Water splitting for hydrogen production is limited by high cell voltage and low energy conversion efficiencies due to the slow kinetic process of the oxygen evolution reaction (OER). Here, an electrolytic system is constructed in which the cathode and anode co-release H at ultra-low input voltage using formaldehyde oxidation reaction (FOR) instead of OER. The prepared RuCe co-doped CuO nanotubes on copper foam (RuCe-CuO/CF) are used as electrode materials for the HER-FOR system. A current density of 0.8 A cm is achieved at 0.55 V, and a stable hydrogen production process is realized at both the cathode and anode. Density functional theory (DFT) studies show that the synergistic effect of Ru and Ce drives: i) the d-band center of RuCe-CuO/CF away from the Fermi energy level; ii) the energy barrier for the C─H cracking of the HC(OH)O intermediate in FOR is lowered, which promotes the formation of H from H, and iii) ΔG tends to 0 (-0.1 eV), optimizing the reaction kinetics of HER. This work provides a new design for an efficient catalyst for dual hydrogen production systems from water splitting.
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http://dx.doi.org/10.1002/smll.202406107 | DOI Listing |
J Am Chem Soc
January 2025
Department of Chemistry, University of Houston, Houston, Texas 77204-5003, United States.
Monoanionic, bidentate-auxiliary-directed, cobalt-catalyzed C-H bond functionalization has become a very useful tool in organic synthesis. A comprehensive investigation into isolated organometallic intermediates and their reactivity within the catalytic cycle is lacking. We report here mechanistic studies of cobalt-catalyzed, aminoquinoline-directed C(sp)-H bond functionalization.
View Article and Find Full Text PDFNano Lett
January 2025
Center for High Pressure Science and Technology Advanced Research, Beijing 100193, P. R. China.
Saturated sp-carbon nanothreads (CNTh) have garnered significant interest due to their predicted high Young's modulus and thermal conductivity. While the incorporation of heteroatoms into the central ring has been shown to influence the formation of CNTh and yield chemically homogeneous products, the impact of pendant groups on the polymerization process remains underexplored. In this study, we investigate the pressure-induced polymerization of phenol, revealing two phase transitions occurring below 0.
View Article and Find Full Text PDFSci Adv
January 2025
Department of Chemical Engineering, Kansas State University, Manhattan, KS, USA.
Protonic ceramic electrochemical cells (PCECs) can operate at intermediate temperatures (450° to 600°C) for power generation and hydrogen production. However, the operating temperature is still too high to revolutionize ceramic electrochemical cell technology. Lowering the operating temperature to <450°C will enable a wider material choice and reduce system costs.
View Article and Find Full Text PDFACS Nano
January 2025
Department of Chemistry and Biochemistry, Queens College, Flushing, New York 11367, United States.
Semiconductor nanomaterials and nanostructured interfaces have important technological applications, ranging from fuel production to electrosynthesis. Their photocatalytic activity is known to be highly heterogeneous, both in an ensemble of nanomaterials and within a single entity. Photoelectrochemical imaging techniques are potentially useful for high-resolution mapping of photo(electro)catalytic active sites; however, the nanoscale spatial resolution required for such experiments has not yet been attained.
View Article and Find Full Text PDFPhys Chem Chem Phys
January 2025
The Fritz Haber Center for Molecular Dynamics, Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem 91904, Israel.
Peroxy radicals are key intermediates in many atmospheric processes. Reactions between such radicals are of particular interest as they can lead to accretion products capable of participating in new particle formation (NPF). These reactions proceed through a tetroxide intermediate, which then decomposes to a complex of two alkoxy radicals and O, with spin conservation dictating that the complex must be formed in the triplet state.
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