The two-dimensional lamellar materials disperse platinum sites and minimize noble-metal usage for fuel cells, while mass transport resistance at the stacked layers spurs device failure with a significant performance decline in membrane electrode assembly (MEA). Herein, we implant porous and rigid sulfonated covalent organic frameworks (COF) into the graphene-based catalytic layer for the construction of steric mass-charge channels, which highly facilitates the activity of oxygen reduction reactions in both the rotating disk electrode (RDE) measurements and MEA device tests. Specifically, the normalized mass activity is remarkably boosted by 3.7 times to 1.56 A mgpt-1 after additions of suitable COF modifications in the RDE tests. Especially, an excellent maximum power density of 1.015 W cm-2 is realized on the MEA in H2/Air condition, representing a 22% improvement through such constructions of steric mass-charge channels. Meanwhile, the open-circuit voltage of fuel cells demonstrates only 0.8% reductions after 10,000 cycles of stability tests. We further extended such methodology of constructing mass-charge channels to granular PtCo and commercial Pt/C catalysts, which demonstrates a significant impetus for stimulating the catalytic activity in fuel cells.
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http://dx.doi.org/10.1002/anie.202424179 | DOI Listing |
Angew Chem Int Ed Engl
January 2025
Central South University, chemistry, CHINA.
The two-dimensional lamellar materials disperse platinum sites and minimize noble-metal usage for fuel cells, while mass transport resistance at the stacked layers spurs device failure with a significant performance decline in membrane electrode assembly (MEA). Herein, we implant porous and rigid sulfonated covalent organic frameworks (COF) into the graphene-based catalytic layer for the construction of steric mass-charge channels, which highly facilitates the activity of oxygen reduction reactions in both the rotating disk electrode (RDE) measurements and MEA device tests. Specifically, the normalized mass activity is remarkably boosted by 3.
View Article and Find Full Text PDFAdv Sci (Weinh)
October 2024
Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong, SAR, 999077, P. R. China.
Designing high-entropy oxyhydroxides (HEOs) electrocatalysts with controlled nanostructures is vital for efficient and stable water-splitting electrocatalysts. Herein, a novel HEOs material (FeCoNiWCuOOH@Cu) containing five non-noble metal elements derived by electrodeposition on a 3D double-continuous porous Cu support is created. This support, prepared via the liquid metal dealloying method, offers a high specific surface area and rapid mass/charge transfer channels.
View Article and Find Full Text PDFAdv Mater
June 2024
Department of Biomedical Engineering, Technion-IIT, Haifa, 3200003, Israel.
Emerging single-molecule protein sensing techniques are ushering in a transformative era in biomedical research. Nevertheless, challenges persist in realizing ultra-fast full-length protein sensing, including loss of molecular integrity due to protein fragmentation, biases introduced by antibodies affinity, identification of proteoforms, and low throughputs. Here, a single-molecule method for parallel protein separation and tracking is introduced, yielding multi-dimensional molecular properties used for their identification.
View Article and Find Full Text PDFiScience
February 2024
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
MXenes are promising materials for electrocatalysis due to their excellent metallic conductivity, hydrophilicity, high specific surface area, and excellent electrochemical properties. Herein, we summarize the recent advancement of MXene-based materials for electrocatalysis and highlight their key challenges and opportunities. In particular, this review emphasizes on the major design principles of MXene-based electrocatalysts, including (1) coupling MXene with active materials or heteroatomic doping to create highly active synergistic catalyst sites; (2) construction of 3D MXene structure or introducing interlayer spacers to increase active areas and form fast mass-charge transfer channel; and (3) protecting edge of MXene or transforming the surface of MXene to stable active substance that inhibits the oxidation of MXene and then enhances the stability.
View Article and Find Full Text PDFAdv Mater
January 2024
Tsinghua-Berkeley Shenzhen Institute & Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen, 518055, P. R. China.
The localized reaction heterogeneity of the sulfur cathode and the uneven Li deposition on the Li anode are intractable issues for lithium-sulfur (Li-S) batteries under practical operation. Despite impressive progress in separately optimizing the sulfur cathode or Li anode, a comprehensive understanding of the highly coupled relationship between the cathode and anode is still lacking. In this work, inspired by the Butler-Volmer equation, a binary descriptor (I ) assisting the rational structural design of sulfur cathode by simultaneously considering the mass-transport index (I ) and the charge-transfer index (I ) is identified, and subsequently the relationship between I and the morphological evolution of Li anode is established.
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