Metal-free sites with multidimensional structure modifications for selective electrochemical CO2 reduction

Mohamed, Aya Gomaa Abdelkader; Huang, Yiyin; Xie, Jiafang; Borse, Rahul Anil; Ganji, Parameswaram; Wang, Yaobing

doi:10.1016/j.nantod.2020.100891

Cited by 26 publications

(23 citation statements)

References 69 publications

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“…For DG electrocatalyst, Han et al 151 stated that their catalyst was stable for more than 10 h. Stability test at –0.6 V RHE showed that after 10 h, the current density dropped slowly from 2.1 to 1.5 mA cm −2 , whereas FE still retained over 70% during the entire process. They also compared their DG catalyst with previously reported graphene‐based catalysts and found that their catalyst was more stable under room temperature than previously reported ones 129,130,152–156 . Wu et al 131 found that their NGF catalyst was stable for at least 5 h, although the current density needs to be improved.…”

Section: Carbon‐based Metal‐free Electrocatalystsmentioning

confidence: 96%

“…The authors stated that CO 2 activation efficiently occurred on Si@G due to a strong binding capability of -0.83 eV at the armchair edge and -0.65 eV at the zigzag edge, respectively. In addition to well-known N and B-doped carbons, O-carbon chemical bonds (e.g., −OH, −COOH, C−O −C, C═O) also have high reactivity for eCO 2 R. 154 The eCO 2 R on a single-layer graphene nanodisk (GND) catalyst decorated with controlled surface oxygen contents was studied by Yang et al 155 It was found that the enhanced catalytic activity towards the reduction of CO 2 is attributed to the surface contents of carboxyl groups. Furthermore, | 37 DFT calculation demonstrated that this high catalytic activity was attributed to the synergistic effect between neighboring other groups (carbonyl, epoxide, and hydroxyl) and carboxyl groups on GND.…”

Section: Graphenementioning

confidence: 99%

“…They also compared their DG catalyst with previously reported graphene-based catalysts and found that their catalyst was more stable under room temperature than previously reported ones. 129,130,[152][153][154][155][156] Wu et al 131 found that their NGF catalyst was stable for at least 5 h, although the current density needs to be improved.…”

Section: Stabilitymentioning

confidence: 99%

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Carbon‐based metal‐free catalysts for electrochemical CO₂ reduction: Activity, selectivity, and stability

et al. 2020

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Zero or negative emissions of carbon dioxide (CO2) is the need of the times, as inexorable rising and alarming levels of CO2 in the atmosphere lead to global warming and severe climate change. The electrochemical CO2 reduction (eCO2R) to value‐added fuels and chemicals by using renewable electricity provides a cleaner and more sustainable route with economic benefits, in which the key is to develop clean and economical electrocatalysts. Carbon‐based catalyst materials possess desirable properties such as high offset potential for H2 evolution and chemical stability at the negative applied potential. Although it is still challenging to achieve highly efficient carbon‐based catalysts, considerable efforts have been devoted to overcoming the low selectivity, activity, and stability. Here, we summarize and discuss the recent progress in carbon‐based metal‐free catalysts including carbon nanotubes, carbon nanofibers, carbon nanoribbons, graphene, carbon nitride, and diamonds with an emphasis on their activity, product selectivity, and stability. In addition, the key challenges and future potential approaches for efficient eCO2R to low carbon‐based fuels are highlighted. For a good understanding of the whole history of the development of eCO2R, the CO2 reduction reactions, principles, and techniques including the role of electrolytes, electrochemical cell design and evaluation, product selectivity, and structural composition are also discussed. The metal/metal oxides decorated with carbon‐based electrocatalysts are also summarized. We aim to provide insights for further development of carbon‐based metal‐free electrocatalysts for CO2 reduction from the perspective of both fundamental understanding and technological applications in the future.

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Section: Carbon‐based Metal‐free Electrocatalystsmentioning

confidence: 96%

Section: Graphenementioning

confidence: 99%

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Carbon‐based metal‐free catalysts for electrochemical CO₂ reduction: Activity, selectivity, and stability

et al. 2020

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“…The selectivity and the reaction steps depend on the intermediate stabilization at the active sites (Figure 2); essentially, for the production of CO or HCOOH, a strong CO 2 adsorption energy is required to stabilize the intermediate COOH*, but also a weak adsorption of these products is necessary to avoid further reduction or catalyst poisoning [52,56]. In the case of obtaining high selectivity towards multi-carbon products, it is due to the stabilization of the initial C1-type intermediates such as CO or HCOOH, which need to be strongly adsorbed to continue reducing them, taking advantage of the high electron densities of the medium [57]. The N content and type can affect the adsorption and activation of CO 2 molecules as well as the bond strength between the intermediates or adsorbed products with Nfunctionalities, affecting the selectivity of the process.…”

Section: N-doped Carbon-based Materialsmentioning

confidence: 99%

From CO2 to Value-Added Products: A Review about Carbon-Based Materials for Electro-Chemical CO2 Conversion

et al. 2021

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The global warming and the dangerous climate change arising from the massive emission of CO2 from the burning of fossil fuels have motivated the search for alternative clean and sustainable energy sources. However, the industrial development and population necessities make the decoupling of economic growth from fossil fuels unimaginable and, consequently, the capture and conversion of CO2 to fuels seems to be, nowadays, one of the most promising and attractive solutions in a world with high energy demand. In this respect, the electrochemical CO2 conversion using renewable electricity provides a promising solution. However, faradaic efficiency of common electro-catalysts is low, and therefore, the design of highly selective, energy-efficient, and cost-effective electrocatalysts is critical. Carbon-based materials present some advantages such as relatively low cost and renewability, excellent electrical conductivity, and tunable textural and chemical surface, which show them as competitive materials for the electro-reduction of CO2. In this review, an overview of the recent progress of carbon-based electro-catalysts in the conversion of CO2 to valuable products is presented, focusing on the role of the different carbon properties, which provides a useful understanding for the materials design progress in this field. Development opportunities and challenges in the field are also summarized.

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“…[ 18,20,22 ] Pyridinic‐N configuration‐doped carbons are considered as the most favorable environment for ECR activity. [ 11,23–28 ] The basic pyridinic‐N sites offer anchoring sites to attract the Lewis acidic CO 2 molecule and further stabilize the

{CO}_{2}^{- .}

species, consequently reducing the energy of the rate‐determining step and enhancing ECR activity. [ 29 ] Inspired by these insights, tuning the M–N x configuration with specific pyridinic N could be feasible for wide potential CO 2 electrocatalysis.…”

Section: Introductionmentioning

confidence: 99%

Wide Potential CO₂‐to‐CO Electroreduction Relies on Pyridinic‐N/Ni–N_x Sites and Its Zn–CO₂ Battery Application

et al. 2021

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Although metal–N‐doped carbons are promising electrocatalysts for CO2‐to‐CO conversion due to their high conversion efficiency and current density, their commercial application is still challenging due to their narrow potential/current range. In general, a wide potential/current electrocatalyst is in high demand for industrial CO2 electrocatalysis. Controllable strategy to tune N configurations toward pyridinic‐enriched metal–Nx active sites is attractive. The synergetic effect of the ability of pyridinic N to capture Lewis acidic CO2 and the characteristics of Ni–N active sites to inhibit the hydrogen evolution reaction (HER) can achieve a wide potential window, which has high practical value. Herein, the well‐chosen precursors resulting in a pyridinic‐enriched Ni–Nx site can selectively catalyze CO2 toward CO generation in aqueous media with a high Faradaic efficiency (FE) of 100% with an overpotential of 680 mV. Continuous CO FE > 90% was recorded under a wide range of potentials without decay. Motivated by its practical characteristics in CO2 electrocatalysts, a Zn–CO2 battery is assembled achieving a CO2–CO conversion efficiency of more than 90% in a wide discharge current window. Therefore, the results highlight that pyridinic‐enriched Ni–Nx holds great promise as simultaneous CO‐selective electrocatalyst by suitably tuning M–N configurations as new perspective strategy.

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Metal-free sites with multidimensional structure modifications for selective electrochemical CO2 reduction

Cited by 26 publications

References 69 publications

Carbon‐based metal‐free catalysts for electrochemical CO₂ reduction: Activity, selectivity, and stability

Carbon‐based metal‐free catalysts for electrochemical CO₂ reduction: Activity, selectivity, and stability

From CO2 to Value-Added Products: A Review about Carbon-Based Materials for Electro-Chemical CO2 Conversion

Wide Potential CO₂‐to‐CO Electroreduction Relies on Pyridinic‐N/Ni–N_x Sites and Its Zn–CO₂ Battery Application

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Metal-free sites with multidimensional structure modifications for selective electrochemical CO2 reduction

Cited by 26 publications

References 69 publications

Carbon‐based metal‐free catalysts for electrochemical CO2 reduction: Activity, selectivity, and stability

Carbon‐based metal‐free catalysts for electrochemical CO2 reduction: Activity, selectivity, and stability

From CO2 to Value-Added Products: A Review about Carbon-Based Materials for Electro-Chemical CO2 Conversion

Wide Potential CO2‐to‐CO Electroreduction Relies on Pyridinic‐N/Ni–Nx Sites and Its Zn–CO2 Battery Application

Contact Info

Product

Resources

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Carbon‐based metal‐free catalysts for electrochemical CO₂ reduction: Activity, selectivity, and stability

Carbon‐based metal‐free catalysts for electrochemical CO₂ reduction: Activity, selectivity, and stability

Wide Potential CO₂‐to‐CO Electroreduction Relies on Pyridinic‐N/Ni–N_x Sites and Its Zn–CO₂ Battery Application