Although lithium-sulfur batteries(Li SBs)are regarded as one of the most promising candidates for the next-generation energy storage system,the actual industrial application is hindered by the sluggish solid–liquid p...Although lithium-sulfur batteries(Li SBs)are regarded as one of the most promising candidates for the next-generation energy storage system,the actual industrial application is hindered by the sluggish solid–liquid phase conversion kinetics,severe shuttle effect,and low sulfur loadings.Herein,a zeolitic imidazolate framework(ZIF)derived heterogeneous ZnSe-CoSe nanoparticles encapsulated in hollow N-doped carbon nanocage(ZnSe-CoSe-HNC)was designed by etching with tannic acid as a multifunctional electrocatalyst to boost the polysulfide conversion kinetics in LiSBs.The hollow structure in ZIF ensures large inner voids for sulfur and buffering volume expansions.Abundant exposed ZnSe-CoSe heterogeneous interfaces serve as bifunctional adsorption-catalytic centers to accelerate the conversion kinetics and alleviate the shuttle effect.Together with the highly conductive framework,the ZnSe-CoSeHNC/S cathode exhibits a high initial reversible capacity of 1305.3 m A h g-1at 0.2 C,high-rate capability,and reliable cycling stability under high sulfur loading and lean electrolyte(maintaining at 745 m A h g-1after 200 cycles with a high sulfur loading of 6.4 mg cm-2and a low electrolyte/sulfur ratio of 6μL mg^(-1)).Theoretical calculations have demonstrated the heterostructures of ZnSe-CoSe offer higher binding energy to lithium polysulfides than that of ZnSe or CoSe,facilitating the electron transfer to lithium polysulfides.This work provides a novel heterostructure with superior catalytic ability and hollow conductive architecture,paving the way for the practical application of functional sulfur electrodes.展开更多
MoS_(2) is a promising anode material in sodium-ion battery technologies for possessing high theoretical capacity.However,the sluggish Na^(+) diffusion kinetics and low electronic conductivity hinder the promises.Here...MoS_(2) is a promising anode material in sodium-ion battery technologies for possessing high theoretical capacity.However,the sluggish Na^(+) diffusion kinetics and low electronic conductivity hinder the promises.Herein,a unique MoS_(2)/FeS_(2)/C heterojunction with abundant defects and hollow structure(MFCHHS)was constructed.The synergy of defect engineering in MoS_(2),FeS_(2),and the carbon layer of MFCHHS with a larger specific surface area provides multiple storage sites of Na^(+)corresponding to the surface-controlled process.The MoS_(2)/FeS_(2)/C heterostructure and rich defects in MoS_(2) and carbon layer lower the Na^(+) diffusion energy barrier.Additionally,the construction of MoS_(2)/FeS_(2) heterojunction promotes electron transfer at the interface,accompanying with excellent conductivity of the carbon layer to facilitate reversible electrochemical reactions.The abundant defects and mismatches at the interface of MoS_(2)/FeS_(2) and MoS_(2)/C heterojunctions could relieve lattice stress and volume change sequentially.As a result,the MFCHHS anode exhibits the high capacity of 613.1 mA h g^(-1)at 0.5 A g^(-1) and 306.1 mA h g^(-1) at 20 A g^(-1).The capacity retention of 85.0%after 1400 cycles at 5.0 A g^(-1) is achieved.The density functional theory(DFT)calculation and in situ transmission electron microscope(TEM),Raman,ex-situ X-ray photon spectroscopy(XPS)studies confirm the low volume change during intercalation/deintercalation process and the efficient Na^(+)storage in the layered structure of MoS_(2) and carbon layer,as well as the defects and heterostructures in MFCHHS.We believe this work could provide an inspiration for constructing heterojunction with abundant defects to foster fast electron and Na^(+) diffusion kinetics,resulting in excellent rate capability and cycling stability.展开更多
Metallic Sn has provoked tremendous progress as an anode material for sodium-ion batteries(SIBs).However,Sn anodes suffer from a dramatic capacity fading,owing to pulverization induced by drastic volume expansion duri...Metallic Sn has provoked tremendous progress as an anode material for sodium-ion batteries(SIBs).However,Sn anodes suffer from a dramatic capacity fading,owing to pulverization induced by drastic volume expansion during cycling.Herein,a flexible three-dimensional(3D)hierarchical conductive network electrode is designed by constructing Sn quantum dots(QDs)encapsulated in one-dimensional N,S codoped carbon nanofibers(NS-CNFs)sheathed within two-dimensional(2D)reduced graphene oxide(rGO)scrolls.In this ingenious strategy,1D NS-CNFs are regarded as building blocks to prevent the aggregation and pulverization of Sn QDs during sodiation/desodiation,2D rGO acts as electrical roads and“bridges”among NS-CNFs to improve the conductivity of the electrode and enlarge the contact area with electrolyte.Because of the unique structural merits,the flexible 3D hierarchical conductive network was directly used as binder-and current collectorfree anode for SIBs,exhibiting ultra-long cycling life(373 mAh g?1 after 5000 cycles at 1 A g?1),and excellent high-rate capability(189 mAh g?1 at 10 A g?1).This work provides a facile and efficient engineering method to construct 3D hierarchical conductive electrodes for other flexible energy storage devices.展开更多
This study is focused on the prediction of mining subsidence and its impact on the environment in the Hongqi mining area. The study was carried out by means of a probability integral model based, in first instance bas...This study is focused on the prediction of mining subsidence and its impact on the environment in the Hongqi mining area. The study was carried out by means of a probability integral model based, in first instance based on field surveys and the analysis of data collected from this area. Isolines of mining sub- sidence were then drawn and the impact caused by mining subsidence on the environment was analyzed quantitatively by spatial analysis with Geographic Information System (GIS). The results indicate that the subsidence area of the first working-mine can be as large as 2.54 km2, the maximum subsidence is 3440 mrn which will cause 1524 houses to be relocated. The entire subsidence area of the mine can reach 8.09 km2, with a maximum subsidence of 3590 ram. Under these circumstances the value of the loss of ecosystem services Will reach 5.371 million Yuan and the cost of relocating buildings will increase to 6.858 million Yuan.展开更多
The design strategy and efficiency optimization of a Ge-based n-type metal-oxide-semiconductor field-effect transistor(n-MOSFET)with a Si_(0.14)Ge_(0.72)Sn_(0.14)-Ge_(0.82)Sn_(0.18)-Ge quantum structure used for 2.45 ...The design strategy and efficiency optimization of a Ge-based n-type metal-oxide-semiconductor field-effect transistor(n-MOSFET)with a Si_(0.14)Ge_(0.72)Sn_(0.14)-Ge_(0.82)Sn_(0.18)-Ge quantum structure used for 2.45 GHz weak energy microwave wireless energy transmission is reported.The quantum structure combined withδ-doping technology is used to reduce the scattering of the device and improve its electron mobility;at the same time,the generation of surface channels is suppressed by the Si_(0.14)Ge_(0.72)Sn_(0.14) cap layer.By adjusting the threshold voltage of the device to 91 mV,setting the device aspect ratio to 1μm/0.4μm and adopting a novel diode connection method,the rectification efficiency of the device is improved.With simulation by Silvaco TCAD software,good performance is displayed in the transfer and output characteristics.For a simple half-wave rectifier circuit with a load of 1 pf and 20 kΩ,the rectification efficiency of the device can reach 7.14%at an input power of-10 dBm,which is 4.2 times that of a Si MOSFET(with a threshold voltage of 80 mV)under the same conditions;this device shows a better rectification effect than a Si MOSFET in the range of-30 dBm to 6.9 dBm.展开更多
In order to enhance the ionic conductivity of solid polymer electrolytes(SPEs)and their structural rigidity against lithium dendrite during lithium-ion battery(LIB)cycling,we propose porous garnet Li6.4La3Zr2Al0.2O12(...In order to enhance the ionic conductivity of solid polymer electrolytes(SPEs)and their structural rigidity against lithium dendrite during lithium-ion battery(LIB)cycling,we propose porous garnet Li6.4La3Zr2Al0.2O12(LLZO),as the filler to SPEs.The porous LLZO with interlinked grains was synthesized via a resol-assisted cationic coordinative co-assembly approach.The porous structure of LLZO with high specific surface area facilitates the interaction between polymer and filler and provides sufficient entrance for Li^(+)migration into the LLZO phase.Furthermore,the interconnection of LLZO grains forms continuous inorganic pathways for fast Li^(+)migration,which avoid the multiple diffusion for Li^(+)in interface.As a result,the SPEs with porous LLZO(SPE-PL)show a high ionic conductive of 0.73 mS·cm^(-1) at 30℃ and lithium-ion transference number of 0.40.The porous LLZO with uniformly dispersed pores also acts as an ion distributor to regulate ionic flux.The lithium-symmetrical batteries assembled with SPE-PL show a highly stable Li plating/stripping cycling for nearly 3000 h at 0.1 mA·cm^(-2).The corresponding Li/LiFePO_(4) batteries also exhibit excellent cyclic performance with capacity retention of 75%after nearly 500 cycles.This work brings new insights into the design of conductive fillers and the optimization of SPEs.展开更多
UltrasmaU Au10 clusters have a unique electronic structure and can act as a charge reservoir to donate electrons or accept charges. This is particularly important for catalysis, since it leads to facile charge transfe...UltrasmaU Au10 clusters have a unique electronic structure and can act as a charge reservoir to donate electrons or accept charges. This is particularly important for catalysis, since it leads to facile charge transfer across the interface between the gold species and the oxide substrate. To determine the electronic and structural effects of Au10 on the catalytic oxidation, a TiO2 charge carrier was chosen as the substrate to anchor Au10 for olefin oxidation. Au10 supported on TiO2-RP (RP = pyramid-capped columnar structure) exhibited superior catalytic activity to Au10/TiO2 nanotubes and Au10/P25. In addition, the supported Au10 clusters gave rise to higher activity than supported Au20, Au144 clusters, and 5 nm Au nanocrystals. The superior catalytic ability of Au^0fFiO2-RP arises from the charge/discharge effect of the Au10/TiO2-RP interface, which effectively improves the formation of active oxygen species on electron-rich gold atoms at the terminal position of Au10, and promotes the activation of olefin C--C bonds on the electron-deficient gold atoms of Au10.展开更多
基金financially supported by the Natural Science Foundation of Shandong Province,China(ZR2021QE192)the National Natural Science Foundation of China(21975154,22179078)+1 种基金the Postdoctoral Science Foundation of China(2018M63074)Qingdao Post-doctoral Applied Research Project(QDBSH20220202040)。
文摘Although lithium-sulfur batteries(Li SBs)are regarded as one of the most promising candidates for the next-generation energy storage system,the actual industrial application is hindered by the sluggish solid–liquid phase conversion kinetics,severe shuttle effect,and low sulfur loadings.Herein,a zeolitic imidazolate framework(ZIF)derived heterogeneous ZnSe-CoSe nanoparticles encapsulated in hollow N-doped carbon nanocage(ZnSe-CoSe-HNC)was designed by etching with tannic acid as a multifunctional electrocatalyst to boost the polysulfide conversion kinetics in LiSBs.The hollow structure in ZIF ensures large inner voids for sulfur and buffering volume expansions.Abundant exposed ZnSe-CoSe heterogeneous interfaces serve as bifunctional adsorption-catalytic centers to accelerate the conversion kinetics and alleviate the shuttle effect.Together with the highly conductive framework,the ZnSe-CoSeHNC/S cathode exhibits a high initial reversible capacity of 1305.3 m A h g-1at 0.2 C,high-rate capability,and reliable cycling stability under high sulfur loading and lean electrolyte(maintaining at 745 m A h g-1after 200 cycles with a high sulfur loading of 6.4 mg cm-2and a low electrolyte/sulfur ratio of 6μL mg^(-1)).Theoretical calculations have demonstrated the heterostructures of ZnSe-CoSe offer higher binding energy to lithium polysulfides than that of ZnSe or CoSe,facilitating the electron transfer to lithium polysulfides.This work provides a novel heterostructure with superior catalytic ability and hollow conductive architecture,paving the way for the practical application of functional sulfur electrodes.
基金the National Natural Science Foundation of China(NSFC)(22105059,22279112)the Talent Introduction Program of Hebei Agricultural University(YJ201810)+5 种基金the Youth Topnotch Talent Foundation of Hebei Provincial Universities(BJK2022023)the Natural Science Foundation of Hebei Province(B2022203018)the Fok Ying-Tong Education Foundation of China(171064)the Natural Science Foundation of Shandong Province,China(ZR2021QE192)the China Postdoctoral Science Foundation(2018M630747)the 333 Talent Program of Hebei Province(C20221018)for their support。
文摘MoS_(2) is a promising anode material in sodium-ion battery technologies for possessing high theoretical capacity.However,the sluggish Na^(+) diffusion kinetics and low electronic conductivity hinder the promises.Herein,a unique MoS_(2)/FeS_(2)/C heterojunction with abundant defects and hollow structure(MFCHHS)was constructed.The synergy of defect engineering in MoS_(2),FeS_(2),and the carbon layer of MFCHHS with a larger specific surface area provides multiple storage sites of Na^(+)corresponding to the surface-controlled process.The MoS_(2)/FeS_(2)/C heterostructure and rich defects in MoS_(2) and carbon layer lower the Na^(+) diffusion energy barrier.Additionally,the construction of MoS_(2)/FeS_(2) heterojunction promotes electron transfer at the interface,accompanying with excellent conductivity of the carbon layer to facilitate reversible electrochemical reactions.The abundant defects and mismatches at the interface of MoS_(2)/FeS_(2) and MoS_(2)/C heterojunctions could relieve lattice stress and volume change sequentially.As a result,the MFCHHS anode exhibits the high capacity of 613.1 mA h g^(-1)at 0.5 A g^(-1) and 306.1 mA h g^(-1) at 20 A g^(-1).The capacity retention of 85.0%after 1400 cycles at 5.0 A g^(-1) is achieved.The density functional theory(DFT)calculation and in situ transmission electron microscope(TEM),Raman,ex-situ X-ray photon spectroscopy(XPS)studies confirm the low volume change during intercalation/deintercalation process and the efficient Na^(+)storage in the layered structure of MoS_(2) and carbon layer,as well as the defects and heterostructures in MFCHHS.We believe this work could provide an inspiration for constructing heterojunction with abundant defects to foster fast electron and Na^(+) diffusion kinetics,resulting in excellent rate capability and cycling stability.
基金financially supported by the Natural Science Foundation of Shandong Province,China(ZR2018JL021,ZR2014EMQ011)the Applied Basic Research Foundation of Qingdao City(17-1-1-84-jch)+2 种基金the National Natural Science Foundation of China(51402160)supported by Taishan Scholar Program of Shandong Province,China,and National Demonstration Center for Experimental Applied Physics Education(Qingdao University)support from the China Postdoctoral Science Foundation Funded Project(2018M630747)and Qingdao Postdoctoral Applied Research Project.
文摘Metallic Sn has provoked tremendous progress as an anode material for sodium-ion batteries(SIBs).However,Sn anodes suffer from a dramatic capacity fading,owing to pulverization induced by drastic volume expansion during cycling.Herein,a flexible three-dimensional(3D)hierarchical conductive network electrode is designed by constructing Sn quantum dots(QDs)encapsulated in one-dimensional N,S codoped carbon nanofibers(NS-CNFs)sheathed within two-dimensional(2D)reduced graphene oxide(rGO)scrolls.In this ingenious strategy,1D NS-CNFs are regarded as building blocks to prevent the aggregation and pulverization of Sn QDs during sodiation/desodiation,2D rGO acts as electrical roads and“bridges”among NS-CNFs to improve the conductivity of the electrode and enlarge the contact area with electrolyte.Because of the unique structural merits,the flexible 3D hierarchical conductive network was directly used as binder-and current collectorfree anode for SIBs,exhibiting ultra-long cycling life(373 mAh g?1 after 5000 cycles at 1 A g?1),and excellent high-rate capability(189 mAh g?1 at 10 A g?1).This work provides a facile and efficient engineering method to construct 3D hierarchical conductive electrodes for other flexible energy storage devices.
基金Support for this work, provided by the Science and Technology Project of the Land and Resources Department of Henan Province (No.0979)
文摘This study is focused on the prediction of mining subsidence and its impact on the environment in the Hongqi mining area. The study was carried out by means of a probability integral model based, in first instance based on field surveys and the analysis of data collected from this area. Isolines of mining sub- sidence were then drawn and the impact caused by mining subsidence on the environment was analyzed quantitatively by spatial analysis with Geographic Information System (GIS). The results indicate that the subsidence area of the first working-mine can be as large as 2.54 km2, the maximum subsidence is 3440 mrn which will cause 1524 houses to be relocated. The entire subsidence area of the mine can reach 8.09 km2, with a maximum subsidence of 3590 ram. Under these circumstances the value of the loss of ecosystem services Will reach 5.371 million Yuan and the cost of relocating buildings will increase to 6.858 million Yuan.
基金supported by the National 111 Center(Grant No.B12026)Research on***Technology of Intelligent Reconfigurable General System(Grant No.F020250058)。
文摘The design strategy and efficiency optimization of a Ge-based n-type metal-oxide-semiconductor field-effect transistor(n-MOSFET)with a Si_(0.14)Ge_(0.72)Sn_(0.14)-Ge_(0.82)Sn_(0.18)-Ge quantum structure used for 2.45 GHz weak energy microwave wireless energy transmission is reported.The quantum structure combined withδ-doping technology is used to reduce the scattering of the device and improve its electron mobility;at the same time,the generation of surface channels is suppressed by the Si_(0.14)Ge_(0.72)Sn_(0.14) cap layer.By adjusting the threshold voltage of the device to 91 mV,setting the device aspect ratio to 1μm/0.4μm and adopting a novel diode connection method,the rectification efficiency of the device is improved.With simulation by Silvaco TCAD software,good performance is displayed in the transfer and output characteristics.For a simple half-wave rectifier circuit with a load of 1 pf and 20 kΩ,the rectification efficiency of the device can reach 7.14%at an input power of-10 dBm,which is 4.2 times that of a Si MOSFET(with a threshold voltage of 80 mV)under the same conditions;this device shows a better rectification effect than a Si MOSFET in the range of-30 dBm to 6.9 dBm.
基金supported by the National Natural Science Foundation of China(No.21805147)Natural Science Foundation of Shandong Province(No.ZR202211240080).
文摘In order to enhance the ionic conductivity of solid polymer electrolytes(SPEs)and their structural rigidity against lithium dendrite during lithium-ion battery(LIB)cycling,we propose porous garnet Li6.4La3Zr2Al0.2O12(LLZO),as the filler to SPEs.The porous LLZO with interlinked grains was synthesized via a resol-assisted cationic coordinative co-assembly approach.The porous structure of LLZO with high specific surface area facilitates the interaction between polymer and filler and provides sufficient entrance for Li^(+)migration into the LLZO phase.Furthermore,the interconnection of LLZO grains forms continuous inorganic pathways for fast Li^(+)migration,which avoid the multiple diffusion for Li^(+)in interface.As a result,the SPEs with porous LLZO(SPE-PL)show a high ionic conductive of 0.73 mS·cm^(-1) at 30℃ and lithium-ion transference number of 0.40.The porous LLZO with uniformly dispersed pores also acts as an ion distributor to regulate ionic flux.The lithium-symmetrical batteries assembled with SPE-PL show a highly stable Li plating/stripping cycling for nearly 3000 h at 0.1 mA·cm^(-2).The corresponding Li/LiFePO_(4) batteries also exhibit excellent cyclic performance with capacity retention of 75%after nearly 500 cycles.This work brings new insights into the design of conductive fillers and the optimization of SPEs.
基金We are grateful for financial support by the National Natural Science Foundation of China (No. 21273151), and Hundred Talent Program of Chinese Academy of Sciences. Y. Z. acknowledges support by Ministry of Education for returned overseas Chinese scholars.
文摘UltrasmaU Au10 clusters have a unique electronic structure and can act as a charge reservoir to donate electrons or accept charges. This is particularly important for catalysis, since it leads to facile charge transfer across the interface between the gold species and the oxide substrate. To determine the electronic and structural effects of Au10 on the catalytic oxidation, a TiO2 charge carrier was chosen as the substrate to anchor Au10 for olefin oxidation. Au10 supported on TiO2-RP (RP = pyramid-capped columnar structure) exhibited superior catalytic activity to Au10/TiO2 nanotubes and Au10/P25. In addition, the supported Au10 clusters gave rise to higher activity than supported Au20, Au144 clusters, and 5 nm Au nanocrystals. The superior catalytic ability of Au^0fFiO2-RP arises from the charge/discharge effect of the Au10/TiO2-RP interface, which effectively improves the formation of active oxygen species on electron-rich gold atoms at the terminal position of Au10, and promotes the activation of olefin C--C bonds on the electron-deficient gold atoms of Au10.