Highly homogeneous, well dispersed SiO_2@Au@TiO_2(SAT) microspheres decorated with Au nanoparticles(AuNPs) were prepared and incorporated into the photoanode with an optimized concentration gradientascent. The effects...Highly homogeneous, well dispersed SiO_2@Au@TiO_2(SAT) microspheres decorated with Au nanoparticles(AuNPs) were prepared and incorporated into the photoanode with an optimized concentration gradientascent. The effects of SAT microspheres and the gradient-ascent architecture on the light absorption and the photoelectric conversion efficiency(PCE) of the dye-sensitized solar cells(DSSCs) were investigated.Studies indicate that the introduction of SAT microspheres and the gradient-ascent architecture in the photoanode significantly enhance the light scattering and harvesting capability of the photoanode. The DSSC with the optimized SAT gradient-ascent photoanode has the maximum short circuit current density(J_(sc)) of 17.7 mA cm^(-2) and PCE of 7.75%, remarkably higher than those of the conventional DSSC by 23.7%and 28.0%, respectively. This significantly enhancement of the performance of the DSSC can be attributed to the excellent light reflection/scattering of SAT, the localized surface plasma resonance(LSPR) effect of AuNPs within the microspheres, and the gradient-ascent architecture of SAT microspheres inside the photoanode. This study demonstrates that the tri-synergies of the scattering of SAT microspheres, the LSPR of AuNPs and the gradient-ascent architecture can effectively improve the PCE of DSSC.展开更多
As promising energy storage systems,lithium-sulfur(Li-S)batteries have attracted significant attention because of their ultra-high energy densities.However,Li-S battery suffers problems related to the complex phase co...As promising energy storage systems,lithium-sulfur(Li-S)batteries have attracted significant attention because of their ultra-high energy densities.However,Li-S battery suffers problems related to the complex phase conversion that occurs during the charge-discharge process,particularly the deposition of solid Li2S from the liquid-phase polysulfides,which greatly limits its practical application.In this paper,edge-rich MoS2/C hollow microspheres(Edg-MoS2/C HMs)were designed and used to functionalize separator for Li-S battery,resulting in the uniform deposition of Li2S.The microspheres were fabricated through the facile hydrothermal treatment of MoO3-aniline nanowires and a subsequent carbonization process.The obtained Edg-MoS2/C HMs have a strong chemical absorption capability and high density of Li2S binding sites,and exhibit excellent electrocatalytic performance and can effectively hinder the polysulfide shuttle effect and guide the uniform nucleation and growth of Li2S.Furthermore,we demonstrate that the Edg-MoS2/C HMs can effectively regulate the deposition of Li2S and significantly improve the reversibility of the phase conversion of the active sulfur species,especially at high sulfur loadings and high C-rates.As a result,a cell containing a separator functionalized with Edg-MoS2/C HMs exhibited an initial discharge capacity of 935 mAh g-1 at 1.0 C and maintained a capacity of 494 mAh g-1 after 1000 cycles with a sulfur loading of 1.7 mg cm-2.Impressively,at a high sulfur loading of 6.1 mg cm-2 and high rate of 0.5 C,the cell still delivered a high reversible discharge capacity of 478 mAh g-1 after 300 cycles.This work provides fresh insights into energy storage systems related to complex phase conversions.展开更多
Herein,N-Ti3C2@CNT microspheres are successfully synthesized by the simple spray drying method.In the preparation process,HCl-treated melamine(HTM)is selected as the sources of carbon and nitrogen.It not only realizes...Herein,N-Ti3C2@CNT microspheres are successfully synthesized by the simple spray drying method.In the preparation process,HCl-treated melamine(HTM)is selected as the sources of carbon and nitrogen.It not only realizes in situ growth of CNTs on the surface of MXene nanosheets with the catalysis of Ni,but also introduces efficient N-doping in both MXene and CNTs.Within the microsphere,MXene nanosheets interconnect with CNTs to form porous and conductive network.In addition,N-doped MXene and CNTs can provide strong chemical immobilization for polysulfides and effectively entrap them within the porous microspheres.Above-mentioned merits enable N-Ti3C2@CNT microspheres to be ideal sulfur host.When used in lithium–sulfur(Li–S)battery,the N-Ti3C2@CNT microspheres/S cathode delivers initial specific capacity of 927 mAh g−1 at 1 C and retains high capacity of 775 mAh g−1 after 1000 cycles with extremely low fading rate(FR)of 0.016%per cycle.Furthermore,the cathode still shows high cycling stability at high C-rate of 4 C(capacity of 647 mAh g−1 after 650 cycles,FR 0.027%)and high sulfur loading of 3 and 6 mg cm−2 for Li–S batteries.展开更多
Core-shell structured SiO2/poly(N-isopropylacrylamide) (SiO2/PNIPAM) microspheres were successfully fabricated through hydrolysis and condensation reaction of tertraethyl orthosilicate (TEOS) on the surface of P...Core-shell structured SiO2/poly(N-isopropylacrylamide) (SiO2/PNIPAM) microspheres were successfully fabricated through hydrolysis and condensation reaction of tertraethyl orthosilicate (TEOS) on the surface of PNIPAM template at 50 ~C. The PNIPAM template can be easily removed by water at room temperature so that SiO2 hollow microspheres were finally obtained. The transmission electron microscope and scanning electron microscope observations indicated that SiO2 hollow microspheres with an average diameter of 150 nm can be formed only if there are enough concentration of PNIPAM and TEOS, and the hy- drolysis time of TEOS. FTIR analysis showed that part of PNIPAM remained on the wall of SiO2 because of the strong interaction between PNIPAM and silica. This work provides a clean and efficient way to prepare hollow microspheres.展开更多
基金supported financially by the National Natural Science Foundation of China (Nos.51572102,11504101,11604089 and 11364018)
文摘Highly homogeneous, well dispersed SiO_2@Au@TiO_2(SAT) microspheres decorated with Au nanoparticles(AuNPs) were prepared and incorporated into the photoanode with an optimized concentration gradientascent. The effects of SAT microspheres and the gradient-ascent architecture on the light absorption and the photoelectric conversion efficiency(PCE) of the dye-sensitized solar cells(DSSCs) were investigated.Studies indicate that the introduction of SAT microspheres and the gradient-ascent architecture in the photoanode significantly enhance the light scattering and harvesting capability of the photoanode. The DSSC with the optimized SAT gradient-ascent photoanode has the maximum short circuit current density(J_(sc)) of 17.7 mA cm^(-2) and PCE of 7.75%, remarkably higher than those of the conventional DSSC by 23.7%and 28.0%, respectively. This significantly enhancement of the performance of the DSSC can be attributed to the excellent light reflection/scattering of SAT, the localized surface plasma resonance(LSPR) effect of AuNPs within the microspheres, and the gradient-ascent architecture of SAT microspheres inside the photoanode. This study demonstrates that the tri-synergies of the scattering of SAT microspheres, the LSPR of AuNPs and the gradient-ascent architecture can effectively improve the PCE of DSSC.
基金financially supported by National Natural Science Foundation of China (No. 51672083)Program of Shanghai Academic/Technology Research Leader (18XD1401400)+3 种基金Basic Research Program of Shanghai (17JC1404702)Leading talents in Shanghai in 2018The 111 project (B14018)the Fundamental Research Funds for the Central Universities (222201718002)
文摘As promising energy storage systems,lithium-sulfur(Li-S)batteries have attracted significant attention because of their ultra-high energy densities.However,Li-S battery suffers problems related to the complex phase conversion that occurs during the charge-discharge process,particularly the deposition of solid Li2S from the liquid-phase polysulfides,which greatly limits its practical application.In this paper,edge-rich MoS2/C hollow microspheres(Edg-MoS2/C HMs)were designed and used to functionalize separator for Li-S battery,resulting in the uniform deposition of Li2S.The microspheres were fabricated through the facile hydrothermal treatment of MoO3-aniline nanowires and a subsequent carbonization process.The obtained Edg-MoS2/C HMs have a strong chemical absorption capability and high density of Li2S binding sites,and exhibit excellent electrocatalytic performance and can effectively hinder the polysulfide shuttle effect and guide the uniform nucleation and growth of Li2S.Furthermore,we demonstrate that the Edg-MoS2/C HMs can effectively regulate the deposition of Li2S and significantly improve the reversibility of the phase conversion of the active sulfur species,especially at high sulfur loadings and high C-rates.As a result,a cell containing a separator functionalized with Edg-MoS2/C HMs exhibited an initial discharge capacity of 935 mAh g-1 at 1.0 C and maintained a capacity of 494 mAh g-1 after 1000 cycles with a sulfur loading of 1.7 mg cm-2.Impressively,at a high sulfur loading of 6.1 mg cm-2 and high rate of 0.5 C,the cell still delivered a high reversible discharge capacity of 478 mAh g-1 after 300 cycles.This work provides fresh insights into energy storage systems related to complex phase conversions.
文摘Herein,N-Ti3C2@CNT microspheres are successfully synthesized by the simple spray drying method.In the preparation process,HCl-treated melamine(HTM)is selected as the sources of carbon and nitrogen.It not only realizes in situ growth of CNTs on the surface of MXene nanosheets with the catalysis of Ni,but also introduces efficient N-doping in both MXene and CNTs.Within the microsphere,MXene nanosheets interconnect with CNTs to form porous and conductive network.In addition,N-doped MXene and CNTs can provide strong chemical immobilization for polysulfides and effectively entrap them within the porous microspheres.Above-mentioned merits enable N-Ti3C2@CNT microspheres to be ideal sulfur host.When used in lithium–sulfur(Li–S)battery,the N-Ti3C2@CNT microspheres/S cathode delivers initial specific capacity of 927 mAh g−1 at 1 C and retains high capacity of 775 mAh g−1 after 1000 cycles with extremely low fading rate(FR)of 0.016%per cycle.Furthermore,the cathode still shows high cycling stability at high C-rate of 4 C(capacity of 647 mAh g−1 after 650 cycles,FR 0.027%)and high sulfur loading of 3 and 6 mg cm−2 for Li–S batteries.
文摘Core-shell structured SiO2/poly(N-isopropylacrylamide) (SiO2/PNIPAM) microspheres were successfully fabricated through hydrolysis and condensation reaction of tertraethyl orthosilicate (TEOS) on the surface of PNIPAM template at 50 ~C. The PNIPAM template can be easily removed by water at room temperature so that SiO2 hollow microspheres were finally obtained. The transmission electron microscope and scanning electron microscope observations indicated that SiO2 hollow microspheres with an average diameter of 150 nm can be formed only if there are enough concentration of PNIPAM and TEOS, and the hy- drolysis time of TEOS. FTIR analysis showed that part of PNIPAM remained on the wall of SiO2 because of the strong interaction between PNIPAM and silica. This work provides a clean and efficient way to prepare hollow microspheres.