Oxidative dehydrogenation of propane (ODHP) is a key technology for producing propene from shale gas, but conventional metal oxide catalysts are prone to overoxidation to form valueless COx. Boron-based catalysts were recently found to be selective for this reaction, and B–O–B oligomers are generally regarded as active centers. We show here that the isolated boron in a zeolite framework without such oligomers exhibits high activity and selectivity for ODHP, which also hinders full hydrolysis for boron leaching in a humid atmosphere because of the B–O–SiOx linkage, achieving superior durability in a long-period test. Furthermore, we demonstrate an isolated boron with a –B[OH…O(H)–Si]2 structure in borosilicate zeolite as the active center, which enables the activation of oxygen and a carbon–hydrogen bond to catalyze the ODHP.
Organic cathode materials have attracted extensive attention because of their diverse structures,f acile synthesis, and environmental friendliness.H owever,t hey often suffer from insufficient cycling stability caused by the dissolution problem, poor rate performance,a nd lowv oltages.A ni nsitu electropolymerization method was developed to stabilize and enhance organic cathodes for lithium batteries.4 ,4',4''-Tris-(carbazol-9-yl)-triphenylamine (TCTA) was employed because carbazole groups can be polymerized under an electric field and they may serve as high-voltage redox-active centers. The electropolymerized TCTAe lectrodes demonstrated excellent electrochemical performance with ah igh discharge voltage of 3.95 V, ultrafast rate capability of 20 Ag À1 ,a nd al ong cycle life of 5000 cycles.O ur findings provideanew strategy to address the dissolution issue and they explore the molecular design of organic electrode materials for use in rechargeable batteries.
Organic batteries using redox-active polymers and small organic compounds have become promising candidates for next-generation energy storage devices due to the abundance, environmental benignity, and diverse nature of organic resources. To date, tremendous research efforts have been devoted to developing advanced organic electrode materials and understanding the material structure–performance correlation in organic batteries. In contrast, less attention was paid to the correlation between electrolyte structure and battery performance, despite the critical roles of electrolytes for the dissolution of organic electrode materials, the formation of the electrode–electrolyte interphase, and the solvation/desolvation of charge carriers. In this review, we discuss the prospects and challenges of organic batteries with an emphasis on electrolytes. The differences between organic and inorganic batteries in terms of electrolyte property requirements and charge storage mechanisms are elucidated. To provide a comprehensive and thorough overview of the electrolyte development in organic batteries, the electrolytes are divided into four categories including organic liquid electrolytes, aqueous electrolytes, inorganic solid electrolytes, and polymer-based electrolytes, to introduce different components, concentrations, additives, and applications in various organic batteries with different charge carriers, interphases, and separators. The perspectives and outlook for the future development of advanced electrolytes are also discussed to provide a guidance for the electrolyte design and optimization in organic batteries. We believe that this review will stimulate an in-depth study of electrolytes and accelerate the commercialization of organic batteries.
p-Benzoquinone (BQ) is a promising cathode material for lithium-ion batteries (LIBs) due to its high theoretical specific capacity and voltage. However, it suffers from a serious dissolution problem in organic electrolytes, leading to poor electrochemical performance. Herein, two BQ-derived molecules with a near-plane structure and relative large skeleton: 1,4-bis(p-benzoquinonyl)benzene (BBQB) and 1,3,5-tris(p-benzoquinonyl)benzene (TBQB) are designed and synthesized. They show greatly decreased solubility as a result of strong intermolecular interactions. As cathode materials for LIBs, they exhibit high carbonyl utilizations of 100% with high initial capacities of 367 and 397 mAh g −1 , respectively. Especially, BBQB with better planarity presents remarkably improved cyclability, retaining a high capacity of 306 mAh g −1 after 100 cycles. The cycling stability of BBQB surpasses all reported BQ-derived small molecules and most polymers. This work provides a new molecular structure design strategy to suppress the dissolution of organic electrode materials for achieving high performance rechargeable batteries.
Organic cathode materials have gained substantial attention in sodium‐ion batteries (SIBs) because of their low cost, structure versatility, and environmental friendliness. Nevertheless, the use of organic materials is plagued by the unsatisfactory cycling performance caused by dissolution of organic electrode materials, use of inappropriate electrolytes, and/or poor interfacial compatibility. In this work, an ultralong cycle life of SIBs through coupling an insoluble organic cathode, N, N′‐bis(glycinyl) naphthalene diimide, with ether‐based electrolytes, is realized. A thin and stable inorganic‐rich solid electrolyte interphase is constructed through a prior reduction of salt in the organic solvents in the ether‐based electrolytes, promising fast charge transfer kinetics and stable cycling performance of organic electrodes in SIBs. A superb long cycle life of 70 000 cycles at 10C is demonstrated, which is a new record for organic cathode materials in SIBs. The findings highlight the key role of electrolytes and electrolyte/electrode interfaces in furthering the practical prospects of organic electrodes.
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