Atomic-level-designed copper atoms on hierarchically porous gold architectures for high-efficiency electrochemical CO2 reduction

Zhao, Yang; Liu, Xunlin; Chen, Dechao; Liu, Zhixiao; Yang, Qingcheng; Lin, Xin; Peng, Ming; Liu, Pan; Tan, Yongwen

doi:10.1007/s40843-020-1583-4

Cited by 31 publications

(19 citation statements)

References 50 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Cu-based materials are promising electrocatalysts in CO 2 RR [57][58][59]. To investigate the CO 2 RR performance of helical CuTCPP, H-CuTCPP@Cu(OH) 2 , nH-CuTCPP-Cu(OH) 2 , and Cu(OH) 2 nanoarrays were investigated using a three-electrode system.…”

Section: Co 2 Rr Performancementioning

confidence: 99%

Helical copper-porphyrinic framework nanoarrays for highly efficient CO2 electroreduction

et al. 2021

View full text Add to dashboard Cite

In recent years, metal-organic frameworks (MOFs) have been extensively investigated as electrocatalysts due to their highly efficient electroreduction of CO 2 . Herein, the electrocatalytic CO 2 reduction reaction was investigated by growing helical Cu-porphyrinic MOF Cu meso-tetra(4-carboxyphenyl)porphyrin (TCPP) on Cu(OH) 2 nanoarrays (H-CuTCPP@Cu(OH) 2 ) using a sacrificial template method. The electrocatalytic results showed that the H-CuTCPP@Cu(OH) 2 nanoarrays exhibited a high acetic acid Faradaic efficiency (FE) of 26.1% at −1.6 V vs. Ag/Ag + , which is much higher than the value of 19.8% obtained for non-helical CuTCPP@ Cu(OH) 2 (nH-CuTCPP@Cu(OH) 2 ). The higher efficiency may be because space was more effectively utilized in the helical MOF nanoarrays, resulting in a greater number of active catalytic sites. Furthermore, in situ diffuse reflectance infrared Fourier transform spectra showed that the H-CuTCPP@ Cu(OH) 2 nanoarrays have much stronger CO linear adsorption, indicating a better selectivity of acetic acid than that of nH-CuTCPP@Cu(OH) 2 . In this study, we develop new helical nanomaterials and propose a new route to enhance the reduction of CO 2 .

show abstract

Section: Co 2 Rr Performancementioning

confidence: 99%

Helical copper-porphyrinic framework nanoarrays for highly efficient CO2 electroreduction

et al. 2021

View full text Add to dashboard Cite

show abstract

“…The catalytic current usually depends on the surface structure of NPGs and local environments during the CO 2 ER, which are normally considered from thermodynamic and kinetic aspects. On one hand, the detailed structures of NPG in previous investigation include pore size, [15,16,41] crystalline facets, [32,42,43] ECSA, [46] and atomic doping [44,45] for various electrochemical catalysis. On the other hand, physical and chemical environments also affect catalytic activity from the viewpoint of local pH value, temperature, reactant/product concentration, and mass transport of different species.…”

Section: Resultsmentioning

confidence: 99%

Intrinsic Contribution of Mass Transport within Nanoscale Channels of Nanoporous Gold for CO₂ Electrochemical Reduction

Zhou

Chen

et al. 2022

Adv Materials Inter

Self Cite

View full text Add to dashboard Cite

monoxide, methanol, and ethanol) and electrochemical reduction (oxygen, carbon dioxide). [3][4][5][6][7][8][9] Crystalline surfaces of metallic skeletons with unique curvature may expose a large number of active sites, extrinsically depending on pore size, crystal facets, surface strain, and atomic coordination. [9][10][11][12][13][14] Different from metallic nanoparticles, nanoporous metals possess a large amount of geometrically necessary atomic steps and crystalline facets where surface atoms with low coordination are normally active for many electrocatalytic reactions. [15,16] In our previous investigation, nanoporous gold (NPG) with abundant surface steps by electrochemical dealloying of potential cycling, enabling the conversion of CO 2 into CO with Faradaic efficiency (FE) as high as 98%. [17] Besides the unique geometries of metallic skeletons, the interconnected porous channels and their spatial geometries may exhibit a complex impact on reaction kinetics correlating with mass transport, that is, extrinsically reflected by different electrochemical parameters including local pH at the electrode/electrolyte interface and local concentration of reactants/products. [18,19] Mass transport that is widely investigated in heterogeneous catalysis usually plays a critical role in changing physical and chemical environments localized on catalyst Electrochemical reduction enables the conversion of CO 2 into fuel in favor of its global circulation. Nanoporous metals with interconnected and unique skeletons contain large amounts of active sites for effective catalysis, while reaction dynamics are usually stuck by mass transport limited by nanoscale channels. In this work, nanoporous gold (NPG) with different pore sizes is utilized to evaluate the intrinsic behavior of mass transport within nanoscale channels. By defining one comprehensive parameter to exclude the effect of crystalline facets, the intrinsic contribution of mass transport within nanoscale channels to catalytic activity is experimentally identified. Identical correlations between pore size and specific current density are observed in two kinds of NPG that contain crystalline facets with obviously different fractions and comparable fractions. Therefore, the specific current density of CO production monotonously increases with pore size, with a subsequent saturation in both NPG. The critical size of 46 nm correlating with mass transport within nanoscale channels offers one fundamental principle to design hierarchically porous catalysts with high electrochemical activity in the future.

show abstract

“…Recently, Tan et al reported a hierarchically porous Cu 1 Au SAAs as a highly efficient catalyst for CO 2 electroreduction. 65 Beneting from the hierarchically porous architectures with abundant vacancy defects, the as-prepared nanoporous Cu 1 Au SAAs catalyst shows remarkable CO 2 RR activity with nearly 100% CO Faraday efficiency in a wide potential range (À0.4 to À0.9 V vs. RHE) (Fig. 11i).…”

Section: Synergistic Single-atomic Catalysis In the Co 2 Rrmentioning

confidence: 98%

“…Another commonly used method for the synthesis of SAAs is selective dealloying, which can stabilize isolated metal atoms on the surface of another host metal. For instance, Tan et al proposed a facile route to prepare atomic Cu dispersed on hierarchically nanoporous gold architectures (denoted as np-Cu 1 Au SAAs) through a dealloying method, 65 and the fabrication process is illustrated in Fig. 6a.…”

Section: Single-atomic Alloys (Saas)mentioning

confidence: 99%

Synergistically enhanced single-atomic site catalysts for clean energy conversion

2022

J. Mater. Chem. A

View full text Add to dashboard Cite

show abstract

Atomic-level-designed copper atoms on hierarchically porous gold architectures for high-efficiency electrochemical CO2 reduction

Cited by 31 publications

References 50 publications

Helical copper-porphyrinic framework nanoarrays for highly efficient CO2 electroreduction

Helical copper-porphyrinic framework nanoarrays for highly efficient CO2 electroreduction

Intrinsic Contribution of Mass Transport within Nanoscale Channels of Nanoporous Gold for CO₂ Electrochemical Reduction

Synergistically enhanced single-atomic site catalysts for clean energy conversion

Contact Info

Product

Resources

About

Atomic-level-designed copper atoms on hierarchically porous gold architectures for high-efficiency electrochemical CO2 reduction

Cited by 31 publications

References 50 publications

Helical copper-porphyrinic framework nanoarrays for highly efficient CO2 electroreduction

Helical copper-porphyrinic framework nanoarrays for highly efficient CO2 electroreduction

Intrinsic Contribution of Mass Transport within Nanoscale Channels of Nanoporous Gold for CO2 Electrochemical Reduction

Synergistically enhanced single-atomic site catalysts for clean energy conversion

Contact Info

Product

Resources

About

Intrinsic Contribution of Mass Transport within Nanoscale Channels of Nanoporous Gold for CO₂ Electrochemical Reduction