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1.
J Phys Chem Lett ; 15(35): 9122-9128, 2024 Sep 05.
Artigo em Inglês | MEDLINE | ID: mdl-39207063

RESUMO

The application of membrane electrode assembly (MEA) in electrocatalytic CO2 reduction (ECO2R) technology is an essential step toward industrialization. Nevertheless, the issue of ECO2R failure in MEA during extended operation hinders its industrial application. In this work, we employed in situ, nondestructive electrochemical impedance spectroscopy (EIS) techniques combined with distribution of relaxation times (DRT) methodology to diagnose the causes of the failure. By systematically investigating the variations in polarization resistance throughout the degradation process and utilizing a controlled variable approach to identify the origin of polarization, we diagnosed the degeneration of ionomers as the primary cause of the performance degradation of ECO2R in this instance. We further confirmed the reliability of our findings through material characterization and respraying ionomers onto the catalyst surface. This research provides an effective diagnostic method for the failure analysis of ECO2R performance in MEA, which is crucial for advancing industrialization of ECO2R technology.

2.
Small ; : e2307970, 2023 Dec 06.
Artigo em Inglês | MEDLINE | ID: mdl-38054785

RESUMO

Surface engineering offers opportunities for the design and synthesis of Pt-based alloyed electrocatalysts with high mass activity and resistance to CO poisoning, which is of great significance for methanol electrooxidation. Surface curvature regulation may endow electrocatalysts with enhanced atomic utilization and abundance of unsaturated atoms; however, a reliable synthetic route for controlled construction of tailorable curved surface is still lacking. Here, a colloidal-chemical method to synthesize two types of PtCu branched-structured electrocatalysts, where the concave curvature can be customized is reported. These studies show that, among various synthesis parameters, the concentration of CuCl2 ·2H2 O precursor is the key factor in manipulating the reaction kinetics and determining the concave surface curvature. Significantly, PtCu branched nanocrystals with long and sharp arms (PtCu BNCs-L), featuring a high concave surface curvature, exhibit remarkable activity and stability toward MOR, which is mainly attributed to advanced features of a highly concave surface and the synergistically bifunctional effect from introduced oxophilic Cu metal. In situ Raman spectroscopy and CO stripping test demonstrates weakened CO adsorption and accelerated CO removal on PtCu BNCs-L. This work highlights the importance of surface curvature, opening up an appealing route for the design and synthesis of advanced electrocatalysts with well-defined surface configurations.

3.
Chem Commun (Camb) ; 57(81): 10580-10583, 2021 Oct 12.
Artigo em Inglês | MEDLINE | ID: mdl-34558580

RESUMO

Dual-confined porous Si@c-ZIF@carbon nanofibers (Si@c-ZIF@CNFs) are fabricated that possess excellent antioxidant capacity, high surface area and abundant pores, which enhances conductivity, relieves volume expansion and facilitates electrolyte penetration during cycling. When evaluated as self-supporting anodes for lithium-ion batteries, the Si@c-ZIF@CNFs exhibit excellent cycling and rate performance.

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