Intermetallic CuAu nanoalloy for stable electrochemical CO2 reduction

Kuang, Siyu; Li, Minglu; Chen, Xiaoyi; Chi, Haoyuan; Lin, Jianlong; Hu, Zheng; Hu, Shengsun; Zhang, Sheng; Ma, Xinbin

doi:10.1016/j.cclet.2022.108013

Cited by 13 publications

(5 citation statements)

References 35 publications

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“…As shown in Figure S4b, the vibration bands at approximately 1255 cm À 1 and 1515 cm À 1 are assigned to the characteristic vibration adsorption of CO 2 *À and *OCCO on Cu nanoparticles, respectively, which is aligned with the mechanisms of single electron pre-equilibrium on Cu nanoparticles. [25,26] Two CO 2 *À radicals combine to generate OOCÀ COO (oxalate) and then further reduced to *OCCO. As shown in Figure S5, symmetric CO 2 stretch (1350 cm À 1 ) was detected under CO 2 as carbon source, which proved that oxalate is the key intermediate of CO 2 reaction process.…”

Section: Resultsmentioning

confidence: 99%

Acetamide Electrosynthesis from CO₂ and Nitrite in Water

Kuang,

Xiao,

Chi

et al. 2024

Angew Chem Int Ed

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Renewable electricities driven electrocatalytic CO2 reduction reaction (CO2RR) is a promising solution to carbon neutralization, which mainly generate simple carbon products. It is of great importance to produce more valuable C‐N chemicals from CO2 and nitrogen species. However, it is challenging to co‐reduce CO2 and NO3‐/NO2‐ to generate aldoxime an important intermediate in the electrocatalytic C‐N coupling process. Herein, we report the successful electrochemical conversion of CO2 and NO2‐ to acetamide for the first time over copper catalysts under alkaline condition through a gas diffusion electrode. Operando spectroelectrochemical characterizations and DFT calculations, suggest acetaldehyde and hydroxylamine identified as key intermediates undergo a nucleophilic addition reaction to produce acetaldoxime, which is then dehydrated to acetonitrile and followed by hydrolysis to give acetamide under highly local alkaline environment and electric field. Moreover, the above mechanism was successfully extended to the formation of phenylacetamide. This study provides a new strategy to synthesize highly valued amides from CO2 and wastewater.

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Section: Resultsmentioning

confidence: 99%

Acetamide Electrosynthesis from CO₂ and Nitrite in Water

Kuang,

Xiao,

Chi

et al. 2024

Angew Chem Int Ed

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“…Among the Cu–M bimetallic catalysts (where M = Ag, Au, , Zn, Pd, etc. ), Ag and Au metals are promising candidates for oxygenate conversion due to their weak H and O affinity. , For example, Cu 3 Au showed a high FE ethanol of over 29%, possibly attributed to the tuned d-band center below the Fermi-level energy (Figure C) . The changed electronic structure originated from lattice disorder by introducing Au and induced a shorter C–O length of intermediates than pure Cu, thus leading to a high ethanol conversion over ethylene through a higher energy barrier for breaking C–O bonds.…”

Section: Electrocatalystsmentioning

confidence: 99%

Multiscale CO₂ Electrocatalysis to C₂₊ Products: Reaction Mechanisms, Catalyst Design, and Device Fabrication

Yan,

Chen,

Kumari

et al. 2023

Chem. Rev.

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111

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Electrosynthesis of value-added chemicals, directly from CO 2 , could foster achievement of carbon neutral through an alternative electrical approach to the energyintensive thermochemical industry for carbon utilization. Progress in this area, based on electrogeneration of multicarbon products through CO 2 electroreduction, however, lags far behind that for C 1 products. Reaction routes are complicated and kinetics are slow with scale up to the high levels required for commercialization, posing significant problems. In this review, we identify and summarize state-of-art progress in multicarbon synthesis with a multiscale perspective and discuss current hurdles to be resolved for multicarbon generation from CO 2 reduction including atomistic mechanisms, nanoscale electrocatalysts, microscale electrodes, and macroscale electrolyzers with guidelines for future research. The review ends with a cross-scale perspective that links discrepancies between different approaches with extensions to performance and stability issues that arise from extensions to an industrial environment.

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“…The huge demand for fossil fuels leads to a drastic enhancement in the atmospheric concentration of carbon dioxide (CO2), triggering serious environmental issues for sustainable development [4][5][6] . As the main component of greenhouse gases, CO2 is also an ideal economical carbon feedstock to produce value-added chemicals 3,[7][8][9][10][11][12] . However, the conversion of CO2 into liquid fuels and value-added chemicals features a great challenge because of its intrinsic properties.…”

Section: Introductionmentioning

confidence: 99%

Effects of Electron Density Variation of Active Sites in CO2 Activation and Photoreduction: A Review

Cao¹,

Guo²,

Ma³

et al. 2024

Acta Physico-Chimica Sinica

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Photocatalytic reduction of CO2 into value-added chemicals is a feasible approach to harvest solar light energy and storing energy in the form of chemical fuels as well as to mitigate the effects of global climate change and help achieve an artificial carbon cycle. However, the efficiency of CO2 photoreduction is low for commercial purposes. This is mainly due to the difficult adsorption and activation process of CO2 molecules, the unsatisfactory selectivity of target products, and the uncontrolled-subsequent reaction process of the generated carbon products. CO2 photoreduction requires substantial electrons for participation. Hence, these issues are due to the electron density modulation of the active sites of catalysts. Unfortunately, the CO2 photoreduction process involves multi-fundamental steps, which leads to different requirements in electron density modulation. The performance might not be effectively improved by directly enhancing or weakening the total electron density of active sites. In this paper, we summarize recent advances in the influence of electron density variation of the active sites in strengthening the adsorption and activation of CO2 molecules, enhancing the selectivity of target carbon products and modulating the subsequent reaction process of the generated carbon products. This review begins with the effect of different types of active sites in strengthening the adsorption and activation of the CO2 molecules and the related methods for modulating the electron density of active sites. Active sites with high electron densities can significantly enhance the adsorption and activation of CO2. Introducing metal and fabricating the defects on catalyst surfaces are effective strategies for fabricating the electron-rich active sites. After that, we discuss the influence of electron density variation in enhancing the selectivity of target carbon products in detail. In this part, the related effects in the multielectron donation from the catalyst surface, the reactive intermediates, and the competition hydrogen evolution reaction are summarized. Enhancing the electron density of active sites strengthens the former two processes. For multielectron donation, introducing cocatalysts or fabricating heterostructures are the most effective methods for enhancing the electron density of active sites. The adsorption and conversion process of intermediates are mainly affected by the accumulation sites of electrons. The active sites with low coordination are more favorable to achieving the generation of multi-electronic carbon products. In contrast, the hydrogen evolution reaction is significantly inhibited by reducing the electron density of active sites. Moreover, elemental doping is considered one of the most effective strategies. Finally, we describe the method for weakening the electron density of active sites to promote product desorption and inhibit the photooxidation of reactive products.

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Intermetallic CuAu nanoalloy for stable electrochemical CO2 reduction

Cited by 13 publications

References 35 publications

Acetamide Electrosynthesis from CO₂ and Nitrite in Water

Acetamide Electrosynthesis from CO₂ and Nitrite in Water

Multiscale CO₂ Electrocatalysis to C₂₊ Products: Reaction Mechanisms, Catalyst Design, and Device Fabrication

Effects of Electron Density Variation of Active Sites in CO2 Activation and Photoreduction: A Review

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Intermetallic CuAu nanoalloy for stable electrochemical CO2 reduction

Cited by 13 publications

References 35 publications

Acetamide Electrosynthesis from CO2 and Nitrite in Water

Acetamide Electrosynthesis from CO2 and Nitrite in Water

Multiscale CO2 Electrocatalysis to C2+ Products: Reaction Mechanisms, Catalyst Design, and Device Fabrication

Effects of Electron Density Variation of Active Sites in CO2 Activation and Photoreduction: A Review

Contact Info

Product

Resources

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Acetamide Electrosynthesis from CO₂ and Nitrite in Water

Acetamide Electrosynthesis from CO₂ and Nitrite in Water

Multiscale CO₂ Electrocatalysis to C₂₊ Products: Reaction Mechanisms, Catalyst Design, and Device Fabrication