Modulated Sn Oxidation States over a Cu<sub>2</sub>O-Derived Substrate for Selective Electrochemical CO<sub>2</sub> Reduction

Li, Mengran; Tian, Xiaohe; Garg, Sahil; Rufford, Thomas E.; Zhao, Peiyao; Wu, Yuming; Yago, Anya; Ge, Lei; Rudolph, Victor; Wang, Geoff

doi:10.1021/acsami.0c00412

Cited by 41 publications

(39 citation statements)

References 42 publications

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“…Previous studies have shown that Cu–Sn alloys can realize both CO 2 -to-CO 27 , 28 and CO 2 -to-formate reaction pathways 29 , 30 (see Supplementary Table 2 ). Although insights have been gained in terms of morphology 31 , structure 30 , valence state 32 , and composition 29 , the mechanistic understanding of Cu–Sn alloys at the isolated atomic interfaces and the root behind different CO 2 RR pathways remain elusive. In this study, the three-dimensional atomic structure of the Cu–Sn surface alloy is established by using the atom probe tomography (APT) and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM).…”

Section: Introductionmentioning

confidence: 99%

Isolated copper–tin atomic interfaces tuning electrocatalytic CO2 conversion

et al. 2021

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Direct experimental observations of the interface structure can provide vital insights into heterogeneous catalysis. Examples of interface design based on single atom and surface science are, however, extremely rare. Here, we report Cu–Sn single-atom surface alloys, where isolated Sn sites with high surface densities (up to 8%) are anchored on the Cu host, for efficient electrocatalytic CO2 reduction. The unique geometric and electronic structure of the Cu–Sn surface alloys (Cu97Sn3 and Cu99Sn1) enables distinct catalytic selectivity from pure Cu100 and Cu70Sn30 bulk alloy. The Cu97Sn3 catalyst achieves a CO Faradaic efficiency of 98% at a tiny overpotential of 30 mV in an alkaline flow cell, where a high CO current density of 100 mA cm−2 is obtained at an overpotential of 340 mV. Density functional theory simulation reveals that it is not only the elemental composition that dictates the electrocatalytic reactivity of Cu–Sn alloys; the local coordination environment of atomically dispersed, isolated Cu–Sn bonding plays the most critical role.

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Section: Introductionmentioning

confidence: 99%

Isolated copper–tin atomic interfaces tuning electrocatalytic CO2 conversion

et al. 2021

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“…However, achieving high product selectivity at industrially relevant current densities remains a crucial challenge in the large‐scale deployment of CO 2 R technologies [2] . Advances in new electrocatalyst materials for CO 2 R [3–12] provide a crucial strategy to improve the selectivity and activity. Still, there is a need to better understand how CO 2 and electrolytes interact with the catalysts and how these interactions during CO 2 R can play a significant role in enhancing CO 2 R selectivity and activity [13–16] .…”

Section: Introductionmentioning

confidence: 99%

Understanding the Effects of Anion Interactions with Ag Electrodes on Electrochemical CO₂ Reduction in Choline Halide Electrolytes

Garg

et al. 2021

ChemSusChem

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Interactions of electrolyte ions at electrocatalyst surfaces influence the selectivity of electrochemical CO2 reduction (CO2R) to chemical feedstocks like CO. We investigated the effects of anion type in aqueous choline halide solutions (ChCl, ChBr, and ChI) on the selectivity of CO2R to CO over an Ag foil cathode. Using an H‐type cell, we observed that halide‐specific adsorption at the Ag surface limits CO faradaic efficiency (FECO) at potentials more positive than −1.0 V vs. reversible hydrogen electrode (RHE). At these conditions, FECO increased from I−90 %) in ChCl (at −0.75±0.06 Vvs. RHE) and ChI (at −0.78±0.17 V vs. RHE) could be achieved at a current density of 150 mA cm−2 in a continuous flow‐cell electrolyser with Ag nanoparticles on a commercial gas diffusion electrode. This study provides new insights to understand the interactions of anions with catalysts and offers a new method to modify electrocatalyst surfaces.

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“…Gas chromatograph (GC‐7820, Zhongkehuifen, China) equipped with both thermal conductivity detector (TCD) and flame ionization detector (FID) was used to quantify the gas‐phase products. The FE i of gas product species‐CO and H 2 was calculated by [34]

true F E_{i} = (n_{i} \times F \times P \times v \times c_{i}) / (R \times T \times j) \times 100 %

…”

Section: Methodsmentioning

confidence: 99%

Engineering Bimetallic Copper‐Tin Based Core‐Shell Alloy@Oxide Nanowire as Efficient Catalyst for Electrochemical CO₂ Reduction

Deng

Yuan

et al. 2021

ChemElectroChem

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Pursuing both high effective and selective electrocatalysts is significant for efficient and low-cost electrochemical carbon dioxide (CO 2 ) reduction. Here, we design a novel bimetallic alloy/oxide nanowire catalyst with core-shell configuration. A typical CuSn alloy core provides high electrical conductivity while the amorphous Cu doped SnO 2 shell guarantees the catalytic activity and selectivity for CO 2 reduction process. Computational studies further elucidate the important role of Cu doped SnO 2 layer in the electrocatalytic selectivity for formate and the restraint of hydrogen production. Benefited from the well-designed components and hierarchical configuration, the as-prepared electrocatalyst displays a partial current density of 30 mA cm À 2 with a Faradaic efficiency of 78 % at À 0.9 V vs. reversible hydrogen electrode (RHE) for formate. This work provides a new pathway to design advanced electrocatalyst for CO 2 electrochemical reduction.

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Modulated Sn Oxidation States over a Cu₂O-Derived Substrate for Selective Electrochemical CO₂ Reduction

Cited by 41 publications

References 42 publications

Isolated copper–tin atomic interfaces tuning electrocatalytic CO2 conversion

Isolated copper–tin atomic interfaces tuning electrocatalytic CO2 conversion

Understanding the Effects of Anion Interactions with Ag Electrodes on Electrochemical CO₂ Reduction in Choline Halide Electrolytes

Engineering Bimetallic Copper‐Tin Based Core‐Shell Alloy@Oxide Nanowire as Efficient Catalyst for Electrochemical CO₂ Reduction

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Modulated Sn Oxidation States over a Cu2O-Derived Substrate for Selective Electrochemical CO2 Reduction

Cited by 41 publications

References 42 publications

Isolated copper–tin atomic interfaces tuning electrocatalytic CO2 conversion

Isolated copper–tin atomic interfaces tuning electrocatalytic CO2 conversion

Understanding the Effects of Anion Interactions with Ag Electrodes on Electrochemical CO2 Reduction in Choline Halide Electrolytes

Engineering Bimetallic Copper‐Tin Based Core‐Shell Alloy@Oxide Nanowire as Efficient Catalyst for Electrochemical CO2 Reduction

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Product

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Modulated Sn Oxidation States over a Cu₂O-Derived Substrate for Selective Electrochemical CO₂ Reduction

Understanding the Effects of Anion Interactions with Ag Electrodes on Electrochemical CO₂ Reduction in Choline Halide Electrolytes

Engineering Bimetallic Copper‐Tin Based Core‐Shell Alloy@Oxide Nanowire as Efficient Catalyst for Electrochemical CO₂ Reduction