Earth-abundant magnetite(Fe_(3)O_(4))as cathode materials in aqueous zinc-ion batteries(ZIBs)is limited by its very low capacity and poor cycling.Here,a combined strategy based on carbon coating and electrolyte optimi...Earth-abundant magnetite(Fe_(3)O_(4))as cathode materials in aqueous zinc-ion batteries(ZIBs)is limited by its very low capacity and poor cycling.Here,a combined strategy based on carbon coating and electrolyte optimization is adopted to improve the performance of Fe_(3)O_(4).The Zn-Fe_(3)O_(4)@C batteries display specific capacities of 93 mAh g^(−1) and 81%capacity retention after 200 cycles.Such performance is attributed to the enhanced electrical conductivity and structural stability of Fe_(3)O_(4)@C nanocomposites with suppressed iron dissolution.Experimental analysis reveals that the charge storage is contributed by diffusion-limited redox reactions and surface-controlled pseudocapacitance.A stretchable Zn-Fe_(3)O_(4)@C battery is further fabricated,showing stable performance when it is bent or stretched.Fe_(3)O_(4) is a promising cathode material for cost-effective,safe,sustainable and wearable energy supplies.展开更多
Active sites of two-dimensional(2D)electrocatalysts are often partially blocked owing to their inevitable stacking and hydrophobic polymeric binders in macroscale electrodes,therefore impeding their applications in ef...Active sites of two-dimensional(2D)electrocatalysts are often partially blocked owing to their inevitable stacking and hydrophobic polymeric binders in macroscale electrodes,therefore impeding their applications in efficient electrolyzers.Here,using layered double hydroxide(LDH)nanosheets as a model 2D electrocatalyst,we demonstrate that their performance toward water splitting can be boosted when they are electrostatically assembled into an organized structure pillared by hydrophilic polyelectrolytes or nanoparticles in a layer-by-layer(LbL)fashion.In particular,their mass activity on a planar electrode can be as large as 2.267 mA·μg^(-1) toward oxygen evolution reaction(OER),when NiFe-LDH nanosheets are electrostatically connected by poly(sodium 4-styrenesulfonate)(PSS),while drop-casted NiFe-LDH nanosheets only have a mass activity of 0.116 mA·μg^(-1).In addition,these homogeneous NiFe-LDH nanofilms can be easily deposited on three-dimensional(3D)surfaces with high areas,such as carbon cloths,to serve as practical electrodes with overpotentials of 328 mV at a current density of 100 mA·cm^(-2),and stability for 40 h.Furthermore,Pt nanoparticles can be LbL assembled with NiFe-LDH as bifunctional electrodes for synergistically boosted oxygen and hydrogen evolution reactions(HER),leading to successful overall water splitting powered by a 1.5 V battery.This study heralds the spatial control of 2D nanomaterials in nanoscale precision as an efficient strategy for the design of advanced electrocatalysts.展开更多
Recently discovered bismuth oxychalcogenide(Bi_(2) O_(2) Se) has aroused great interest due to its ultrahigh carrier mobility,tunable band gap and good environmental stability,making it a promising candidate for high-...Recently discovered bismuth oxychalcogenide(Bi_(2) O_(2) Se) has aroused great interest due to its ultrahigh carrier mobility,tunable band gap and good environmental stability,making it a promising candidate for high-performance electronics and optoelectronics.Their synthesis by colloidal approaches represents a cost-effective alternative to well-established chemical vapor deposition methods,and the resulting electronic-grade inks are important for large-area printed or wearable electronics.However,it is still challenging to control the colloidal growth of Bi_(2) O_(2) Se nanosheets in solution in addition to their assembly into high-performance thin films.Here,we report a two-step colloidal synthesis of Bi_(2) O_(2) Se nanosheets by separating the seeding and growth steps,thereby achieving controllable production of nanosheets with a lateral size of 1.4 mm and a thickness of 10 nm at optimized reaction conditions.These Bi_(2) O_(2) Se nanosheets are electrostatically assembled into large-area thin films,from which a photodetector is fabricated with a responsivity of 6.1 A/W and a short response time of 368 ms under the 520-nm laser illumination.The device exhibits fast response to modulations as high as 100 k Hz,along with a à3 dB bandwidth of 1 kHz.This work provides an important understanding of the controlled colloidal synthesis of Bi_(2) O_(2) Se nanosheets,and demonstrates their potential applications in fast photodetectors.展开更多
The polypnictide complexes of rare earth cations have drawn the attention of the scientific community for their uncommon bonding modes and potential applications.Herein,we present a systematic and comprehensive summar...The polypnictide complexes of rare earth cations have drawn the attention of the scientific community for their uncommon bonding modes and potential applications.Herein,we present a systematic and comprehensive summary on recent advances in the field of rare earth polypnictides,focusing on their synthesis,structures,and reactivities.The structural stbilizing effects imposed by the electropositive rare earth cations as well as the reducing capability of rare earth precursors in the synthesis of these polypnictide complexes are described in this review.We also disscuss in detail the bonding interactions and coordination modes between rare earth cations and polypnictide clusters as well as the similarities and the peculiarity of some structures.展开更多
Fabrication of large-area and uniform semiconducting thin films of two-dimensional(2D)materials is paramount for the full exploitation of their atomic thicknesses and smooth surfaces in integrated circuits.In addition...Fabrication of large-area and uniform semiconducting thin films of two-dimensional(2D)materials is paramount for the full exploitation of their atomic thicknesses and smooth surfaces in integrated circuits.In addition to elaborate vapor-based synthesis techniques for the wafer-scale growth of 2D films,solution-based approaches for high-quality thin films from the liquid dispersions of 2D flakes,despite underdeveloped,are alternative cost-effective tactics.Here,we present layer-by-layer(LbL)assembly as an effective approach to obtaining scalable semiconducting films of molybdenum disulfide(MoS_(2))for field-effect transistors(FETs).LbL assembly is achieved by coordinating electrochemically exfoliated MoS_(2) with cationic poly(diallyldimethylammonium chloride)(PDDA)through electrostatic interactions.The PDDA/MoS_(2) percolating nanofilms show controlled and self-limited growth on a variety of substrates,and are easily patterned through lift-off processes.Ion gel gated FETs are fabricated on these MoS_(2) nanofilms,and they show mobilities of 9.8 cm^(2)·V^(−1)·s^(−1),on/off ratios of 2.1×10^(5) with operating voltages less than 2 V.The annealing temperature in the fabrication process can be as low as 200℃,thereby permitting the fabrication of flexible FETs on polyethylene terephthalate substrates.The LbL assembly technique holds great promise for the large-scale fabrication of flexible electronics based on solution-processed 2D semiconductors.展开更多
基金This work was supported by National Natural Science Foundation of China(51873088)the Tianjin Municipal Science and Technology Commission(18JCZDJC38400)in China.
文摘Earth-abundant magnetite(Fe_(3)O_(4))as cathode materials in aqueous zinc-ion batteries(ZIBs)is limited by its very low capacity and poor cycling.Here,a combined strategy based on carbon coating and electrolyte optimization is adopted to improve the performance of Fe_(3)O_(4).The Zn-Fe_(3)O_(4)@C batteries display specific capacities of 93 mAh g^(−1) and 81%capacity retention after 200 cycles.Such performance is attributed to the enhanced electrical conductivity and structural stability of Fe_(3)O_(4)@C nanocomposites with suppressed iron dissolution.Experimental analysis reveals that the charge storage is contributed by diffusion-limited redox reactions and surface-controlled pseudocapacitance.A stretchable Zn-Fe_(3)O_(4)@C battery is further fabricated,showing stable performance when it is bent or stretched.Fe_(3)O_(4) is a promising cathode material for cost-effective,safe,sustainable and wearable energy supplies.
基金supported by the National Natural Science Foundation of China(NSFC)(Nos.52273076,52111540268,and 12004195)the 111 Project(No.B18030)in China+1 种基金The authors also acknowledge the financial support by Haihe Laboratory of Sustainable Chemical Transformations(No.YYJC202101)Open Research Fund Program of the State Key Laboratory of Low Dimensional Quantum Physics(No.KF202113).
文摘Active sites of two-dimensional(2D)electrocatalysts are often partially blocked owing to their inevitable stacking and hydrophobic polymeric binders in macroscale electrodes,therefore impeding their applications in efficient electrolyzers.Here,using layered double hydroxide(LDH)nanosheets as a model 2D electrocatalyst,we demonstrate that their performance toward water splitting can be boosted when they are electrostatically assembled into an organized structure pillared by hydrophilic polyelectrolytes or nanoparticles in a layer-by-layer(LbL)fashion.In particular,their mass activity on a planar electrode can be as large as 2.267 mA·μg^(-1) toward oxygen evolution reaction(OER),when NiFe-LDH nanosheets are electrostatically connected by poly(sodium 4-styrenesulfonate)(PSS),while drop-casted NiFe-LDH nanosheets only have a mass activity of 0.116 mA·μg^(-1).In addition,these homogeneous NiFe-LDH nanofilms can be easily deposited on three-dimensional(3D)surfaces with high areas,such as carbon cloths,to serve as practical electrodes with overpotentials of 328 mV at a current density of 100 mA·cm^(-2),and stability for 40 h.Furthermore,Pt nanoparticles can be LbL assembled with NiFe-LDH as bifunctional electrodes for synergistically boosted oxygen and hydrogen evolution reactions(HER),leading to successful overall water splitting powered by a 1.5 V battery.This study heralds the spatial control of 2D nanomaterials in nanoscale precision as an efficient strategy for the design of advanced electrocatalysts.
基金supported by National Science Foundations of China (Nos.51873088, 12004195)Natural Science Foundations of Tianjin (No.20JCQNJC01820)+2 种基金Tianjin Municipal Science and Technology Commission (No.18JCZDJC38400)“111” Project of China’s Higher Education (No.B18030)Fundamental Research Funds for the Central Universities from Nankai University (No.63201061)。
文摘Recently discovered bismuth oxychalcogenide(Bi_(2) O_(2) Se) has aroused great interest due to its ultrahigh carrier mobility,tunable band gap and good environmental stability,making it a promising candidate for high-performance electronics and optoelectronics.Their synthesis by colloidal approaches represents a cost-effective alternative to well-established chemical vapor deposition methods,and the resulting electronic-grade inks are important for large-area printed or wearable electronics.However,it is still challenging to control the colloidal growth of Bi_(2) O_(2) Se nanosheets in solution in addition to their assembly into high-performance thin films.Here,we report a two-step colloidal synthesis of Bi_(2) O_(2) Se nanosheets by separating the seeding and growth steps,thereby achieving controllable production of nanosheets with a lateral size of 1.4 mm and a thickness of 10 nm at optimized reaction conditions.These Bi_(2) O_(2) Se nanosheets are electrostatically assembled into large-area thin films,from which a photodetector is fabricated with a responsivity of 6.1 A/W and a short response time of 368 ms under the 520-nm laser illumination.The device exhibits fast response to modulations as high as 100 k Hz,along with a à3 dB bandwidth of 1 kHz.This work provides an important understanding of the controlled colloidal synthesis of Bi_(2) O_(2) Se nanosheets,and demonstrates their potential applications in fast photodetectors.
基金the National Natural Science Foundation of China(Nos.21971118 and 21722106 to ZMS).
文摘The polypnictide complexes of rare earth cations have drawn the attention of the scientific community for their uncommon bonding modes and potential applications.Herein,we present a systematic and comprehensive summary on recent advances in the field of rare earth polypnictides,focusing on their synthesis,structures,and reactivities.The structural stbilizing effects imposed by the electropositive rare earth cations as well as the reducing capability of rare earth precursors in the synthesis of these polypnictide complexes are described in this review.We also disscuss in detail the bonding interactions and coordination modes between rare earth cations and polypnictide clusters as well as the similarities and the peculiarity of some structures.
基金The work was supported by the National Natural Science Foundation of China(No.51873088)Tianjin Municipal Science and Technology Commission(No.18JCZDJC38400)111 Project(B18030)in China.
文摘Fabrication of large-area and uniform semiconducting thin films of two-dimensional(2D)materials is paramount for the full exploitation of their atomic thicknesses and smooth surfaces in integrated circuits.In addition to elaborate vapor-based synthesis techniques for the wafer-scale growth of 2D films,solution-based approaches for high-quality thin films from the liquid dispersions of 2D flakes,despite underdeveloped,are alternative cost-effective tactics.Here,we present layer-by-layer(LbL)assembly as an effective approach to obtaining scalable semiconducting films of molybdenum disulfide(MoS_(2))for field-effect transistors(FETs).LbL assembly is achieved by coordinating electrochemically exfoliated MoS_(2) with cationic poly(diallyldimethylammonium chloride)(PDDA)through electrostatic interactions.The PDDA/MoS_(2) percolating nanofilms show controlled and self-limited growth on a variety of substrates,and are easily patterned through lift-off processes.Ion gel gated FETs are fabricated on these MoS_(2) nanofilms,and they show mobilities of 9.8 cm^(2)·V^(−1)·s^(−1),on/off ratios of 2.1×10^(5) with operating voltages less than 2 V.The annealing temperature in the fabrication process can be as low as 200℃,thereby permitting the fabrication of flexible FETs on polyethylene terephthalate substrates.The LbL assembly technique holds great promise for the large-scale fabrication of flexible electronics based on solution-processed 2D semiconductors.
基金supported by the National Natural Science Foundation of China (51873088)Tianjin Municipal Science and Technology Commission (18JCZDJC38400) in China“the Fundamental Research Funds for the Central Universities”, Nankai University (023/63191303)
基金supported by the National Natural Science Foundation of China (21722702 and 21872102)Tianjin Municipal Science and Technology Bureau (18YFZCSF00730, 18YFZCSF00770, 18ZXSZSF00230 and 19YFZCSF00740)。