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  • Chemistry/Pharmacy  (17)
  • 1
    Online Resource
    Online Resource
    Selective Photocatalytic Oxidative Coupling of Methane via Regulating Methyl Intermediates over Metal/ZnO Nanoparticles
    Wiley ; 2023
    In:  Angewandte Chemie Vol. 135, No. 23 ( 2023-06-05)
    Details
    In: Angewandte Chemie, Wiley, Vol. 135, No. 23 ( 2023-06-05)
    Abstract: Methane conversion to higher hydrocarbons requires harsh reaction conditions due to high energy barriers associated with C−H bond activation. Herein, we report a systematic investigation of photocatalytic oxidative coupling of methane (OCM) over transition‐metal‐loaded ZnO photocatalysts. A 1 wt % Au/ZnO delivered a remarkable C 2 ‐C 4 hydrocarbon production rate of 683 μmol g −1  h −1 (83 % C 2 ‐C 4 selectivity) under light irradiation with excellent photostability over two days. The metal type and its interaction with ZnO strongly influence the selectivity toward C−C coupling products. Photogenerated Zn + ‐O − sites enable CH 4 activation to methyl intermediates (*CH 3 ) migrating onto adjacent metal nanoparticles. The nature of the *CH 3 ‐metal interaction controls the OCM products. In the case of Au, strong d‐σ orbital hybridization reduces metal‐C−H bond angles and steric hindrance, thereby enabling efficient methyl coupling. Findings indicate the d‐σ center may be a suitable descriptor for predicting product selectivity during OCM over metal/ZnO photocatalysts.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    URL: Article
    DOI: 10.1002/ange.v135.23
    DOI: 10.1002/ange.202304301
    RVK:
    VA 2100
    RVK:
    VN 5020
    Language: English
    Publisher: Wiley
    Publication Date: 2023
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    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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  • 2
    Online Resource
    Online Resource
    Selective Photocatalytic Oxidative Coupling of Methane via Regulating Methyl Intermediates over Metal/ZnO Nanoparticles
    Wiley ; 2023
    In:  Angewandte Chemie International Edition Vol. 62, No. 23 ( 2023-06-05)
    Details
    In: Angewandte Chemie International Edition, Wiley, Vol. 62, No. 23 ( 2023-06-05)
    Abstract: Methane conversion to higher hydrocarbons requires harsh reaction conditions due to high energy barriers associated with C−H bond activation. Herein, we report a systematic investigation of photocatalytic oxidative coupling of methane (OCM) over transition‐metal‐loaded ZnO photocatalysts. A 1 wt % Au/ZnO delivered a remarkable C 2 ‐C 4 hydrocarbon production rate of 683 μmol g −1  h −1 (83 % C 2 ‐C 4 selectivity) under light irradiation with excellent photostability over two days. The metal type and its interaction with ZnO strongly influence the selectivity toward C−C coupling products. Photogenerated Zn + ‐O − sites enable CH 4 activation to methyl intermediates (*CH 3 ) migrating onto adjacent metal nanoparticles. The nature of the *CH 3 ‐metal interaction controls the OCM products. In the case of Au, strong d‐σ orbital hybridization reduces metal‐C−H bond angles and steric hindrance, thereby enabling efficient methyl coupling. Findings indicate the d‐σ center may be a suitable descriptor for predicting product selectivity during OCM over metal/ZnO photocatalysts.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    URL: Article
    DOI: 10.1002/anie.v62.23
    DOI: 10.1002/anie.202304301
    RVK:
    VA 2100
    Language: English
    Publisher: Wiley
    Publication Date: 2023
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
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  • 3
    Online Resource
    Online Resource
    Revealing Ammonia Quantification Minefield in Photo/Electrocatalysis
    Wiley ; 2021
    In:  Angewandte Chemie International Edition Vol. 60, No. 40 ( 2021-09-27), p. 21728-21731
    Details
    In: Angewandte Chemie International Edition, Wiley, Vol. 60, No. 40 ( 2021-09-27), p. 21728-21731
    Abstract: Photo/electrocatalytic ammonia synthesis has recently developed fast while the ammonia yields over state‐of‐the‐art photo/electrocatalysts are still very moderate. Such low concentration of synthesized NH3 brings about a challenge to the reliable quantification of the product in photo/electrocatalysis. Notably, we found that the quantitative detection of ammonia concentration below 0.2 ppm is error‐prone, which is likely the case happening in the majority of photo/electrocatalytic NH3 synthesis, thus arising concerns about the rationality and accuracy for low‐concentration ammonia quantification in these processes. Herein, we discuss the methodology used and analyze the reliability of various detection methods for the detection of trace ammonia in aqueous media. The challenges facing the detection of low concentration of ammonia in photo/electrocatalysis can be overcome by integration with multiple detection methods. According to the data presented, we also propose an effective criterion for precise quantification of ammonia, avoiding the unreasonable comparisons in photo/electrocatalytic ammonia synthesis.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    URL: Article
    DOI: 10.1002/anie.v60.40
    DOI: 10.1002/anie.202108769
    RVK:
    VA 2100
    Language: English
    Publisher: Wiley
    Publication Date: 2021
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
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  • 4
    Online Resource
    Online Resource
    Revealing Ammonia Quantification Minefield in Photo/Electrocatalysis
    Wiley ; 2021
    In:  Angewandte Chemie Vol. 133, No. 40 ( 2021-09-27), p. 21896-21899
    Details
    In: Angewandte Chemie, Wiley, Vol. 133, No. 40 ( 2021-09-27), p. 21896-21899
    Abstract: Photo/electrocatalytic ammonia synthesis has recently developed fast while the ammonia yields over state‐of‐the‐art photo/electrocatalysts are still very moderate. Such low concentration of synthesized NH3 brings about a challenge to the reliable quantification of the product in photo/electrocatalysis. Notably, we found that the quantitative detection of ammonia concentration below 0.2 ppm is error‐prone, which is likely the case happening in the majority of photo/electrocatalytic NH3 synthesis, thus arising concerns about the rationality and accuracy for low‐concentration ammonia quantification in these processes. Herein, we discuss the methodology used and analyze the reliability of various detection methods for the detection of trace ammonia in aqueous media. The challenges facing the detection of low concentration of ammonia in photo/electrocatalysis can be overcome by integration with multiple detection methods. According to the data presented, we also propose an effective criterion for precise quantification of ammonia, avoiding the unreasonable comparisons in photo/electrocatalytic ammonia synthesis.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    URL: Article
    DOI: 10.1002/ange.v133.40
    DOI: 10.1002/ange.202108769
    RVK:
    VA 2100
    RVK:
    VN 5020
    Language: English
    Publisher: Wiley
    Publication Date: 2021
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    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
    Promoted Electron Transfer along the Newly Formed BiOS Bond in Bi2O(OH)2SO4
    American Chemical Society (ACS) ; 2016
    In:  The Journal of Physical Chemistry A Vol. 120, No. 17 ( 2016-05-05), p. 2657-2666
    Details
    In: The Journal of Physical Chemistry A, American Chemical Society (ACS), Vol. 120, No. 17 ( 2016-05-05), p. 2657-2666
    Type of Medium: Online Resource
    ISSN: 1089-5639 , 1520-5215
    URL: Article
    URL: Article
    DOI: 10.1021/acs.jpca.6b01908
    DOI: 10.1021/acs.jpca.6b01908.s001
    RVK:
    VA 5430.A
    Language: English
    Publisher: American Chemical Society (ACS)
    Publication Date: 2016
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    detail.hit.zdb_id: 1357795-5
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  • 6
    Online Resource
    Online Resource
    Exploiting Ru‐Induced Lattice Strain in CoRu Nanoalloys for Robust Bifunctional Hydrogen Production
    Wiley ; 2021
    In:  Angewandte Chemie International Edition Vol. 60, No. 6 ( 2021-02-08), p. 3290-3298
    Details
    In: Angewandte Chemie International Edition, Wiley, Vol. 60, No. 6 ( 2021-02-08), p. 3290-3298
    Abstract: Designing bifunctional catalysts capable of driving the electrochemical hydrogen evolution reaction (HER) and also H 2 evolution via the hydrolysis of hydrogen storage materials such as ammonia borane (AB) is of considerable practical importance for future hydrogen economies. Herein, we systematically examined the effect of tensile lattice strain in CoRu nanoalloys supported on carbon quantum dots (CoRu/CQDs) on hydrogen generation by HER and AB hydrolysis. By varying the Ru content, the lattice parameters and Ru‐induced lattice strain in the CoRu nanoalloys could be tuned. The CoRu 0.5 /CQDs catalyst with an ultra‐low Ru content (1.33 wt.%) exhibited excellent catalytic activity for HER ( η =18 mV at 10 mA cm −2 in 1 M KOH) and extraordinary activity for the hydrolysis of AB with a turnover frequency of 3255.4 mol  mol −1 (Ru)  min −1 or 814.7 mol  mol −1 (cat)  min −1 at 298 K, respectively, representing one of the best activities yet reported for AB hydrolysis over a ruthenium alloy catalyst. Moreover, the CoRu 0.5 /CQDs catalyst displayed excellent stability during each reaction, including seven alternating cycles of HER and AB hydrolysis. Theoretical calculations revealed that the remarkable catalytic performance of CoRu 0.5 /CQDs resulted from the optimal alloy electronic structure realized by incorporating small amounts of Ru, which enabled fast interfacial electron transfer to intermediates, thus benefitting H 2 evolution kinetics. Results support the development of new and improved catalysts HER and AB hydrolysis.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    URL: Article
    DOI: 10.1002/anie.v60.6
    DOI: 10.1002/anie.202013985
    RVK:
    VA 2100
    Language: English
    Publisher: Wiley
    Publication Date: 2021
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
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  • 7
    Online Resource
    Online Resource
    Understanding Aerobic Nitrogen Photooxidation on Titania through In Situ Time‐Resolved Spectroscopy
    Wiley ; 2022
    In:  Angewandte Chemie International Edition Vol. 61, No. 51 ( 2022-12-19)
    Details
    In: Angewandte Chemie International Edition, Wiley, Vol. 61, No. 51 ( 2022-12-19)
    Abstract: Nitrate is an important raw material for chemical fertilizers, but it is industrially manufactured in multiple steps at high temperature and pressure, urgently motivating the design of a green and sustainable strategy for nitrate production. We report the photosynthesis of nitrate from N 2 and O 2 on commercial TiO 2 in a flow reactor under ambient conditions. The TiO 2 photocatalyst offered a high nitrate yield of 1.85 μmol h −1 as well as a solar‐to‐nitrate energy conversion efficiency up to 0.13 %. We combined reactivity and in situ Fourier transform infrared spectroscopy to elucidate the mechanism of nitrate formation and unveil the special role of O 2 in N≡N bond dissociation. The mechanistic insight into charge‐involved N 2 oxidation was further demonstrated by in situ transient absorption spectroscopy and electron paramagnetic resonance. This work exhibits the mechanistic origin of N 2 photooxidation and initiates a potential method for triggering inert catalytic reactions.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    URL: Article
    DOI: 10.1002/anie.v61.51
    DOI: 10.1002/anie.202211469
    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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  • 8
    Online Resource
    Online Resource
    Minimizing Temperature Bias through Reliable Temperature Determination in Gas‐Solid Photothermal Catalytic Reactions
    Wiley ; 2023
    In:  Angewandte Chemie International Edition Vol. 62, No. 24 ( 2023-06-12)
    Details
    In: Angewandte Chemie International Edition, Wiley, Vol. 62, No. 24 ( 2023-06-12)
    Abstract: Enormous advances in photothermal catalysis have been made over the years, whereas the temperature assessment still remains controversial in the majority of photothermal catalytic systems. Herein, we methodically uncovered the phenomenon of temperature determination bias arising from prominent temperature differences in gas‐solid photothermal catalytic systems, which extensively existed yet has been overlooked in most relevant cases. To avoid the interference of temperature bias, we developed a universal protocol for reliable temperature evaluation of gas‐solid photothermal catalytic reactions, with emphasis on eliminating the temperature gradient and temperature fluctuation of catalyst layer via optimizing the reaction system. This work presents a functional and credible practice for temperature detection, calling attention to addressing the effects of temperature differences, and reassessing the actual temperature‐based performances in gas‐solid photothermal catalysis.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    URL: Article
    DOI: 10.1002/anie.v62.24
    DOI: 10.1002/anie.202219340
    RVK:
    VA 2100
    Language: English
    Publisher: Wiley
    Publication Date: 2023
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
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  • 9
    Online Resource
    Online Resource
    Understanding Aerobic Nitrogen Photooxidation on Titania through In Situ Time‐Resolved Spectroscopy
    Wiley ; 2022
    In:  Angewandte Chemie Vol. 134, No. 51 ( 2022-12-19)
    Details
    In: Angewandte Chemie, Wiley, Vol. 134, No. 51 ( 2022-12-19)
    Abstract: Nitrate is an important raw material for chemical fertilizers, but it is industrially manufactured in multiple steps at high temperature and pressure, urgently motivating the design of a green and sustainable strategy for nitrate production. We report the photosynthesis of nitrate from N 2 and O 2 on commercial TiO 2 in a flow reactor under ambient conditions. The TiO 2 photocatalyst offered a high nitrate yield of 1.85 μmol h −1 as well as a solar‐to‐nitrate energy conversion efficiency up to 0.13 %. We combined reactivity and in situ Fourier transform infrared spectroscopy to elucidate the mechanism of nitrate formation and unveil the special role of O 2 in N≡N bond dissociation. The mechanistic insight into charge‐involved N 2 oxidation was further demonstrated by in situ transient absorption spectroscopy and electron paramagnetic resonance. This work exhibits the mechanistic origin of N 2 photooxidation and initiates a potential method for triggering inert catalytic reactions.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    URL: Article
    DOI: 10.1002/ange.v134.51
    DOI: 10.1002/ange.202211469
    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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  • 10
    Online Resource
    Online Resource
    Sub‐3 nm Ultrafine Cu 2 O for Visible Light Driven Nitrogen Fixation
    Wiley ; 2021
    In:  Angewandte Chemie International Edition Vol. 60, No. 5 ( 2021-02), p. 2554-2560
    Details
    In: Angewandte Chemie International Edition, Wiley, Vol. 60, No. 5 ( 2021-02), p. 2554-2560
    Abstract: Cu 2 O, a low‐cost, visible light responsive semiconductor photocatalyst represents an ideal candidate for visible light driven photocatalytic reduction of N 2 to NH 3 from the viewpoint of thermodynamics, but it remains unexplored. Reported here is the successful synthesis of uniformly sized and ultrafine Cu 2 O platelets, with a lateral size of 〈 3 nm, by the in situ topotactic reduction of a Cu II ‐containing layered double hydroxide with ascorbic acid. The supported ultrafine Cu 2 O offered excellent performance and stability for the visible light driven photocatalytic reduction of N 2 to NH 3 (the Cu 2 O‐mass‐normalized rate as high as 4.10 mmol g −1  h −1 at λ 〉 400 nm), with the origin of the high activity being long‐lived photoexcited electrons in trap states, an abundance of exposed active sites, and the underlying support structure. This work guides the future design of ultrafine catalysts for NH 3 synthesis and other applications.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    URL: Article
    DOI: 10.1002/anie.v60.5
    DOI: 10.1002/anie.202013594
    RVK:
    VA 2100
    Language: English
    Publisher: Wiley
    Publication Date: 2021
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
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