The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered architectures.Polypyrrole(PPy)emerges as an exceedingly co...The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered architectures.Polypyrrole(PPy)emerges as an exceedingly conductive polymer and a prospective pseudocapacitive materials for supercapacitors,yet the inferior cyclic stability and unpredictable polymerization patterns severely impede its real-world applicability.Here,for the first time,an innovative seed-induced in-situ polymerization assisted 3D printing strategy is proposed to fabricate PPy-reduced graphene oxide/poly(vinylidene difluoride-cohexafluoropropylene)(PVDF-HFP)(PPy-rGO/PH)electrodes with controllable polymerization behavior and exceptional areal mass loading.The preferred active sites uniformly pre-planted on the 3D-printed graphene substrates serve as reliable seeds to induce efficient polypyrrole deposition,achieving an impressive mass loading of 185.6 mg cm^(-2)(particularly 79.2 mg cm^(-2)for polypyrrole)and a superior areal capacitance of 25.2 F cm^(-2)at 2 mA cm^(-2)for a 12-layer electrode.In agreement with theses appealing features,an unprecedented areal energy density of 1.47 mW h cm^(-2)for a symmetrical device is registered,a rarely achieved value for other PPy/rGO-based supercapacitors.This work highlights a promising route to preparing high energy density energy storage modules for real-world applications.展开更多
Carbon-based electric double layer capacitors(EDLCs)hold tremendous potentials due to their high-power performance and excellent cycle stability.However,the practical use of EDLCs is limited by the low energy density ...Carbon-based electric double layer capacitors(EDLCs)hold tremendous potentials due to their high-power performance and excellent cycle stability.However,the practical use of EDLCs is limited by the low energy density in aqueous electrolyte and sluggish diffusion kinetics in organic or/and ionic liquids electrolyte.Herein,3D carbon frameworks(3DCFs)constructed by interconnected nanocages(10-20 nm)with an ultrathin wall of ca.2 nm have been fabricated,which possess high specific surface area,hierarchical porosity and good conductive network.After deoxidization,the deoxidized 3DCF(3DCFDO)exhibits a record low IR drop of 0.064 V at 100 A g^−1 and ultrafast charge/discharge rate up to 10 V s^−1.The related device can be charged up to 77.4%of its maximum capacitance in 0.65 s at 100 A g^−1 in 6 M KOH.It has been found that the 3DCF-DO has a great affinity to EMIMBF4,resulting in a high specific capacitance of 174 F g^−1 at 1 A g^−1,and a high energy density of 34 Wh kg^−1 at an ultrahigh power density of 150 kW kg^−1 at 4 V after a fast charge in 1.11 s.This work provides a facile fabrication of novel 3D carbon frameworks for supercapacitors with ultrafast charge/discharge rate and high energy-power density.展开更多
Lithium-sulfur(Li-S) batteries are one of the most promising rechargeable storage devices due to the high theoretical energy density.However,the low areal sulfur loading impedes their commercial development.Herein,a 3...Lithium-sulfur(Li-S) batteries are one of the most promising rechargeable storage devices due to the high theoretical energy density.However,the low areal sulfur loading impedes their commercial development.Herein,a 3 D free-standing sulfur cathode scaffold is rationally designed and fabricated by coaxially coating polar Ti_3 C_2 T_x flakes on sulfur-impregnated carbon cloth(Ti_3 C_2 T_x@S/CC) to achieve high loading and high energy density Li-S batteries,in which,the flexible CC substrate with highly porous structure can accommodate large amounts of sulfur and ensure fast electron transfer,while the outer-coated Ti_3 C_2 T_x can serve as a polar and conductive protective layer to further promote the conductivity of the whole electrode,achieve physical blocking and chemical anchoring of lithium-polysulfides as well as catalyze their conversion.Due to these advantages,at a sulfur loading of 4 mg cm^(-2),Li-S cells with Ti_3 C_2 T_x@S/CC cathodes can deliver outstanding cycling stability(746.1 mAh g^(-1) after 200 cycles at1 C),superb rate performance(866.8 mAh g^(-1) up to 2 C) and a high specific energy density(564.2 Wh kg^(-1) after 100 cycles at 0.5 C).More significantly,they also show the commercial potential that can compete with current lithium-ion batteries due to the high areal capacity of 6.7 mAh cm^(-2) at the increased loading of 8 mg cm^(-2).展开更多
Developing high-performing oxygen evolution reaction(OER)electrocatalysts under high-current operation conditions is critical for future commercial applications of alkaline water electrolysis for clean energy generati...Developing high-performing oxygen evolution reaction(OER)electrocatalysts under high-current operation conditions is critical for future commercial applications of alkaline water electrolysis for clean energy generation.Herein,we prepared a three-dimensional(3D)bimetallic oxyhydroxide hybrid grown on a Ni foam(NiFeOOH/NF)prepared by immersing Ni foam(NF)into Fe(NO_(3))_(3) solution.In this unique 3D structure,the NiFeOOH/NF hybrid was composed of crystalline Ni(OH)_(2) and amorphous FeOOH evenly grown on the NF surface.As a bimetallic oxyhydroxide electrocatalyst,the NiFeOOH/NF hybrid exhibited excellent catalytic activity,surpassing not only the other reported Ni–Fe based electrocatalysts,but also the commercial Ir/C catalyst.In situ electrochemical Raman spectroscopy demonstrated the active FeOOH and NiOOH phases involved in the OER process.Profiting from the synergy of Fe and Ni catalytic sites,the NiFeOOH/NF hybrid delivered an outstanding OER performance under challenging industrial conditions in a 10.0 mol·L^(-1) KOH electrolyte at 80℃,requiring potentials as small as 1.47 and 1.51 V to achieve the super-high catalytic current densities of 100 and 500mA∙cm^(-2),respectively.展开更多
Multi-stages volcanic are available in HX area, shielding the seismic waves. Previous seismic acquisitions of large size bin, less fold coverage and narrow azimuth result in indistinct fault images, low S/N ratio and ...Multi-stages volcanic are available in HX area, shielding the seismic waves. Previous seismic acquisitions of large size bin, less fold coverage and narrow azimuth result in indistinct fault images, low S/N ratio and the difficulty of multi-stages volcanic characterization. In reference to the successful experience of domestic and overseas volcanic exploration, the low frequency excitation and receiving, and survey with wide range, high coverage, wide azimuth should be paid more attention, associated with two-dimensional and three-dimensional wave equation forward modeling and real data processing contrast analysis method. The image of underlying strata and fault are remarkably improved in the new method, according to the processing results of new seismic data. The new method will provide technical reference for the similar volcanic development area in the future seismic acquisition design.展开更多
We report a wire-shaped three-dimensional(3D)-hybrid supercapacitor with high volumetric capacitance and high energy density due to an interconnected 3D-configuration of the electrode allowing for large number of elec...We report a wire-shaped three-dimensional(3D)-hybrid supercapacitor with high volumetric capacitance and high energy density due to an interconnected 3D-configuration of the electrode allowing for large number of electrochemical active sites,easy access of electrolyte ions,and facile charge transport for flexible wearable applications.The interconnected and compact electrode delivers a high volumetric capacitance(gravimetric capacitance)of 73 F cm−3(2446 F g−1),excellent rate capability,and cycle stability.The 3D-nickel cobalt-layered double hydroxide onto 3D-nickel wire(NiCo LDH/3D-Ni)//the 3D-manganese oxide onto 3D-nickel wire(Mn3O4/3D-Ni)hybrid supercapacitor exhibits energy density of 153.3 Wh kg−1 and power density of 8810 W kg−1.The red lightemitting diode powered by the as-prepared hybrid supercapacitor can operate for 80 min after being charged for tens of seconds and exhibit excellent electrochemical stability under various deformation conditions.The results verify that such wire-shaped 3D-hybrid supercapacitors are promising alternatives for batteries with long charge–discharge times,for smart wearable and implantable devices.展开更多
The actual manufacture of supercapacitors(SCs)is restricted by the inadequate energy density,and the energy density of devices can be properly promoted by assembling zinc-ion capacitors(ZICs)which used capacitive cath...The actual manufacture of supercapacitors(SCs)is restricted by the inadequate energy density,and the energy density of devices can be properly promoted by assembling zinc-ion capacitors(ZICs)which used capacitive cathode and battery-type anode.Two-dimensional(2D)MXene has brought great focuses in the electrode research on the foundation of large redox-active surface,but the specific capacitance is still affected by the tight stacking of interlaminations.Ti_(3)C_(2)T_(x)@polyaniline(PANI)heterostructures are prepared by uniformly depositing the conductive polymer PANI nanorods as the intercalation agent into the external of Ti_(3)C_(2)T_(x)nanosheets to inhibit stacking.Subsequently,by using graphene oxide(GO)-assisted low-temperature hydrothermal self-assembly manufacture,2D heterostructures are assembled into the three-dimensional(3D)porous crosslinked Ti_(3)C_(2)T_(x)@PANI-reduced graphene oxide(RGO)hydrogels.Attributed to the synergistic work of PANI nanorods,Ti_(3)C_(2)T_(X)nanosheets,and 3D crosslinking frameworks of RGO to match capacitive and battery effects,3D porous hierarchical Ti_(3)C_(2)T_(x)@PANI-RGO heterostructure hydrogels have rich ion transport channels,a large number of active sites,and excellent reaction kinetics.ZIC is assembled by using Ti_(3)C_(2)T_(x)@PANI-RGO heterostructure hydrogels as cathodes and zinc foil as anodes.In this work,Ti_(3)C_(2)T_(x)@PANI-RGO//Zn ZIC exhibits a wide working window(2.0 V),marked specific capacitance(589.89 F·g^(−1)at 0.5 A·g−1),salient energy density(327.71 Wh·kg^(−1)at 513.61 W·kg^(−1)and 192.20 Wh·kg^(−1)at 13,005.87 W·kg^(−1)),and durable cycling stability(97.87%capacitance retention after 10,000 cycles at 10 A·g^(−1)).This study emphasizes the device design of ZICs and the broad prospect of Ti_(3)C_(2)T_(x)-based hydrogels as viable cathodes for ZICs.展开更多
基金financially supported by the National Natural Science Foundation of China(No.51933007,No.52373047,No.52302106)the Sichuan Youth Science and Technology Innovation Research Team Project(No.2022JDTD0012)+2 种基金the Program for Featured Directions of Engineering Multidisciplines of Sichuan University(No.2020SCUNG203)the Natural Science Foundation of Sichuan Province(No.2023NSFSC0418)the Program for State Key Laboratory of Polymer Materials Engineering(No.sklpme2022-3-10)。
文摘The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered architectures.Polypyrrole(PPy)emerges as an exceedingly conductive polymer and a prospective pseudocapacitive materials for supercapacitors,yet the inferior cyclic stability and unpredictable polymerization patterns severely impede its real-world applicability.Here,for the first time,an innovative seed-induced in-situ polymerization assisted 3D printing strategy is proposed to fabricate PPy-reduced graphene oxide/poly(vinylidene difluoride-cohexafluoropropylene)(PVDF-HFP)(PPy-rGO/PH)electrodes with controllable polymerization behavior and exceptional areal mass loading.The preferred active sites uniformly pre-planted on the 3D-printed graphene substrates serve as reliable seeds to induce efficient polypyrrole deposition,achieving an impressive mass loading of 185.6 mg cm^(-2)(particularly 79.2 mg cm^(-2)for polypyrrole)and a superior areal capacitance of 25.2 F cm^(-2)at 2 mA cm^(-2)for a 12-layer electrode.In agreement with theses appealing features,an unprecedented areal energy density of 1.47 mW h cm^(-2)for a symmetrical device is registered,a rarely achieved value for other PPy/rGO-based supercapacitors.This work highlights a promising route to preparing high energy density energy storage modules for real-world applications.
基金the financial support from the National Natural Science Foundation of China(51672033,U1610255,U1703251).
文摘Carbon-based electric double layer capacitors(EDLCs)hold tremendous potentials due to their high-power performance and excellent cycle stability.However,the practical use of EDLCs is limited by the low energy density in aqueous electrolyte and sluggish diffusion kinetics in organic or/and ionic liquids electrolyte.Herein,3D carbon frameworks(3DCFs)constructed by interconnected nanocages(10-20 nm)with an ultrathin wall of ca.2 nm have been fabricated,which possess high specific surface area,hierarchical porosity and good conductive network.After deoxidization,the deoxidized 3DCF(3DCFDO)exhibits a record low IR drop of 0.064 V at 100 A g^−1 and ultrafast charge/discharge rate up to 10 V s^−1.The related device can be charged up to 77.4%of its maximum capacitance in 0.65 s at 100 A g^−1 in 6 M KOH.It has been found that the 3DCF-DO has a great affinity to EMIMBF4,resulting in a high specific capacitance of 174 F g^−1 at 1 A g^−1,and a high energy density of 34 Wh kg^−1 at an ultrahigh power density of 150 kW kg^−1 at 4 V after a fast charge in 1.11 s.This work provides a facile fabrication of novel 3D carbon frameworks for supercapacitors with ultrafast charge/discharge rate and high energy-power density.
基金supported by the National Natural Science Foundation of China (51772069)。
文摘Lithium-sulfur(Li-S) batteries are one of the most promising rechargeable storage devices due to the high theoretical energy density.However,the low areal sulfur loading impedes their commercial development.Herein,a 3 D free-standing sulfur cathode scaffold is rationally designed and fabricated by coaxially coating polar Ti_3 C_2 T_x flakes on sulfur-impregnated carbon cloth(Ti_3 C_2 T_x@S/CC) to achieve high loading and high energy density Li-S batteries,in which,the flexible CC substrate with highly porous structure can accommodate large amounts of sulfur and ensure fast electron transfer,while the outer-coated Ti_3 C_2 T_x can serve as a polar and conductive protective layer to further promote the conductivity of the whole electrode,achieve physical blocking and chemical anchoring of lithium-polysulfides as well as catalyze their conversion.Due to these advantages,at a sulfur loading of 4 mg cm^(-2),Li-S cells with Ti_3 C_2 T_x@S/CC cathodes can deliver outstanding cycling stability(746.1 mAh g^(-1) after 200 cycles at1 C),superb rate performance(866.8 mAh g^(-1) up to 2 C) and a high specific energy density(564.2 Wh kg^(-1) after 100 cycles at 0.5 C).More significantly,they also show the commercial potential that can compete with current lithium-ion batteries due to the high areal capacity of 6.7 mAh cm^(-2) at the increased loading of 8 mg cm^(-2).
基金Y.Hou expresses appreciation for the assistance of the National Natural Science Foundation of China(21922811,21878270,and 21961160742)the Zhejiang Provincial Natural Science Foundation of China(LR19B060002)+2 种基金the Fundamental Research Funds for the Central Universities(2020XZZX002-09)the Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang(2019R01006)the Startup Foundation for Hundred-Talent Program of Zhejiang University.K.Ostrikov acknowledges partial assistance from the Australian Research Council.
文摘Developing high-performing oxygen evolution reaction(OER)electrocatalysts under high-current operation conditions is critical for future commercial applications of alkaline water electrolysis for clean energy generation.Herein,we prepared a three-dimensional(3D)bimetallic oxyhydroxide hybrid grown on a Ni foam(NiFeOOH/NF)prepared by immersing Ni foam(NF)into Fe(NO_(3))_(3) solution.In this unique 3D structure,the NiFeOOH/NF hybrid was composed of crystalline Ni(OH)_(2) and amorphous FeOOH evenly grown on the NF surface.As a bimetallic oxyhydroxide electrocatalyst,the NiFeOOH/NF hybrid exhibited excellent catalytic activity,surpassing not only the other reported Ni–Fe based electrocatalysts,but also the commercial Ir/C catalyst.In situ electrochemical Raman spectroscopy demonstrated the active FeOOH and NiOOH phases involved in the OER process.Profiting from the synergy of Fe and Ni catalytic sites,the NiFeOOH/NF hybrid delivered an outstanding OER performance under challenging industrial conditions in a 10.0 mol·L^(-1) KOH electrolyte at 80℃,requiring potentials as small as 1.47 and 1.51 V to achieve the super-high catalytic current densities of 100 and 500mA∙cm^(-2),respectively.
文摘Multi-stages volcanic are available in HX area, shielding the seismic waves. Previous seismic acquisitions of large size bin, less fold coverage and narrow azimuth result in indistinct fault images, low S/N ratio and the difficulty of multi-stages volcanic characterization. In reference to the successful experience of domestic and overseas volcanic exploration, the low frequency excitation and receiving, and survey with wide range, high coverage, wide azimuth should be paid more attention, associated with two-dimensional and three-dimensional wave equation forward modeling and real data processing contrast analysis method. The image of underlying strata and fault are remarkably improved in the new method, according to the processing results of new seismic data. The new method will provide technical reference for the similar volcanic development area in the future seismic acquisition design.
基金supported by national research foundation of Korea(NRF)(No.NRF-2019R1H1A2039743)S-Oil corporation,and “Human Resources Program in Energy Technology” of the Korea Institute of Energy Technology Evaluation and Planning(KETEP)granted financial resource from the Ministry of Trade,Industry and Energy,Republic of Korea(No.20194010201890)
文摘We report a wire-shaped three-dimensional(3D)-hybrid supercapacitor with high volumetric capacitance and high energy density due to an interconnected 3D-configuration of the electrode allowing for large number of electrochemical active sites,easy access of electrolyte ions,and facile charge transport for flexible wearable applications.The interconnected and compact electrode delivers a high volumetric capacitance(gravimetric capacitance)of 73 F cm−3(2446 F g−1),excellent rate capability,and cycle stability.The 3D-nickel cobalt-layered double hydroxide onto 3D-nickel wire(NiCo LDH/3D-Ni)//the 3D-manganese oxide onto 3D-nickel wire(Mn3O4/3D-Ni)hybrid supercapacitor exhibits energy density of 153.3 Wh kg−1 and power density of 8810 W kg−1.The red lightemitting diode powered by the as-prepared hybrid supercapacitor can operate for 80 min after being charged for tens of seconds and exhibit excellent electrochemical stability under various deformation conditions.The results verify that such wire-shaped 3D-hybrid supercapacitors are promising alternatives for batteries with long charge–discharge times,for smart wearable and implantable devices.
基金the National Key Research and Development Program of China(No.2022YFC2105900)the National Natural Science Foundation of China(No.52073022).
文摘The actual manufacture of supercapacitors(SCs)is restricted by the inadequate energy density,and the energy density of devices can be properly promoted by assembling zinc-ion capacitors(ZICs)which used capacitive cathode and battery-type anode.Two-dimensional(2D)MXene has brought great focuses in the electrode research on the foundation of large redox-active surface,but the specific capacitance is still affected by the tight stacking of interlaminations.Ti_(3)C_(2)T_(x)@polyaniline(PANI)heterostructures are prepared by uniformly depositing the conductive polymer PANI nanorods as the intercalation agent into the external of Ti_(3)C_(2)T_(x)nanosheets to inhibit stacking.Subsequently,by using graphene oxide(GO)-assisted low-temperature hydrothermal self-assembly manufacture,2D heterostructures are assembled into the three-dimensional(3D)porous crosslinked Ti_(3)C_(2)T_(x)@PANI-reduced graphene oxide(RGO)hydrogels.Attributed to the synergistic work of PANI nanorods,Ti_(3)C_(2)T_(X)nanosheets,and 3D crosslinking frameworks of RGO to match capacitive and battery effects,3D porous hierarchical Ti_(3)C_(2)T_(x)@PANI-RGO heterostructure hydrogels have rich ion transport channels,a large number of active sites,and excellent reaction kinetics.ZIC is assembled by using Ti_(3)C_(2)T_(x)@PANI-RGO heterostructure hydrogels as cathodes and zinc foil as anodes.In this work,Ti_(3)C_(2)T_(x)@PANI-RGO//Zn ZIC exhibits a wide working window(2.0 V),marked specific capacitance(589.89 F·g^(−1)at 0.5 A·g−1),salient energy density(327.71 Wh·kg^(−1)at 513.61 W·kg^(−1)and 192.20 Wh·kg^(−1)at 13,005.87 W·kg^(−1)),and durable cycling stability(97.87%capacitance retention after 10,000 cycles at 10 A·g^(−1)).This study emphasizes the device design of ZICs and the broad prospect of Ti_(3)C_(2)T_(x)-based hydrogels as viable cathodes for ZICs.
