Unraveling the pH-Dependent Oxygen Reduction Performance on Single-Atom Catalysts: From Single- to Dual-Sabatier Optima

M-N-C single-atom catalysts (SACs) have emerged as a potential substitute for the costly platinum-group catalysts in oxygen reduction reaction (ORR). However, several critical aspects of M-N-C SACs in ORR remain poorly understood, including their pH-dependent activity, selectivity for 2- or 4-electron transfer pathways, and the identification of the rate-determining steps. Herein, analyzing >100 M-N-C structures and >2000 sets of energetics, we unveil for the first time a pH-dependent evolution in ORR activity volcanos from a single-peak in alkaline media to a double-peak in acids. We found that this pH-dependent behavior in M-N-C catalysts fundamentally stems from their moderate dipole moments and polarizability for O* and HOO* adsorbates, as well as unique scaling relations among ORR adsorbates. To validate our theoretical discovery, we synthesized a series of molecular M-N-C catalysts, each characterized by well-defined atomic coordination environments. Impressively, the experiments matched our theoretical predictions on kinetic current, Tafel slope, and turnover frequency in both acidic and alkaline environments. These new insights also refine the famous Sabatier principle by emphasizing the need to avoid an "acid trap" while designing M-N-C catalysts for ORR or any other pH-dependent electrochemical applications.Comment: 24 pages, 5 Figure

Amorphous carbon films doped with silver and chromium to achieve ultra-low interfacial electrical resistance and long-term durability in the application of proton exchange membrane fuel cells

Amorphous carbon films doped with silver and chromium to achieve ultra-low interfacial electrical resistance and long-term durability in the application of proton exchange membrane fuel cell

Numerical Simulation of Corroded Reinforced Concrete Beam Strengthened by a Steel Plate with Different Strengthening Schemes

This paper proposes 3D nonlinear finite element (FE) models to predict the response of corroded reinforced concrete (RC) beam strengthened using a steel plate. Five FE models are developed based on the tests carried out by the authors in a previous investigation, in which three models are used to simulate the corroded RC beams with different schemes. The FE models use the coupled damaged-plasticity constitutive law for concrete in tension and compression and consider the bond-slip between the corroded tensile steel bar and concrete. The cohesive element is also used to model the cohesive bond between the steel plate and concrete. The FE results of load-deflection and the crack distribution are compared with the test data. The FE results are consistent with the test results. The influence of the thickness of the steel plate, the thickness, and location of the U-shaped steel strip on the bearing capacity of the strengthened corroded beam is analyzed through FE models. The results show that the thickness of the steel plate on the bottom surface should not exceed 4 mm for the flexure-strengthened and combined strengthened beams with a 10% corrosion rate. It is most reasonable to improve the bearing capacity using the 3 mm and 2 mm of thick U-shaped steel strips for the shear-strengthened and combined strengthened beams, respectively. The most reasonable location of the U-shaped steel plate is at the end of the steel plate for beams with a 10% corrosion rate

Flow channel design for metallic bipolar plates in proton exchange membrane fuel cells: Experiments

This study offers an efficient design method of flow channels of metallic bipolar plates (BPPs) to improve manufacturing technique of BPPs and maximize power density in proton exchange membrane (PEM) fuel cells. Stamped thin metallic BPPs with anticorrosive and conductive coating are promising candidates for replacing conventional carbon-based BPPs. Nevertheless, unlike carbon-based BPPs, the flow channel design of metallic BPPs should take into account not only the reaction efficiency, but also formability due to the possible rupture of the metallic channel during the micro-forming process. In our previous study, a forming limit model was first proposed to predict the maximum allowable channel height by the forming process. This study is conducted to further propose the method of the design and fabrication of metallic BPPs based on the numerical model. In order to determine channel geometry design from formability perspective, response surface method is utilized to build a formability model. Combining the formability model and reaction efficiency, flow field design for metallic BPPs (channel width of 0.9 mm, rib width of 0.9 mm, channel depth of 0.4 mm and radius of 0.15 mm) is proposed. Experiments on BPP fabrication and assembled 20-cell fuel cell testing are conducted to observe forming quality of micro channel and output performance on the real fuel cell. It is shown that the stamping force grows with increasing channel depth in a nonlinear manner and a blank holder is needed to eliminate the sheet wrinkle in the forming process. The uniformity of the voltage distribution in the 1000 W-class stack further proves the reliability of metallic BPPs designed by our method. The methodology developed is beneficial to the fabrication management of metallic BPPs and effective supplement to the channel design principle for PEM fuel cells