N2- and CO2-saturated 0.1 mol•L–1 KHCO3 solutions) with 10 mV•s–1; (b) CO Faradaic efficiency at different potentials; (c) CO current density at different potentials; (d) Tafel plots for CO; (e) correlation curves between current density and sweep speed; (f) durability test of Ag/Ni-N-OMMC at a constant potential of –0.7 V vs. RHE

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镍氮掺杂有序大孔/介孔碳负载银纳米颗粒用于高效电催化CO₂还原

Nickel-Nitrogen-Doped Ordered Macro-/Mesoporous Carbon Supported Ag Nanoparticles for Efficient Electrocatalytic CO₂ Reduction

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镍氮掺杂有序大孔/介孔碳负载银纳米颗粒用于高效电催化CO2还原