For the large-scale sustainable implementation of polymer electrolyte membrane fuel cells in vehicles, high-performance electrocatalysts with low platinum consumption are desirable for use as cathode material during the oxygen reduction reaction in fuel cells. Here we report a carbon black-supported cost-effective, efficient and durable platinum single-atom electrocatalyst with carbon monoxide/methanol tolerance for the cathodic oxygen reduction reaction. The acidic single-cell with such a catalyst as cathode delivers high performance, with power density up to 680 mW cm−2 at 80 °C with a low platinum loading of 0.09 mgPt cm−2, corresponding to a platinum utilization of 0.13 gPt kW−1 in the fuel cell. Good fuel cell durability is also observed. Theoretical calculations reveal that the main effective sites on such platinum single-atom electrocatalysts are single-pyridinic-nitrogen-atom-anchored single-platinum-atom centres, which are tolerant to carbon monoxide/methanol, but highly active for the oxygen reduction reaction.
Multi-elemental alloy nanoparticles (MEA-NPs) hold great promise for catalyst discovery in a virtually unlimited compositional space. However, rational and controllable synthesize of these intrinsically complex structures remains a challenge. Here, we report the computationally aided, entropy-driven design and synthesis of highly efficient and durable catalyst MEA-NPs. The computational strategy includes prescreening of millions of compositions, prediction of alloy formation by density functional theory calculations, and examination of structural stability by a hybrid Monte Carlo and molecular dynamics method. Selected compositions can be efficiently and rapidly synthesized at high temperature (e.g., 1500 K, 0.5 s) with excellent thermal stability. We applied these MEA-NPs for catalytic NH 3 decomposition and observed outstanding performance due to the synergistic effect of multielemental mixing, their small size, and the alloy phase. We anticipate that the computationally aided rational design and rapid synthesis of MEA-NPs are broadly applicable for various catalytic reactions and will accelerate material discovery. Computationally aided, entropy-driven synthesis of highly efficient and durable multi-elemental alloy catalysts.(11), eaaz0510. 6 Sci Adv ARTICLE TOOLS
Maximizing the platinum utilization in electrocatalysts toward oxygen reduction reaction (ORR) is very desirable for large‐scale sustainable application of Pt in energy systems. A cost‐effective carbon‐supported carbon‐defect‐anchored platinum single‐atom electrocatalysts (Pt1/C) with remarkable ORR performance is reported. An acidic H2/O2 single cell with Pt1/C as cathode delivers a maximum power density of 520 mW cm−2 at 80 °C, corresponding to a superhigh platinum utilization of 0.09 gPt kW−1. Further physical characterization and density functional theory computations reveal that single Pt atoms anchored stably by four carbon atoms in carbon divacancies (Pt‐C4) are the main active centers for the observed high ORR performance.
Plastic waste has been increasingly transferred from land into the ocean and has accumulated within the food chain, causing a great threat to the environment and human health, indicating that fabricating an eco‐friendly and biodegradable replacement is urgent. Paper made of cellulose is attractive in terms of its favorable biodegradability, resource abundance, large manufacturing scale, and low material cost, but is usually hindered by its inferior stability against water and poor mechanical strength for plastic replacement. Here, inspired by the reinforcement principle of cellulose and lignin in natural wood, a strong and hydrostable cellulosic material is developed by integrating lignin into the cellulose. Lignin as a reinforced matrix is incorporated to the cellulose fiber scaffold by successive infiltration and mechanical hot‐pressing treatments. The resulting lignin‐cellulose composite exhibits an outstanding isotropic tensile strength of 200 MPa, which is significantly higher than that of conventional cellulose paper (40 MPa) and some commercial petroleum‐based plastics. Additionally, the composite demonstrates a superior wet strength of 50 MPa. Adding lignin also improves the thermostability and UV‐blocking performance of cellulose paper. The demonstrated lignin‐cellulose composite is biodegradable and eco‐friendly with both components from natural wood, which represents a promising alternative that can potentially replace the nonbiodegradable plastics.
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