Nitrogen-doped Carbon-CoOx Nanohybrids: A Precious Metal Free Cathode that Exceeds 1.0†W cm-2 Peak Power and 100†h Life in Anion-Exchange Membrane Fuel Cells.

Efficient and durable nonprecious metal electrocatalysts for the oxygen reduction (ORR) are highly desirable for several electrochemical devices, including anion exchange membrane fuel cells (AEMFCs). Here, a 2D planar electrocatalyst with CoOx embedded in nitrogen-doped graphitic carbon (N-C-CoOx ) was created through the direct pyrolysis of a metal-organic complex with a NaCl template. The N-C-CoOx catalyst showed high ORR activity, indicated by excellent half-wave (0.84 V vs. RHE) and onset (1.01 V vs. RHE) potentials. This high intrinsic activity was also observed in operating AEMFCs where the kinetic current was 100 mA cm-2 at 0.85 V. When paired with a radiation-grafted ETFE powder ionomer, the N-C-CoOx AEMFC cathode was able to achieve extremely high peak power density (1.05 W cm-2 ) and mass transport limited current (3 A cm-2 ) for a precious metal free electrode. The N-C-CoOx cathode also showed good stability over 100 hours of operation with a voltage decay of only 15 % at 600 mA cm-2 under H2 /air (CO2 -free) reacting gas feeds. The N-C-CoOx cathode catalyst was also paired with a very low loading PtRu/C anode catalyst, to create AEMFCs with a total PGM loading of only 0.10 mgPt-Ru cm-2 capable of achieving 7.4 W mg-1 PGM as well as supporting a current of 0.7 A cm-2 at 0.6 V with H2 /air (CO2 free)-creating a cell that was able to meet the 2019 U.S. Department of Energy initial performance target of 0.6 V at 0.6 A cm-2 under H2 /air with a PGM loading <0.125 mg cm-2 with AEMFCs for the first time.

Using operando techniques to understand and design high performance and stable alkaline membrane fuel cells.

There is a need to understand the water dynamics of alkaline membrane fuel cells under various operating conditions to create electrodes that enable high performance and stable, long-term operation. Here we show, via operando neutron imaging and operando micro X-ray computed tomography, visualizations of the spatial and temporal distribution of liquid water in operating cells. We provide direct evidence for liquid water accumulation at the anode, which causes severe ionomer swelling and performance loss, as well as cell dryout from undesirably low water content in the cathode. We observe that the operating conditions leading to the highest power density during polarization are not generally the conditions that allow for long-term stable operation. This observation leads to new catalyst layer designs and gas diffusion layers. This study reports alkaline membrane fuel cells that can be operated continuously for over 1000 h at 600 mA cm-2 with voltage decay rate of only 32-µV h-1 - the best-reported durability to date.