Recent advances of organometallic complexes for rechargeable batteries

Wang, Dan-Yang; Liu, Ruilan; Guo, Wei; Li, Gang; Fu, Yongzhu

doi:10.1016/j.ccr.2020.213650

Cited by 57 publications

(44 citation statements)

References 146 publications

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“…[1] In the light of promoting efficient, safe, and low-polluting electrochemical energy storage systems, [2] electroactive organic materials (EOMs) have sparked considerable attention in recent compounds, [53] and the most recently reported N-substituted salts of viologen derivatives. [52] Since 2008 (a year witnessed as the modern area revival of EOMs), dozens of review articles have been published from different perspectives (e.g., molecular design, [20,22,23,27,41,42,49,50,[54][55][56][57][58][59][60][61][62][63][64][65][66][67][68][69] sustainability, [70,71] opportunity, [3,[72][73][74] practicability, [75][76][77][78] and technology [79][80][81][82] ). It is worth noting that most reviews are focused on OPEMs with less consideration to ONEMs, except two reviews dedicated to ONEMs for Na/K-ion batteries, [37,83] yet presenting only a summary of advances and no critical discussion or suggested solutions for remai...…”

Section: Introductionmentioning

confidence: 99%

Organic Negative Electrode Materials for Metal‐Ion and Molecular‐Ion Batteries: Progress and Challenges from a Molecular Engineering Perspective

Lakraychi

Dolhem

Vlad

et al. 2021

Advanced Energy Materials

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Thanks to their versatility and flexibility, EOMs have shown broad applicability as bulky solid [3] or dissolved [4,5] active material, in aqueous [6][7][8] or non-aqueous electrolyte, [9][10][11] for portable and stationary batteries, respectively. In practice, OEMs are explored as main active materials in LIBs, [12] beyond Li systems (e.g., hydrogen, [13,14] Na-ion, [15][16][17][18][19] K-ion, [20][21][22][23][24] and multivalent batteries like magnesium, [25,26] zinc, [27] or aluminum [28,29] ) and also redox flow batteries; [30] or as supporting active materials such as redox mediators for Li-O 2 batteries, [31] Li-source sacrificial materials for Li-ion capacitor [32] and redox electrolytes for high-energy supercapacitors. [33] In contrast to the state-of-the-art inorganic materials, whose reactivity is based on redox of transition metal center and consequently Li + de/insertion, [34,35] the redox reaction of EOMs is based on the charge state change of the redox moiety, [12] for which the charge compensation during redox can be either made by cations, referring to n-type systems, or by anions, belonging then to p-type system, according to the proposed Hünig's classification. [36,37] The richness of organic chemistry coupled with molecular modifications have provided thus far a plethora of molecules and architectures operating within a large potential window with high specific capacities, extended cycling stability and high cycling rate. This has enabled building a broad database of electroactive compounds for both positive and negative electrode applications. Organic positive electrode materials (OPEMs) certainly benefit from larger attention since there are more possibilities to explore, for example, conducting polymers, [38,39] nitroxides, and other stable organic radicals, [40][41][42][43] sulfur compounds, [11] as well as conjugated amines, [44][45][46] conjugated sulfonamides, [47] nitro-aromatics, [48] and carbonyls. [49,50] The latter being certainly the most explored category owing to major advances attained so far but also to opportunities for further improvements to attain simultaneously high energy and power densities combined with good cycling stability. [12] On the opposite side, the chemical library is less rich for organic negative electrode materials (ONEMs), primarily due to much focus on positive electrode chemistries, for which many issues and strategies are to be addressed and explored, respectively. Today, the ONEMs database counts fewer redox families as OPEMs one, with also less specific chemistries within each class. To cite some: the most studied conjugated dicarboxylates, [51] Hückel-stabilized Schiff base, [52] nitrogen-redox azo

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Section: Introductionmentioning

confidence: 99%

Organic Negative Electrode Materials for Metal‐Ion and Molecular‐Ion Batteries: Progress and Challenges from a Molecular Engineering Perspective

Lakraychi

Dolhem

Vlad

et al. 2021

Advanced Energy Materials

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“…13 In the context of alkali-ion storage, many MOFs have been reported as both positive and negative electrode materials. 6,8,10,11,13,20 Despite the high specific capacities attained, MOF-based negative electrodes (anode materials) require further improvements, and in particular to lower the redox potential, reduce the voltage hysteresis (and thus increase the energy efficiency), and augment the first-cycle Coulombic efficiency. MOF-based positive electrodes (cathode materials) are more challenging to design, and further innovation is desired with structure−composition−property synergy between organic linkers and metal nodes.…”

Section: Introductionmentioning

confidence: 99%

An Electrically Conducting Li-Ion Metal–Organic Framework

et al. 2021

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Metal–organic frameworks (MOFs) have emerged as an important, yet highly challenging class of electrochemical energy storage materials. The chemical principles for electroactive MOFs remain, however, poorly explored because precise chemical and structural control is mandatory. For instance, no anionic MOF with a lithium cation reservoir and reversible redox (like a conventional Li-ion cathode) has been synthesized to date. Herein, we report on electrically conducting Li-ion MOF cathodes with the generic formula Li2-M-DOBDC (wherein M = Mg2+ or Mn2+; DOBDC4– = 2,5-dioxido-1,4-benzenedicarboxylate), by rational control of the ligand to transition metal stoichiometry and secondary building unit (SBU) topology in the archetypal CPO-27. The accurate chemical and structural changes not only enable reversible redox but also induce a million-fold electrical conductivity increase by virtue of efficient electronic self-exchange facilitated by mix-in redox: 10–7 S/cm for Li2-Mn-DOBDC vs 10–13 S/cm for the isoreticular H2-Mn-DOBDC and Li2-Mg-DOBDC, or the Mn-CPO-27 compositional analogues. This particular SBU topology also considerably augments the redox potential of the DOBDC4– linker (from 2.4 V up to 3.2 V, vs Li+/Li0), a highly practical feature for Li-ion battery assembly and energy evaluation. As a particular cathode material, Li2-Mn-DOBDC displays an average discharge potential of 3.2 V vs Li+/Li0, demonstrates excellent capacity retention over 100 cycles, while also handling fast cycling rates, inherent to the intrinsic electronic conductivity. The Li2-M-DOBDC material validates the concept of reversible redox activity and electronic conductivity in MOFs by accommodating the ligand’s noncoordinating redox center through composition and SBU design.

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“…Although the long cycle success is to a certain extent due to the excellent conductivity and confinement, it still encounters the obstacle that carbon-based materials are less efficient in restricting polar polysulfides owing to their nonpolar properties. To further capture the polysulfide species, various approaches have been devoted to tune the polarity of the host materials (i.e., heteroatom doping carbon materials with N, P, and S) − or incorporate them with polar materials (metals, polar metallic oxides (Fe 3 O 4 , TiO 2 , Ti 4 O 7 , MnO 2 ), transition metal sulfide, metal organic frameworks (MOFs), MXene) into organometallic complexes (OMC) composed of organic and metal active parts (porphyrins, phthalocyanines), which offer an enhanced anchor effect to immobilize the soluble polysulfide species and dramatically alleviate the “shuttle effect”, thereby significantly promoting the cycling stability. Even though these composites have shown improved electrochemical performance, their electrochemical properties usually deteriorate in subsequent cycles because these composites designed for the physical encapsulation of sulfur within conductive carbon matrices are not enough to trap the polysulfides especially under long-term cycling, which leads to rapid cell failure.…”

Section: Introductionmentioning

confidence: 99%

Lithiated Sulfur-Incorporated, Polymeric Cathode for Durable Lithium–Sulfur Batteries with Promoted Redox Kinetics

Dong

Peng

et al. 2021

ACS Nano

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Even though lithium−sulfur (Li−S) batteries have made much progress in terms of the delivered specific capacity and cycling stability by the encapsulation of sulfur within conductive carbon matrixes or polar materials, challenges such as low active sulfur utilization and unacceptable Coulombic efficiency are still hindering their commercial use. Herein, a lithium-rich conjugated sulfur-incorporated, polymeric material based on poly(Li 2 S 6 -r-1,3diisopropenylbenzene) (DIB) is developed as a cathode material for high rate and stable Li−S batteries. Motivated by extra Li + ions affording fast Li + redox kinetics across the conjugated aromatic backbones, the Li-rich sulfur-based copolymer exhibits high delivery capacities (934 mAh g −1 at 120 cycles), impressive rate capabilities (727 mAh g −1 even under a current of 2 A g −1 ), and long electrochemical cycling performance over 500 cycles. Moreover, by use of the elastic nature and thermoplastic properties of the sulfur-incorporated, polymeric material, a prototype of a flexible Li−S pouch cell is constructed by using a poly(Li 2 S 6 -r-DIB) copolymer cathode and paired with the flexible carbon cloth/Si/Li anode, which exhibits stable electrochemical performance (658 mAh g −1 after 100 cycles) and operational capability even under folding at various angle (30°, 60°, 90°, 120°, 150°, 180°). This work extends the molecular-design approach to obtaining a high-performance organosulfur cathode material by introducing extra Li + ions to promote redox kinetics, which provides valuable guidance for the development of high-performance Li−S batteries for practical applications.

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Recent advances of organometallic complexes for rechargeable batteries

Cited by 57 publications

References 146 publications

Organic Negative Electrode Materials for Metal‐Ion and Molecular‐Ion Batteries: Progress and Challenges from a Molecular Engineering Perspective

Organic Negative Electrode Materials for Metal‐Ion and Molecular‐Ion Batteries: Progress and Challenges from a Molecular Engineering Perspective

An Electrically Conducting Li-Ion Metal–Organic Framework

Lithiated Sulfur-Incorporated, Polymeric Cathode for Durable Lithium–Sulfur Batteries with Promoted Redox Kinetics

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