ORCID Profile
0000-0002-9279-3815
Current Organisations
Delft University of Technology
,
Massachusetts Institute of Technology
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Publisher: American Chemical Society (ACS)
Date: 17-06-2022
Publisher: Springer Science and Business Media LLC
Date: 14-09-2022
DOI: 10.1038/S41467-022-33145-8
Abstract: Integrating carbon dioxide (CO 2 ) electrolysis with CO 2 capture provides exciting new opportunities for energy reductions by simultaneously removing the energy-demanding regeneration step in CO 2 capture and avoiding critical issues faced by CO 2 gas-fed electrolysers. However, understanding the potential energy advantages of an integrated process is not straightforward due to the interconnected processes which require knowledge of both capture and electrochemical conversion processes. Here, we identify the upper limits of the integrated process from an energy perspective by comparing the working principles and performance of integrated and sequential approaches. Our high-level energy analyses unveil that an integrated electrolyser must show similar performance to the gas-fed electrolyser to ensure an energy benefit of up to 44% versus the sequential route. However, such energy benefits diminish if future gas-fed electrolysers resolve the CO 2 utilisation issue and if an integrated electrolyser shows lower conversion efficiencies than the gas-fed system.
Publisher: Wiley
Date: 09-04-2023
Abstract: The electrochemical CO 2 reduction reaction (CO 2 RR) is an attractive method to produce renewable fuel and chemical feedstock using clean energy sources. Formate production represents one of the most economical target products from CO 2 RR but is primarily produced using post‐transition metal catalysts that require comparatively high overpotentials. Here a composition of bimetallic Cu–Pd is formulated on 2D Ti 3 C 2 T x (MXene) nanosheets that are lyophilized into a highly porous 3D aerogel, resulting in formate production much more efficient than post‐transition metals. Using a membrane electrode assembly (MEA), formate selectivities % are achieved with a current density of 150 mA cm −2 resulting in the highest ever reported overall energy efficiency of 47% (cell potentials of −2.8 V), over 5 h of operation. A comparable Cu‐Pd aerogel achieves near‐unity CO production without the MXene templating. This simple strategy represents an important step toward the experimental demonstration of 3D‐MXenes‐based electrocatalysts for CO 2 RR application and opens a new platform for the fabrication of macroscale aerogel MXene‐based electrocatalysts.
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2NR03310K
Abstract: This review paper provides an overview of the fundamental and applied aspects of advancing carbon dioxide electrolysis for the integrated amine-based CO 2 capture and conversion.
Publisher: Wiley
Date: 03-02-2023
Abstract: The electrochemical reduction of carbon dioxide (CO 2 ) to value‐added chemicals is a promising strategy to mitigate climate change. Metalloporphyrins have been used as a promising class of stable and tunable catalysts for the electrochemical reduction reaction of CO 2 (CO 2 RR) but have been primarily restricted to single‐carbon reduction products. Here, we utilize functionalized earth‐abundant manganese tetraphenylporphyrin‐based (Mn‐TPP) molecular electrocatalysts that have been immobilized via electrografting onto a glassy carbon electrode (GCE) to convert CO 2 with overall 94 % Faradaic efficiencies, with 62 % being converted to acetate. Tuning of Mn‐TPP with electron‐withdrawing sulfonate groups (Mn‐TPPS) introduced mechanistic changes arising from the electrostatic interaction between the sulfonate groups and water molecules, resulting in better surface coverage, which facilitated higher conversion rates than the non‐functionalized Mn‐TPP. For Mn‐TPP only carbon monoxide and formate were detected as CO 2 reduction products. Density‐functional theory (DFT) calculations confirm that the additional sulfonate groups could alter the C−C coupling pathway from *CO→*COH→*COH‐CO to *CO→*CO‐CO→*COH‐CO, reducing the free energy barrier of C−C coupling in the case of Mn‐TPPS. This opens a new approach to designing metalloporphyrin catalysts for two carbon products in CO 2 RR.
Publisher: Research Square Platform LLC
Date: 25-01-2022
DOI: 10.21203/RS.3.RS-1274022/V1
Abstract: The electrochemical reduction of carbon dioxide (CO2) to value-added materials has received considerable attention. Both bulk transition metal catalysts, and molecular catalysts affixed to conductive non-catalytic solid supports, represents a promising approach towards electroreduction of CO2. Here, we report a combined silver (Ag) and pyridine catalyst through a green and irreversible electrografting process, which demonstrates enhanced CO2 conversion versus the in idual counterparts. We find by tailoring the pyridine carbon chain length, a 200 mV shift in the onset potential is obtainable compared to the bare silver electrode. A 10-fold activity enhancement at -0.7 V vs RHE is then observed with demonstratable higher partial current densities for CO indicating a co-catalytic effect is attainable through the integration of the two different catalytic structures. We extended performance to a flow cell operating at 150 mA/cm2, demonstrating the approach’s potential for substantial adaption with various transition metals as supports, and electrografted molecular co-catalysts.
Publisher: American Chemical Society (ACS)
Date: 28-11-2022
Location: United States of America
No related grants have been discovered for Maryam Abdinejad.