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• W2904603525 abstract "In the November issue of Chem, Dong and co-workers developed a unique soluble electrocatalyst, a Ru(II) polypyridyl complex (RuPC), for Li-O2 batteries. As a result of the specific interactions between the Ru(II) center and O2−/LiO2 species, reversible formation and decomposition of Li2O2 occur in the electrolyte solution, and the Li-O2 cell sees drastic improvement in performance. In the November issue of Chem, Dong and co-workers developed a unique soluble electrocatalyst, a Ru(II) polypyridyl complex (RuPC), for Li-O2 batteries. As a result of the specific interactions between the Ru(II) center and O2−/LiO2 species, reversible formation and decomposition of Li2O2 occur in the electrolyte solution, and the Li-O2 cell sees drastic improvement in performance. Rechargeable Li-ion batteries have evolved into a necessity for people’s daily lives.1Tarascon J.M. Armand M. Issues and challenges facing rechargeable lithium batteries.Nature. 2001; 414: 359-367Crossref PubMed Scopus (16278) Google Scholar However, limited by their intrinsic intercalation chemistries, Li-ion batteries are approaching their theoretical capacity limits and would not satisfy the ever-growing energy-density demands of large-scale applications (e.g., electric vehicles with a driving range > 500 km) even if they were fully developed.1Tarascon J.M. Armand M. Issues and challenges facing rechargeable lithium batteries.Nature. 2001; 414: 359-367Crossref PubMed Scopus (16278) Google Scholar This situation has led to a surge of research activity toward exploring radically new battery chemistries with specific energy (or energy density) beyond what the best Li-ion batteries can achieve.2Bruce P.G. Freunberger S.A. Hardwick L.J. Tarascon J.M. Li-O2 and Li-S batteries with high energy storage.Nat. Mater. 2011; 11: 19-29Crossref PubMed Scopus (7410) Google Scholar Among these high-energy-density battery chemistries, the aprotic Li-O2 battery has attracted much attention because its theoretical specific energy is higher than that of any other rechargeable system.2Bruce P.G. Freunberger S.A. Hardwick L.J. Tarascon J.M. Li-O2 and Li-S batteries with high energy storage.Nat. Mater. 2011; 11: 19-29Crossref PubMed Scopus (7410) Google Scholar Typically, a Li-O2 battery consists of a Li anode separated from a porous O2 cathode by a Li+ conducting electrolyte, and the operation of a Li-O2 battery requires the O2 reduction reaction producing solid Li2O2 on discharge and reverse Li2O2 oxidation to O2 on recharge. Because the discharge product Li2O2 is a wide-band-gap insulator and can hardly dissolve in commonly used organic solvents, accumulation of Li2O2 on the cathode surface can easily result in the so-called “sudden-death” phenomenon, and only a very limited discharge capacity, far below the theoretical promise of Li-O2 electrochemistry, is realized by current Li-O2 batteries. Toward unlocking the energy capabilities of Li-O2 batteries, a great deal of research effort has been devoted to a fundamental understanding of the Li-O2 electrochemistry, and it has been found that the “sudden death” associated with current Li-O2 batteries can be addressed through the discharge (and decomposition) of Li2O2 in the electrolyte solution rather than on the electrode surface with the assistance of soluble electrocatalysts (or redox mediators).3Aurbach D. McCloskey B.D. Nazar L.F. Bruce P.G. Advances in understanding mechanisms underpinning lithium–air batteries.Nat. Energy. 2016; 1: 16128Crossref Scopus (835) Google Scholar In the November issue of Chem, Dong and co-workers from Xiamen University reported a remarkable redox mediator of a Ru(II) polypyridyl complex (RuPC) that can interact favorably with O2−/LiO2 intermediates in the electrolyte solution, facilitate both the charge and discharge processes, and suppress superoxide- and peroxide-related side reactions (see Figure 1).4Lin X. Yuan R. Cao Y. Ding X. Cai S. Han B. Hong Y. Zhou Z. Yang X. Gong L. et al.Controlling reversible expansion of Li2O2 formation and decomposition by modifying electrolyte in Li-O2 batteries.Chem. 2018; 4: 2685-2698Abstract Full Text Full Text PDF Scopus (42) Google Scholar Specifically, upon discharge, O2 is reduced to O2− via a one-electron reaction, and then O2− rapidly combines with Li+, RuPC, and DMSO to form a less reactive intermediate of RuPC(LiO2-3DMSO) in the electrolyte solution:O2(sol) + e− + Li+ + 3DMSO + RuPC(sol) → RuPC(LiO2-3DMSO)(Equation 1) Subsequently, the final discharge product Li2O2 is produced by a second reduction of the RuPC(LiO2-3DMSO) intermediates:RuPC(LiO2-3DMSO) + e− + Li+ → Li2O2 + 3DMSO + RuPC(Equation 2) Upon charging, again with the assistance of RuPC and DMSO, the Li2O2 product is first oxidized to the RuPC(LiO2-3DMSO) intermediate via a one-electron delithiation reaction:Li2O2 + 3DMSO + RuPC(sol) → RuPC(LiO2-3DMSO) + Li+ + e−(Equation 3) Then, the RuPC(LiO2-3DMSO) intermediate proceeds with a second oxidation reaction to release O2 and regenerate the RuPC catalyst:RuPC(LiO2-3DMSO) → O2 + Li+ + e− + 3DMSO + RuPC(Equation 4) It is notable that the above charge-discharge mechanisms in the RuPC-catalyzed Li-O2 cell are very different from the O2 electrochemistry in pristine Li-O2 batteries.5Park J.-B. Lee S.H. Jung H.-G. Aurbach D. Sun Y.-K. Redox mediators for Li–O2 batteries: status and perspectives.Adv. Mater. 2018; 30: 1704162Crossref Scopus (233) Google Scholar For the discharge process, the RuPC catalyst in its reduced form can effectively combine with the very reactive O2−/LiO2 species to form a less reactive RuPC(LiO2-3DMSO) intermediate, which makes the cell components (e.g., cathode material and electrolyte solvent) free from attack by O2−/LiO2 and therefore significantly suppresses the superoxide-related side reactions. The RuPC(LiO2-3DMSO) intermediate is soluble and can effectively promote the formation of Li2O2 in the electrolyte solution. As a result, the problem of cathode passivation by the discharged Li2O2 can be significantly alleviated. Moreover, the RuPC can also interact with the surface O atoms of Li2O2, and therefore the reactive O sites of the Li2O2 are stabilized and the undesirable side reaction between Li2O2 and the cell components is minimized. For the charging process, the problems associated with the Li2O2 oxidation at the solid-solid interface (electrode-Li2O2) in conventional Li-O2 batteries can also be solved with the redox mediators of RuPC. Because of the favorable interaction between RuPC and LiO2 in the presence of DMSO, the initial delithiation pathway of Li2O2 oxidation via a one-electron process producing soluble intermediates of RuPC(LiO2-3DMSO) can be realized. Compared with the previously proposed two-electron pathway, the one-electron delithiation pathway is more kinetically favorable and chemically reversible.6Peng Z. Freunberger S.A. Hardwick L.J. Chen Y. Giordani V. Bardé F. Novák P. Graham D. Tarascon J.M. Bruce P.G. Oxygen reactions in a non-aqueous Li+ electrolyte.Angew. Chem. Int. Ed. 2011; 50: 6351-6355Crossref PubMed Scopus (481) Google Scholar As expected, the charge overpotential of the RuPC-catalyzed Li-O2 cell has been significantly reduced. Given all of the advantages mentioned above for the RuPC electrocatalysts, Dong and co-workers have achieved outstanding electrochemical performance, including a high discharge capacity (∼9,281 mAh g−1), an ultralong cycle life (371 cycles), and a low charge overpotential (0.54 V), for the RuPC-catalyzed Li-O2 cells. The O2 electrochemistry in Li-O2 batteries is intrinsically complex because the cathode is a gas-diffuse-type electrode and the discharge product Li2O2 is an insulating solid. The Dong group’s strategy of catalyzing and promoting in solution by using soluble electrocatalyst of RuPC is smart and promising for a better Li-O2 battery with enhanced kinetics and reduced side reactions.4Lin X. Yuan R. Cao Y. Ding X. Cai S. Han B. Hong Y. Zhou Z. Yang X. Gong L. et al.Controlling reversible expansion of Li2O2 formation and decomposition by modifying electrolyte in Li-O2 batteries.Chem. 2018; 4: 2685-2698Abstract Full Text Full Text PDF Scopus (42) Google Scholar Recently, a similar concept was reported by Bruce and co-workers, who employed dual redox mediators (one for discharge and the other for charge) to facilitate both discharge and charge of Li-O2 batteries.7Gao X. Chen Y. Johnson L.R. Jovanov Z.P. Bruce P.G. A rechargeable lithium–oxygen battery with dual mediators stabilizing the carbon cathode.Nat. Energy. 2017; 2: 17118Crossref Scopus (185) Google Scholar However, when two redox mediators with different redox potentials are used at the same time, it is necessary to consider the compatibility of these two redox mediators to ensure that they do not interfere with each other and can work independently upon charge and discharge. Assigning solution-phase catalytic capabilities of both the O2 reduction reaction and the O2 evolution reaction to one single redox mediator (e.g., RuPC) can solve the above technical issue. Because Li-O2 batteries work with a Li-metal anode, one possible drawback of the redox-mediator-catalyzed Li-O2 battery is that the soluble catalysts could shuttle from the O2 cathode to the Li anode and decompose thereon, gradually degrading their functionalities. However, this issue could be addressed through the use of a protected Li anode (such as a solid-state electrolyte)8Zhou B. Guo L. Zhang Y. Wang J. Ma L. Zhang W.H. Fu Z. Peng Z. A high-performance Li-O2 battery with a strongly solvating hexamethylphosphoramide electrolyte and a LiPON-protected lithium anode.Adv. Mater. 2017; 29: 1701568Crossref Scopus (120) Google Scholar or immobilized redox mediators (such as polymerized redox mediators),9Liu Z. Ma L. Guo L. Peng Z. Promoting solution discharge of Li-O2 batteries with immobilized redox mediators.J. Phys. Chem. Lett. 2018; 9: 5915-5920Crossref PubMed Scopus (25) Google Scholar two evolving research directions of next-generation Li-O2 batteries. Controlling Reversible Expansion of Li2O2 Formation and Decomposition by Modifying Electrolyte in Li-O2 BatteriesLin et al.ChemSeptember 20, 2018In BriefThe development of the Li-O2 battery is critically hindered by cathode passivation, large polarization, and severe parasitic reactions. Here, Dong and co-workers employ a Ru(II) polypyridyl complex (RuPC) as a multifunctional soluble electrocatalyst for Li-O2 batteries to address these issues. Benefiting from the interaction between the Ru(II) center and O2−/LiO2 species, the RuPC can not only reversibly expand Li2O2 formation and decomposition with a low overpotential but also limit the side reactions. As a result, the RuPC-catalyzed Li-O2 batteries exhibit excellent performance. Full-Text PDF Open Archive" @default.
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• W2904603525 title "Making Li2O2 Different in Solution" @default.
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