Sulfurization-derived Cu0–Cu+ sites for electrochemical CO2 reduction to ethanol

Dou, Tong; Du, Jiawei; He, Jinqing; Wang, Yiping; Zhao, Xuhui; Zhang, Fazhi; Lei, Xiaodong

doi:10.1016/j.jpowsour.2022.231393

Cited by 22 publications

(8 citation statements)

References 40 publications

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“…As shown in Figure S6, the peaks located at 932.9 eV in Cu 2p XPS spectra were associated with Cu 0 or Cu + . The Cu LMM Auger electron spectroscopy (AES) further proved that Cu 0 and Cu + coexisted in p-Cu@m-SiO 2 and porous-Cu (Figure b) . However, the previous PXRD spectra and TEM images both proved that no copper oxide existed in the as-prepared samples.…”

Section: Resultsmentioning

confidence: 89%

Steering CO₂ Electroreduction Selectivity U-Turn to Ethylene by Cu–Si Bonded Interface

Xiong,

Si,

et al. 2023

J. Am. Chem. Soc.

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Copper (Cu), with the advantage of producing a deep reduction product, is a unique catalyst for the electrochemical reduction of CO 2 (CO 2 RR). Designing a Cu-based catalyst to trigger CO 2 RR to a multicarbon product and understanding the accurate structure−activity relationship for elucidating reaction mechanisms still remain a challenge. Herein, we demonstrate a rational design of a core−shell structured silica-copper catalyst (p-Cu@m-SiO 2 ) through Cu−Si direct bonding for efficient and selective CO 2 RR. The Cu−Si interface fulfills the inversion in CO 2 RR product selectivity. The product ratio of C 2 H 4 /CH 4 changes from 0.6 to 14.4 after silica modification, and the current density reaches a high of up to 450 mA cm −2 . The kinetic isotopic effect, in situ attenuated total reflection Fourier-transform infrared spectra, and density functional theory were applied to elucidate the reaction mechanism. The SiO 2 shell stabilizes the *H intermediate by forming Si−O−H and inhibits the hydrogen evolution reaction effectively. Moreover, the direct-bonded Cu−Si interface makes bare Cu sites with larger charge density. Such bare Cu sites and Si−O−H sites stabilized the *CHO and activated the *CO, promoting the coupling of *CHO and *CO intermediates to form C 2 H 4 . This work provides a promising strategy for designing Cu-based catalysts with high C 2 H 4 catalytic activity.

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Section: Resultsmentioning

confidence: 89%

Steering CO₂ Electroreduction Selectivity U-Turn to Ethylene by Cu–Si Bonded Interface

Xiong,

Si,

et al. 2023

J. Am. Chem. Soc.

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“…Besides, other copper compounds have also been studied as the precursors to obtain derived Cu catalysts for CO 2 ERR. For instance, a CuI-derived Cu catalyst showing a 71.2% C 2+ faradaic efficiency with 290 mA cm –2 stands out among cuprous-halide-derived Cu catalysts. − A Cu 3 N-derived Cu catalyst provided a 68% C 2+ faradaic efficiency at 18.5 mA cm –2 , while a Cu 2 S-derived Cu catalyst gave a 13.5% ethanol faradaic efficiency at 100 mA cm –2 . , Both a copper phthalocyanine-derived Cu catalyst and a Cu–Al hydrotalcite-derived AlO x -modified Cu catalyst exhibited 70% C 2+ faradaic efficiencies at 200 mA cm –2 . , These progresses have shown great practical potential of copper compound-derived Cu catalysts and aroused the demand of further investigations toward more efficient CO 2 ERR catalyst designs.…”

Section: Introductionmentioning

confidence: 98%

“…faradaic efficiency at 100 mA cm −2 . 31,32 Both a copper phthalocyanine-derived Cu catalyst and a Cu−Al hydrotalcite-derived AlO x -modified Cu catalyst exhibited 70% C 2+ faradaic efficiencies at 200 mA cm −2 . 1,33 These progresses have shown great practical potential of copper compound-derived Cu catalysts and aroused the demand of further investigations toward more efficient CO 2 ERR catalyst designs.…”

Section: Introductionmentioning

confidence: 99%

Phosphate-Derived Copper-Based Catalysts for Efficient CO₂ Reduction to Multicarbon Products

Gao,

Gu,

et al. 2023

Energy Fuels

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“…Catalysts containing Cu + sites have been widely studied for their advantages in CO 2 activation and *CO dimerization , (* means adsorbed). For example, it has shown that Cu/Cu 2 S catalysts prepared in situ on copper mesh generated high density of Cu 0 and Cu + pairs during reduction, which facilitated the adsorption of key intermediate *CH 2 CHO and decreased the energy barrier of the ethanol pathway . Different Cu-based catalysts have different reduction rates and structural evolution, so they have different mechanisms and active sites for electroreduction of CO 2.…”

Section: Introductionmentioning

confidence: 99%

“…For example, it has shown that Cu/Cu 2 S catalysts prepared in situ on copper mesh generated high density of Cu 0 and Cu + pairs during reduction, which facilitated the adsorption of key intermediate *CH 2 CHO and decreased the energy barrier of the ethanol pathway. 30 Different Cu-based catalysts have different reduction rates and structural evolution, so they have different mechanisms and active sites for electroreduction of CO 2. 31 However, there is still a long way to go to improve the selectivity of electroreduction of CO 2 .…”

Section: ■ Introductionmentioning

confidence: 99%

Cu/Fe₃O₄ Nanocomposites from Layered Double Hydroxides as Catalysts for Selective Electroreduction of Carbon Dioxide

Dou

Diao

et al. 2023

ACS Appl. Nano Mater.

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The reduction of carbon dioxide to valuable chemical products is a hot topic of current research. In this article, Cu nanoparticle-decorated Fe 3 O 4 (Cu/Fe 3 O 4 ) is prepared by using layered double hydroxide (LDH) as the precursor. The CuFe-LDH is synthesized using the coprecipitation method and further reduced to obtain the final material Cu/Fe 3 O 4 . The uniform layered structure of LDH results in highly dispersed metallic elements in the corresponding Cu/Fe 3 O 4 , in which Cu atoms provide Cu 0 and Cu + pairs and good electrical conductivity during the reduction process with Fe 3 O 4 as the framework. Therefore, Cu/Fe 3 O 4 shows high selectivity for CO 2 electroreduction to ethanol, in which the Faraday efficiency is 50.9% at −0.3 V vs RHE. Experimental results show that Cu/Fe 3 O 4 generates uniformly distributed Cu + sites during CO 2 electroreduction, which is conducive to the formation of *CHO, a key intermediate to ethanol. This study provides a design method for catalysts of CO 2 electroreduction with feasibility.

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Sulfurization-derived Cu0–Cu+ sites for electrochemical CO2 reduction to ethanol

Cited by 22 publications

References 40 publications

Steering CO₂ Electroreduction Selectivity U-Turn to Ethylene by Cu–Si Bonded Interface

Steering CO₂ Electroreduction Selectivity U-Turn to Ethylene by Cu–Si Bonded Interface

Phosphate-Derived Copper-Based Catalysts for Efficient CO₂ Reduction to Multicarbon Products

Cu/Fe₃O₄ Nanocomposites from Layered Double Hydroxides as Catalysts for Selective Electroreduction of Carbon Dioxide

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Sulfurization-derived Cu0–Cu+ sites for electrochemical CO2 reduction to ethanol

Cited by 22 publications

References 40 publications

Steering CO2 Electroreduction Selectivity U-Turn to Ethylene by Cu–Si Bonded Interface

Steering CO2 Electroreduction Selectivity U-Turn to Ethylene by Cu–Si Bonded Interface

Phosphate-Derived Copper-Based Catalysts for Efficient CO2 Reduction to Multicarbon Products

Cu/Fe3O4 Nanocomposites from Layered Double Hydroxides as Catalysts for Selective Electroreduction of Carbon Dioxide

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Steering CO₂ Electroreduction Selectivity U-Turn to Ethylene by Cu–Si Bonded Interface

Steering CO₂ Electroreduction Selectivity U-Turn to Ethylene by Cu–Si Bonded Interface

Phosphate-Derived Copper-Based Catalysts for Efficient CO₂ Reduction to Multicarbon Products

Cu/Fe₃O₄ Nanocomposites from Layered Double Hydroxides as Catalysts for Selective Electroreduction of Carbon Dioxide