Solvent-free mechanochemical synthesis of efficient and low-cost double perovskite (DP), like a cage of Prussian blue (PB) and PB analogs (PBAs), is a promising approach for different applications such as chemical sensing, energy storage, and conversion. Although the solvent-free mechanochemical grinding approach has been extensively used to create halide-based perovskites, no such reports have been made for cyanide-based double perovskites. Herein, an innovative solvent-free mechanochemical synthetic strategy is demonstrated for synthesizing Fe[Fe(CN)], Co[Fe(CN)], and Ni[Fe(CN)], where defect sites such as carbon-nitrogen vacancies are inherently introduced during the synthesis. Among all the synthesized PB analogs, the Ni analog manifests a considerable electrocatalytic oxygen evolution reaction (OER) with a low overpotential of 288 mV to obtain the current benchmark density of 20 mA cm. We hypothesize that incorporating defects, such as carbon-nitrogen vacancies, and synergistic effects contribute to high catalytic activity. Our findings pave the way for an easy and inexpensive large-scale production of earth-abundant non-toxic electrocatalysts with vacancy-mediated defects for oxygen evolution reaction.
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http://dx.doi.org/10.3390/nano13172459 | DOI Listing |
ACS Nano
January 2025
School of Science and Engineering, The Chinese University of Hong Kong, Shenzhen 518000, China.
Electrochemical nitrate reduction (NORR) to ammonia presents a promising alternative strategy to the traditional Haber-Bosch process. However, the competitive hydrogen evolution reaction (HER) reduces the Faradaic efficiency toward ammonia, while the oxygen evolution reaction (OER) increases the energy consumption. This study designs IrCu alloy nanoparticles as a bifunctional catalyst to achieve efficient NORR and OER while suppressing the unwanted HER.
View Article and Find Full Text PDFNat Commun
January 2025
WA School of Mines: Minerals, Energy and Chemical Engineering (WASM-MECE), Curtin University, Perth, WA, 6102, Australia.
Reducing green hydrogen production cost is critical for its widespread application. Proton-exchange-membrane water electrolyzers are among the most promising technologies, and significant research has been focused on developing more active, durable, and cost-effective catalysts to replace expensive iridium in the anode. Ruthenium oxide is a leading alternative while its stability is inadequate.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Anhui Normal University, School of Chemistry and Materials Science, CHINA.
The space charge effect induced by high-quality heterojunctions is essential for efficient electrocatalytic processes. Herein, we delicately manipulate intermolecular charge transfer by modifying substituents (-g = -CH3, -H, -NO2) with various electron donating/withdrawing capabilities in CoPc-g/CoS organic-inorganic heterostructures. CoPc-CH3, as a typical electron donor, transfers more electrons to CoS due to the presence of -CH3, forming the strongest space electric field and thus regulating the dual active sites at the interface.
View Article and Find Full Text PDFACS Nano
January 2025
Key Laboratory for Liquid-Solid Structural Evolution and Processing of Materials, Ministry of Education, School of Materials Science and Engineering, Shandong University, Jinan 250061, P. R. China.
To achieve a long cycle life and high-capacity performance for Li-O batteries, it is critical to rationally modulate the formation and decomposition pathway of the discharge product LiO. Herein, we designed a highly efficient catalyst containing dual catalytic active sites of Pt single atoms (Pt) paired with high-entropy alloy (HEA) nanoparticles for oxygen reduction reaction (ORR) in Li-O batteries. HEA is designed with a moderate d-band center to enhance the surface adsorbed LiO intermediate (LiO(ads)), while Pt active sites exhibit weak adsorption energy and promote the soluble LiO pathway (LiO(sol)).
View Article and Find Full Text PDFJ Colloid Interface Sci
January 2025
State Key Laboratory of Chem/Bio-Sensing and Chemometrics, Advanced Catalytic Engineering Research Center of the Ministry of Education, College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082 PR China. Electronic address:
High-entropy phosphides (HEPs) have garnered increasing interest as innovative electrocatalysts for water splitting, highlighted by their distinctive catalytic activity, elemental synergy, and tunable electronic configuration. Herein, a novel electrode comprising CoNiCuZnFeP nanocubes with rich phosphorus vacancies was fabricated through coprecipitation and phosphorization two-step method. The synergistic interaction among metal elements and the modulation of the electronic configuration by phosphorus vacancies augmentation enhance the catalytic performance for both the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER).
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