以钼酸钠(Na_2MoO_4·2H_2O)、硫脲(NH_2CSNH_2)、CTAB为原料,利用水热法合成了MoS_2/C球状纳米花复合材料。通过XRD、SEM、TEM、TG等分析测试方法,研究了不同CTAB添加量对MoS_2/C复合材料的微观结构、表面形貌的影响规律,结果显示...以钼酸钠(Na_2MoO_4·2H_2O)、硫脲(NH_2CSNH_2)、CTAB为原料,利用水热法合成了MoS_2/C球状纳米花复合材料。通过XRD、SEM、TEM、TG等分析测试方法,研究了不同CTAB添加量对MoS_2/C复合材料的微观结构、表面形貌的影响规律,结果显示,有部分无定形碳嵌入了MoS_2层间,并抑制了MoS_2(002)面的堆积。电化学测试表明:与纯MoS_2相比,MoS_2/C复合材料具有更好的电化学性能,当加入0.025 g CTAB时首次放电比容量达到730 m Ah/g,在100 m A/g的电流密度下经过100次循环比容量稳定在415 m Ah/g。在此基础上讨论了MoS_2/C球状纳米花复合材料的可能生长机理以及对材料电化学性能的影响规律。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
MoS_2-decorated C_3N_4(C_3N_4/MoS_2) nanosheets hybrid photocatalysts were prepared by a simple sonication-impregnation method. Face-to-face lamellar heterojunctions were well established between two dimension(2D) C_3...MoS_2-decorated C_3N_4(C_3N_4/MoS_2) nanosheets hybrid photocatalysts were prepared by a simple sonication-impregnation method. Face-to-face lamellar heterojunctions were well established between two dimension(2D) C_3N_4 and MoS_2 nanosheets. The effects of MoS_2 content on the light absorption, charge transfer and photocatalytic activity of the hybrid samples were investigated. Characterization results show that MoS_2 nanosheets are well anchored on the face of C_3N_4 nanosheets and the composites have well dispersed layered morphology. After loading with MoS_2, the light absorption of composites was much improved, especially in visible-light region. The photocatalytic activities of C_3N_4/MoS_2 samples were evaluated based on the H_2 evolution under visible light irradiation(λ > 400 nm). When the loading amount of MoS_2 was increased to 5 wt%, the highest H_2 evolution rate(274 μmol·g^(-1)·h^(-1)) was obtained. Compared with samples obtained from direct impregnation method, sonication pretreatment is favorable for the formation of 2D layered heterojuctions and thus improve the photocatalytic activity. Slightly deactivation of C_3N_4/MoS_2 composites could be observed when recycled due to the mild photocorrosion of MoS_2. Based on the band alignments of C_3N_4 and MoS_2, a possible photocatalytic mechanism was discussed, where MoS_2 could efficiently promote the separation of the photogenerated carriers of C_3N_4.展开更多
Constructing heterostructures by combining COFs and TMD is a new strategy to design efficient photocatalysts for CO2 reduction reaction(CO2RR) due to their good stability,tunable band gaps and efficient charge separat...Constructing heterostructures by combining COFs and TMD is a new strategy to design efficient photocatalysts for CO2 reduction reaction(CO2RR) due to their good stability,tunable band gaps and efficient charge separation.Based on the synthesis of completely novel C4N-COF in our previous re ported work,a new C4N/MoS2 heterostructure was constructed and then the related structural,electronic and optical properties were also studied using first principle calculations.The interlayer coupling effect and charge transfer between the C4N and MoS2 layer are systematically illuminated.The reduced band gap of the C4N/MoS2 heterostructure is beneficial to absorb more visible light.For the formation of type-Ⅱ band alignment,a built-in electric field appears which separates the photogene rated electrons and holes into different layers efficiently and produces redox active sites.The band alignment of the heterostructure ensures its photocatalytic activities of the whole CO2 reduction reaction.Furthermore,the charge density difference and charge carrier mobility confirm the existence of the built-in electric field at the interface of the C4N/MoS2 heterostructure directly.Finally,the high optical absorption indicates it is an efficient visible light harvesting photocatalyst.Therefore,this wo rk could provide strong insights into the internal mechanism and high photocatalytic activity of the C4N/MoS2 heterostructure and offer guiding of designing and synthesizing COF/TMD heterostructure photocatalysts.展开更多
Rational design of advanced polar hosts with high sulfur loading,facilitated ionic/electronic transport and effectively suppressed shuttling effect has great potential for high performance lithium-sulfur batteries,yet...Rational design of advanced polar hosts with high sulfur loading,facilitated ionic/electronic transport and effectively suppressed shuttling effect has great potential for high performance lithium-sulfur batteries,yet it remains challenging.Here we propose a novel templated spherical coassembly strategy to fabricate the MoS_(2)/C hollow spheres as an efficient sulfur host material.The unique hollow structure provides enough interior space for accommodating a substantial amount of sulfur,and effectively suppresses the diffusion of dissolved polysulfides by both physical confinement and chemical adsorption.Moreover,the ionic transport as well as the ability to mitigate volume variation upon cycling is also improved,thereby maximizing the utilization of sulfur.Owing to these merits,when evaluated as a sulfur host for lithiumsulfur batteries,the MoS_(2)/C hollow spheres exhibit appealing electrochemical performance with an impressive specific capacity of 1082 mA hg^(-1)at 0.1 C,excellent rate capability and superior cycling stability with a low fading rate of 0.04%per cycle.展开更多
文摘以钼酸钠(Na_2MoO_4·2H_2O)、硫脲(NH_2CSNH_2)、CTAB为原料,利用水热法合成了MoS_2/C球状纳米花复合材料。通过XRD、SEM、TEM、TG等分析测试方法,研究了不同CTAB添加量对MoS_2/C复合材料的微观结构、表面形貌的影响规律,结果显示,有部分无定形碳嵌入了MoS_2层间,并抑制了MoS_2(002)面的堆积。电化学测试表明:与纯MoS_2相比,MoS_2/C复合材料具有更好的电化学性能,当加入0.025 g CTAB时首次放电比容量达到730 m Ah/g,在100 m A/g的电流密度下经过100次循环比容量稳定在415 m Ah/g。在此基础上讨论了MoS_2/C球状纳米花复合材料的可能生长机理以及对材料电化学性能的影响规律。
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.
基金Funded by the National Natural Science Foundation of China(No.21503096)
文摘MoS_2-decorated C_3N_4(C_3N_4/MoS_2) nanosheets hybrid photocatalysts were prepared by a simple sonication-impregnation method. Face-to-face lamellar heterojunctions were well established between two dimension(2D) C_3N_4 and MoS_2 nanosheets. The effects of MoS_2 content on the light absorption, charge transfer and photocatalytic activity of the hybrid samples were investigated. Characterization results show that MoS_2 nanosheets are well anchored on the face of C_3N_4 nanosheets and the composites have well dispersed layered morphology. After loading with MoS_2, the light absorption of composites was much improved, especially in visible-light region. The photocatalytic activities of C_3N_4/MoS_2 samples were evaluated based on the H_2 evolution under visible light irradiation(λ > 400 nm). When the loading amount of MoS_2 was increased to 5 wt%, the highest H_2 evolution rate(274 μmol·g^(-1)·h^(-1)) was obtained. Compared with samples obtained from direct impregnation method, sonication pretreatment is favorable for the formation of 2D layered heterojuctions and thus improve the photocatalytic activity. Slightly deactivation of C_3N_4/MoS_2 composites could be observed when recycled due to the mild photocorrosion of MoS_2. Based on the band alignments of C_3N_4 and MoS_2, a possible photocatalytic mechanism was discussed, where MoS_2 could efficiently promote the separation of the photogenerated carriers of C_3N_4.
基金supported by Technological Innovation Talents of Harbin Science and Technology Bureau(No.2017RAQXJ101)the Fundamental Research Foundation for Universities of Heilongjiang Province(No.LGYC2018JC008)+1 种基金supported by the Beijing National Laboratory for Molecular Sciences(No.BNLMS201911)the Young Scholar Training Program of Jilin University。
文摘Constructing heterostructures by combining COFs and TMD is a new strategy to design efficient photocatalysts for CO2 reduction reaction(CO2RR) due to their good stability,tunable band gaps and efficient charge separation.Based on the synthesis of completely novel C4N-COF in our previous re ported work,a new C4N/MoS2 heterostructure was constructed and then the related structural,electronic and optical properties were also studied using first principle calculations.The interlayer coupling effect and charge transfer between the C4N and MoS2 layer are systematically illuminated.The reduced band gap of the C4N/MoS2 heterostructure is beneficial to absorb more visible light.For the formation of type-Ⅱ band alignment,a built-in electric field appears which separates the photogene rated electrons and holes into different layers efficiently and produces redox active sites.The band alignment of the heterostructure ensures its photocatalytic activities of the whole CO2 reduction reaction.Furthermore,the charge density difference and charge carrier mobility confirm the existence of the built-in electric field at the interface of the C4N/MoS2 heterostructure directly.Finally,the high optical absorption indicates it is an efficient visible light harvesting photocatalyst.Therefore,this wo rk could provide strong insights into the internal mechanism and high photocatalytic activity of the C4N/MoS2 heterostructure and offer guiding of designing and synthesizing COF/TMD heterostructure photocatalysts.
基金financially supported by the National Natural Science Foundation(51972235)the China Postdoctoral Science Foundation(2020M680538)+3 种基金Natural Science Foundation of Shanghai(17ZR1447800)Jiangsu Key R&D Plan(BE2018006-4)the Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learningthe Fundamental Research Funds for the Central Universities
文摘Rational design of advanced polar hosts with high sulfur loading,facilitated ionic/electronic transport and effectively suppressed shuttling effect has great potential for high performance lithium-sulfur batteries,yet it remains challenging.Here we propose a novel templated spherical coassembly strategy to fabricate the MoS_(2)/C hollow spheres as an efficient sulfur host material.The unique hollow structure provides enough interior space for accommodating a substantial amount of sulfur,and effectively suppresses the diffusion of dissolved polysulfides by both physical confinement and chemical adsorption.Moreover,the ionic transport as well as the ability to mitigate volume variation upon cycling is also improved,thereby maximizing the utilization of sulfur.Owing to these merits,when evaluated as a sulfur host for lithiumsulfur batteries,the MoS_(2)/C hollow spheres exhibit appealing electrochemical performance with an impressive specific capacity of 1082 mA hg^(-1)at 0.1 C,excellent rate capability and superior cycling stability with a low fading rate of 0.04%per cycle.
