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• W2945113119 abstract "In their recent publication in Nature, Kang Xu, Chunsheng Wang, and co-authors reported for the first time on a novel halogen conversion-intercalation graphite cathode chemistry for the development of high-energy aqueous batteries. As evidenced by experimental works and modeling, a densely packed stage-1 graphite intercalation compound (GIC) with a stoichiometry of C3.5[Br0.5Cl0.5] is reversibly formed in a water-in-bisalt (WiBS) electrolyte, enabling an outstandingly high specific cathode capacity of 243 mAh g−1 at an average potential of 4.2 V versus Li/Li+. In their recent publication in Nature, Kang Xu, Chunsheng Wang, and co-authors reported for the first time on a novel halogen conversion-intercalation graphite cathode chemistry for the development of high-energy aqueous batteries. As evidenced by experimental works and modeling, a densely packed stage-1 graphite intercalation compound (GIC) with a stoichiometry of C3.5[Br0.5Cl0.5] is reversibly formed in a water-in-bisalt (WiBS) electrolyte, enabling an outstandingly high specific cathode capacity of 243 mAh g−1 at an average potential of 4.2 V versus Li/Li+. The lithium-ion battery (LIB) technology revolutionized energy storage since its market introduction in 1991 and still shows an evolutionary development with continuously increasing specific energy (Wh kg−1) and energy density (Wh L−1). LIBs not only dominate the small format battery market for portable electronic devices but also have been successfully implemented as the technology of choice for electrochemical power sources in electromobility1Schmuch R. Wagner R. Hörpel G. Placke T. Winter M. Performance and cost of materials for lithium-based rechargeable automotive batteries.Nat. Energy. 2018; 3: 267-278Crossref Scopus (1538) Google Scholar and stationary energy (“grid”) storage. A major focus of future battery research and development lies on the further improvement of the battery key performance indicators (KPIs), in particular to increase the energy content per weight and volume and to decrease cost, which is mandatory to achieve a broad customer acceptance.1Schmuch R. Wagner R. Hörpel G. Placke T. Winter M. Performance and cost of materials for lithium-based rechargeable automotive batteries.Nat. Energy. 2018; 3: 267-278Crossref Scopus (1538) Google Scholar Additionally, a high operational safety needs to be guaranteed and has to go hand in hand with the increase of the energy content. In addition, it is rather clear that there will be further KPIs that need to be considered when designing advanced batteries, which especially include a decreased CO2 footprint of the battery over the whole lifetime and the use of more sustainable or “green” materials, components, and production routes. State-of-the-art LIBs are based on non-aqueous electrolytes, i.e., LiPF6 dissolved in a mixture of carbonate-based solvents, offering the best performance for high-energy LIBs. However, these electrolytes give rise to safety and environmental concerns, as they exhibit intrinsic drawbacks, including flammability, toxicity, and high sensitivity toward moisture. In particular, the undesired combination of high-energy cathode materials, which can release oxygen, and flammable electrolytes as combustibles is considered as a major threat for the large-scale application of LIBs. A suitable strategy to address these safety concerns is the replacement of non-aqueous by aqueous electrolytes, which, however, sets an intrinsic limit to the battery’s practical energy by the narrow electrochemical stability window (ESW) of water (1.23 V). Aqueous LIBs gained significant attention, as Kang Xu, Chuncheng Wang, and colleagues addressed this challenge and made ground-breaking efforts by expanding the ESW of water to >3.0 V when first introducing the concept of the “water-in-salt” electrolyte class (WiSE), based on highly or super-concentrated lithium salts (>21 mol kg−1 LiTFSI).2Suo L. Borodin O. Gao T. Olguin M. Ho J. Fan X. Luo C. Wang C. Xu K. “Water-in-salt” electrolyte enables high-voltage aqueous lithium-ion chemistries.Science. 2015; 350: 938-943Crossref PubMed Scopus (1923) Google Scholar, 3Yang C. Chen J. Qing T. Fan X. Sun W. von Cresce A. Ding M.S. Borodin O. Vatamanu J. Schroeder M.A. et al.4.0 V Aqueous Li-Ion Batteries.Joule. 2017; 1: 122-132Abstract Full Text Full Text PDF Scopus (349) Google Scholar Inspired by this work, they developed a mixed salt system, named “water-in-bisalt” (WiBS) electrolyte, consisting of 21 mol kg−1 LiTFSI and 7 mol kg−1 LiOTf, which was proven to further enhance the ESW in a 2.5 V aqueous LIB cell (carbon-coated TiO2‖LiMn2O4) delivering an outstanding high specific energy of 100 Wh kg−1.4Suo L. Borodin O. Sun W. Fan X. Yang C. Wang F. Gao T. Ma Z. Schroeder M. von Cresce A. et al.Advanced High-Voltage Aqueous Lithium-Ion Battery Enabled by “Water-in-Bisalt” Electrolyte.Angew. Chem. Int. Ed. Engl. 2016; 55: 7136-7141Crossref PubMed Scopus (480) Google Scholar Furthermore, they marked another major step forward by developing a fluorinating protective coating for the negative electrode, enabling a reversible cycling of graphite and Li metal electrodes in aqueous electrolytes, thus leading to 4.0 V aqueous LIBs and paving the path to a series of new aqueous cell chemistries.3Yang C. Chen J. Qing T. Fan X. Sun W. von Cresce A. Ding M.S. Borodin O. Vatamanu J. Schroeder M.A. et al.4.0 V Aqueous Li-Ion Batteries.Joule. 2017; 1: 122-132Abstract Full Text Full Text PDF Scopus (349) Google Scholar In their recent publication in Nature, Chunsheng Wang, Kang Xu, and colleagues introduced a novel storage concept for the positive electrode of high-energy aqueous batteries on the basis of a halogen conversion-intercalation chemistry by use of a graphite cathode, thus enabling the highly reversible formation of a graphite intercalation compound (GIC) in the WiBS electrolyte (Figure 1).5Yang C. Chen J. Ji X. Pollard T.P. Lü X. Sun C.J. Hou S. Liu Q. Liu C. Qing T. et al.Aqueous Li-ion Battery Enabled by Halogen Conversion-Intercalation Chemistry in Graphite.Nature. 2019; (Published online May 9, 2019)https://doi.org/10.1038/s41586-019-1175-6Crossref Scopus (435) Google Scholar With this pioneering work, they addressed the rather low specific capacities of typical transition metal oxide-based cathodes (<200 mAh g−1) and reported an outstandingly high specific capacity of 243 mAh g−1 for the graphite cathode, which is obtained at an average discharge potential of 4.2 V versus Li/Li+. Furthermore, they coupled this novel graphite cathode chemistry with a graphite anode, protected by a highly fluorinated ether polymer gel,3Yang C. Chen J. Qing T. Fan X. Sun W. von Cresce A. Ding M.S. Borodin O. Vatamanu J. Schroeder M.A. et al.4.0 V Aqueous Li-Ion Batteries.Joule. 2017; 1: 122-132Abstract Full Text Full Text PDF Scopus (349) Google Scholar resulting in a 4.0 V graphite‖graphite aqueous battery cell, offering a specific energy of 460 Wh kg−1, considering the mass of both the graphite anode and cathode.5Yang C. Chen J. Ji X. Pollard T.P. Lü X. Sun C.J. Hou S. Liu Q. Liu C. Qing T. et al.Aqueous Li-ion Battery Enabled by Halogen Conversion-Intercalation Chemistry in Graphite.Nature. 2019; (Published online May 9, 2019)https://doi.org/10.1038/s41586-019-1175-6Crossref Scopus (435) Google Scholar Graphite as a redox-amphoteric host material can incorporate a broad range of different guest species, yielding the well-known donor-type or acceptor-type GICs by intercalation of cations or anions, respectively, which can be prepared by various chemical or electrochemical procedures.6Besenhard J.O. Fritz H.P. The Electrochemistry of Black Carbons.Angew. Chem. Int. Ed. Engl. 1983; 22: 950-975Crossref Scopus (257) Google Scholar Fundamental research on GICs has been performed for more than 150 years, while GICs have been researched and used for various application purposes, e.g., as adsorbents, highly conductive materials, or for battery applications. In general, graphite is a highly versatile host material, enabling various battery cell chemistries, as can be recognized by the broad spectrum of cations (e.g., Li+, K+, etc.) capable of reversibly forming donor-type GICs according to Equation 1 and of anions (e.g., BF4−, PF6−, TFSI−, etc.) able to form acceptor-type GICs, as described by Equation 2.6Besenhard J.O. Fritz H.P. The Electrochemistry of Black Carbons.Angew. Chem. Int. Ed. Engl. 1983; 22: 950-975Crossref Scopus (257) Google ScholarCn + x·M+ + x·e− ⇌ MxCn (donor-type GIC)(Equation 1) Cn + x·A− ⇌ AxCn + x·e− (acceptor-type GIC)(Equation 2) While lithium-intercalated graphite used as state-of-the-art negative electrode in LIBs is the most prominent donor-type GIC,1Schmuch R. Wagner R. Hörpel G. Placke T. Winter M. Performance and cost of materials for lithium-based rechargeable automotive batteries.Nat. Energy. 2018; 3: 267-278Crossref Scopus (1538) Google Scholar acceptor-type GICs recently got significant attention as positive electrode material in the so-called dual-ion battery (DIB) technology and their special forms, the dual-carbon battery (DCB) or dual-graphite battery (DGB).7Placke T. Heckmann A. Schmuch R. Meister P. Beltrop K. Winter M. Perspective on Performance, Cost, and Technical Challenges for Practical Dual-Ion Batteries.Joule. 2018; 2: 2528-2550Abstract Full Text Full Text PDF Scopus (212) Google Scholar The latter DGB systems typically use graphitic carbons as both the negative and positive electrode material and are considered a promising option for grid applications, displaying environmental, safety, and, in particular, cost benefits over state-of-the-art LIBs.7Placke T. Heckmann A. Schmuch R. Meister P. Beltrop K. Winter M. Perspective on Performance, Cost, and Technical Challenges for Practical Dual-Ion Batteries.Joule. 2018; 2: 2528-2550Abstract Full Text Full Text PDF Scopus (212) Google Scholar, 8Rothermel S. Meister P. Schmuelling G. Fromm O. Meyer H.W. Nowak S. Winter M. Placke T. Dual-Graphite Cells based on the Reversible Intercalation of Bis(trifluoromethanesulfonyl)imide Anions from an Ionic Liquid Electrolyte.Energy Environ. Sci. 2014; 7: 3412-3423Crossref Google Scholar The general storage mechanism of DGBs is based on the simultaneous intercalation of the cations and anions, typically from non-aqueous electrolytes,7Placke T. Heckmann A. Schmuch R. Meister P. Beltrop K. Winter M. Perspective on Performance, Cost, and Technical Challenges for Practical Dual-Ion Batteries.Joule. 2018; 2: 2528-2550Abstract Full Text Full Text PDF Scopus (212) Google Scholar, 8Rothermel S. Meister P. Schmuelling G. Fromm O. Meyer H.W. Nowak S. Winter M. Placke T. Dual-Graphite Cells based on the Reversible Intercalation of Bis(trifluoromethanesulfonyl)imide Anions from an Ionic Liquid Electrolyte.Energy Environ. Sci. 2014; 7: 3412-3423Crossref Google Scholar into the graphite negative and positive electrode, respectively. In 1938, Rüdorff and Hofmann reported for the first time on a dual-graphite rocking chair battery in which HSO4− anions were shuttled between the two graphite electrodes and reversibly intercalated from an aqueous electrolyte based on highly concentrated sulfuric acid.9Rüdorff W. Hofmann U. Über Graphitsalze.Z. Anorg. Allg. Chem. 1938; 238: 1-50Crossref Scopus (247) Google Scholar With this work, they marked a milestone, as this battery system was based on the shuttling mechanism of anions and thus can be regarded as the earliest ancestor of today’s LIB.9Rüdorff W. Hofmann U. Über Graphitsalze.Z. Anorg. Allg. Chem. 1938; 238: 1-50Crossref Scopus (247) Google Scholar Even though DGBs offer a relatively high average discharge voltage of up to 4.5 V, the specific capacity of the graphite cathode is limited by the relatively low packing density of complex anions, resulting in capacities < 150 mAh g−1, even for stage-1 GICs, meaning that each graphite interlayer gap is occupied by the guest species.7Placke T. Heckmann A. Schmuch R. Meister P. Beltrop K. Winter M. Perspective on Performance, Cost, and Technical Challenges for Practical Dual-Ion Batteries.Joule. 2018; 2: 2528-2550Abstract Full Text Full Text PDF Scopus (212) Google Scholar The highest reversible capacities have been reported for CnTFSI (121 mAh g−1), CnPF6 (140 mAh g−1), and for CnAlCl4 (150 mAh g−1).7Placke T. Heckmann A. Schmuch R. Meister P. Beltrop K. Winter M. Perspective on Performance, Cost, and Technical Challenges for Practical Dual-Ion Batteries.Joule. 2018; 2: 2528-2550Abstract Full Text Full Text PDF Scopus (212) Google Scholar In their work, Chunsheng Wang, Kang Xu, and co-authors presented Cn[BrxCly] as a novel GIC cathode material, offering a remarkably high reversible capacity of 243 mAh g−1, based on the total weight of the cathode, and a high reversibility as displayed by a Coulombic efficiency close to 100%.5Yang C. Chen J. Ji X. Pollard T.P. Lü X. Sun C.J. Hou S. Liu Q. Liu C. Qing T. et al.Aqueous Li-ion Battery Enabled by Halogen Conversion-Intercalation Chemistry in Graphite.Nature. 2019; (Published online May 9, 2019)https://doi.org/10.1038/s41586-019-1175-6Crossref Scopus (435) Google Scholar In particular, they synthesized a composite cathode by mixing anhydrous LiBr and LiCl with graphite, containing equimolar lithium halide salts, i.e., (LiBr)0.5(LiCl)0.5-graphite, noted as LBC-G. In contact with the WiBS aqueous gel electrolyte, a hydrated LiBr/LiCl layer is formed at the LBC-G surface (Figure 1), accelerating the halogen’s redox reactions, i.e., the Br− intercalation in a potential range of 4.0–4.2 V versus Li/Li+ and the Cl− intercalation in a potential range of 4.2–4.5 V versus Li/Li+, as observed from the cyclic voltammetry results (Figure 2) and summarized by Equations 3 and 4, respectively. In this two-step redox reaction, a mixed intercalation compound, i.e., Cn[BrxCly], is formed in the second step, while the oxidation of each halogen involves a one-electron transfer and the release of one Li+ to the bulk electrolyte.Cn + x·LiBr ⇌ Cn[Brx] + x·Li+ + x·e− (4.0–4.2 V versus Li/Li+)(Equation 3) Cn[Brx] + y·LiCl ⇌ Cn[BrxCly] + y·Li+ + y·e− (4.2–4.5 V versus Li/Li+)(Equation 4) The authors comprehensively studied the structural properties of the formed GICs and calculated among others the intercalant gallery heights and the nearest in-plane distances of the halogen intercalants. Evidenced by density functional theory (DFT) calculations and extended X-ray absorption fine structure (EXAFS) measurements, they found nearest in-plane distances of 2.4–3.2 Å for the Br-Br or Br-Cl intercalants, which are much shorter than those of alkali metal GICs (e.g., 4.31 Å for Li+-Li+) as well as for large anions (e.g., 9.8 Å for PF6−-PF6−).10Placke T. Schmuelling G. Kloepsch R. Meister P. Fromm O. Hilbig P. Meyer H.W. Winter M. In situ X-ray Diffraction Studies of Cation and Anion Intercalation into Graphitic Carbons for Electrochemical Energy Storage Applications.Z. Anorg. Allg. Chem. 2014; 640: 1996-2006Crossref Google Scholar This work presents another milestone in the development of high-energy, safe, and low-cost aqueous batteries by offering a high-capacity graphite cathode chemistry approach based on an intercalation-conversion mechanism. This 4.0 V graphite‖graphite cell chemistry may either be named “aqueous lithium-ion battery” or “aqueous dual-ion battery,” according to the proposed working mechanism during charge/discharge." @default.
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• W2945113119 title "Boosting Aqueous Batteries by Conversion-Intercalation Graphite Cathode Chemistry" @default.
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