Visualization of CO2 electrolysis using optical coherence tomography.

Electrolysers offer an appealing technology for conversion of CO2 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 CO2 electrolyser. This platform was designed to capture three-dimensional images and videos at high spatial and temporal resolutions. We recorded 12 h of footage of an electrolyser containing a porous electrode separated by a membrane, converting a continuous feed of liquid KHCO3 to reduce CO2 into CO at applied current densities of 50-800 mA cm-2. This platform visualized reactants, intermediates and products, and captured the strikingly dynamic movement of the cathode and membrane components during electrolysis. It also linked CO production to regions of the electrolyser in which CO2 was in direct contact with both membrane and catalyst layers. These results highlight how this platform can be used to track reactions in continuous flow electrochemical reactors.

High-Efficiency Perovskite Solar Cells with Sputtered Metal Contacts.

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. We support this claim by making PSCs sputtered with Au contacts that exhibit higher efficiencies (18.7%) and stabilities than those made with thermally evaporated Au contacts (18.4%). We performed a series of experiments that show that the post-sputtering oxidation step reconstructs the molecular order of the hole transport layer (HTL) and reverses Au atom diffusion into the HTL. This potential restoration was previously neglected in PSC fabrication recipes because metal contact deposition is generally performed after the HTL oxidation. This result is important for scaling PSCs because sputtering is a superior method for manufacturing optimal-quality coatings or large-area devices.

Electrolysis Can Be Used to Resolve Hydrogenation Pathways at Palladium Surfaces in a Membrane Reactor.

For common hydrogenation chemistries that occur at high temperatures (where H2 is adsorbed and activated at the same surface which the substrate must also adsorb for reaction), there is often little consensus on how the reactions (e.g., hydro(deoxy)genation) actually occur. We demonstrate here that an electrocatalytic palladium membrane reactor (ePMR) can be used to study hydrogenation reaction mechanisms at ambient temperatures, where the catalyst does not necessarily undergo structural reorganization. The ePMR uses electrolysis and a hydrogen-selective palladium membrane to deliver reactive hydrogen to a catalyst surface in an adjacent compartment for reaction with an organic substrate. This process forms the requisite metal-hydride surface for hydrogenation chemistry, but at ambient temperature and pressure, and without a H2 source. We demonstrate the utility of this analytical tool by studying the hydrogenation of benzaldehyde at palladium nanocubes with dimensions of 13-24 nm. This experimental design enabled us to resolve that the alcohol product forms at the facial sites, whereas the hydrodeoxygenation step occurs at edge sites. These observations enabled us to develop the first site-specific definition of how a carbonyl species undergoes hydro(deoxy)genation.