In this paper,porous partially fluorinated graphene(PFG)for supercapacitors(SCs)was fabricated by a mild and secure one-pot hydrothermal method utilizing weakly coordinating anion BF_(4)^(-) as the fluorine source.The...In this paper,porous partially fluorinated graphene(PFG)for supercapacitors(SCs)was fabricated by a mild and secure one-pot hydrothermal method utilizing weakly coordinating anion BF_(4)^(-) as the fluorine source.The hydrolysis rate of sodium fluoroborate was adjusted by controlling the reaction temperature and PFG containing semi-ionic C-F bonds was obtained,where the content of semi-ionic C-F bonds in PFG can be easily regulated.The final experimental results show that the incorporation of fluorine not only modulates the electrochemical properties of the material,but also creates abundant pores.When assembled in a symmetric supercapacitor,the PFG shows a high specific capacitance of 269.7 F g^(-1) at 1 A g^(-1) and a superior rate capability with 89.3%capacitance retained,as the current density is increased from 1 A g^(-1)even to 20 A g^(-1).Furthermore,the resultant energy density for PFG is 9.4 Wh kg^(-1) at a power density of 250.0 W kg^(-1)(1 A g^(-1)).All these results confirm that as-prepared partially fluorinated graphene is appropriate for the application in SCs and mass production.展开更多
Synthesis of stable main-group element-based radicals represents one of the most interesting topics in contemporary organometallic chem- istry, because of their vital roles in organic, inorganic and biological chemist...Synthesis of stable main-group element-based radicals represents one of the most interesting topics in contemporary organometallic chem- istry, because of their vital roles in organic, inorganic and biological chemistry as well as materials science. However, the access of stable main-group element-based radicals is highly challenging owing to the lack of energetically accessible orbitals in the main-group elements. During the last decades, several synthetic strategies have been developed in obtaining these reactive species. Among them, utilizing the stericaliy demanding substituents and x-conjugated ligands has proven to be an effective approach. Weakly coordinating ions (WCAs) have also been found to be exceptionally practical in synthesizing radical cations of main-group elements. By introducing these stabilization methods, we have successfully prepared a variety of radical ions of p-block elements in the crystalline forms, and investigated their properties by different experimental and quantum chemical calculation methods. According to the investigations, magnetic stability was observed, resulting from the intramolecular electron-exchange interaction. Furthermore, we also found that the singlet-triptet energy gaps of the bis(triarylamine) diradical dications can be tunable by varying the temperature. These investigations open new avenues of the main-group element-based radicals for a large variety of applications.展开更多
基金supported by National Natural Science Foundation of China(21905304)Natural Science Foundation of Shandong Province(ZX20210028)the Fundamental Research Funds for the Central Universities(19CX05001A).
文摘In this paper,porous partially fluorinated graphene(PFG)for supercapacitors(SCs)was fabricated by a mild and secure one-pot hydrothermal method utilizing weakly coordinating anion BF_(4)^(-) as the fluorine source.The hydrolysis rate of sodium fluoroborate was adjusted by controlling the reaction temperature and PFG containing semi-ionic C-F bonds was obtained,where the content of semi-ionic C-F bonds in PFG can be easily regulated.The final experimental results show that the incorporation of fluorine not only modulates the electrochemical properties of the material,but also creates abundant pores.When assembled in a symmetric supercapacitor,the PFG shows a high specific capacitance of 269.7 F g^(-1) at 1 A g^(-1) and a superior rate capability with 89.3%capacitance retained,as the current density is increased from 1 A g^(-1)even to 20 A g^(-1).Furthermore,the resultant energy density for PFG is 9.4 Wh kg^(-1) at a power density of 250.0 W kg^(-1)(1 A g^(-1)).All these results confirm that as-prepared partially fluorinated graphene is appropriate for the application in SCs and mass production.
基金We thank the National Key R&D Program of China (Grant 2016YFA0300404, X.W.) and the National Natural Science Foundation of China (Grants 21525102, 21690062, X.W. and 21601082, G.T.) for financial support. Dr. Li Zhang is acknowledged for proofreading the manuscript.
文摘Synthesis of stable main-group element-based radicals represents one of the most interesting topics in contemporary organometallic chem- istry, because of their vital roles in organic, inorganic and biological chemistry as well as materials science. However, the access of stable main-group element-based radicals is highly challenging owing to the lack of energetically accessible orbitals in the main-group elements. During the last decades, several synthetic strategies have been developed in obtaining these reactive species. Among them, utilizing the stericaliy demanding substituents and x-conjugated ligands has proven to be an effective approach. Weakly coordinating ions (WCAs) have also been found to be exceptionally practical in synthesizing radical cations of main-group elements. By introducing these stabilization methods, we have successfully prepared a variety of radical ions of p-block elements in the crystalline forms, and investigated their properties by different experimental and quantum chemical calculation methods. According to the investigations, magnetic stability was observed, resulting from the intramolecular electron-exchange interaction. Furthermore, we also found that the singlet-triptet energy gaps of the bis(triarylamine) diradical dications can be tunable by varying the temperature. These investigations open new avenues of the main-group element-based radicals for a large variety of applications.