Two‐dimensional (2D) graphitic carbon nitride (g‐CN) is a promising anode material for sodium‐ion batteries (SIBs), but its insufficient interlayer spacing and poor electronic conductivity impede its sodium storage capacity and cycling stability. Herein, we report the fabrication of a fullerene (C60)‐modified graphitic carbon nitride (C60@CN) material which as an anode material for SIBs shows a high‐reversible capacity (430.5 mA h g−1 at 0.05 A g−1, about 3 times higher than that of pristine g‐CN), excellent rate capability (226.6 mA h g−1 at 1 A g−1) and ultra‐long cycle life (101.2 mA h g−1 after 5000 cycles at 5 A g−1). Even at a high‐active mass loading of 3.7 mg cm−2, a reversible capacity of 316.3 mA h g−1 can be obtained after 100 cycles. Such outstanding performance of C60@CN is attributed to the C60 molecules distributed in the g‐CN nanosheets, which enhance the electronic conductivity and prevent g‐CN sheets from restacking, thus resulting in enlarged interlayer spacing and exposed edge N defects (pyridinic N and pyrrolic N) for sodium‐ion storage. Furthermore, a sodium‐ion full cell combining C60@CN anode and NVPF@rGO cathode provides high‐coulombic efficiency (>96.5%), exceptionally high‐energy density (359.8 W h kganode−1 at power density of 105.1 W kganode−1) and excellent cycling stability (89.2% capacity retention over 500 cycles at 1 A ganode−1). This work brings new insights into the field of carbon‐based anode materials for SIBs.
Reaction
of AgCC
t
Bu with (EtO)2PS2Na at room temperature leads to the isolation
of two new silver(I)-ethynide compounds incorporating the dithiophosphate
ligand, namely, {CO3@(Ag3)4(CC
t
Bu)4(EtO)2PS2]6}·0.5H2O (1) and {(CO3)2@Ag26(CC
t
Bu)16[(EtO)2PS2]4}·2(OH)·4MeOH·6H2O (2). Besides,
we obtain another three silver(I)-ethynide clusters S@Ag11(CC
t
Bu)2[(EtO)2PS2]7 (3), {S@Ag14(CCPh)8[(EtO)2PS2]4(TMEDA)2}·5MeOH (4), and {S@Ag14(CCPh)8[(
i
PrO)2PS2]4(TMEDA)2}·7CH3OH (5), with AgCCR (R=
t
Bu, Ph) and (RO)2PS2Na (R= Et,
i
Pr) as the starting materials. Complexes 1–2 are templated by a carbonate anion in situ
generated from the fixation of atmospheric CO2 in a basic
TMEDA-containing solution, and TMEDA can also lead to the disassembly
of dithiophosphate to give a sulfide ion as the template for the generation
of 3–5.
Phosphonate can act as the intermediate connector to link two silver ethynide clusters functionalized by hfac ligands together to enlarge the silver cluster.
Four copper(I) alkynyl complexes
incorporating phosphate ligands,
namely, [Cu16(
t
BuCC)12(PhOPO3)2]
n
(1; PhOPO3 = phenyl phosphate), [Cu16(
t
BuCC)12(1-NaphOPO3)2]
n
(2; 1-NaphOPO3 = 1-naphthyl phosphate), [VO4@Cu25(
t
BuCC)19(1-NaphOPO3)](PF6)0.5(F)0.5 (3), and [PO4@Cu25(
t
BuCC)19(1-NaphOPO3)](PF6)0.5(F)0.5 (4), were solvothermally
synthesized and well-characterized by IR spectroscopy, powder X-ray
diffraction, and single-crystal X-ray diffraction. Single-crystal
X-ray analysis revealed that the Cu16 cluster-based coordination
chain polymers 1 and 2 are formed by assembly
during crystallization, while 3 and 4 contain
high-nuclearity copper(I) composite clusters enclosing orthovanadate
and phosphate template ions, respectively, that are supported by ROPO3
2– ligands. Complexes 1–4 exhibit crystallization-induced emission enhancement. Their
crystalline state shows strong luminescence, in striking contrast
to the weak emission of the amorphous state and solution phase. A
detailed investigation of the crystal structure suggests that well-arranged
C–H···π and π···π
interactions between the ligands are the major factors for this enhanced
emission. Clusters 3 and 4 also exhibit
photocurrent responses upon visible-light illumination.
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