ORCID Profile
0000-0003-4650-5226
Current Organisation
Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences
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Publisher: American Association for the Advancement of Science (AAAS)
Date: 10-12-2021
Abstract: Manipulating perovskite surface reconstruction offers a new path for developing advanced water oxidation catalysts.
Publisher: American Chemical Society (ACS)
Date: 08-06-2018
Publisher: Springer Science and Business Media LLC
Date: 20-09-2022
DOI: 10.1038/S41467-022-33000-W
Abstract: Developing efficient catalysts is of paramount importance to oxygen evolution, a sluggish anodic reaction that provides essential electrons and protons for various electrochemical processes, such as hydrogen generation. Here, we report that the oxygen evolution reaction (OER) can be efficiently catalyzed by cobalt tetrahedra, which are stabilized over the surface of a Swedenborgite-type YBCo 4 O 7 material. We reveal that the surface of YBaCo 4 O 7 possesses strong resilience towards structural amorphization during OER, which originates from its distinctive structural evolution toward electrochemical oxidation. The bulk of YBaCo 4 O 7 composes of corner-sharing only CoO 4 tetrahedra, which can flexibly alter their positions to accommodate the insertion of interstitial oxygen ions and mediate the stress during the electrochemical oxidation. The density functional theory calculations demonstrate that the OER is efficiently catalyzed by a binuclear active site of dual corner-shared cobalt tetrahedra, which have a coordination number switching between 3 and 4 during the reaction. We expect that the reported active structural motif of dual corner-shared cobalt tetrahedra in this study could enable further development of compounds for catalyzing the OER.
Publisher: American Association for the Advancement of Science (AAAS)
Date: 25-08-2023
Abstract: Developing technologies based on the concept of methanol electrochemical refinery (e-refinery) is promising for carbon-neutral chemical manufacturing. However, a lack of mechanism understanding and material properties that control the methanol e-refinery catalytic performances hinders the discovery of efficient catalysts. Here, using 18 O isotope–labeled catalysts, we find that the oxygen atoms in formate generated during the methanol e-refinery reaction can originate from the catalysts’ lattice oxygen and the O-2p-band center levels can serve as an effective descriptor to predict the catalytic performance of the catalysts, namely, the formate production rates and Faradaic efficiencies. Moreover, the identified descriptor is consolidated by additional catalysts and theoretical mechanisms from density functional theory. This work provides direct experimental evidence of lattice oxygen participation and offers an efficient design principle for the methanol e-refinery reaction to formate, which may open up new research directions in understanding and designing electrified conversions of small molecules.
Publisher: Wiley
Date: 18-02-2021
Publisher: Springer Science and Business Media LLC
Date: 04-02-2019
DOI: 10.1038/S41467-019-08532-3
Abstract: Exploring robust catalysts for water oxidation in acidic electrolyte is challenging due to the limited material choice. Iridium (Ir) is the only active element with a high resistance to the acid corrosion during water electrolysis. However, Ir is rare, and its large-scale application could only be possible if the intrinsic activity of Ir could be greatly enhanced. Here, a pseudo-cubic SrCo 0.9 Ir 0.1 O 3-δ perovskite, containing corner-shared IrO6 octahedrons, is designed. The Ir in the SrCo 0.9 Ir 0.1 O 3-δ catalyst shows an extremely high intrinsic activity as reflected from its high turnover frequency, which is more than two orders of magnitude higher than that of IrO 2 . During the electrochemical cycling, a surface reconstruction, with Sr and Co leaching, over SrCo 0.9 Ir 0.1 O 3-δ occurs. Such reconstructed surface region, likely contains a high amount of structural domains with corner-shared and under-coordinated IrO x octahedrons, is responsible for the observed high activity.
Publisher: Springer Science and Business Media LLC
Date: 28-04-2023
DOI: 10.1038/S41467-023-38017-3
Abstract: Understanding and mastering the structural evolution of water oxidation electrocatalysts lays the foundation to finetune their catalytic activity. Herein, we demonstrate that surface reconstruction of spinel oxides originates from the metal-oxygen covalency polarity in the M T –O–M O backbone. A stronger M O –O covalency relative to M T –O covalency is found beneficial for a more thorough reconstruction towards oxyhydroxides. The structure-reconstruction relationship allows precise prediction of the reconstruction ability of spinel pre-catalysts, based on which the reconstruction degree towards the in situ generated oxyhydroxides can be controlled. The investigations of oxyhydroxides generated from spinel pre-catalysts with the same reconstruction ability provide guidelines to navigate the cation selection in spinel pre-catalysts design. This work reveals the fundamentals for manipulating the surface reconstruction of spinel pre-catalysts for water oxidation.
Location: China
No related grants have been discovered for Yuanmiao Sun.