Insight into the decay mechanism of cycling capacitance for layered double hydroxides at subnanometer scale

Zhao, Jie; Guo, Yue; Yang, Yuqi; Shen, Zhen; Wu, Qiang; Yang, Lijun; Wang, Xizhang; Zheng, Hu

doi:10.1039/d2cc02633c

Cited by 20 publications

(4 citation statements)

References 36 publications

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“…Due to a bunch of advantages, the poor cycling stability is its Achille's heel. [ 10 ] The unremitting redox reaction of transition metal ions, [ 11 ] Jahn–Teller distortion, [ 12 ] phase change, [ 13 ] weak interaction between LDHs, and current collector [ 14 ] could cause serious volume change, agglomeration, exfoliation, and performance degradation of LDHs after hundreds of cycles, preventing it from practical applications.…”

Section: Introductionmentioning

confidence: 99%

Exceeding 50 000 Cycle Durability of Layered Hydroxide‐Based Hybrid Supercapacitor Through Scandium Doping‐Induced Superlong Activation Process

Hu,

et al. 2024

Small Structures

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Layered double hydroxides (LDHs) are a class of promising cathode materials for supercapacitors. However, the bad cycling performance has always been the Achilles’ heel of LDHs‐based supercapacitors. In this contribution, a nonelectrochemical active element Scandium (Sc) is doped into NiCo‐LDHs to greatly improve the intrinsic cycling performance of active materials. The trimetallic NiCoSc‐LDHs exhibit an ultralong cycle lifespan with 40 000 charge–discharge cycles (exceeding 50 days) and a high specific capacity of 196 mAh g−1 (1695 F g−1). Sc doping greatly changes the degradation mode of NiCo‐LDHs from rapid decay in thousands of cycles to a two‐stage performance evolution, which consists of a superlong activation process of about 10 000 cycles and then extremely slow degradation. Moreover, Sc doping enhances the electrochemical activity of Ni3+, so as to not only avoid its Jahn–Teller distortion, but also perform as a structural stabilizer to alleviate the local strain of host layer. The assembled asymmetric supercapacitor delivers an ultralong cycling lifespan with 101% capacity retention even after 50 000 cycles. This work presents a new pathway to significantly improve the electrochemical performance, especially the cycling stability of LDH‐based electrodes for high‐performance supercapacitors.

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Section: Introductionmentioning

confidence: 99%

Exceeding 50 000 Cycle Durability of Layered Hydroxide‐Based Hybrid Supercapacitor Through Scandium Doping‐Induced Superlong Activation Process

Hu,

et al. 2024

Small Structures

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“…78 The energy density can be increased through designing and fabricating electrode materials. [79][80][81][82] 2D layered double hydroxides (LDHs) 83,84 have a high specific surface area and abundant ion insertion sites and have received focus because of high theoretical specific capacitance, [85][86][87][88][89] showing good prospects for applications in supercapacitors. There are mainly metal cations (M 2+ , M 3+ ) and interlayer anions (A nÀ ) and solvent molecules (H 2 O) in the hydroxide layer.…”

Section: Introductionmentioning

confidence: 99%

Progress of layered double hydroxide-based materials for supercapacitors

Ren

Sridhar³

et al. 2023

Mater. Chem. Front.

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“…Specifically, oxygen vacancies in LDHs have been proven as active sites for the chemisorption of N 2 molecules, optimizing the reaction kinetics and lowering the reaction energy barrier as confirmed by theoretical and experimental results. − On the other hand, the adjustable interlayer spacing of LDHs allows the interlayer anions to be exchanged by a wide variety of anionic species (CO 3 2– , dicarboxylic acid, organic ionic liquids, etc.) for improving the inherent functionality in catalysis. − In this stage, polyoxometalates (POMs), a typical class of high-valence early transition polyoxoanions, act as a promising candidate to combine with defect LDH materials through an anion exchange strategy because (i) POMs as intercalated anion species can support layered metal laminates via intermolecular interactions, such as electrostatic and hydrogen bond networks, due to their high-negative charge surface, which is in favor of constructing accessible POM-LDH composite materials. (ii) Reduced POMs (mixed-valence POMs) are well known for a broad and strong absorption spectrum including the near-infrared and visible regions due to their metal-to-metal charge transfer or intervalence charge transfer (IVCT), manifesting a fire-new type of light absorber species as a driving force that can promote the nitrogen photofixation reaction.…”

Section: Introductionmentioning

confidence: 99%

Photochemical Ammonia Synthesis over Reduced Polyoxovanadate-Intercalated Defective ZnAl Layered Double Hydroxide Nanosheets

Chen

et al. 2023

Inorg. Chem.

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The exploration of efficient and stable N 2 fixation photocatalysts featuring a broad absorption spectrum and N 2 fixation active sites has become specifically conspicuous. Herein, a series of reduced polyoxovanadates (POVs) were intercalated into copper-induced ZnAl layered double hydroxide (0.5%-ZnAl LDH) nanosheets with oxygen vacancies via an anion exchange strategy toward green ammonia production. The intervalence charge transfer arising from mixedvalence POV materials is responsible for its light-harvesting behavior, and the LDHs lay the foundation for the chemical adsorption and activation process of nitrogen molecules; both contributions facilitate the nitrogen photofixation performance of such composite materials. As predicted, the catalytic efficiency of V 34 /0.5%-ZnAl is 7.0 times higher than 0.5%-ZnAl LDH. Therefore, such an all-inorganic system exhibits an apparent quantum efficiency of 0.3137% at 500 nm. The strategy of "working in tandem" established by POV-based light-absorber species and oxygen vacancies as the sites for N 2 activation is extremely vital for enhanced ammonia formation. This work opens up a versatile insight for the rational design of an efficient photo-driven nitrogenreduction composite catalyst toward sustainable ammonia production compared to the industrial Haber−Bosch process.

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Insight into the decay mechanism of cycling capacitance for layered double hydroxides at subnanometer scale

Abstract: The application of layered double hydroxides (LDHs) in supercapacitors is encouraged by their high capacitances but still limited by deficient cycling stability. The remarkable capacitance decay of LDHs during cycling...

Cited by 20 publications

References 36 publications

Exceeding 50 000 Cycle Durability of Layered Hydroxide‐Based Hybrid Supercapacitor Through Scandium Doping‐Induced Superlong Activation Process

Exceeding 50 000 Cycle Durability of Layered Hydroxide‐Based Hybrid Supercapacitor Through Scandium Doping‐Induced Superlong Activation Process

Progress of layered double hydroxide-based materials for supercapacitors

Photochemical Ammonia Synthesis over Reduced Polyoxovanadate-Intercalated Defective ZnAl Layered Double Hydroxide Nanosheets

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