Developing highly active methanol oxidation electrocatalysts with superior anti-CO poisoning capability remains a grand challenge. Herein, a simple strategy was employed to prepare distinctive PtFeIr jagged nanowires with Ir located at the shell and Pt/Fe located at the core. The PtFeIr jagged nanowire possesses an optimal mass activity of 2.13 A mg and specific activity of 4.25 mA cm, giving the catalyst a great edge over PtFe jagged nanowire (1.63 A mg and 3.75 mA cm) and Pt/C (0.38 A mg and 0.76 mA cm). The in-situ Fourier transform infrared (FTIR) spectroscopy and differential electrochemical mass spectrometry (DEMS) unravel the origin of extraordinary CO tolerance in terms of key reaction intermediates in the non-CO pathway. Density functional theory (DFT) calculations add to the body of evidence that the surface Ir incorporation transforms the selectivity from CO pathway to non-CO pathway. Meanwhile, the presence of Ir serves to optimize surface electronic structure with weakened CO binding strength. We believe this work will advance the understanding of methanol oxidation catalytic mechanism and provide some insight into structural design of efficient electrocatalysts.
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http://dx.doi.org/10.1016/j.jcis.2023.02.126 | DOI Listing |
J Colloid Interface Sci
December 2024
School of Petrochemical Engineering, Lanzhou University of Technology, Lanzhou 730050, PR China; Key Laboratory of Low Carbon Energy and Chemical Engineering of Gansu Province, Lanzhou 730050, PR China.
Heteroatom-doped carbon materials are widely used to improve the electrocatalytic oxidation of methanol; however, the underlying mechanisms driving this enhancement remain poorly understood. A major challenge lies in developing non-doped carbon supports with tunable intrinsic defect types tailored for metal-based catalysts. In this study, we synthesize a series of ordered mesoporous carbon (OMC) supports with adjustable edge defect densities by varying roasting temperatures and employing a zinc (Zn) evaporation strategy to systematically investigate the impact of edge defects on methanol oxidation reaction (MOR) performance.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
December 2024
Department of Chemistry, Capital Normal University, Beijing, 100048, P. R. China.
Whether the catalyst can realize the non-CO pathway is the key to greatly improve the catalytic activity and stability of methanol oxidation reaction (MOR). It is feasible to optimize the reaction path selectivity by modifying organic ligands and constructing single-atom systems. At the same time, heterogeneous metal nanosheets with atomic thickness have been shown to significantly enhance the catalytic activity of materials due to their ultra-high exposure of active sites and synergistic effects.
View Article and Find Full Text PDFSci Total Environ
October 2024
Dept. Environ. Sci. & Engn., Hebei Key Lab. Power Plant Flue Gas Multipollutant, North China Elect. Power Univ., Baoding 071003, PR China; Coll. Environm. Sci. & Engn, MOE Key Lab Resources & Environm. Syst. Optimizat., North China Elect. Power Univ., Beijing 102206, PR China. Electronic address:
With the clarification of the CO abatement targets and pathways, the management and control of non-CO greenhouse gases (GHGs) have been widely emphasized. As the potent GHGs restricted by the Kyoto Protocol, methane (CH) and sulfur hexafluoride (SF) emissions contribute to a significant and increasing share of the total global GHG emissions, resulting in a continuous impact on the environment. Hence, the abatement of CH and SF, the potent GHGs, is a matter of urgency.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2024
School of Nuclear Science and Technology, Key Laboratory of Precision and Intelligent Chemistry, Hefei National Research Center for Physical Sciences at the Microscale, National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, P.R. China.
Rational design of efficient methanol oxidation reaction (MOR) catalyst that undergo non-CO pathway is essential to resolve the long-standing poisoning issue. However, it remains a huge challenge due to the rather difficulty in maximizing the non-CO pathway by the selective coupling between the key *CHO and *OH intermediates. Here, we report a high-performance electrocatalyst of patchy atomic-layer Pt epitaxial growth on CeO nanocube (Pt ALs/CeO) with maximum electronic metal-support interaction for enhancing the coupling selectively.
View Article and Find Full Text PDFAdv Sci (Weinh)
May 2024
College of sciences, Henan Agricultural University, Zhengzhou, Henan, 450000, P. R. China.
Designing high efficiency platinum (Pt)-based catalysts for methanol oxidation reaction (MOR) with high "non-CO" pathway selectivity is strongly desired and remains a grand challenge. Herein, PtRuNiCoFeGaPbW HEA ultrathin nanowires (HEA-8 UNWs) are synthesized, featuring unique cascaded p-d orbital hybridization interaction by inducing dual p-block metals (Ga and Pb). In comparison with Pt/C, HEA-8 UNWs exhibit 15.
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