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  • Online Resource  (7)
  • Wiley  (7)
  • Zhou, Zhiyou  (7)
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  • Online Resource  (7)
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  • Wiley  (7)
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  • 1
    Online Resource
    Online Resource
    p–d Orbital Hybridization Induced by a Monodispersed Ga Site on a Pt 3 Mn Nanocatalyst Boosts Ethanol Electrooxidation
    Wiley ; 2022
    In:  Angewandte Chemie International Edition Vol. 61, No. 12 ( 2022-03-14)
    Details
    In: Angewandte Chemie International Edition, Wiley, Vol. 61, No. 12 ( 2022-03-14)
    Abstract: Constructing monodispersed metal sites in heterocatalysis is an efficient strategy to boost their catalytic performance. Herein, a new strategy using monodispersed metal sites to tailor Pt‐based nanocatalysts is addressed by engineering unconventional p–d orbital hybridization. Thus, monodispersed Ga on Pt 3 Mn nanocrystals (Ga‐O‐Pt 3 Mn) with high‐indexed facets was constructed for the first time to drive ethanol electrooxidation reaction (EOR). Strikingly, the Ga‐O‐Pt 3 Mn nanocatalyst shows an enhanced EOR performance with achieving 8.41 times of specific activity than that of Pt/C. The electrochemical in situ Fourier transform infrared spectroscopy results and theoretical calculations disclose that the Ga‐O‐Pt 3 Mn nanocatalyst featuring an unconventional p–d orbital hybridization not only promote the C−C bond‐breaking and rapid oxidation of ‐OH of ethanol, but also inhibit the generation of poisonous CO intermediate species. This work discloses a promising strategy to construct a novel nanocatalysts tailored by monodispersed metal site as efficient fuel cell catalysts.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    URL: Article
    DOI: 10.1002/anie.v61.12
    DOI: 10.1002/anie.202115735
    RVK:
    VA 2100
    Language: English
    Publisher: Wiley
    Publication Date: 2022
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
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    Online Resource
  • 2
    Online Resource
    Online Resource
    p–d Orbital Hybridization Induced by a Monodispersed Ga Site on a Pt 3 Mn Nanocatalyst Boosts Ethanol Electrooxidation
    Wiley ; 2022
    In:  Angewandte Chemie Vol. 134, No. 12 ( 2022-03-14)
    Details
    In: Angewandte Chemie, Wiley, Vol. 134, No. 12 ( 2022-03-14)
    Abstract: Constructing monodispersed metal sites in heterocatalysis is an efficient strategy to boost their catalytic performance. Herein, a new strategy using monodispersed metal sites to tailor Pt‐based nanocatalysts is addressed by engineering unconventional p–d orbital hybridization. Thus, monodispersed Ga on Pt 3 Mn nanocrystals (Ga‐O‐Pt 3 Mn) with high‐indexed facets was constructed for the first time to drive ethanol electrooxidation reaction (EOR). Strikingly, the Ga‐O‐Pt 3 Mn nanocatalyst shows an enhanced EOR performance with achieving 8.41 times of specific activity than that of Pt/C. The electrochemical in situ Fourier transform infrared spectroscopy results and theoretical calculations disclose that the Ga‐O‐Pt 3 Mn nanocatalyst featuring an unconventional p–d orbital hybridization not only promote the C−C bond‐breaking and rapid oxidation of ‐OH of ethanol, but also inhibit the generation of poisonous CO intermediate species. This work discloses a promising strategy to construct a novel nanocatalysts tailored by monodispersed metal site as efficient fuel cell catalysts.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    URL: Article
    DOI: 10.1002/ange.v134.12
    DOI: 10.1002/ange.202115735
    RVK:
    VA 2100
    RVK:
    VN 5020
    Language: English
    Publisher: Wiley
    Publication Date: 2022
    detail.hit.zdb_id: 505868-5
    detail.hit.zdb_id: 506609-8
    detail.hit.zdb_id: 514305-6
    detail.hit.zdb_id: 505872-7
    detail.hit.zdb_id: 1479266-7
    detail.hit.zdb_id: 505867-3
    detail.hit.zdb_id: 506259-7
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    Online Resource
  • 3
    Online Resource
    Online Resource
    Ultrasmall Pd‐Cu‐Pt Trimetallic Twin Icosahedrons Boost the Electrocatalytic Performance of Glycerol Oxidation at the Operating Temperature of Fuel Cells
    Wiley ; 2020
    In:  Advanced Functional Materials Vol. 30, No. 11 ( 2020-03)
    Details
    In: Advanced Functional Materials, Wiley, Vol. 30, No. 11 ( 2020-03)
    Abstract: Recently, in order to improve the energy conversion efficiency of direct polyol fuel cells, the engineering of effective Pd‐ and/or Pt‐based electrocatalysts to rupture CC bonds has received increasing attention. Here, an example is shown to synthesize highly uniform sub‐10 nm Pd‐Cu‐Pt twin icosahedrons by controlling the nucleation phase. Because of the synergies of the electronic effect, synergistic effect, geometric effect, and abundant surface active sites originating from the formation of near surface alloy and special icosahedral shape, the Pd‐Cu‐Pt twin icosahedrons exhibit excellent electrocatalytic performance in glycerol electrocatalysis at the operating temperature of direct alcohol fuel cells (70 °C) in KOH electrolyte. The Pd 50.2 Cu 38.4 Pt 11.4 icosahedrons show mass activities of 9.7 A mg −1 Pd+Pt and 13.7 A mg −1 Pd . Furthermore, the Pd 50.2 Cu 38.4 Pt 11.4 icosahedrons demonstrate long‐term durability in current–time test for 36 000 s and high in situ anti‐CO poisoning performance. In addition, the introduction of CO can enhance electro‐oxidation endurance on Pd 50.2 Cu 38.4 Pt 11.4 icosahedrons, and the peak mass activity can reach to 14.4 A mg −1 Pd+Pt . The in situ Fourier transform infrared spectroscopy spectra indicate that the Pd 50.2 Cu 38.4 Pt 11.4 icosahedrons possess a high capacity to break CC bonds and may efficiently convert glycerol into CO 2 , thus improving the utilization efficiency of energy‐containing molecule glycerol.
    Type of Medium: Online Resource
    ISSN: 1616-301X , 1616-3028
    URL: Issue
    URL: Article
    DOI: 10.1002/adfm.v30.11
    DOI: 10.1002/adfm.201908235
    Language: English
    Publisher: Wiley
    Publication Date: 2020
    detail.hit.zdb_id: 2029061-5
    detail.hit.zdb_id: 2039420-2
    SSG: 11
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  • 4
    Online Resource
    Online Resource
    A Lattice‐Oxygen‐Involved Reaction Pathway to Boost Urea Oxidation
    Wiley ; 2019
    In:  Angewandte Chemie Vol. 131, No. 47 ( 2019-11-18), p. 16976-16981
    Details
    In: Angewandte Chemie, Wiley, Vol. 131, No. 47 ( 2019-11-18), p. 16976-16981
    Abstract: The electrocatalytic urea oxidation reaction (UOR) provides more economic electrons than water oxidation for various renewable energy‐related systems owing to its lower thermodynamic barriers. However, it is limited by sluggish reaction kinetics, especially by CO 2 desorption steps, masking its energetic advantage compared with water oxidation. Now, a lattice‐oxygen‐involved UOR mechanism on Ni 4+ active sites is reported that has significantly faster reaction kinetics than the conventional UOR mechanisms. Combined DFT, 18 O isotope‐labeling mass spectrometry, and in situ IR spectroscopy show that lattice oxygen is directly involved in transforming *CO to CO 2 and accelerating the UOR rate. The resultant Ni 4+ catalyst on a glassy carbon electrode exhibits a high current density (264 mA cm −2 at 1.6 V versus RHE), outperforming the state‐of‐the‐art catalysts, and the turnover frequency of Ni 4+ active sites towards UOR is 5 times higher than that of Ni 3+ active sites.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    URL: Article
    DOI: 10.1002/ange.v131.47
    DOI: 10.1002/ange.201909832
    RVK:
    VA 2100
    RVK:
    VN 5020
    Language: English
    Publisher: Wiley
    Publication Date: 2019
    detail.hit.zdb_id: 505868-5
    detail.hit.zdb_id: 506609-8
    detail.hit.zdb_id: 514305-6
    detail.hit.zdb_id: 505872-7
    detail.hit.zdb_id: 1479266-7
    detail.hit.zdb_id: 505867-3
    detail.hit.zdb_id: 506259-7
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  • 5
    Online Resource
    Online Resource
    Conjugated Coordination Polymer as a New Platform for Efficient and Selective Electroreduction of Nitrate into Ammonia
    Wiley ; 2023
    In:  Advanced Materials Vol. 35, No. 10 ( 2023-03)
    Details
    In: Advanced Materials, Wiley, Vol. 35, No. 10 ( 2023-03)
    Abstract: Electroreduction of nitrate into ammonia (NRA) provides a sustainable route to convert the widespread nitrate pollutants into high‐value‐added products under ambient conditions, which unfortunately suffers from unsatisfactory selectivity due to the competitive hydrogen evolution reaction (HER). Previous strategies of modifying the metal sites of catalysts often met a dilemma for simultaneously promoting activity and selectivity toward NRA. Here, a general strategy is reported to enable an efficient and selective NRA process through coordination modulation of single‐atom catalysts to tailor the local proton concentration at the catalyst surface. By contrast, two analogous Ni‐single‐atom enriched conjugated coordination polymers (NiO 4 ‐CCP and NiN 4 ‐CCP) with different coordination motifs are investigated for the proof‐of‐concept study. The NiO 4 ‐CCP catalyst exhibits an ammonia yield rate as high as 1.83 mmol h −1 mg −1 with a Faradaic efficiency of 94.7% under a current density of 125 mA cm −2 , outperforming the NiN 4 ‐CCP catalyst. These experimental and theoretical studies both suggest that the strategy of coordination modulation can not only accelerate the NRA by adjusting the adsorption energies of NRA intermediates on the metal sites but also inhibit the HER through regulating the proton migration with contributions from the metal‐hydrated cations adsorbed at the catalyst surface, thus achieving simultaneous enhancement of NRA selectivity and activity.
    Type of Medium: Online Resource
    ISSN: 0935-9648 , 1521-4095
    URL: Issue
    URL: Article
    DOI: 10.1002/adma.v35.10
    DOI: 10.1002/adma.202209855
    RVK:
    UA 1538
    Language: English
    Publisher: Wiley
    Publication Date: 2023
    detail.hit.zdb_id: 1474949-X
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  • 6
    Online Resource
    Online Resource
    A Lattice‐Oxygen‐Involved Reaction Pathway to Boost Urea Oxidation
    Wiley ; 2019
    In:  Angewandte Chemie International Edition Vol. 58, No. 47 ( 2019-11-18), p. 16820-16825
    Details
    In: Angewandte Chemie International Edition, Wiley, Vol. 58, No. 47 ( 2019-11-18), p. 16820-16825
    Abstract: The electrocatalytic urea oxidation reaction (UOR) provides more economic electrons than water oxidation for various renewable energy‐related systems owing to its lower thermodynamic barriers. However, it is limited by sluggish reaction kinetics, especially by CO 2 desorption steps, masking its energetic advantage compared with water oxidation. Now, a lattice‐oxygen‐involved UOR mechanism on Ni 4+ active sites is reported that has significantly faster reaction kinetics than the conventional UOR mechanisms. Combined DFT, 18 O isotope‐labeling mass spectrometry, and in situ IR spectroscopy show that lattice oxygen is directly involved in transforming *CO to CO 2 and accelerating the UOR rate. The resultant Ni 4+ catalyst on a glassy carbon electrode exhibits a high current density (264 mA cm −2 at 1.6 V versus RHE), outperforming the state‐of‐the‐art catalysts, and the turnover frequency of Ni 4+ active sites towards UOR is 5 times higher than that of Ni 3+ active sites.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    URL: Article
    DOI: 10.1002/anie.v58.47
    DOI: 10.1002/anie.201909832
    RVK:
    VA 2100
    Language: English
    Publisher: Wiley
    Publication Date: 2019
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
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  • 7
    Online Resource
    Online Resource
    Relay Catalysis of Multi‐Sites Promotes Oxygen Reduction Reaction
    Wiley ; 2023
    In:  Advanced Functional Materials Vol. 33, No. 30 ( 2023-07)
    Details
    In: Advanced Functional Materials, Wiley, Vol. 33, No. 30 ( 2023-07)
    Abstract: The two‐electron pathway to form hydrogen peroxide (H 2 O 2 ) is undesirable for the oxygen reduction reaction (ORR) in iron and nitrogen doped carbon (Fe–N–C) material as it not only lowers the catalytic efficiency but also impairs the catalyst durability. In this study, a relay catalysis pathway is designed to minimize the two‐electron selectivity of Fe–N–C catalyst. Such a design is achieved by introducing two other sites, that is, MnN 4 site and α‐Fe(110) face. A combination of transmission electron microscopy image and X‐ray absorption spectra verify the three site formation. Electrochemical test coupled with post‐treatment confirm the improvement of MnN 4 site and α‐Fe(110) face on catalyst performance. Theoretical calculation proposes a relay catalysis pathway of three sites, that is, H 2 O 2 released from the FeN 4 site migrates to the MnN 4 site or α‐Fe(110) face, on which the captive H 2 O 2 is further reduced to H 2 O. The relay catalysis pathway positioned the as‐prepared catalyst among the best ORR catalysts in both aqueous electrode and alkaline direct methanol fuel cell test. This study examples an interesting relay catalysis pathway of multi‐sites for the ORR, which offers insights into the design of efficient electrocatalysts for fuel cells or beyond.
    Type of Medium: Online Resource
    ISSN: 1616-301X , 1616-3028
    URL: Issue
    URL: Article
    DOI: 10.1002/adfm.v33.30
    DOI: 10.1002/adfm.202215021
    Language: English
    Publisher: Wiley
    Publication Date: 2023
    detail.hit.zdb_id: 2029061-5
    detail.hit.zdb_id: 2039420-2
    SSG: 11
    Location Call Number Limitation Availability
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