Electrolysers offer an appealing technology for conversion of CO into high-value chemicals. However, there are few tools available to track the reactions that occur within electrolysers. Here we report an electrolysis optical coherence tomography platform to visualize the chemical reactions occurring in a CO electrolyser.
View Article and Find Full Text PDFHere, we detail how the catalytic behavior of immobilized molecular electrocatalysts for the CO reduction reaction (CORR) can be impacted by catalyst aggregation. Raman spectroscopy was used to study the CORR mediated by a layer of cobalt phthalocyanine (CoPc) immobilized on the cathode of an electrochemical flow reactor. We demonstrate that during electrolysis, the oxidation state of CoPc in the catalyst layer is dependent upon the degree of catalyst aggregation.
View Article and Find Full Text PDFACS Appl Mater Interfaces
November 2022
Sputter deposition produces dense, uniform, adhesive, and scalable metal contacts for perovskite solar cells (PSCs). However, sputter deposition damages the other layers of the PSC. We here report that the damage caused by sputtering metal contacts can be reversed by aerial oxidation.
View Article and Find Full Text PDFElectrolyzers are now capable of reducing carbon dioxide (CO) into products at high reaction rates but are often characterized by low energy efficiencies and low CO utilization efficiencies. We report here an electrolyzer that reduces 3.0 M KHCO(aq) into CO(g) at a high rate (partial current density for CO of 220 mA cm) and a CO utilization efficiency of 40%, at a voltage of merely 2.
View Article and Find Full Text PDFElectrochemical conversion of CO to useful products at temperatures below 100 °C is nearing the commercial scale. Pilot units for CO conversion to CO are already being tested. Units to convert CO to formic acid are projected to reach pilot scale in the next year.
View Article and Find Full Text PDFMolecular catalysts that combine high product selectivity and high current density for CO electrochemical reduction to CO or other chemical feedstocks are urgently needed. While earth-abundant metal-based molecular electrocatalysts with high selectivity for CO to CO conversion are known, they are characterized by current densities that are significantly lower than those obtained with solid-state metal materials. Here, we report that a cobalt phthalocyanine bearing a trimethyl ammonium group appended to the phthalocyanine macrocycle is capable of reducing CO to CO in water with high activity over a broad pH range from 4 to 14.
View Article and Find Full Text PDFPractical electrochemical carbon dioxide (CO) conversion requires a catalyst capable of mediating the efficient formation of a single product with high selectivity at high current densities. Solid-state electrocatalysts achieve the CO reduction reaction (CORR) at current densities ≥ 150 milliamperes per square centimeter (mA/cm), but maintaining high selectivities at high current densities and efficiencies remains a challenge. Molecular CORR catalysts can be designed to achieve high selectivities and low overpotentials but only at current densities irrelevant to commercial operation.
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