Rational construction of efficient carbon-supported rare earth cerium nanoclusters as oxygen reduction reaction (ORR) is of great significance to promote the practical application of zinc-air batteries (ZABs). Herein, N doped conductive carbon black anchored CeO nanoclusters (CeO Clusters/NC) for the ORR is reported. The volatile cerium species vaporized by CeO nanoclusters at high temperatures are captured by nitrogen-rich carbon carriers to form highly dispersed Ce-Nx active sites. Benefiting from the coupling effect between oxygen vacancies-enriched CeO nanoclusters and highly dispersed Ce-Nx sites, the prepared 2CeO Clusters/NC catalyst possesses an ORR half-wave potential of 0.88 V, superior electrochemical stability, and better methanol tolerance compared to commercial Pt/C catalysts. Moreover, the 2CeO Clusters/NC involved liquid ZABs show excellent energy efficiency, superior stability, and a high energy density of 982 Wh kg at 10 mA cm.
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http://dx.doi.org/10.1016/j.jcis.2023.12.124 | DOI Listing |
Inorg Chem
December 2024
College of Materials Science and Engineering, Fuzhou University, Fuzhou 350108, PR China.
Angew Chem Int Ed Engl
January 2025
Department of Chemical Engineering, University of California, Santa Barbara, Santa Barbara, CA 93106-5080, United States.
Redox reactions on the surface of transition metal oxides are of broad interest in thermo, photo, and electrocatalysis. H temperature-programmed reduction (H-TPR) is commonly used to probe oxide reducibility by measuring the rate of H consumption during temperature ramps, assuming that this rate is controlled by oxide reduction. However, oxide reduction involves several elementary steps, such as H dissociation and H-spillover, before surface reduction and HO formation occur.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Department of Endocrinology, Institute of Endocrine and Metabolic Diseases, The First Affiliated Hospital of USTC, Division of Life Sciences and Medicine, University of Science and Technology of China, Hefei, 230026, China.
Regulating appropriate valence states of metal active centers, such as Ce/Ce and Mn/Mn, as well as surface vacancy defects, is crucial for enhancing the catalytic activity of cerium-based and manganese-based nanozymes. Drawing inspiration from the efficient substance exchange in rhizobia-colonized root cells of legumes, we developed a symbiosis nanozyme system with rhizobia-like CeO nanoclusters robustly anchored onto root-like MnO nanosupports (CeO/MnO). The process of "substance exchange" between Ce and Mn atoms-reminiscent of electron transfer-not only fine-tunes the metal active sites to achieve optimal Ce/Ce and Mn/Mn ratios but also enhances the vacancy ratio through interface defect engineering.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310058, P. R. China.
Strong metal-support interaction (SMSI) plays a vital role in tuning the geometric and electronic structures of metal species. Generally, a high-temperature treatment (>500 °C) in reducing atmosphere is required for constructing SMSI, which may induce the sintering of metal species. Herein, we use molten salts as the reaction media to trigger the formation of high-intensity SMSI at reduced temperatures.
View Article and Find Full Text PDFNanotechnology
September 2024
State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310032, Zhejiang, People's Republic of China.
It is a challenge to improve the long-term durability of Pd-based electrocatalysts for oxygen reduction reaction (ORR) in fuel cells. Herein, Pd/CeO-C-T (= 800 °C, 900 °C and 1000 °C) hybrid catalysts with metal-support interaction are prepared from Ce-based metal organic framework precursor. Abundant tiny CeOnanoclusters are produced to form nanorod structures with uniformly distributed carbon through a calcination process.
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