In the interlayer expansion of the layered zeolite precursor COK-5, a Sn, salt, bis（2,4-pentanedionate）- dichlorotin [Sn（acac）2CL2], instead of a silylating agent was used to link the layers at 180 ℃. The obtaine...In the interlayer expansion of the layered zeolite precursor COK-5, a Sn, salt, bis（2,4-pentanedionate）- dichlorotin [Sn（acac）2CL2], instead of a silylating agent was used to link the layers at 180 ℃. The obtained material, which is designed as Sn-COE-5, shows a shift of the first XRD reflection, which is very similar to that of COK-5 interlayer expanded with dichlorodimethylsilane （DCDMS）, indicating an increase in interlayer distance. X-ray diffraction （XRD）, N2 sorption isotherms, inductively coupled plasma （ICP）, and X-ray photo- electron spectroscopy （XPS） support the incorporation of isolated Sn sites in the sample. In the conversion of glucose to levulinic acid. Sn-COE-5 exhibits much higher activity than COK-5, which is due to the presence of Lewis acidic sites in the Sn-COE-5.展开更多
Aqueous zinc-ion batteries(AZIBs)have attracted extensive attention owing to their environmental friendliness and low cost.However,the application of AZIBs is hindered by the lack of suitable cathode materials due to ...Aqueous zinc-ion batteries(AZIBs)have attracted extensive attention owing to their environmental friendliness and low cost.However,the application of AZIBs is hindered by the lack of suitable cathode materials due to the sluggish kinetics of divalent Zn^(2+)in host materials.Herein,Se doped MoS_(2)nanosheets(MoS_(1.8)Se_(0.2))grown on reduced graphene oxide(rGO)are proposed as a promising cathode for AZIBs.Se doping generates expanded interlayer spacing and a high 1T phase(up to 64%)of MoS_(2),which improve its ion diffusion kinetics and electronic conductivity.Remarkably,the MoS_(1.8)Se_(0.2)/rGO cathode exhibits a high capacity of 213.6 mA h g^(-1)at 0.1 A g^(-1),excellent rate capability of 62.2 mA h g^(-1)at 8.0 A g^(-1),and long-term stability with 74.1%capacity retention after 1000 cycles at 1.0 A g^(-1).Moreover,reversible H^(+)/Zn^(2+)co-insertion/extraction behaviors of MoS_(1.8)Se_(0.2)/rGO are revealed.This study proves that anion doping of metal sulfides is a feasible method to develop high-performance cathodes for AZIBs.展开更多
Developing advanced cathode modification strategies to address the inherent high charge density of Al^(3+) is essential for achieving high-energy-density and long-cycle-life rechargeable aluminum batteries(RABs).Herei...Developing advanced cathode modification strategies to address the inherent high charge density of Al^(3+) is essential for achieving high-energy-density and long-cycle-life rechargeable aluminum batteries(RABs).Herein,we engineer tetraethylammonium(TEA)cation intercalation as a dual-function strategy that concurrently enables interlayer distance enlargement and electrostatic shielding effects,resolving Al^(3+) polarization-induced sluggish kinetics and cathode degradation in RABs.TEA intercalation triggers exceptional V2O5 interlayer expansion from 4.37 to 13.10Å,while the modulated charge distribution generates an electrostatic shielding effect that significantly weakens the Coulombic interactions between Al^(3+) and V2O5 frameworks.This dual mechanism collectively enhances ion diffusion kinetics and suppresses lattice stress accumulation.Ex situ X-ray diffraction and transmission electron microscopy analyses confirm that the“molecular pillar effect”of TEA enables minimal and highly reversible structural deformation of the cathode(<2.0%volume change after 200 cycles),demonstrating zero-strain aluminum-storage behavior.The optimized cathode delivers a high reversible capacity of 258 mAh g^(−1) at 0.5 A g^(−1),maintains 99%capacity retention at 5.0 A g^(−1),and exhibits an ultralow capacity decay rate of 0.01%per cycle over 6000 cycles.This work opens new pathways for designing stable high-performance RAB cathodes through synergistic modulation of electronic and lattice structures.展开更多
A highly efficient and reusable plane‐curved and interlayer‐expanded MoS2nanocatalyst with increased exposure of active sites was prepared.The catalyst was used for the heterogeneous hydrogen transfer reaction of ni...A highly efficient and reusable plane‐curved and interlayer‐expanded MoS2nanocatalyst with increased exposure of active sites was prepared.The catalyst was used for the heterogeneous hydrogen transfer reaction of nitroarenes with hydrazine monohydrate as a reductant under mild reaction conditions without pressure and base,which was different from other hydrogen transfer systems that require the presence of a base(e.g.,propan‐2‐ol/KOH).The sandwiching of carbon between the MoS2nanosheets increased the distance between the layers of MoS2and exposed more Mo sites,resulting in superior catalytic performance compared with that of bulk MoS2catalyst.The active hydrogen(H*)generated from N2H4could directly transfer to the–NO2groups of nitrobenzene to form aniline followed by N2emission,which was confirmed by detecting the gas emission with mass spectrometry during the decomposition of hydrazine or the co‐existence of nitrobenzene and hydrazine.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved.展开更多
Potassium-ion batteries are regarded as the low-cost alternative to lithium-ion batteries.However,their development is hampered by the lack of suitable electrode materials.In this work,we demonstrate that MoS2 with ex...Potassium-ion batteries are regarded as the low-cost alternative to lithium-ion batteries.However,their development is hampered by the lack of suitable electrode materials.In this work,we demonstrate that MoS2 with expanded interlayers represents a promising candidate for the electrochemical storage of potassium ions.Hierarchical interlayer-expanded MoS2 assemblies supported on carbon nanotubes are prepared via a straightforward solution method.The increased interlayer spacing not only enables the better accommodation of foreign ions,but also lowers the diffusion energy barrier and improves diffusion kinetics of ions.When investigated as the anode material of potassium ion batteries,our interlayer-expanded MoS2 assemblies exhibit an excellent electrochemical performance with large capacity(up to∼520 mAhg^−1),good rate capability(∼310 mAhg^−1 at 1,000 mAg^−1)and impressive cycling stability,superior to most competitors.展开更多
基金supported by the National Natural Science Foundation of China (21422306 and 21403192)Zhejiang Provincial Natural Science Foundation of China under grant no. LR15B030001the Fundamental Research Funds for the Central Universities (2015XZZX004-04)
文摘In the interlayer expansion of the layered zeolite precursor COK-5, a Sn, salt, bis（2,4-pentanedionate）- dichlorotin [Sn（acac）2CL2], instead of a silylating agent was used to link the layers at 180 ℃. The obtained material, which is designed as Sn-COE-5, shows a shift of the first XRD reflection, which is very similar to that of COK-5 interlayer expanded with dichlorodimethylsilane （DCDMS）, indicating an increase in interlayer distance. X-ray diffraction （XRD）, N2 sorption isotherms, inductively coupled plasma （ICP）, and X-ray photo- electron spectroscopy （XPS） support the incorporation of isolated Sn sites in the sample. In the conversion of glucose to levulinic acid. Sn-COE-5 exhibits much higher activity than COK-5, which is due to the presence of Lewis acidic sites in the Sn-COE-5.
基金supported by the Natural Science Foundation of Hunan Province(2021JJ30094)the National Natural Science Foundation of China(22379041 and 52103313)the Science and Technology Innovation Program of Hunan Province(2023RC1045).
文摘Aqueous zinc-ion batteries(AZIBs)have attracted extensive attention owing to their environmental friendliness and low cost.However,the application of AZIBs is hindered by the lack of suitable cathode materials due to the sluggish kinetics of divalent Zn^(2+)in host materials.Herein,Se doped MoS_(2)nanosheets(MoS_(1.8)Se_(0.2))grown on reduced graphene oxide(rGO)are proposed as a promising cathode for AZIBs.Se doping generates expanded interlayer spacing and a high 1T phase(up to 64%)of MoS_(2),which improve its ion diffusion kinetics and electronic conductivity.Remarkably,the MoS_(1.8)Se_(0.2)/rGO cathode exhibits a high capacity of 213.6 mA h g^(-1)at 0.1 A g^(-1),excellent rate capability of 62.2 mA h g^(-1)at 8.0 A g^(-1),and long-term stability with 74.1%capacity retention after 1000 cycles at 1.0 A g^(-1).Moreover,reversible H^(+)/Zn^(2+)co-insertion/extraction behaviors of MoS_(1.8)Se_(0.2)/rGO are revealed.This study proves that anion doping of metal sulfides is a feasible method to develop high-performance cathodes for AZIBs.
基金supported by the Key R&D Program of Zaozhuang city,China(2024GH12)the Zaozhuang Gathering of Talents Program。
文摘Developing advanced cathode modification strategies to address the inherent high charge density of Al^(3+) is essential for achieving high-energy-density and long-cycle-life rechargeable aluminum batteries(RABs).Herein,we engineer tetraethylammonium(TEA)cation intercalation as a dual-function strategy that concurrently enables interlayer distance enlargement and electrostatic shielding effects,resolving Al^(3+) polarization-induced sluggish kinetics and cathode degradation in RABs.TEA intercalation triggers exceptional V2O5 interlayer expansion from 4.37 to 13.10Å,while the modulated charge distribution generates an electrostatic shielding effect that significantly weakens the Coulombic interactions between Al^(3+) and V2O5 frameworks.This dual mechanism collectively enhances ion diffusion kinetics and suppresses lattice stress accumulation.Ex situ X-ray diffraction and transmission electron microscopy analyses confirm that the“molecular pillar effect”of TEA enables minimal and highly reversible structural deformation of the cathode(<2.0%volume change after 200 cycles),demonstrating zero-strain aluminum-storage behavior.The optimized cathode delivers a high reversible capacity of 258 mAh g^(−1) at 0.5 A g^(−1),maintains 99%capacity retention at 5.0 A g^(−1),and exhibits an ultralow capacity decay rate of 0.01%per cycle over 6000 cycles.This work opens new pathways for designing stable high-performance RAB cathodes through synergistic modulation of electronic and lattice structures.
基金supported by the Ministry of Science and Technology(MOST,2016YFA0204100 and 2011CBA00504)the National Natural Science Foundation of China(21573254,91545110)+1 种基金the Youth Innovation Promotion Association(CAS)the Sinopec China~~
文摘A highly efficient and reusable plane‐curved and interlayer‐expanded MoS2nanocatalyst with increased exposure of active sites was prepared.The catalyst was used for the heterogeneous hydrogen transfer reaction of nitroarenes with hydrazine monohydrate as a reductant under mild reaction conditions without pressure and base,which was different from other hydrogen transfer systems that require the presence of a base(e.g.,propan‐2‐ol/KOH).The sandwiching of carbon between the MoS2nanosheets increased the distance between the layers of MoS2and exposed more Mo sites,resulting in superior catalytic performance compared with that of bulk MoS2catalyst.The active hydrogen(H*)generated from N2H4could directly transfer to the–NO2groups of nitrobenzene to form aniline followed by N2emission,which was confirmed by detecting the gas emission with mass spectrometry during the decomposition of hydrazine or the co‐existence of nitrobenzene and hydrazine.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved.
基金supported by the National Natural Science Foundation of China(No.51972219)the Priority Academic Program Development of Jiangsu Higher Education Institutions and Collaborative Innovation Center of Suzhou Nano Science and Technology.
文摘Potassium-ion batteries are regarded as the low-cost alternative to lithium-ion batteries.However,their development is hampered by the lack of suitable electrode materials.In this work,we demonstrate that MoS2 with expanded interlayers represents a promising candidate for the electrochemical storage of potassium ions.Hierarchical interlayer-expanded MoS2 assemblies supported on carbon nanotubes are prepared via a straightforward solution method.The increased interlayer spacing not only enables the better accommodation of foreign ions,but also lowers the diffusion energy barrier and improves diffusion kinetics of ions.When investigated as the anode material of potassium ion batteries,our interlayer-expanded MoS2 assemblies exhibit an excellent electrochemical performance with large capacity(up to∼520 mAhg^−1),good rate capability(∼310 mAhg^−1 at 1,000 mAg^−1)and impressive cycling stability,superior to most competitors.
