Stabilizing Copper by a Reconstruction-Resistant Atomic Cu–O–Si Interface for Electrochemical CO<sub>2</sub> Reduction

Tan, Xin; Sun, Kaian; Zhuang, Zewen; Hu, Botao; Liu, Qinggang; He, Chang; Zhi-Yuan, XU; Chen, Chang; Xiao, Hai; Chen, Chen

doi:10.1021/jacs.3c01638

Cited by 22 publications

(30 citation statements)

References 57 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…(c) CH 4 FEs at −1.18 V (vs RHE) on Pd, Pd 7 @Cu 1 , Pd 7 @Cu 2 , Pd 7 @Cu 3 , and Cu. (d) Comparison of this work with previous studies on the electrocatalytic CO 2 -to-CH 4 reaction in 1 M KOH by a flow cell device (refs − ). (e) Potential versus time of Pd 7 @Cu 2 at a constant current density of 100 mA·cm –2 and the corresponding CH 4 FE.…”

Section: Resultsmentioning

confidence: 80%

A Surfactant-Free and General Strategy for the Synthesis of Bimetallic Core–Shell Nanocrystals on Reduced Graphene Oxide through Targeted Photodeposition

Liu

et al. 2023

ACS Nano

View full text Add to dashboard Cite

Tunable physicochemical properties of bimetallic core–shell heterostructured nanocrystals (HNCs) have shown enormous potential in electrocatalytic reactions. In many cases, HNCs are required to load on supports to inhibit catalyst aggregation. However, the introduction of supports during the process of growing core–shell HNCs makes the synthesis much more complicated and difficult to control precisely. Herein, we reported a universal photochemical synthetic strategy for the controlled synthesis of well-defined surfactant-free core–shell metal HNCs on a reduced graphene oxide (rGO) support, which was assisted by the fine control of photogenerated electrons directly transferring to the targeted metal seeds via rGO and the precisely tuned adsorption capacity of the added second metal precursors. The surface photovoltage microscopy (SPVM) platform proved that photogenerated electrons flowed through rGO to Pd particles under illumination. We have successfully synthesized 24 different core–shell metal HNCs, i.,e., MA@MB (MA = Pd, Au, and Pt; MB = Au, Ag, Pt, Pd, Ir, Ru, Rh, Ni and Cu), on the rGO supports. The as-prepared Pd@Cu core–shell HNCs showed outstanding performance in the electrocatalytic reduction of CO2 to CH4. This work could shed light on the controlled synthesis of more functional bimetallic nanostructured materials on diverse supports for various applications.

show abstract

Section: Resultsmentioning

confidence: 80%

A Surfactant-Free and General Strategy for the Synthesis of Bimetallic Core–Shell Nanocrystals on Reduced Graphene Oxide through Targeted Photodeposition

Liu

et al. 2023

ACS Nano

View full text Add to dashboard Cite

show abstract

“…They claimed that the formation of strong Si–O or Si–C bonds at the Cu-SiO x step site accelerated C 2 H 4 production. Chen et al demonstrated that CuSiO x catalysts with abundant Cu–O–Si interfacial sites exhibited high CO 2 -to-CH 4 selectivity . However, no attention has been paid to the effect of Cu–Si bonds in previous reports.…”

Section: Resultsmentioning

confidence: 99%

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

Xiong,

Si,

et al. 2023

J. Am. Chem. Soc.

View full text Add to dashboard Cite

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.

show abstract

“…Cu atoms on the F-substituted GDY exhibited the positive Cu δ+ centers, which accelerated water dissociation to promote the hydrogenation of intermediates toward the CH 4 production (Figure e). SiO 2 was used as a support to stabilize the Cu species, which formed abundant atomic Cu–O–Si interfacial sites . The strong interaction between Cu and SiO 2 made the Cu–O–Si interfacial sites show ultrahigh reconstruction resistance (Figure g).…”

Section: Ad Cu Catalysts For C1 Productsmentioning

confidence: 99%

Insight on Atomically Dispersed Cu Catalysts for Electrochemical CO₂ Reduction

Wang,

Deng,

et al. 2023

ACS Nano

View full text Add to dashboard Cite

Electrochemical CO2 reduction (ECO2R) with renewable electricity is an advanced carbon conversion technology. At present, copper is the only metal to selectively convert CO2 into multicarbon (C2+) products. Among them, atomically dispersed (AD) Cu catalysts have received great attention due to the relatively single chemical environment, which are able to minimize the negative impact of morphology, valence state, and crystallographic properties, etc. on product selectivity. Furthermore, the completely exposed atomic Cu sites not only provide space and bonding electrons for the adsorption of reactants in favor of better catalytic activity but also provide an ideal platform for studying its reaction mechanism. This review summarizes the recent progress of AD Cu catalysts as a chemically tunable platform for ECO2R, including the atomic Cu sites dynamic evolution, the catalytic performance, and mechanism. Furthermore, the prospects and challenges of AD Cu catalysts for ECO2R are carefully discussed. We sincerely hope that this review can contribute to the rational design of AD Cu catalysts with enhanced performance for ECO2R.

show abstract

Stabilizing Copper by a Reconstruction-Resistant Atomic Cu–O–Si Interface for Electrochemical CO₂ Reduction

Cited by 22 publications

References 57 publications

A Surfactant-Free and General Strategy for the Synthesis of Bimetallic Core–Shell Nanocrystals on Reduced Graphene Oxide through Targeted Photodeposition

A Surfactant-Free and General Strategy for the Synthesis of Bimetallic Core–Shell Nanocrystals on Reduced Graphene Oxide through Targeted Photodeposition

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

Insight on Atomically Dispersed Cu Catalysts for Electrochemical CO₂ Reduction

Contact Info

Product

Resources

About

Stabilizing Copper by a Reconstruction-Resistant Atomic Cu–O–Si Interface for Electrochemical CO2 Reduction

Cited by 22 publications

References 57 publications

A Surfactant-Free and General Strategy for the Synthesis of Bimetallic Core–Shell Nanocrystals on Reduced Graphene Oxide through Targeted Photodeposition

A Surfactant-Free and General Strategy for the Synthesis of Bimetallic Core–Shell Nanocrystals on Reduced Graphene Oxide through Targeted Photodeposition

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

Insight on Atomically Dispersed Cu Catalysts for Electrochemical CO2 Reduction

Contact Info

Product

Resources

About

Stabilizing Copper by a Reconstruction-Resistant Atomic Cu–O–Si Interface for Electrochemical CO₂ Reduction

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

Insight on Atomically Dispersed Cu Catalysts for Electrochemical CO₂ Reduction