As a sustainable and promising approach of removing of nitrogen oxides (NO), catalytic reduction of NO with H is highly desirable with a precise understanding to the structure-activity relationship of supported catalysts. In particular, the dynamic evolution of support at microscopic scale may play a critical role in heterogeneous catalysis, however, identifying the in situ structural change of support under working condition with atomic precision and revealing its role in catalysis is still a grand challenge. Herein, we visually capture the surface lattice expansion of WO support in Pt-WO catalyst induced by NO in the exemplified reduction of NO with H using in situ transmission electron microscopy and first reveal its important role in enhancing catalysis. We find that NO can adsorb on the oxygen vacancy sites of WO and favorably induce the reversible stretching of W-O-W bonds during the reaction, which can reduce the adsorption energy of NO on Pt centers and the energy barrier of the rate-determining step. The comprehensive studies reveal that lattice expansion of WO support can tune the catalytic performance of Pt-WO catalyst, leading to 20% catalytic activity enhancement for the exemplified reduction of NO with H. This work reveals that the lattice expansion of defective support can tune and optimize the catalytic performance at the atomic scale.
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http://dx.doi.org/10.1073/pnas.2311180121 | DOI Listing |
ACS Appl Mater Interfaces
December 2024
Institute for Composites Science Innovation (InCSI), School of Materials Science and Engineering, Zhejiang University, 38 Zheda Road, Hangzhou 310027, China.
Electrically conducting 2D metal-organic frameworks (MOFs) with hexagonal 2D lattices like other 2D van der Waals stacked materials are attracting increasing interest. The conductivity can be effectively regulated through electronic structure adjustment thanks to the chemical and physical flexibility and adjustability of MOFs. In this regard, through a simple and rapid electrochemical method, 2D conductive iron-quinoid MOFs were synthesized.
View Article and Find Full Text PDFChem Sci
December 2024
College of Materials Science and Engineering, Zhengzhou University Zhengzhou 450052 P. R. China
Preparation of two-dimensional (2D) ferromagnetic nanomaterials and the study of their magnetic sources are crucial for the exploration of new materials with multiple applications. Herein, two-dimensional room-temperature ferromagnetic (FM) CaTiO nanosheets are successfully constructed with the assistance of supercritical carbon dioxide (SC CO). In this process, the SC CO-induced strain effect can lead to lattice expansion and introduction of O vacancies.
View Article and Find Full Text PDFSmall
December 2024
Key Laboratory of Advanced Structural Materials, Ministry of Education & School of Materials Science and Engineering, Changchun University of Technology, Changchun, 130012, China.
2D layered embedding materials have shown promising applications in rapidly rechargeable sodium-ion batteries (SIBs). However, the most commonly used embedding structures are susceptible to damage and collapse with increasing cycles, which in turn leads to a degradation of the overall performance of the batteries. In order to address this issue, a "stress-strain transition" mechanism is proposed to form a heterostructure by introducing pyramid-like MnSe into the MoS lattice to reduce the irreversible reconstruction under deep discharge.
View Article and Find Full Text PDFSmall Methods
December 2024
Institute of Photonics Technologies, National Tsing Hua University, Hsinchu, 30013, Taiwan.
Nano Lett
December 2024
Key Laboratory of Physics and Technology for Advanced Batteries (Ministry of Education), College of Physics, Jilin University, Changchun 130012, China.
Dendrite growth, corrosion, passivation, and other side reactions during Zn plating and stripping have consistently hindered the capacity and lifespan of Zn metal batteries. In this study, we employ first-principles calculations to unravel the epitaxial electroplating mechanism of Zn (002) planes on various substrate surfaces. We identify six critical factors, including interfacial stability, zincophilicity, surface atomic arrangement, lattice mismatch, responsiveness, and adaptability, that profoundly influence the electrochemical behavior of zinc deposition.
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