Developing efficient catalysts to accelerate the rate of oxygen evolution reaction (OER) is critical for photocatalytic water-splitting. In this work, metallic Ir, IrO(OH), and core-shell Ir@IrO(OH) were synthesized and employed as OER catalysts for photocatalytic water oxidation. It was found that the Ir@IrO(OH) core-shell heterostructure catalyst showed the best photocatalytic performance among these three catalysts, with the oxygen evolution rate as high as 59.63 mmol g h. Detailed investigations revealed that the excellent photocatalytic activity of Ir@IrO(OH) could be attributed to both the outstanding intrinsic activity of IrO(OH) shell and the efficient electron transfer between the photosensitizer and catalyst.
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http://dx.doi.org/10.1088/1361-6528/aad3f4 | DOI Listing |
Chem Sci
January 2025
Interdisciplinary Research Center for Sustainable Energy Science and Engineering (IRC4SE2), School of Chemical Engineering, Zhengzhou University Henan 450001 China
The exceptional oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) performances of core-shell catalysts are well documented, yet their activity and durability origins have been interpreted only based on the static structures. Herein we employ a NiFe alloy coated with a nitrogen-doped graphene-based carbon shell (NiFe@NC) as a model system to elucidate the active structure and stability mechanism for the ORR and OER by combining constant potential computations, molecular dynamic simulations, and experiments. The results reveal that the synergistic effects between the alloy core and carbon shell facilitate the formation of Fe-N-C active sites and replenish metal sites when central metal atoms detach.
View Article and Find Full Text PDFFerroelectric polarization is considered to be an effective strategy to improve the oxygen evolution reaction (OER) of photoelectrocatalysis. The primary challenge is to clarify how the polarization field controls the OER dynamic pathway at a molecular level. Here, electrochemical fingerprint tests were used, together with theoretical calculations, to systematically investigate the free energy change in oxo and hydroxyl intermediates on TiO-BaTiO core-shell nanowires (BTO@TiO) upon polarization in different pH environments.
View Article and Find Full Text PDFChem Commun (Camb)
January 2025
Key Laboratory for Ultrafine Materials of Ministry of Education, School of Materials Science and Engineering, East China University of Science and Technology, Shanghai 200237, China.
In this study, we present a novel approach to achieve the template-free fabrication of nanocage-shaped SrTiO (N-STO) single crystals molten salt flux treatment. Systematic characterizations demonstrate the high crystallinity and low defect density of N-STO. The N-STO single crystals enable overall water splitting (OWS) with hydrogen and oxygen evolution rates of 100.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
East China University of Science and Technology, School of Chemical Engineering, CHINA.
The development of efficient and durable oxygen evolution reaction (OER) catalysts is crucial for advancing proton exchange membrane water electrolysis (PEMWE) technology, especially in the pursuit of non-iridium alternatives. Herein, we report a Zn, W co-doping Ru3Zn0.85W0.
View Article and Find Full Text PDFPhys Chem Chem Phys
September 2020
State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing 102249, P. R. China.
The lower limit of overpotential derived from the scaling relationship in the generally proposed adsorbate evolution mechanism (AEM) greatly hinders the oxygen evolution reaction (OER) activity in electrochemical energy conversion. The lattice oxygen mechanism tends to be triggered on oxygen-enriched surfaces under conditions; however, the required specific geometry and electronic structure need in-depth exploration. Here, tunable CoO is used as a model material, where the reconstruction of dominantly exposed (110) surface under reaction conditions is first presented using an thermodynamic approach.
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