Attracted by high energy density and considerable conductivity of selenium(Se),Na-Se batteries have been deemed promising energy-storage systems.But,it still suffers from sluggish kinetic behaviors and similar“shuttl...Attracted by high energy density and considerable conductivity of selenium(Se),Na-Se batteries have been deemed promising energy-storage systems.But,it still suffers from sluggish kinetic behaviors and similar“shuttling effect”to S-electrodes.Herein,utilizing uniform hollow carbon spheres as precursors,Se-material is effectively loaded through vapor-infiltration method.Owing to the distribution of optimized pores,the content of microspores could be up to~60%(<2 nm),serving important roles for the physical confinement effect.Meanwhile,the rich oxygen-containing groups and N-elements could be noted,inducing the evolution of electron-moving behaviors.More significantly,assisted by the interfacial C-Se bonds and tiny Se distributions,Se electrodes are activated during cycling.Used as cathodes for Na-Se systems,the as-resulted samples display a capacity of 593.9 mA h g^(-1)after 100 cycles at the current density of 0.1 C.Even after 6000 cycles,the capacity could be still kept at about 225 mA h g^(-1)at 5.0 C.Supported by the detailed kinetic analysis,the designed microspores size induces the increasing redox reaction of nano Se,whilst the surface traits further render the enhancement of pseudo-capacitive contributions.Moreover,after cycling,the product Sex(x<4)in pores serves as the primary active material.Given this,the work is anticipated to provide an effective strategy for advanced electrodes for Na-Se systems.展开更多
Despite the intriguing merits of lithium-sulfur(Li-S) systems, they still suffer from the notorious‘‘shuttling-effect" of polysulfides. Herein, carbon materials with rational tailoring of morphology and pores w...Despite the intriguing merits of lithium-sulfur(Li-S) systems, they still suffer from the notorious‘‘shuttling-effect" of polysulfides. Herein, carbon materials with rational tailoring of morphology and pores were designed for strong loading/adsorption with the controlling of energy-storage ability.Through rational tailoring, it is strongly verified that such engineering of evolutions result in variational of sulfur immobilization in the obtained carbon. As expected, the targeted sample delivers a stable capacity of 925 m Ah g^(-1) after 100 loops. Supporting by the "cutting-off" manners, it is disclosed that mesopores in carbon possess more fascinated traits than micro/macropores in improving the utilization of sulfur and restraining Li_(2)S_x(4≤x≤8). Moreover, the long-chain polysulfide could be further consolidated by auto-doping oxygen groups. Supported by in-depth kinetic analysis, it is confirmed that the kinetics of ion/e-transfer during charging and discharging could be accelerated by mesopores, especially in stages of the formation of solid S_(8) and Li_(2)S, further improving the capacity of ion-storage in Li-S battery. Given this, the elaborate study provide significant insights into the effect of pore structure on kinetic performance about Li-storage behaviors in Li-S battery, and give guidance for improving sulfur immobilization.展开更多
Inspired by the success of CH-series acceptors, a small-molecular acceptor, CH-Tz was reported by adopting a new conjugationextended electron-deficient unit([1,2,5]thiadiazolo[3,4-b]pyrazine) on the central core. Owin...Inspired by the success of CH-series acceptors, a small-molecular acceptor, CH-Tz was reported by adopting a new conjugationextended electron-deficient unit([1,2,5]thiadiazolo[3,4-b]pyrazine) on the central core. Owing to the enhanced inter-/intramolecular interactions, CH-Tz exhibited near-infrared absorption and an effective three-dimensional molecular packing network in its single crystal. When blended with polymer donor PM6, the binary device achieved a high power conversion efficiency(PCE) of 18.54%, with a notable short-circuit current density(J_(sc)) of 27.54 m A cm-2and an excellent fill factor(FF) over 80%,which can be partly ascribed to the balanced charge transport properties in the blend film. After employing D18-Cl as the third component, an enhanced PCE of 18.85% was achieved due to a more obvious fiber network. Impressively, the CH-Tz-based OSC devices show excellent thermal stability and thickness insensitivity. Record-breaking Jscof 28.92 m A cm-2was reached for PM6:D18-Cl:CH-Tz ternary device with a thickness of 560 nm. Besides, CH-Tz shows potential in fabricating multicomponent high-performance organic solar cells, where over 19% efficiency could be realized in the quaternary device. Our work advances the strong influence of electron-deficient central units on molecular photovoltaic properties and guides the design of acceptors for stable and large-thickness organic solar cells.展开更多
基金financially supported by the National Natural Science Foundation of China(No.21973028,52004334)the outstanding youth science fund of Henan Normal University(No.2021JQ02),Natural Science Foundation of Hunan Province(2021JJ20073)+2 种基金National Key Research and Development Program of China(2018YFC1901601 and 2019YFC1907801)Scientific Research Fund of Hunan Provincial Education Department,grant number(20C0085)Collaborative Innovation Center for Clean and Efficient Utilization of Strategic Metal Mineral Resources,Foundation of State Key Laboratory of Mineral Processing(BGRIMM-KJSKL-2017-13)。
文摘Attracted by high energy density and considerable conductivity of selenium(Se),Na-Se batteries have been deemed promising energy-storage systems.But,it still suffers from sluggish kinetic behaviors and similar“shuttling effect”to S-electrodes.Herein,utilizing uniform hollow carbon spheres as precursors,Se-material is effectively loaded through vapor-infiltration method.Owing to the distribution of optimized pores,the content of microspores could be up to~60%(<2 nm),serving important roles for the physical confinement effect.Meanwhile,the rich oxygen-containing groups and N-elements could be noted,inducing the evolution of electron-moving behaviors.More significantly,assisted by the interfacial C-Se bonds and tiny Se distributions,Se electrodes are activated during cycling.Used as cathodes for Na-Se systems,the as-resulted samples display a capacity of 593.9 mA h g^(-1)after 100 cycles at the current density of 0.1 C.Even after 6000 cycles,the capacity could be still kept at about 225 mA h g^(-1)at 5.0 C.Supported by the detailed kinetic analysis,the designed microspores size induces the increasing redox reaction of nano Se,whilst the surface traits further render the enhancement of pseudo-capacitive contributions.Moreover,after cycling,the product Sex(x<4)in pores serves as the primary active material.Given this,the work is anticipated to provide an effective strategy for advanced electrodes for Na-Se systems.
基金financially supported by National National Key Research and Development Program of China (2019YFC1907801, 2018YFC1900305, 2018YFC1901601, 2018YFC1901602)the Natural Science Foundation of China (52004334, 51622406, 51634009 and U1704252)+4 种基金National 111 Project (No. B14034)the National Key R&D Program of China (2018YFC1901901)the Collab-orative Innovation Center for Clean and Efficient Utilization of Strategic Metal Mineral Resources, Found of State Key Laboratory of Mineral Processing (BGRIMM-KJSKL-2017-13)the Fundamental Research Funds for the Central Universities of Central South University (2019zzts1712020zzts203)the Hunan Provincial Innovation Foundation for Postgraduate (CX20190227)。
文摘Despite the intriguing merits of lithium-sulfur(Li-S) systems, they still suffer from the notorious‘‘shuttling-effect" of polysulfides. Herein, carbon materials with rational tailoring of morphology and pores were designed for strong loading/adsorption with the controlling of energy-storage ability.Through rational tailoring, it is strongly verified that such engineering of evolutions result in variational of sulfur immobilization in the obtained carbon. As expected, the targeted sample delivers a stable capacity of 925 m Ah g^(-1) after 100 loops. Supporting by the "cutting-off" manners, it is disclosed that mesopores in carbon possess more fascinated traits than micro/macropores in improving the utilization of sulfur and restraining Li_(2)S_x(4≤x≤8). Moreover, the long-chain polysulfide could be further consolidated by auto-doping oxygen groups. Supported by in-depth kinetic analysis, it is confirmed that the kinetics of ion/e-transfer during charging and discharging could be accelerated by mesopores, especially in stages of the formation of solid S_(8) and Li_(2)S, further improving the capacity of ion-storage in Li-S battery. Given this, the elaborate study provide significant insights into the effect of pore structure on kinetic performance about Li-storage behaviors in Li-S battery, and give guidance for improving sulfur immobilization.
基金supported by the Ministry of Science and Technology of China (2022YFB4200400, 2019YFA0705900,2023YFE0210400)the National Natural Science Foundation of China(21935007, 52025033, 52303237, 22361132530)。
文摘Inspired by the success of CH-series acceptors, a small-molecular acceptor, CH-Tz was reported by adopting a new conjugationextended electron-deficient unit([1,2,5]thiadiazolo[3,4-b]pyrazine) on the central core. Owing to the enhanced inter-/intramolecular interactions, CH-Tz exhibited near-infrared absorption and an effective three-dimensional molecular packing network in its single crystal. When blended with polymer donor PM6, the binary device achieved a high power conversion efficiency(PCE) of 18.54%, with a notable short-circuit current density(J_(sc)) of 27.54 m A cm-2and an excellent fill factor(FF) over 80%,which can be partly ascribed to the balanced charge transport properties in the blend film. After employing D18-Cl as the third component, an enhanced PCE of 18.85% was achieved due to a more obvious fiber network. Impressively, the CH-Tz-based OSC devices show excellent thermal stability and thickness insensitivity. Record-breaking Jscof 28.92 m A cm-2was reached for PM6:D18-Cl:CH-Tz ternary device with a thickness of 560 nm. Besides, CH-Tz shows potential in fabricating multicomponent high-performance organic solar cells, where over 19% efficiency could be realized in the quaternary device. Our work advances the strong influence of electron-deficient central units on molecular photovoltaic properties and guides the design of acceptors for stable and large-thickness organic solar cells.