Boosting electrochemical CO2 reduction on ternary heteroatoms-doped porous carbon

Yang, Fubin; Yu, Haoming; Mao, Xinyu; Meng, Qiangguo; Chen, Shixia; Deng, Qiang; Zeng, Zheling; Wang, Jun; Deng, Shuguang

doi:10.1016/j.cej.2021.131661

Cited by 25 publications

(17 citation statements)

References 49 publications

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“…The electrolytic cell without mass transfer constraints can significantly increase the partial current density, such as gas/liquid cells (gas diffusion electrodes), flow cells, and fully gas‐fed cells (membrane electrode assembly). The partial current density of CO at −1.0 V (vs. RHE) for NSP‐HPC is 11.0 mA/cm 2 in H‐type cells and 183.2 mA/cm 2 in flow‐cell 78 . The H‐type cells may limit the role of electrocatalysts for converting CO 2 to value‐added fuels and chemicals production.…”

Section: Discussionmentioning

confidence: 99%

“…The partial current density of CO at −1.0 V (vs. RHE) for NSP-HPC is 11.0 mA/cm 2 in H-type cells and 183.2 mA/cm 2 in flowcell. 78 The H-type cells may limit the role of electrocatalysts for converting CO 2 to value-added fuels and chemicals production. In addition, ionic liquids can also improve the selectivity of target product by increasing the solubility of CO 2 and inhibiting the competing HER.…”

Section: Discussionmentioning

confidence: 99%

“…Compared with single heteroatom doping, multiheteroatoms (N, S-, N, P-, and N, B-) doping with different electronegativity can more effectively regulate the electronic structure of MFEs, which is beneficial to promote CO 2 localization, decrease reaction barriers, provide abundant active sites, and further enhance the electrochemical activity of CO 2 RR. 78,80,121 For example, the N,P co-doping metal-free carbon electrocatalyst possessed more defects and outstanding selectivity of CO (over 6.6 times) than single N doping ones. 81 The polarization of Fermi level is induced by P doping, which remarkably improved the reaction activity of active centers and reduced the free energy of the *COOH intermediates.…”

Section: Doped Defectmentioning

confidence: 99%

“…Recently, the synergistic effects between the heteroatoms of different electron negativities have shown excellent CO 2 RR performance. 78 The fullerene-like carbon structure with N and P coordination (N,P-FC) was prepared using polyethylene glycol (PEG) as a soft template. 64 The CO 2 RR activity of N,P-FC strongly depended on the N/P atomic ratio.…”

Section: Synergymentioning

confidence: 99%

“…The N, S, and P ternary-doped carbon catalyst (NSP-HPC) has a high activity for electrochemical reduction of CO 2 (FE CO of 92% at −0.7 V in conventional H-cell, FE CO of 98% and high current density of 245 mA/cm 2 in flow cell). 78 Doping P can increase the charge delocalization of C atoms. The introduction of S can increase the spin density of the catalyst.…”

Section: Intermediate Stabilizationmentioning

confidence: 99%

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Surface and interface chemistry in metal‐free electrocatalysts for electrochemical CO₂ reduction

Zhang

Jia

et al. 2022

SmartMat

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The electrochemical reduction of carbon dioxide (CO2) into value‐added fuels and chemicals presents a sustainable route to alleviate CO2 emissions, promote carbon‐neutral cycles and reduce the dependence on fossil fuels. Considering the thermodynamic stability of the CO2 molecule and sluggish reaction kinetics, it is still a challenge to design highly efficient electrocatalysts for the CO2 reduction reaction (CO2RR). It has been found that the surface and interface chemistry of electrocatalysts can modulate the electronic structure and increase the active sites, which is favorable for CO2 adsorption, electron transfer, mass transport, and optimizing adsorption strength of reaction intermediates. However, the effect of surface and interface chemistry on metal‐free electrocatalysts (MFEs) for CO2RR has not been comprehensively reviewed. Herein, we discuss the importance of the surface and interface chemistry on MFEs for improving the electrochemical CO2RR performance based on thermodynamic and kinetic views. The fundamentals and challenges of CO2RR are firstly presented. Then, the recent advances of the surface and interface chemistry in improving reaction rate and overcoming reaction constraints are reviewed from regulating electronic structure, active sites, electron transfer, mass transport, and intermediate binding energy. Finally, the research challenges and prospects are proposed to suggest the future designs of advanced MFEs in CO2RR.

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Section: Discussionmentioning

confidence: 99%

Section: Discussionmentioning

confidence: 99%

Section: Doped Defectmentioning

confidence: 99%

Section: Synergymentioning

confidence: 99%

Section: Intermediate Stabilizationmentioning

confidence: 99%

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Surface and interface chemistry in metal‐free electrocatalysts for electrochemical CO₂ reduction

Zhang

Jia

et al. 2022

SmartMat

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Phosphorus‐Doped Graphene Aerogel as Self‐Supported Electrocatalyst for CO₂‐to‐Ethanol Conversion

Yang

Liang

et al. 2022

Advanced Science

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Electrochemical reduction of carbon dioxide (CO2) to ethanol is a promising strategy for global warming mitigation and resource utilization. However, due to the intricacy of C─C coupling and multiple proton–electron transfers, CO2‐to‐ethanol conversion remains a great challenge with low activity and selectivity. Herein, it is reported a P‐doped graphene aerogel as a self‐supporting electrocatalyst for CO2 reduction to ethanol. High ethanol Faradaic efficiency (FE) of 48.7% and long stability of 70 h are achieved at −0.8 VRHE. Meanwhile, an outstanding ethanol yield of 14.62 µmol h−1 cm−2 can be obtained, outperforming most reported electrocatalysts. In situ Raman spectra indicate the important role of adsorbed *CO intermediates in CO2‐to‐ethanol conversion. Furthermore, the possible active sites and optimal pathway for ethanol formation are revealed by density functional theory calculations. The graphene zigzag edges with P doping enhance the adsorption of *CO intermediate and increase the coverage of *CO on the catalyst surface, which facilitates the *CO dimerization and boosts the EtOH formation. In addition, the hierarchical pore structure of P‐doped graphene aerogels exposes abundant active sites and facilitates mass/charge transfer. This work provides inventive insight into designing metal‐free catalysts for liquid products from CO2 electroreduction.

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Transition Metal‐Nitrogen‐Carbon Single‐Atom Catalysts Enhanced CO₂ Electroreduction Reaction: A Review

Ji,

Du,

Chen

et al. 2024

ChemSusChem

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As the global energy crisis and environmental challenges worsen, CO2 conversion has emerged as a focal point in international research. CO2 electroreduction reaction (CO2ER) is a green and sustainable technology that converts CO2 into high‐value chemicals, thereby achieving the recycling of carbon resources. However, the activity and selectivity are constrained by the performance of the catalyst. Although traditional N‐doped carbon‐based catalysts exhibit excellent performance toward CO2ER, the atomic utilization rate in these materials is far from 100 %. Single atom catalysts (SACs) can attain nearly 100 % atomic utilization efficiency because of the fully exposing metal atoms. Therefore, SACs have emerged as one of the hot research materials in the field of CO2ER. Recently, transition metal‐nitrogen‐carbon single‐atom catalysts (TM−N−C SACs) have flourished because of their extraordinary catalytic activity, low cost, and excellent stability, demonstrating enormous application prospects in CO2ER. In this review, we concentrate on TM−N−C SACs that electrochemically reduce CO2 to high value products. A comprehensive and detailed discussion were conducted on the synthesis method, chemical structure, chemical characterization of TM−N−C SACs, as well as their catalytic performance, active sources, and mechanism exploration for CO2ER. Finally, challenges and prospects for commercial application of TM−N−C SACs catalysts suitable for CO2ER are proposed.

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Boosting electrochemical CO2 reduction on ternary heteroatoms-doped porous carbon

Cited by 25 publications

References 49 publications

Surface and interface chemistry in metal‐free electrocatalysts for electrochemical CO₂ reduction

Surface and interface chemistry in metal‐free electrocatalysts for electrochemical CO₂ reduction

Phosphorus‐Doped Graphene Aerogel as Self‐Supported Electrocatalyst for CO₂‐to‐Ethanol Conversion

Transition Metal‐Nitrogen‐Carbon Single‐Atom Catalysts Enhanced CO₂ Electroreduction Reaction: A Review

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Boosting electrochemical CO2 reduction on ternary heteroatoms-doped porous carbon

Cited by 25 publications

References 49 publications

Surface and interface chemistry in metal‐free electrocatalysts for electrochemical CO2 reduction

Surface and interface chemistry in metal‐free electrocatalysts for electrochemical CO2 reduction

Phosphorus‐Doped Graphene Aerogel as Self‐Supported Electrocatalyst for CO2‐to‐Ethanol Conversion

Transition Metal‐Nitrogen‐Carbon Single‐Atom Catalysts Enhanced CO2 Electroreduction Reaction: A Review

Contact Info

Product

Resources

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Surface and interface chemistry in metal‐free electrocatalysts for electrochemical CO₂ reduction

Surface and interface chemistry in metal‐free electrocatalysts for electrochemical CO₂ reduction

Phosphorus‐Doped Graphene Aerogel as Self‐Supported Electrocatalyst for CO₂‐to‐Ethanol Conversion

Transition Metal‐Nitrogen‐Carbon Single‐Atom Catalysts Enhanced CO₂ Electroreduction Reaction: A Review