Potential‐Dependent Morphology of Copper Catalysts During CO₂ Electroreduction Revealed by In Situ Atomic Force Microscopy

Angewandte Chemie International Edition, Год журнала: 2020, Номер 60(5), С. 2561 - 2568

Опубликована: Окт. 9, 2020

Electrochemical AFM is a powerful tool for the real-space characterization of catalysts under realistic electrochemical CO2 reduction (CO2 RR) conditions. The evolution structural features ranging from micrometer to atomic scale could be resolved during RR. Using Cu(100) as model surface, distinct nanoscale surface morphologies and their potential-dependent transformations granular smoothly curved mound-pit surfaces or structures with rectangular terraces are revealed RR in 0.1 m KHCO3 . density undercoordinated copper sites shown increase decreasing potential. In situ atomic-scale imaging reveals specific adsorption occurring at cathodic potentials impacting observed catalyst structure. These results show complex interrelation morphology, structure, defect density, applied potential, electrolyte catalysts.

Язык: Английский

---

Carbon-Based Materials for Electrochemical Reduction of CO₂ to C₂₊ Oxygenates: Recent Progress and Remaining Challenges

ACS Catalysis, Год журнала: 2021, Номер 11(4), С. 2076 - 2097

Опубликована: Фев. 2, 2021

Electrochemical reduction of CO2 to multicarbon (C2+) products is desirable because the higher energy density and economic value C2+ significant scientific issue for coupling multicarbons. However, efficient conversion into remains challenging difficulty in C–C coupling. Recently, numerous papers have reported carbon-based materials production from electrochemical reduction. Because unique properties production, can be used as a potential alternative electrocatalytic CO2. This Review summarized recent progresses formation oxygenates on materials. In this Review, we highlighted strategies available achieving electrocatalysts revealed relationships between intermediate adsorption selectivity oxygenate Moreover, provided understandings fabricating active sites related mechanisms generation. The remaining challenges opportunities were discussed.

Язык: Английский

---

Photocatalytic and electrocatalytic transformations of C1 molecules involving C–C coupling

Energy & Environmental Science, Год журнала: 2020, Номер 14(1), С. 37 - 89

Опубликована: Окт. 31, 2020

Selective transformation of one-carbon (C1) molecules, which are abundant or easily available and inexpensive carbon feedstocks, into value-added multi-carbon (C2+) compounds is a very attractive but highly challenging research target. Photocatalysis electrocatalysis have offered great opportunities for the activation controllable C–C coupling C1 molecules under mild environmentally benign conditions. This article provides critical review on recent advances in photocatalytic electrocatalytic conversions major including CO, CO2, CH4, CH3OH HCHO, C2+ compounds, such as C2H4, C3H6, ethanol ethylene glycol, play essential roles current chemical energy industry. Besides photocatalysts electrocatalysts reported these conversions, structure–performance relationships key factors that control activity product selectivity analysed to provide insights rational design more efficient catalysts synthesis from feedstocks. The active species, reaction intermediates catalyst-functioning mechanism discussed deepen understanding chemistry selective presence solar electrical energy.

Язык: Английский

---

p–d Orbital Hybridization Induced by p-Block Metal-Doped Cu Promotes the Formation of C₂₊ Products in Ampere-Level CO₂ Electroreduction

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(8), С. 4675 - 4682

Опубликована: Фев. 17, 2023

Large-current electrolysis of CO2 to multi-carbon (C2+) products is critical realize the industrial application conversion. However, poor binding strength *CO intermediates on catalyst surface induces multiple competing pathways, which hinder C2+ production. Herein, we report that p-d orbital hybridization induced by Ga-doped Cu (CuGa) could promote efficient electrocatalysis at ampere-level current density. It was found CuGa exhibited highest productivity with a remarkable Faradaic efficiency (FE) 81.5% density 0.9 A/cm2, and potential such high -1.07 V versus reversible hydrogen electrode. At 1.1 still maintained an FE 76.9%. Experimental theoretical studies indicated excellent performance results from Ga, not only enriches reactive sites but also enhances intermediate facilitates C-C coupling. The strategy can be extended other p-block metal-doped catalysts, as CuAl CuGe, boost electroreduction for As far know, this first work electrochemical reduction reaction generate product interaction using catalyst.

Язык: Английский

---

Towards artificial photosynthesis: Sustainable hydrogen utilization for photocatalytic reduction of CO2 to high-value renewable fuels

Chemical Engineering Journal, Год журнала: 2020, Номер 402, С. 126184 - 126184

Опубликована: Июль 8, 2020

Язык: Английский

---