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Interfacial Oxygen Vacancy-Copper Pair Sites on Inverse CeO2/Cu Catalyst Enable Efficient CO2 Electroreduction to Ethanol in Acid.
Angew Chem Int Ed Engl
January 2025
Hunan University, College of Materials Science and Engineering, South Lushan Road 2#, 410082, China, 410082, Changsha, CHINA.
Renewable electricity-driven electrochemical reduction of CO2 offers a promising route for production of high-value ethanol. However, the current state of this technology is hindered by low selectivity and productivity, primarily due to limited understanding of the atomic-level active sites involved in ethanol formation. Herein, we identify that the interfacial oxygen vacancy-neighboring Cu (Ov-Cu) pair sites are the active sites for CO2 electroreduction to ethanol.
View Article and Find Full Text PDFPorphyrin-based Vinylene-linked 3D Covalent Organic Framework with Unprecedented cya Topology for Photocatalytic H2O2 Production.
Angew Chem Int Ed Engl
January 2025
University of Science and Technology Beijing, School of Chemistry and Biological Engineering, CHINA.
Designing and realizing new topologies represent one of the most important ways toward developing new structures and functionalities for molecule-based frameworks including SOFs, MOFs, and COFs. Herein, Aldol condensation between 5,10,15,20-tetrayl(tetrakis(([1,1':3',1''-terphenyl]-4,4''-dicarbaldehyde)))-porphyrin (TTEP) and 2,4,6-trimethyl-1,3,5-triazine (TMT) affords the vinylene-linked 3D covalent organic framework Por-COF-cya. Powder X-ray diffraction (PXRD) in combination with structural simulation reveals its high crystalline structure with an unprecedented cya topology in the molecule-based frameworks reported thus far.
View Article and Find Full Text PDFNickel Nanocluster-Stabilized Unsaturated Ni-N3 Atomic Sites for Efficient CO2-to-CO Electrolysis at Industrial-Level Current.
Angew Chem Int Ed Engl
January 2025
Central South University, School of Physics and Electronics, 932 Lushan Nan Road, 410081, Changsha, CHINA.
Unsaturated Ni single atom catalysts (SACs), Ni-Nx (x=1,2,3), have been investigated to break the conventional Ni-N4 structural limitation and provide more unoccupied 3d orbitals for CO2RR intermediates adsorption, but their intrinsically low structural stability has seriously hindered their applications. Here, we developed a strategy by integrating Ni nanoclusters to stabilize unsaturated Ni-N3 atomic sites for efficient CO2 electroreduction to CO at industrial-level current. DFT calculations revealed that the incorporation of Ni nanocluster effectively stabilizes the unsaturated Ni-N3 atomic sites and modulates their electronic structure to enhance the adsorption of the key intermediate *COOH during CO2RR.
View Article and Find Full Text PDFHeteroarchitectural Gas Diffusion Layer Promotes CO2 Reduction Coupled with Biomass Oxidation at Ampere-Level Current Density.
Angew Chem Int Ed Engl
January 2025
Shanghai Jiao Tong University, School of Environmental Science and Engineering, 800 Dongchuan Road, 200240, Shanghai, CHINA.
Achieving high product selectivity at ampere-level current densities is essential for the industrial application of electrochemical CO2 reduction. However, the operational stability of CO2 electrolyzers at large current density has long been hindered by flooding of gas diffusion layer (GDL). Herein, a new heteroarchitectural GDL is designed to overcome flooding.
View Article and Find Full Text PDFSymmetry Breaking of FeN4 Moiety via Edge Defects for Acidic Oxygen Reduction Reaction.
Angew Chem Int Ed Engl
January 2025
University of Science and Technology of China, National Synchrotron Radiation Laboratory, 42#, South Road of HeZuoHua, 230029, Hefei, CHINA.
Fe-N-C catalysts, with a planar D4h symmetric FeN4 structure, show promising as noble metal-free oxygen reduction reaction catalysts. Nonetheless, the highly symmetric structure restricts the effective manipulation of its geometric and electronic structures, impeding further enhancements in oxygen reduction reaction performance. Here, a high proportion of asymmetric edge-carbon was successfully introduced into Fe-N-C catalysts through morphology engineering, enabling the precise modulation of the FeN4 active site.
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