Incorporation of nickel single atoms into carbon paper as self-standing electrocatalyst for CO<sub>2</sub>reduction

Li, Simin; Ceccato, Marcel; Lu, Xiuyuan; Frank, Sara; Lock, Nina; Roldán, Alberto; Hu, Xin‐Ming; Skrydstrup, Troels; Daasbjerg, Kim

doi:10.1039/d0ta08433f

Cited by 42 publications

(18 citation statements)

References 58 publications

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“…Single-atom catalysts (SACs) featuring a metal–nitrogen co-decorated carbon (M–NC) structure have gained great popularity in heterogeneous catalysis. − Compared with their nanoparticle or bulk counterparts, isolated metal atoms behave differently in the catalysis due to their unique coordination and electronic state. , Moreover, SACs can be used as ideal models for understanding the structure–activity relationship at the atomic level by virtue of their adjustable coordination environments . As a result, atomization of p-block metals may provide a solution for modifying their electronic state and thus activating them for CO 2 -to-CO conversion.…”

Section: Introductionmentioning

confidence: 99%

p-Block Indium Single-Atom Catalyst with Low-Coordinated In–N Motif for Enhanced Electrochemical CO₂ Reduction

Zhao

et al. 2022

ACS Catal.

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Electrochemical CO2 reduction represents a promising path toward the production of value-added chemicals. Atomically dispersed metal sites on nitrogen-doped carbon have demonstrated outstanding catalytic performance in this reaction. However, challenges remain in developing such catalysts beyond transition metals. Herein, we present two types of p-block indium single-atom catalysts: one with four nitrogen coordinated (In–N4) and another with three nitrogen coordinated with one vacancy nearby (In–N3–V). In electrochemical CO2 reduction, the In–N3–V site can achieve maximum CO Faradic efficiency (FECO) of 95% at −0.57 V vs reversible hydrogen electrode (RHE) in an aqueous medium. This outperforms the intact In–N4 catalyst with the maximum FECO of 80% at −0.47 V vs RHE. Density functional theory calculations on the mechanism suggest that structural change from In–N4 to In–N3–V brings the In orbital (s and p z ) energies closer to the Fermi energy. These hybridized orbitals are responsible for lowering the energy barrier for COOH* intermediate formation, thus enhancing the catalytic performance. This work sheds light on the relationship between catalytic performance and structure of In single-atom sites, highlighting the importance of tailoring the electron state of s and p z orbitals in developing efficient p-block single-atom catalysts for electrochemical CO2 reduction.

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Section: Introductionmentioning

confidence: 99%

p-Block Indium Single-Atom Catalyst with Low-Coordinated In–N Motif for Enhanced Electrochemical CO₂ Reduction

Zhao

et al. 2022

ACS Catal.

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“…The inherent electrocatalytic activity and selectivity for CO 2 ‐to‐CO were modulated by S atoms, resulting in improved interaction strength between Fe atom and intermediates. This unique structure and electronic properties endowed the Fe−NS−C electrocatalyst with a FE(CO) of 98 % under an overpotential of 0.49 V. Indeed, the local electronic structures of host atoms could be altered by doping heteroatoms, further influencing catalytic properties [28–30] . Thus, it can be anticipated that the incorporation of proper heteroatoms into carbon sites close to the M−N X center could tune the electronic structure of metal atoms, which would effectively promote the activation of CO 2 and modify the binding strength of intermediates during the ECR process.…”

Section: Introductionmentioning

confidence: 99%

Sulfur‐Decorated Ni−N−C Catalyst for Electrocatalytic CO₂ Reduction with Near 100 % CO Selectivity

Zhang

Mady

et al. 2022

ChemSusChem

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Developing highly efficient electrocatalysts for electrochemical CO2 reduction (ECR) to value‐added products is important for CO2 conversion and utilization technologies. In this work, a sulfur‐doped Ni−N−C catalyst is fabricated through a facile ion‐adsorption and pyrolysis treatment. The resulting Ni−NS−C catalyst exhibits higher activity in ECR to CO than S‐free Ni−N−C, yielding a current density of 20.5 mA cm−2 under −0.80 V versus a reversible hydrogen electrode (vs. RHE) and a maximum CO faradaic efficiency of nearly 100 %. It also displays excellent stability with negligible activity decay after electrocatalysis for 19 h. A combination of experimental investigations and DFT calculations demonstrates that the high activity and selectivity of ECR to CO is due to a synergistic effect of the S and Ni−NX moieties. This work provides insights for the design and synthesis of nonmetal atom‐decorated M−N−C‐based ECR electrocatalysts.

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“…63 The ECSA of S-CP is 1.1 × 10 3 cm 2 /cm 3 , which is 16 times higher than that of CP. This increase in surface area may be related to the pyrolysis of PTFE 64 and the assistance of glucose. 61 The ECSA of MNC and CNF is 7.8 × 10 3 cm 2 /cm 3 and 1.8 × 10 4 cm 2 /cm 3 , respectively, which is 113 times and 261 times higher than that of CP.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Eight-Fold Intensification of Electrochemical Azidooxygenation with a Flow-Through Electrode

Guo

Kim

Siu

et al. 2022

ACS Sustainable Chem. Eng.

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Finding ways to reduce reactor volume while increasing product output for electro-organic reactions would facilitate the broader adoption of such reactions for the production of chemicals in a commercial setting. This work investigates how the use of flow with different electrode structures impacts the productivity (i.e., the rate of product generation) of a TEMPO-mediated azidooxygenation reaction. Comparison of a flow and batch process with carbon paper (CP) demonstrated a 3.8-fold-higher productivity for the flow reactor. Three custom carbon electrodes, sintered carbon paper (S-CP), carbon nanofiber (CNF), and composite carbon microfiber-nanofiber (MNC), were studied in the flow reactor to evaluate how changing the electrode structure affected productivity. Under the optimum conditions, these electrodes achieved productivities 5.4, 6.5, and 7.8 times higher than the average batch reactor, respectively. Recycling the outlet from the flow reactor with the MNC electrode back into the inlet achieved an 81% yield in 36 min, while the batch reactor obtained a 75% yield in 5 h. These findings demonstrate that the productivity of electro-organic reactions can be substantially improved through the use of novel flow-through electrodes.

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Incorporation of nickel single atoms into carbon paper as self-standing electrocatalyst for CO₂reduction

Abstract: The incorporation of Ni single atoms into carbon paper produces self-standing electrode for efficient CO2 reduction to CO in water.

Cited by 42 publications

References 58 publications

p-Block Indium Single-Atom Catalyst with Low-Coordinated In–N Motif for Enhanced Electrochemical CO₂ Reduction

p-Block Indium Single-Atom Catalyst with Low-Coordinated In–N Motif for Enhanced Electrochemical CO₂ Reduction

Sulfur‐Decorated Ni−N−C Catalyst for Electrocatalytic CO₂ Reduction with Near 100 % CO Selectivity

Eight-Fold Intensification of Electrochemical Azidooxygenation with a Flow-Through Electrode

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Incorporation of nickel single atoms into carbon paper as self-standing electrocatalyst for CO2reduction

Abstract: The incorporation of Ni single atoms into carbon paper produces self-standing electrode for efficient CO2 reduction to CO in water.

Cited by 42 publications

References 58 publications

p-Block Indium Single-Atom Catalyst with Low-Coordinated In–N Motif for Enhanced Electrochemical CO2 Reduction

p-Block Indium Single-Atom Catalyst with Low-Coordinated In–N Motif for Enhanced Electrochemical CO2 Reduction

Sulfur‐Decorated Ni−N−C Catalyst for Electrocatalytic CO2 Reduction with Near 100 % CO Selectivity

Eight-Fold Intensification of Electrochemical Azidooxygenation with a Flow-Through Electrode

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Product

Resources

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Incorporation of nickel single atoms into carbon paper as self-standing electrocatalyst for CO₂reduction

p-Block Indium Single-Atom Catalyst with Low-Coordinated In–N Motif for Enhanced Electrochemical CO₂ Reduction

p-Block Indium Single-Atom Catalyst with Low-Coordinated In–N Motif for Enhanced Electrochemical CO₂ Reduction

Sulfur‐Decorated Ni−N−C Catalyst for Electrocatalytic CO₂ Reduction with Near 100 % CO Selectivity