Efficient electrochemical transformation of CO2 to C2/C3 chemicals on benzimidazole-functionalized copper surfaces

Zhong, Shenghong; Yang, Yuting; Cao, Zhen; Dong, Xinglong; Kozlov, Sergey M.; Falivene, Laura; Huang, Jianguo; Zhou, Xiaofeng; Hedhili, Mohamed N.; Lai, Zhiping; Huang, Kuo‐Wei; Han, Yu; Cavallo, Luigi; Li, Lain‐Jong

doi:10.1039/c8cc04735a

Cited by 51 publications

(43 citation statements)

References 28 publications

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“…Enhancement of selectivity is also reported thanks to a chelate effect of benzimidazole (BIM) at copper surface . The conversion of CO 2 to C 2 /C 3 products is observed together with a drastic decrease of the HER process with a much higher yield than bare copper at −1.07 V vs RHE.…”

Section: Surface Functionalization Of Single‐metal Catalystsmentioning

confidence: 86%

“…The conversion of CO 2 to C 2 /C 3 products is observed together with a drastic decrease of the HER process with a much higher yield than bare copper at −1.07 V vs RHE. This enhanced selectivity is ascribed to the formation of a thick Cu(BMI) x layer which is supposed to i) restrict the proton diffusion, hence increasing the local pH at the catalyst surface to suppress HER and ii) be a source of active H δ+ orienting the intermediates formation towards C 2 /C 3 products . Interestingly, the analysis of current density and ESCA indicates that underlying Cu surface rather than Cu(BIM)x complexes are the active surface.…”

Section: Surface Functionalization Of Single‐metal Catalystsmentioning

confidence: 99%

“…They could modify the orientation of the reactants or intermediate species with respect to the catalytic sites, hence governing selectivity . The modifications of the surface may enhance the co‐adsorption of relevant reactants or intermediates and/or facilitates proton transfers or water activation that are of great importance in these processes . They could promote or inhibit certain reaction pathways.…”

Section: Influence Of Organic Ligands On Surface Properties: Steric mentioning

confidence: 99%

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Surface Modification for Promoting Durable, Efficient, and Selective Electrocatalysts

2020

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Intensive research into the design of catalysts involved in energy conversion and fuel cell technologies has allowed great progress in the field. However, durable, efficient and selective electrocatalytic systems for the activation of fuel molecules at the lowest cost are still needed. The most developed strategies consist of tailoring the shape, size and composition of metallic nanomaterials. Yet, deliberate surface modification of the catalysts should be considered as a promising alternative approach. The functionalization of metallic catalysts with organic ligands has been recently demonstrated to promote high catalytic activity. This Review focuses on the functionalization of metallic or alloy catalysts with organic ligands, showing the impact of the surface modification for different materials and different reactions. Hybrid systems based on this alternative strategy could contribute to the elaboration of cutting‐edge systems for electrocatalysis.

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Section: Surface Functionalization Of Single‐metal Catalystsmentioning

confidence: 86%

Section: Surface Functionalization Of Single‐metal Catalystsmentioning

confidence: 99%

Section: Influence Of Organic Ligands On Surface Properties: Steric mentioning

confidence: 99%

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Surface Modification for Promoting Durable, Efficient, and Selective Electrocatalysts

2020

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“…There have been many reports of copper discs and foils requiring extensive purification of both the copper surface and the reaction medium prior to electrocatalysis. 35 Copper foams are active without electropolishing the electrode or scavenging the bicarbonate solution. 34,36 The copper foams reported herein comprise agglomerates of sub-micrometer copper cuboctahedra for the electrocatalytic reduction of CO2 to propanol.…”

Section: Introductionmentioning

confidence: 99%

CO2 Reduction to Propanol by Copper Foams: A Pre- and Post-Catalysis Study

Rudd¹,

Kazimierska²,

Lb³

et al. 2020

Preprint

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The utilization of carbon dioxide is a major incentive for the growing field of carbon capture. Carbon dioxide could be an abundant building block to generate higher value products. Herein, we describe the use of porous copper electrodes to catalyze the reduction of carbon dioxide into higher value products such as ethylene, ethanol and, notably, propanol. For n-propanol production, faradaic efficiencies reach 4.93% at -0.83 V vs RHE, with a geometric partial current density of -1.85 mA/cm2. We have documented the performance of the catalyst in both pristine and urea-modified foams pre- and post-electrolysis. Before electrolysis, the copper electrode consisted of a mixture of cuboctahedra and dendrites. After 35-minute electrolysis, the cuboctahedra and dendrites have undergone structural rearrangement. Changes in the interaction of urea with the catalyst surface have also been observed. These transformations were characterized ex-situ using scanning electron microscopy, X-ray diffraction, and X-ray photoelectron spectroscopy. We found that alterations in the morphology, crystallinity, and surface composition of the catalyst led to the deactivation of the copper foams.

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“…The extensive of fossil fuels produces excess amount of CO 2 , which caused serious ecological issues, therefore the capture and utilization of CO 2 becomes an imperative task . Electrochemical CO 2 reduction is a promising alternative to transform CO 2 to useful fuels, which can be operated in mild reaction condition, such as room temperature, atmospheric pressure and neutral solution .…”

Section: Introductionmentioning

confidence: 99%

Atomic Ni Species Anchored N‐Doped Carbon Hollow Spheres as Nanoreactors for Efficient Electrochemical CO₂ Reduction

Huang

et al. 2019

ChemCatChem

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Electrochemical CO 2 reduction to value-added chemicals is a critical and challenging process for research of sustainable energy. Herein, we synthesize new nickel single atom catalysts embedded in nitrogen doped hollow carbon spheres (NiÀ N/C-x) via thermal treatment of Ni salts and nitrogen doped hollow carbon spheres (N/C-x). The state of Ni species on NiÀ N/C-x can be tuned by the nitrogen species of N/C-x and pyrrolic-N favors the formation of atomic Ni species. Two catalysts, namely, NiÀ N/C-1/4 contains more pyrrolic-N and more amount of atomic Ni species than that on NiÀ N/C-3/2 have been prepared. During all the measurement potential range, NiÀ N/C-1/4 displays a much higher catalytic activity for CO 2 reduction to CO than NiÀ N/C-3/2. Within the potential range of À 0.63 V to À 0.98 V versus reversible hydrogen electrode (RHE), the faradaic efficiencies of CO on NiÀ N/C-1/4 exceed 70 %. Furthermore, NiÀ N/C-1/4 exhibits high selectivity for CO and excellent stability during 4.5 h of CO 2 reduction electrolysis at the potential of À 0.78 V versus RHE.[a] S.

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Efficient electrochemical transformation of CO₂ to C₂/C₃ chemicals on benzimidazole-functionalized copper surfaces

Cited by 51 publications

References 28 publications

Surface Modification for Promoting Durable, Efficient, and Selective Electrocatalysts

Surface Modification for Promoting Durable, Efficient, and Selective Electrocatalysts

CO2 Reduction to Propanol by Copper Foams: A Pre- and Post-Catalysis Study

Atomic Ni Species Anchored N‐Doped Carbon Hollow Spheres as Nanoreactors for Efficient Electrochemical CO₂ Reduction

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Efficient electrochemical transformation of CO2 to C2/C3 chemicals on benzimidazole-functionalized copper surfaces

Cited by 51 publications

References 28 publications

Surface Modification for Promoting Durable, Efficient, and Selective Electrocatalysts

Surface Modification for Promoting Durable, Efficient, and Selective Electrocatalysts

CO2 Reduction to Propanol by Copper Foams: A Pre- and Post-Catalysis Study

Atomic Ni Species Anchored N‐Doped Carbon Hollow Spheres as Nanoreactors for Efficient Electrochemical CO2 Reduction

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Product

Resources

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Efficient electrochemical transformation of CO₂ to C₂/C₃ chemicals on benzimidazole-functionalized copper surfaces

Atomic Ni Species Anchored N‐Doped Carbon Hollow Spheres as Nanoreactors for Efficient Electrochemical CO₂ Reduction