Characterizing CO 2 Reduction Catalysts on Gas Diffusion Electrodes: Comparing Activity, Selectivity, and Stability of Transition Metal Catalysts.
Mark SassenburgReinier de RooijNathan T NesbittRecep KasSanjana ChandrashekarNienke J FiretKailun YangKai LiuMarijn A BlommaertMartin KolenDavide RipepiWilson A SmithEdward H SargentPublished in: ACS applied energy materials (2022)
Continued advancements in the electrochemical reduction of CO 2 (CO 2 RR) have emphasized that reactivity, selectivity, and stability are not explicit material properties but combined effects of the catalyst, double-layer, reaction environment, and system configuration. These realizations have steadily built upon the foundational work performed for a broad array of transition metals performed at 5 mA cm -2 , which historically guided the research field. To encompass the changing advancements and mindset within the research field, an updated baseline at elevated current densities could then be of value. Here we seek to re-characterize the activity, selectivity, and stability of the five most utilized transition metal catalysts for CO 2 RR (Ag, Au, Pd, Sn, and Cu) at elevated reaction rates through electrochemical operation, physical characterization, and varied operating parameters to provide a renewed resource and point of comparison. As a basis, we have employed a common cell architecture, highly controlled catalyst layer morphologies and thicknesses, and fixed current densities. Through a dataset of 88 separate experiments, we provide comparisons between CO-producing catalysts (Ag, Au, and Pd), highlighting CO-limiting current densities on Au and Pd at 72 and 50 mA cm -2 , respectively. We further show the instability of Sn in highly alkaline environments, and the convergence of product selectivity at elevated current densities for a Cu catalyst in neutral and alkaline media. Lastly, we reflect upon the use and limits of reaction rates as a baseline metric by comparing catalytic selectivity at 10 versus 200 mA cm -2 . We hope the collective work provides a resource for researchers setting up CO 2 RR experiments for the first time.
Keyphrases
- transition metal
- highly efficient
- reduced graphene oxide
- visible light
- gold nanoparticles
- metal organic framework
- ionic liquid
- room temperature
- sensitive detection
- carbon dioxide
- structural basis
- mental health
- quantum dots
- electron transfer
- cell therapy
- high throughput
- molecularly imprinted
- high resolution
- mesenchymal stem cells
- bone marrow
- anaerobic digestion
- human health
- crystal structure
- drinking water
- solid state