A bidirectional electrocatalyst for enhancing Li<sub>2</sub>S nucleation and decomposition kinetics in lithium–sulfur batteries

Ren, Yilun; Chang, Shengli; Hu, Libing; Wang, Biao; Sun, Dongyue; Wu, Hao Bin; Ma, Yujie; Yang, Yurong; Tang, Shaochun; Meng, Xiangkang

doi:10.1039/d2ta05046c

Cited by 26 publications

(10 citation statements)

References 59 publications

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“…However, the current investigation is mainly based on the COFs hybrid structure with inorganic semiconductors, which might cause the issue of H 2 O 2 decomposition. Until now, only an example of COF‐based composite integrated with carbon dots (CDs) was designed for H 2 O 2 photosynthesis (see Table 1, entry 38) [66] . More organic materials, such as PCN or graphene nanosheets, should be considered to form hybrids with COFs and exploit their potential in this field.…”

Section: Strategies To Improve Photocatalytic H2o2 Productionmentioning

confidence: 99%

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Solar‐to‐H₂O₂ Catalyzed by Covalent Organic Frameworks

Yong,

2023

Angew Chem Int Ed

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Benefiting from the excellent structural tunability, robust framework, ultrahigh porosity, and rich active sites, covalent organic frameworks (COFs) are widely recognized as promising photocatalysts in chemical conversions, and emerged in the hydrogen peroxide (H2O2) photosynthesis from 2020. H2O2, serving as an environmental‐friendly oxidant and a promising liquid fuel, has attracted increasing researchers to explore its potential. Over the past few years, numerous COFs‐based photocatalysts are developed with encouraging achievements in H2O2 production, whereas no comprehensive review articles exist to summarize this specific and significant area. Herein we provide a systematic overview of the advances and challenges of COFs in photocatalytic H2O2 production. We first introduce the priorities of COFs in H2O2 photosynthesis. Then, various strategies to improve COFs photocatalytic efficiency are discussed. The perspective and outlook for future advances of COFs in this emerging field are finally offered. This timely review will pave the way for the development of highly efficient COFs photocatalysts for practical production of value‐added chemical not limited to H2O2.

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Section: Strategies To Improve Photocatalytic H2o2 Productionmentioning

confidence: 99%

“…Also, due to the porous structure of COFs, it's the perfect platform to introduce co‐catalysts as extra catalytic sites. However, few papers are reported on COFs hybrids [35,62–66] . Therefore, it's urgent to develop COFs hybrids and introduce more active sites for efficient H 2 O 2 production.…”

Section: Perspective and Outlookmentioning

confidence: 99%

Solar‐to‐H₂O₂ Catalyzed by Covalent Organic Frameworks

Yong,

2023

Angew Chem Int Ed

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“…The oxidation peaks at 0.13 and 0.50 V can be assigned to the reversed process of the above‐mentioned reduction reaction. [ 10 ] The largest redox current of MnSA@HNC electrode illustrates the most efficient facilitation of the LiPSs electrochemical conversion. The well‐overlapped CV curves upon several cycles in Figure S11 (Supporting Information) also indicated the excellent redox reversibility and stability of MnSA@HNC.…”

Section: Resultsmentioning

confidence: 99%

“…[3,4] Compared with conventional transition metal compounds such as nitrides, oxides, sulfides, selenides, etc., single atom catalyst (SAC) has unique geometric and electronic structures, maximized atomic utilization as well as high electrocatalytic activity and selectivity. [5][6][7][8][9][10][11][12] In addition, the metal single-atom sites hardly change the specific surface and pore structure of the carbonaceous skeleton, and can enhance the electronic conductivity and polarity of the carbonaceous matrix. [13] Therefore, the carbon-based SAC combining advantage of heterogeneous and homogeneous catalysts becomes a research hotspot in the catalytic realm.…”

Section: Introductionmentioning

confidence: 99%

A Transmetalation Synthetic Strategy to Engineer Atomically Dispersed MnN₂O₂ Electrocatalytic Centers Driving High‐Performance LiS Battery

Zhang

Luo

Xiao

et al. 2023

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Sluggish sulfur redox reaction (SROR) kinetics accompanying lithium polysulfides (LiPSs) shuttle effect becomes a stumbling block for commercial application of LiS battery. High‐efficient single atom catalysts (SACs) are desired to improve the SROR conversion capability; however, the sparse active sites as well as partial sites encapsulated in bulk‐phase are fatal to the catalytic performance. Herein, high loading (5.02 wt.%) atomically dispersed manganese sites (MnSA) on hollow nitrogen‐doped carbonaceous support (HNC) are realized for the MnSA@HNC SAC by a facile transmetalation synthetic strategy. The thin‐walled hollow structure (≈12 nm) anchoring the unique trans‐MnN2O2 sites of MnSA@HNC provides a shuttle buffer zone and catalytic conversion site for LiPSs. Both electrochemical measurement and theoretical calculation indicate that the MnSA@HNC with abundant trans‐MnN2O2 sites have extremely high bidirectional SROR catalytic activity. The assembled LiS battery based on the MnSA@HNC modified separator can deliver a large specific capacity of 1422 mAh g−1 at 0.1 C and stable cycling over 1400 cycles with an ultralow decay rate of 0.033% per cycle at 1 C. More impressively, a flexible pouch cell on account of the MnSA@HNC modified separator may release a high initial specific capacity of 1192 mAh g−1 at 0.1 C and uninterruptedly work after the bending‐unbending processes.

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“…However, most of the reported strategies of electronic structure regulation are based on the assumption that the electrocatalysts are stable under cycling conditions. Meanwhile, the resulting catalytic mechanisms, such as stepwise catalysis, [103][104][105][106] selective catalysis, [107] and bidirectional catalysis, [107][108][109][110][111] also rely on the premise that the electrocatalysts are stable during the testing process. It is very likely that most of the reported electron regulation strategies and the resulting catalytic mechanisms should be re-examined when the electrocatalysts undergo dynamic evolution during the charge/ discharge process.…”

Section: Introductionmentioning

confidence: 99%

In Situ Reconstruction of Electrocatalysts for Lithium–Sulfur Batteries: Progress and Prospects

Zhang

Wang

et al. 2023

Adv Funct Materials

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The current research of Li–S batteries primarily focuses on increasing the catalytic activity of electrocatalysts to inhibit the polysulfide shuttling and enhance the redox kinetics. However, the stability of electrocatalysts is largely neglected, given the premise that they are stable over extended cycles. Notably, the reconstruction of electrocatalysts during the electrochemical reaction process has recently been proposed. Such in situ reconstruction process inevitably leads to varied electrocatalytic behaviors, such as catalytic sites, selectivity, activity, and amounts of catalytic sites. Therefore, a crucial prerequisite for the design of highly effective electrocatalysts for Li–S batteries is an in‐depth understanding of the variation of active sites and the influence factors for the in situ reconstruction behaviors, which has not achieved a fundamental understanding and summary. This review comprehensively summarizes the recent advances in understanding the reconstruction behaviors of different electrocatalysts for Li–S batteries during the electrochemical reaction process, mainly including metal nitrides, metal oxides, metal selenides, metal fluorides, metals/alloys, and metal sulfides. Moreover, the unexplored issues and major challenges of understanding the reconstruction chemistry are summarized and prospected. Based on this review, new perspectives are offered into the reconstruction and true active sites of electrocatalysts for Li–S batteries.

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A bidirectional electrocatalyst for enhancing Li₂S nucleation and decomposition kinetics in lithium–sulfur batteries

Abstract: Accelerating sulfur redox reactions and suppressing the shuttle effect of lithium polysulfide (LiPSs) are crucial for high-performance lithium-sulfur (Li-S) batteries. Herein, we develop a highly efficient bidirectional electrocatalyst (Ti3C2/(NiCo)0.85Se) consisting...

Cited by 26 publications

References 59 publications

Solar‐to‐H₂O₂ Catalyzed by Covalent Organic Frameworks

Solar‐to‐H₂O₂ Catalyzed by Covalent Organic Frameworks

A Transmetalation Synthetic Strategy to Engineer Atomically Dispersed MnN₂O₂ Electrocatalytic Centers Driving High‐Performance LiS Battery

In Situ Reconstruction of Electrocatalysts for Lithium–Sulfur Batteries: Progress and Prospects

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A bidirectional electrocatalyst for enhancing Li2S nucleation and decomposition kinetics in lithium–sulfur batteries

Abstract: Accelerating sulfur redox reactions and suppressing the shuttle effect of lithium polysulfide (LiPSs) are crucial for high-performance lithium-sulfur (Li-S) batteries. Herein, we develop a highly efficient bidirectional electrocatalyst (Ti3C2/(NiCo)0.85Se) consisting...

Cited by 26 publications

References 59 publications

Solar‐to‐H2O2 Catalyzed by Covalent Organic Frameworks

Solar‐to‐H2O2 Catalyzed by Covalent Organic Frameworks

A Transmetalation Synthetic Strategy to Engineer Atomically Dispersed MnN2O2 Electrocatalytic Centers Driving High‐Performance LiS Battery

In Situ Reconstruction of Electrocatalysts for Lithium–Sulfur Batteries: Progress and Prospects

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A bidirectional electrocatalyst for enhancing Li₂S nucleation and decomposition kinetics in lithium–sulfur batteries

Solar‐to‐H₂O₂ Catalyzed by Covalent Organic Frameworks

Solar‐to‐H₂O₂ Catalyzed by Covalent Organic Frameworks

A Transmetalation Synthetic Strategy to Engineer Atomically Dispersed MnN₂O₂ Electrocatalytic Centers Driving High‐Performance LiS Battery