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  • Wiley  (12)
  • Yan, Zhenhua  (12)
  • Chemistry/Pharmacy  (12)
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  • Wiley  (12)
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  • Chemistry/Pharmacy  (12)
RVK
  • 1
    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
    RVK:
    RVK:
    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
    Location Call Number Limitation Availability
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  • 2
    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
    RVK:
    RVK:
    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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  • 3
    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
    RVK:
    Language: English
    Publisher: Wiley
    Publication Date: 2020
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
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  • 4
    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
    RVK:
    Language: English
    Publisher: Wiley
    Publication Date: 2021
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
    Location Call Number Limitation Availability
    BibTip Others were also interested in ...
  • 5
    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
    RVK:
    Language: English
    Publisher: Wiley
    Publication Date: 2022
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
    Location Call Number Limitation Availability
    BibTip Others were also interested in ...
  • 6
    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
    RVK:
    RVK:
    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
    BibTip Others were also interested in ...
  • 7
    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
    RVK:
    RVK:
    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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  • 8
    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
    RVK:
    Language: English
    Publisher: Wiley
    Publication Date: 2024
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
    Location Call Number Limitation Availability
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  • 9
    In: Angewandte Chemie, Wiley, Vol. 134, No. 35 ( 2022-08-26)
    Abstract: Cathode electrolyte interphases (CEIs) are critical to the cycling stability of high‐voltage cathodes for batteries, yet their formation mechanism and properties remain elusive. Here we report that the compositions of CEIs are largely controlled by abundant species in the inner Helmholtz layer (IHL) and can be tuned from material aspects. The IHL of LiCoO 2 (LCO) was found to alter after charging, with a solvent‐rich environment that results in fragile organic‐rich CEIs. By passivated spinel Li 4 Mn 5 O 12 coating, we achieve an anion‐rich IHL after charging, thus enabling robust LiF‐rich CEIs. In situ microscopy reveals that LiF‐rich CEIs maintain mechanical integrity at 500 °C, in sharp contrast to organic‐rich CEIs which undergo severe expansion and subsequent voids/cracks in the cathode. As a result, the spinel‐coated LCO exhibits a high specific capacity of 194 mAh g −1 at 0.05 C and a capacity retention of 83 % after 300 cycles at 0.5 C. Our work sheds new light on modulating CEIs for advanced lithium‐ion batteries.
    Type of Medium: Online Resource
    ISSN: 0044-8249 , 1521-3757
    URL: Issue
    RVK:
    RVK:
    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
    Location Call Number Limitation Availability
    BibTip Others were also interested in ...
  • 10
    In: Angewandte Chemie International Edition, Wiley, Vol. 61, No. 35 ( 2022-08-26)
    Abstract: Cathode electrolyte interphases (CEIs) are critical to the cycling stability of high‐voltage cathodes for batteries, yet their formation mechanism and properties remain elusive. Here we report that the compositions of CEIs are largely controlled by abundant species in the inner Helmholtz layer (IHL) and can be tuned from material aspects. The IHL of LiCoO 2 (LCO) was found to alter after charging, with a solvent‐rich environment that results in fragile organic‐rich CEIs. By passivated spinel Li 4 Mn 5 O 12 coating, we achieve an anion‐rich IHL after charging, thus enabling robust LiF‐rich CEIs. In situ microscopy reveals that LiF‐rich CEIs maintain mechanical integrity at 500 °C, in sharp contrast to organic‐rich CEIs which undergo severe expansion and subsequent voids/cracks in the cathode. As a result, the spinel‐coated LCO exhibits a high specific capacity of 194 mAh g −1 at 0.05 C and a capacity retention of 83 % after 300 cycles at 0.5 C. Our work sheds new light on modulating CEIs for advanced lithium‐ion batteries.
    Type of Medium: Online Resource
    ISSN: 1433-7851 , 1521-3773
    URL: Issue
    RVK:
    Language: English
    Publisher: Wiley
    Publication Date: 2022
    detail.hit.zdb_id: 2011836-3
    detail.hit.zdb_id: 123227-7
    Location Call Number Limitation Availability
    BibTip Others were also interested in ...
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