Overpotential for CO<sub>2</sub> electroreduction lowered on strained penta-twinned Cu nanowires

Chen, Zhengzheng; Zhang, Xu; Lü, Gang

doi:10.1039/c5sc02667a

Cited by 64 publications

(63 citation statements)

References 60 publications

(98 reference statements)

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“…Herein, the free energy changes of the first step for these two reactions (N 2 and H adsorption for NRR and HER, respectively) are adopted as descriptors. Moreover, the reactions with lower free energies are assumed to be more selective . The results are illustrated in Figure k, where the catalysts in the blue and red regions are HER and NRR selective, respectively.…”

Section: Resultsmentioning

confidence: 99%

A General Two‐Step Strategy–Based High‐Throughput Screening of Single Atom Catalysts for Nitrogen Fixation

et al. 2018

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Electrocatalytic or photocatalytic N2 reduction holds great promise for green and sustainable NH3 production under ambient conditions, where an efficient catalyst plays a crucial role but remains a long‐standing challenge. Here, a high‐throughput screening of catalysts for N2 reduction among (nitrogen‐doped) graphene‐supported single atom catalysts is performed based on a general two‐step strategy. 10 promising candidates with excellent performance are extracted from 540 systems. Most strikingly, a single W atom embedded in graphene with three C atom coordination (W1C3) exhibits the best performance with an extremely low onset potential of 0.25 V. This study not only provides a series of promising catalysts for N2 fixation, but also paves a new way for the rational design of catalysts for N2 fixation under ambient conditions.

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Section: Resultsmentioning

confidence: 99%

A General Two‐Step Strategy–Based High‐Throughput Screening of Single Atom Catalysts for Nitrogen Fixation

et al. 2018

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“…In addition, there were no oxide‐related peaks for Cu 2 O or CuO, indicating that our Cu NPLs are mostly composed of metallic Cu. From detailed high‐resolution transmission electron microscopy (HR‐TEM) studies on the as‐grown Cu NWs, we found that the Cu NWs show a fivefold twinned structure in which the growth direction is 〈220〉, which is the well‐known crystalline structure of Cu NWs obtained from solution‐phase synthesis (Figure S4, Supporting Information) . To confirm the crystalline structure of the Cu NPLs by transmission electron microscopy (TEM) analysis, the samples were carefully prepared by dropping them on hollow carbon‐coated nickel TEM grids for top‐view imaging and on silicon oxide substrates for cross‐sectional TEM analysis after focused ion beam modification.…”

Section: Resultsmentioning

confidence: 99%

2D Single‐Crystalline Copper Nanoplates as a Conductive Filler for Electronic Ink Applications

Lee

Han

Lee

et al. 2017

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Large-scale 2D single-crystalline copper nanoplates (Cu NPLs) are synthesized by a simple hydrothermal method. The combination of a mild reductant, stabilizer, and shape modifier allows the dimensional control of the Cu nanocrystals from 1D nanowires (NWs) to 2D nanoplates. High-resolution transmission electron microscopy (HR-TEM) reveals that the prepared Cu NPLs have a single-crystalline structure. From the X-ray photoelectron spectroscopy (XPS) analysis, it is found that iodine plays an important role in the modification of the copper nanocrystals through the formation of an adlayer on the basal plane of the nanoplates. Cu NPLs with an average edge length of 10 μm are successfully synthesized, and these Cu NPLs are the largest copper 2D crystals synthesized by a solution-based process so far. The application of the metallic 2D crystals as a semitransparent electrode proves their feasibility as a conductive filler, exhibiting very low sheet resistance (0.4 Ω ▫ ) compared to Cu NWs and a transmittance near 75%. The efficient charge transport is due to the increased contact area between each Cu NPL, i.e., so-called plane contact (2D electrical contact). In addition, this type of contact enhances the current-carrying capability of the Cu NPL electrodes, implying that the large-size Cu NPLs are promising conductive fillers for printable electrode applications.

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“…In line with the experimental advances in tuning the CNs of Cu, the catalyst models of a Cu 55 nanoparticle [30] and a pentatwinned Cu nanowire [31] were also theoretically investigated by Lim et al and Chen et al, respectively. They found that *CO was adsorbed on the 3-fold site of Cu 55 nanoparticle.…”

Section: Reducing Coordination Numbers (Cns)mentioning

confidence: 98%

Recent Advances in Breaking Scaling Relations for Effective Electrochemical Conversion of CO₂

Sun

2016

Advanced Energy Materials

338

277

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and selectively produce carbon-containing products from CO 2 with reasonably low overpotentials and low cost.From the theoretical point of view, electrochemical CO 2 reduction, similar to many other electrochemical energy conversion processes on metal surfaces, comprise of multiple concerted or sequential proton-electron transfer reactions. In 2004, Nørskov et al. [2] developed a concise and effective scheme to understand the origin of the overpotential, which was denoted as the computational hydrogen electrode (CHE) model. They claimed that due to the relative low proton transfer barriers, the kinetic aspects in the proton transfer was omitted, and the rate-determining step was the one with the most positive free energy change ΔE max . To make the free energy of the rate-determining step become zero, a limiting potentialneeds to be applied. If we denote the equilibrium potential of a given electrochemical reaction as U eq , the overpotential wouldThe overpotential thereby originates from the relative stability between certain adsorbed intermediates. For example, the overpotential for 4-electron oxygen reduction reaction (ORR) is ascribed to the high adsorption free energy barrier of *OOH on the weak binding materials or the high desorption free energy barrier of *OH on the strong binding materials. [3] Similarly, when excluding the Tafel mechanism, the overpotential for hydrogen evolution reaction (HER) originates from either the high adsorption free energy barrier of *H (Volmer step) or the high desorption barrier of the same intermediate (Heyrovsky step). [4] Based on the Sabatier principle, [5] when the maximum electrocatalytic activity is reached in these reactions, the binding of the reaction intermediates should be neither too strong nor too weak. In HER, where only *H is emerged as the reaction intermediate, it is easier to achieve a maximum reactivity with negligible overpotential because the binding energy of *H is not limited and can be tuned freely. If the binding energy of *H on a certain material renders the adsorption free energy of *H close to zero, the overpotential will be negligible. Such an electroactive electrode for HER indeed exists, say the platinum electrode. However, for electrocatalytic reactions with multiple proton-electron transfer steps, the case is much more complex. The overpotential cannot be lowered to a negligible value because the relative The increasing concentration of CO 2 in the atmosphere, and the resulting environmental problems, call for effective ways to convert CO 2 into valuable fuels and chemicals for a sustainable carbon cycle. In such a context, CO 2 electrocatalytic reduction has been hotly studied due to the merits of ambient operational conditions and easy control of the reaction process by changing the applied potential. Among the various systems studied, Cu and Au are found to possess the highest Faradaic efficiency toward cathodic electrocatalytic conversion of CO 2 to hydrocarbons and CO, respectively. However, both of them suffer from large overpotentials ...

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Overpotential for CO₂ electroreduction lowered on strained penta-twinned Cu nanowires

Abstract: Penta-twinned Cu nanowires have a strain-tunable low overpotential for CO2 electroreduction.

Cited by 64 publications

References 60 publications

A General Two‐Step Strategy–Based High‐Throughput Screening of Single Atom Catalysts for Nitrogen Fixation

A General Two‐Step Strategy–Based High‐Throughput Screening of Single Atom Catalysts for Nitrogen Fixation

2D Single‐Crystalline Copper Nanoplates as a Conductive Filler for Electronic Ink Applications

Recent Advances in Breaking Scaling Relations for Effective Electrochemical Conversion of CO₂

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Overpotential for CO2 electroreduction lowered on strained penta-twinned Cu nanowires

Abstract: Penta-twinned Cu nanowires have a strain-tunable low overpotential for CO2 electroreduction.

Cited by 64 publications

References 60 publications

A General Two‐Step Strategy–Based High‐Throughput Screening of Single Atom Catalysts for Nitrogen Fixation

A General Two‐Step Strategy–Based High‐Throughput Screening of Single Atom Catalysts for Nitrogen Fixation

2D Single‐Crystalline Copper Nanoplates as a Conductive Filler for Electronic Ink Applications

Recent Advances in Breaking Scaling Relations for Effective Electrochemical Conversion of CO2

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Overpotential for CO₂ electroreduction lowered on strained penta-twinned Cu nanowires

Recent Advances in Breaking Scaling Relations for Effective Electrochemical Conversion of CO₂