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  • Wiley  (15)
  • Yan, Zhenhua  (15)
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  • Wiley  (15)
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  • 1
    Online Resource
    Online Resource
    Designing Quinone‐Based Anodes with Rapid Kinetics for Rechargeable Proton Batteries
    Wiley ; 2022
    In:  Angewandte Chemie Vol. 134, No. 39 ( 2022-09-26)
    Details
    In: Angewandte Chemie, Wiley, Vol. 134, No. 39 ( 2022-09-26)
    Abstract: Quinone compounds, which are capable of accommodating proton (H + ), are emerging electrodes in aqueous batteries. However, the storage mechanism of proton in quinone compounds is less known and the energy/power density of quinone‐based proton battery is still limited. Here we design a series of quinone anodes and study their electrochemical properties in acidic electrolyte, in which tetramethylquinone (TMBQ) delivers a high capacity of 300 mAh g −1 with an extremely low polarization of 20 mV at 1 C, and maintains over 50 % theoretical capacity in less than 16 seconds. The fast kinetics of TMBQ is attributed to the continuous H + migration channel, high H + diffusion coefficient (10 −6  cm 2  s −1 ), and low H + migration energy barrier (0.26 eV). When coupling with MnO 2 cathode, the battery shows a long lifespan of 4000 cycles with a capacity retention of 77 % at 5 C. This study reveals the proton transport in quinone‐electrodes and offers new insights to design advanced aqueous batteries.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    URL: Article
    DOI: 10.1002/ange.v134.39
    DOI: 10.1002/ange.202209642
    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
  • 2
    Online Resource
    Online Resource
    Insights into the Ionic Conduction Mechanism of Quasi‐Solid Polymer Electrolytes through Multispectral Characterization
    Wiley ; 2021
    In:  Angewandte Chemie Vol. 133, No. 42 ( 2021-10-11), p. 22854-22859
    Details
    In: Angewandte Chemie, Wiley, Vol. 133, No. 42 ( 2021-10-11), p. 22854-22859
    Abstract: Quasi‐solid polymer electrolytes (QPE) composed of Li salts, polymer matrix, and solvent, are beneficial for improving the security and energy density of batteries. However, the ionic conduction mechanism, existential form of solvent molecules, and interactions between different components of QPE remain unclear. Here we develop a multispectral characterization strategy combined with first‐principles calculations to unravel aforesaid mysteries. The results indicate that the existential state of solvent in QPE is quite different from that in liquid electrolyte. The Li cations in gel polymer electrolyte are fully solvated by partial solvent molecules to form a local high concentration of Li + , while the other solvent molecules are fastened by polymer matrix in QPE. As a result, the solvation structure and conduction mechanism of Li + are similar to those in high‐concentrated liquid electrolyte. This work provides a new insight into the ionic conduction mechanism of QPE and will promote its application for safe and high‐energy batteries.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    URL: Article
    DOI: 10.1002/ange.v133.42
    DOI: 10.1002/ange.202107648
    RVK:
    VA 2100
    RVK:
    VN 5020
    Language: English
    Publisher: Wiley
    Publication Date: 2021
    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
    A Universal Graphene Quantum Dot Tethering Design Strategy to Synthesize Single‐Atom Catalysts
    Wiley ; 2020
    In:  Angewandte Chemie International Edition Vol. 59, No. 49 ( 2020-12), p. 21885-21889
    Details
    In: Angewandte Chemie International Edition, Wiley, Vol. 59, No. 49 ( 2020-12), p. 21885-21889
    Abstract: A general graphene quantum dot‐tethering design strategy to synthesize single‐atom catalysts (SACs) is presented. The strategy is applicable to different metals (Cr, Mn, Fe, Co, Ni, Cu, and Zn) and supports (0D carbon nanosphere, 1D carbon nanotube, 2D graphene nanosheet, and 3D graphite foam) with the metal loading of 3.0–4.5 wt %. The direct transmission electron microscopy imaging and X‐ray absorption spectra analyses confirm the atomic dispersed metal in carbon supports. Our study reveals that the abundant oxygenated groups for complexing metal ions and the rich defective sites for incorporating nitrogen are essential to realize the synthesis of SACs. Furthermore, the carbon nanotube supported Ni SACs exhibits high electrocatalytic activity for CO 2 reduction with nearly 100 % CO selectivity. This universal strategy is expected to open up new research avenues to produce SACs for diverse electrocatalytic applications.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    URL: Article
    DOI: 10.1002/anie.v59.49
    DOI: 10.1002/anie.202008422
    RVK:
    VA 2100
    Language: English
    Publisher: Wiley
    Publication Date: 2020
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
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  • 4
    Online Resource
    Online Resource
    Regulating Electrocatalytic Oxygen Reduction Activity of a Metal Coordination Polymer via d–π Conjugation
    Wiley ; 2021
    In:  Angewandte Chemie International Edition Vol. 60, No. 31 ( 2021-07-26), p. 16937-16941
    Details
    In: Angewandte Chemie International Edition, Wiley, Vol. 60, No. 31 ( 2021-07-26), p. 16937-16941
    Abstract: Non‐noble transition metal complexes have attracted growing interest as efficient electrocatalysts for oxygen reduction reaction (ORR) while their activities still lack rational and effective regulation. Herein, we propose a d–π conjugation strategy for rough and fine tuning of ORR activity of TM‐BTA (TM=Mn/Fe/Co/Ni/Cu, BTA=1,2,4,5‐benzenetetramine) coordination polymers. By first‐principle calculations, we elucidate that the strong d–π conjugation elevates the d xz /d yz orbitals of TM centers to enhance intermediate adsorption and strengthens the electronic modulation effect from substitute groups on ligands. Based on this strategy, Co‐TABQ (tetramino benzoquinone) is found to approach the top of ORR activity volcano. The synthesized Co‐TABQ with atomically distributed Co on carbon nanotubes exhibits a half‐wave potential of 0.85 V and a specific current of 127 mA mg metal −1 at 0.8 V, outperforming the benchmark Pt/C. The high activity, low peroxide yield, and considerable durability of Co‐BTA and Co‐TABQ promise their application in oxygen electrocatalysis. This study provides mechanistic insight into the rational design of transition metal complex catalysts.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    URL: Article
    DOI: 10.1002/anie.v60.31
    DOI: 10.1002/anie.202104494
    RVK:
    VA 2100
    Language: English
    Publisher: Wiley
    Publication Date: 2021
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
    Location Call Number Limitation Availability
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    Online Resource
  • 5
    Online Resource
    Online Resource
    Designing Quinone‐Based Anodes with Rapid Kinetics for Rechargeable Proton Batteries
    Wiley ; 2022
    In:  Angewandte Chemie International Edition Vol. 61, No. 39 ( 2022-09-26)
    Details
    In: Angewandte Chemie International Edition, Wiley, Vol. 61, No. 39 ( 2022-09-26)
    Abstract: Quinone compounds, which are capable of accommodating proton (H + ), are emerging electrodes in aqueous batteries. However, the storage mechanism of proton in quinone compounds is less known and the energy/power density of quinone‐based proton battery is still limited. Here we design a series of quinone anodes and study their electrochemical properties in acidic electrolyte, in which tetramethylquinone (TMBQ) delivers a high capacity of 300 mAh g −1 with an extremely low polarization of 20 mV at 1 C, and maintains over 50 % theoretical capacity in less than 16 seconds. The fast kinetics of TMBQ is attributed to the continuous H + migration channel, high H + diffusion coefficient (10 −6  cm 2  s −1 ), and low H + migration energy barrier (0.26 eV). When coupling with MnO 2 cathode, the battery shows a long lifespan of 4000 cycles with a capacity retention of 77 % at 5 C. This study reveals the proton transport in quinone‐electrodes and offers new insights to design advanced aqueous batteries.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    URL: Article
    DOI: 10.1002/anie.v61.39
    DOI: 10.1002/anie.202209642
    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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  • 6
    Online Resource
    Online Resource
    A computational study of Mg m H n nanoclusters with n : m  ≥ 2:1 for efficient hydrogen storage
    Wiley ; 2023
    In:  International Journal of Quantum Chemistry Vol. 123, No. 6 ( 2023-03-15)
    Details
    In: International Journal of Quantum Chemistry, Wiley, Vol. 123, No. 6 ( 2023-03-15)
    Abstract: Magnesium‐based hydrogen storage material (MgH 2 ) has attracted much attention due to its high hydrogen storage density (7.6 wt%). However, the high hydrogen dissociation enthalpy and slow hydrogen dissociation rate in bulk Mg hinder its wide application in the efficient hydrogen storage. In the present work, we study the hydrogen adsorption and desorption reactions of Mg m H n ( m  = 1–6) nanoclusters using density functional theory. From the global search for the configurations of Mg m H n nanoclusters, we found not only stable saturated Mg m H n ( n  = 2 m ) nanoclusters, but four hydrogen‐enriched Mg m H n ( n : m   〉  2:1) nanoclusters, Mg 3 H 7 , Mg 4 H 9 , Mg 5 H 11 , Mg 6 H 13 , with the hydrogen storage density higher than 8.3 wt%. The electronic‐structure calculations indicate that the stability of the hydrogen‐enriched cluster gets relatively higher for larger nanocluster. The ab initio dynamics simulations shows that all hydrogen‐enriched clusters have very fast hydrogen dissociation rates, which is promising for the hydrogen dissociation at ambient temperature and pressure. This work provides valuable insights into the hydrogen storage mechanism of nano‐magnesium materials.
    Type of Medium: Online Resource
    ISSN: 0020-7608 , 1097-461X
    URL: Issue
    URL: Article
    DOI: 10.1002/qua.v123.6
    DOI: 10.1002/qua.27058
    Language: English
    Publisher: Wiley
    Publication Date: 2023
    detail.hit.zdb_id: 1475014-4
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    Online Resource
  • 7
    Online Resource
    Online Resource
    Regulating Electrocatalytic Oxygen Reduction Activity of a Metal Coordination Polymer via d–π Conjugation
    Wiley ; 2021
    In:  Angewandte Chemie Vol. 133, No. 31 ( 2021-07-26), p. 17074-17078
    Details
    In: Angewandte Chemie, Wiley, Vol. 133, No. 31 ( 2021-07-26), p. 17074-17078
    Abstract: Non‐noble transition metal complexes have attracted growing interest as efficient electrocatalysts for oxygen reduction reaction (ORR) while their activities still lack rational and effective regulation. Herein, we propose a d–π conjugation strategy for rough and fine tuning of ORR activity of TM‐BTA (TM=Mn/Fe/Co/Ni/Cu, BTA=1,2,4,5‐benzenetetramine) coordination polymers. By first‐principle calculations, we elucidate that the strong d–π conjugation elevates the d xz /d yz orbitals of TM centers to enhance intermediate adsorption and strengthens the electronic modulation effect from substitute groups on ligands. Based on this strategy, Co‐TABQ (tetramino benzoquinone) is found to approach the top of ORR activity volcano. The synthesized Co‐TABQ with atomically distributed Co on carbon nanotubes exhibits a half‐wave potential of 0.85 V and a specific current of 127 mA mg metal −1 at 0.8 V, outperforming the benchmark Pt/C. The high activity, low peroxide yield, and considerable durability of Co‐BTA and Co‐TABQ promise their application in oxygen electrocatalysis. This study provides mechanistic insight into the rational design of transition metal complex catalysts.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    URL: Article
    DOI: 10.1002/ange.v133.31
    DOI: 10.1002/ange.202104494
    RVK:
    VA 2100
    RVK:
    VN 5020
    Language: English
    Publisher: Wiley
    Publication Date: 2021
    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
    Location Call Number Limitation Availability
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    Online Resource
  • 8
    Online Resource
    Online Resource
    A Universal Graphene Quantum Dot Tethering Design Strategy to Synthesize Single‐Atom Catalysts
    Wiley ; 2020
    In:  Angewandte Chemie Vol. 132, No. 49 ( 2020-12), p. 22069-22073
    Details
    In: Angewandte Chemie, Wiley, Vol. 132, No. 49 ( 2020-12), p. 22069-22073
    Abstract: A general graphene quantum dot‐tethering design strategy to synthesize single‐atom catalysts (SACs) is presented. The strategy is applicable to different metals (Cr, Mn, Fe, Co, Ni, Cu, and Zn) and supports (0D carbon nanosphere, 1D carbon nanotube, 2D graphene nanosheet, and 3D graphite foam) with the metal loading of 3.0–4.5 wt %. The direct transmission electron microscopy imaging and X‐ray absorption spectra analyses confirm the atomic dispersed metal in carbon supports. Our study reveals that the abundant oxygenated groups for complexing metal ions and the rich defective sites for incorporating nitrogen are essential to realize the synthesis of SACs. Furthermore, the carbon nanotube supported Ni SACs exhibits high electrocatalytic activity for CO 2 reduction with nearly 100 % CO selectivity. This universal strategy is expected to open up new research avenues to produce SACs for diverse electrocatalytic applications.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    URL: Article
    DOI: 10.1002/ange.v132.49
    DOI: 10.1002/ange.202008422
    RVK:
    VA 2100
    RVK:
    VN 5020
    Language: English
    Publisher: Wiley
    Publication Date: 2020
    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
    Location Call Number Limitation Availability
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  • 9
    Online Resource
    Online Resource
    Lattice Strained Induced Spin Regulation Hydrogen Bonding in Co‐N/S‐coordination‐framework Enhanced Oxygen Reduction
    Wiley ; 2024
    In:  Angewandte Chemie International Edition
    Details
    In: Angewandte Chemie International Edition, Wiley
    Abstract: Oxygen reduction reaction (ORR) is the bottleneck of metal‐air batteries and fuel cells. Strain regulation can change the geometry and adjust the surface charge distribution of catalysts, which is a powerful strategy to optimize the ORR activity. The introduction of controlled strain to the material is still difficult to achieve. Herein, we present a temperature‐pressure‐induced strategy to achieve the controlled lattice strain for metal coordination polymers. Through the systematic study of the strain effect on ORR performance, the relationship between geometric and electronic effects is further understood and confirmed. The strained Co‐DABDT (DABDT=2,5‐diaminobenzene‐1,4‐dithiol) with 2% lattice compression exhibits a superior half‐wave potential of 0.81 V. Theoretical analysis reveals that the lattice strain changes spin‐charge densities around S atoms for Co‐DABDT, and then regulates the hydrogen bond interaction with intermediates to promote the ORR catalytic process. This work helps to understand the catalytic mechanism from the atomic level.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Article
    DOI: 10.1002/anie.202319518
    RVK:
    VA 2100
    Language: English
    Publisher: Wiley
    Publication Date: 2024
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
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  • 10
    Online Resource
    Online Resource
    Suppressing Bulk Strain and Surface O 2 Release in Li‐rich Cathodes by Just Tuning the Li Content
    Wiley ; 2023
    In:  Advanced Materials
    Details
    In: Advanced Materials, Wiley
    Abstract: Layered oxides represent a prominent class of cathode materials extensively employed in lithium‐ion batteries. The structural degradation of layered cathodes causes the capacity decay during battery cycling, which is generally induced by anisotropic lattice strain in the bulk of the cathode particle and undesirable oxygen release at the surface. However, particularly in lithium‐rich layered oxides (LLOs) that undergo intense oxygen redox reactions, the challenge of simultaneously addressing bulk and surface issues through a singular modification technique remains arduous. Here we construct a thin (1‐nm) and coherent spinel‐like phase on the surface of LLOs particle (Li x Mn 0.54 Ni 0.13 Co 0.13 O 2 ) to suppress bulk strain and surface O 2 release by just adjusting the amount of lithium source during synthesis. The spinel‐like phase hinders the surface O 2 release by accommodating O 2 inside the surface layer, while the trapped O 2 in the bulk lattice impedes strain evolution by about 70% at high voltages compared with unmodified LLOs cathodes. Consequently, the enhanced structural stability in bulk and surface leads to a significantly improved capacity retention of 97.6% and a high Coulombic efficiency of about 99.5% after 100 cycles at a rate of 0.1 C. Our findings provide profound mechanistic insights into the functioning of surface structure and offer guidance for synthesizing high‐capacity cathodes with superior cyclability. This article is protected by copyright. All rights reserved
    Type of Medium: Online Resource
    ISSN: 0935-9648 , 1521-4095
    URL: Article
    DOI: 10.1002/adma.202307617
    RVK:
    UA 1538
    Language: English
    Publisher: Wiley
    Publication Date: 2023
    detail.hit.zdb_id: 1474949-X
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