Sodium-ion batteries have garnered significant attention as a cost-effective alternative to lithium-ion batteries due to the abundance and affordability of sodium precursors.However,the lack of suitable electrode mate...Sodium-ion batteries have garnered significant attention as a cost-effective alternative to lithium-ion batteries due to the abundance and affordability of sodium precursors.However,the lack of suitable electrode materials with both high capacity and excellent stability continues to hinder their practical viability.Herein,we couple lattice strain and sulfur deficiency effects in a tin monosulfide/reduced graphene oxide composite to enhance sodium storage performance.Experimental results and theoretical calculations reveal that the synergistic effects of lattice strain and sulfur vacancies in tin monosulfide promote rapid(de)intercalation near the surface/edge of the material,thereby enhancing its pseudocapacitive sodium storage properties.Consequently,the strained and defective tin monosulfide/reduced graphene oxide composite demonstrates a high reversible capacity of 511.82 mAh g^(-1) at 1 A g^(-1) and an outstanding rate capability of 450.60 mAh g^(-1) at 3 A g^(-1).This study offers an effective strategy for improving sodium storage performance through lattice strain and defect engineering.展开更多
Transition metal chalcogenides have nowadays garnered burgeoning interest owing to their fascinating electronic and catalytic properties,thus possessing great implications for energy conversion and storage application...Transition metal chalcogenides have nowadays garnered burgeoning interest owing to their fascinating electronic and catalytic properties,thus possessing great implications for energy conversion and storage applications.In this regard,their controllable synthesis in a large scale at low cost has readily become a focus of research.Herein we report diatomite-template generic and scalable production of VS2 and other transition metal sulfides targeting emerging energy conversion and storage applications.The conformal growth of VS2over diatomite template would endow them with defect-abundant features.Throughout detailed experimental investigation in combination with theoretical simulation,we reveal that the enriched active sites/sulfur vacancies of thus-derived VS2 architectures would pose positive impacts on the catalytic performance such in electrocatalytic hydrogen evolution reactions.We further show that the favorable electrical conductivity and highly exposed sites of VS2 hold promise for serving as sulfur host in the realm of Li-S batteries.Our work offers new insights into the templated and customized synthesis of defect-rich sulfides in a scalable fashion to benefit multifunctional energy applications.展开更多
The generation process,influence of the laser parameters on the production of zinc metal(Zn^(0)),and the mechanism of interaction between the laser and ZnS were studied.It was observed that an increase in the number o...The generation process,influence of the laser parameters on the production of zinc metal(Zn^(0)),and the mechanism of interaction between the laser and ZnS were studied.It was observed that an increase in the number of S defects enhanced the quantity of Zn^(2+)ejected from the ZnS crystals,which increased the possibility of Zn^(2+)bonding with electrons to produce Zn^(0).A maximum Zn^(0)content of 9.3%in the products was detected upon changing the laser parameters.Upon analyzing the changes in the surface topography during the laser interaction with ZnS,it was shown that the interaction mechanism between laser and ZnS had a synergistic effect comprised of photochemical and photothermal processes,in which the photochemical mechanism predominated.展开更多
High performances of Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)solar cells are heavily influenced by the quality of heterojunctions.Herein,an oxygen(O)doping of CZTSSe/CdS heterojunction is performed to suppress the formation of th...High performances of Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)solar cells are heavily influenced by the quality of heterojunctions.Herein,an oxygen(O)doping of CZTSSe/CdS heterojunction is performed to suppress the formation of the defects by an ultraviolet ozone(UV-O_(3))treatment for the efficient flexible CZTSSe solar cells.The introduction of O reduces the non-radiative recombination and increases the carrier concentration of the CdS films.Furthermore,the defect density of the CdS film has been reduced from 8.24×10^(16)to2.91×10^(16)cm^(-3)by the O-doping.The results indicate that the electron transport is effectively promoted due to the decreased conduction band offset(CBO)at the heterojunction interface.As a result,the champion flexible CZTSSe solar cell achieves a power conversion efficiency(PCE)of 11.21%,with a significantly improved short circuit current density.The study for improving the CZTSSe/CdS heterojunction through O-doping treatment provides a new insight for enhancing the PCE of the flexible CZTSSe solar cells.展开更多
As a promising candidate electrode material in both Li-and Na-ion batteries(L/SIBs),the application of Co_(9)S_(8) is being hindered by its unsatisfactory electrochemical performance caused by the sluggish ion diffusi...As a promising candidate electrode material in both Li-and Na-ion batteries(L/SIBs),the application of Co_(9)S_(8) is being hindered by its unsatisfactory electrochemical performance caused by the sluggish ion diffusion kinetics and drastic volume expansion.Herein,a hybrid material composed of Co_(9)S_(8-x),N-doped carbon foam that seeded with Co nanoparticles(Co_(9)S_(8-x)@Co-NC) is constructed.Particularly,theoretical and experimental results imply that a built-in electric field at the interface of Co and NC is observed due to the variation of Fermi levels,forming rich Mott-Schottky-like heterointerfaces,which can significantly enhance the charge transfer capability between the active materials of Co_(9)S_(8) and conductive NC skeleton.Moreover,the sulfur defects in Co_(9)S_(8-x)can not only effectively lower the energy barrier of the ion diffusion and charge transfer processes,but also endow the target sample with more storage/adsorption/active sites for Li^(+)/Na^(+) ions,thus improving the rate performance of the Co_(9)S_(8-x)@Co-NC composite.As a result,the Co_(9)S_(8-x)@Co-NC exhibits fast surface-controlled redox kinetics and robust cycling stability.For instance,the Co_(9)S_(8-x)@Co-NC displays impressive Li-storage properties in both half and full cells with a high reversible capacity of 1007.4 mA h g^(-1)at 0.1 A g^(-1)after 100 cycles and superior rate capability up to 5 A g^(-1).Moreover,based on these comprehensive merits,the Co_(9)S_(8-x)@Co-NC composite shows decent electrochemical performance(472.2 and 311.1 mA h g^(-1)at 0.1 and 10 A g^(-1),respectively) as an anode for SIBs.This work presents an effective strategy for the construction of Mott-Schottky-like heterointerfaces in Co_(9)S_(8) based materials and provides specific inspiration for future works designing high-performance electrodes via interfacial engineering.展开更多
MoS_(2)is a promising electrocatalyst because of its natural abundance and outstanding electrochemical stability.However,the poor conductivity and low activity limit its catalytic performance;furthermore,MoS_(2)is una...MoS_(2)is a promising electrocatalyst because of its natural abundance and outstanding electrochemical stability.However,the poor conductivity and low activity limit its catalytic performance;furthermore,MoS_(2)is unable to satisfy the requirements of most industrial applications.In this study,to obtain a P-doped MoS_(2)catalyst with S vacancy defects,P is inserted into the MoS_(2)matrix via a solid phase ion exchange at room temperature.The optimal P-doping amount is 11.4 wt%,and the resultant catalyst delivers excellent electrocatalytic properties for the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)with the corresponding overpotentials of 93 and 316 mV at 10 mA cm^(-2) in an alkaline solution;these values surpass the overpotentials of most previously reported MoS_(2)-based materials.Theoretical calculations and results demonstrate that the synergistic effect of the doped P,which forms active centers in the basal plane of MoS_(2),and S vacancy defects caused by P doping intensifies the intrinsic electronic conductivity and electrocatalytic activity of the catalyst.Density functional theory calculations demonstrate that P optimizes the free energy of the MoS_(2)matrix for hydrogen adsorption,thereby considerably increasing the intrinsic activity of the doped catalyst for the HER compared with that observed from pristine MoS_(2).The enhanced catalytic activity of P-doped MoS_(2)for the OER is attributed to the ability of the doped P which facilitates the adsorption of hydroxyl and hydroperoxy intermediates and reduces the reaction energy barrier.This study provides a new environmentally friendly and convenient solid-phase ion exchange method to improve the electrocatalytic capability of two-dimensional transition-metal dichalcogenides in largescale applications.展开更多
基金supported by the National Natural Science Foundation of China(no.22109023,no.22179022,and no.22209027)the Youth Innovation Fund of Fujian Province(no.2021J05043 and no.2022J05046)+5 种基金the National Key Research and Development Program of China(2023YFC3906300)the FuXiaQuan National Independent Innovation Demonstration Zone Collaborative Innovation Platform(no.2022-P-027)the·“Hundred Talents·Plan”of Fujian Provincethe“Top Young Talents of Young Eagle”Program of Fujian Provincethe Award Program for Fujian Minjiang Scholar Professorshipthe Talent Fund Program of Fujian Normal University.
文摘Sodium-ion batteries have garnered significant attention as a cost-effective alternative to lithium-ion batteries due to the abundance and affordability of sodium precursors.However,the lack of suitable electrode materials with both high capacity and excellent stability continues to hinder their practical viability.Herein,we couple lattice strain and sulfur deficiency effects in a tin monosulfide/reduced graphene oxide composite to enhance sodium storage performance.Experimental results and theoretical calculations reveal that the synergistic effects of lattice strain and sulfur vacancies in tin monosulfide promote rapid(de)intercalation near the surface/edge of the material,thereby enhancing its pseudocapacitive sodium storage properties.Consequently,the strained and defective tin monosulfide/reduced graphene oxide composite demonstrates a high reversible capacity of 511.82 mAh g^(-1) at 1 A g^(-1) and an outstanding rate capability of 450.60 mAh g^(-1) at 3 A g^(-1).This study offers an effective strategy for improving sodium storage performance through lattice strain and defect engineering.
基金financially supported by the National Natural Science Foundation of China(nos.51702225,21671059,51702218)Jiangsu Youth Science Foundation(no.BK20170336)Program for Changjiang Scholars and Innovative Research Team in University(IRT-17R36).
文摘Transition metal chalcogenides have nowadays garnered burgeoning interest owing to their fascinating electronic and catalytic properties,thus possessing great implications for energy conversion and storage applications.In this regard,their controllable synthesis in a large scale at low cost has readily become a focus of research.Herein we report diatomite-template generic and scalable production of VS2 and other transition metal sulfides targeting emerging energy conversion and storage applications.The conformal growth of VS2over diatomite template would endow them with defect-abundant features.Throughout detailed experimental investigation in combination with theoretical simulation,we reveal that the enriched active sites/sulfur vacancies of thus-derived VS2 architectures would pose positive impacts on the catalytic performance such in electrocatalytic hydrogen evolution reactions.We further show that the favorable electrical conductivity and highly exposed sites of VS2 hold promise for serving as sulfur host in the realm of Li-S batteries.Our work offers new insights into the templated and customized synthesis of defect-rich sulfides in a scalable fashion to benefit multifunctional energy applications.
基金Shanghai Leading Talent Project,China(No.2022048)National Natural Science Foundation of China(No.52174385)。
文摘The generation process,influence of the laser parameters on the production of zinc metal(Zn^(0)),and the mechanism of interaction between the laser and ZnS were studied.It was observed that an increase in the number of S defects enhanced the quantity of Zn^(2+)ejected from the ZnS crystals,which increased the possibility of Zn^(2+)bonding with electrons to produce Zn^(0).A maximum Zn^(0)content of 9.3%in the products was detected upon changing the laser parameters.Upon analyzing the changes in the surface topography during the laser interaction with ZnS,it was shown that the interaction mechanism between laser and ZnS had a synergistic effect comprised of photochemical and photothermal processes,in which the photochemical mechanism predominated.
基金supported by the National Natural Science Foundation of China(62474043,62074037,52372183)the Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(2021ZZ124)+1 种基金Fujian Provincial Natural Science Foundation of China(2024J09015)the Foundation of Fujian Provincial Department of Industry and Information Technology of China(82318075)。
文摘High performances of Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)solar cells are heavily influenced by the quality of heterojunctions.Herein,an oxygen(O)doping of CZTSSe/CdS heterojunction is performed to suppress the formation of the defects by an ultraviolet ozone(UV-O_(3))treatment for the efficient flexible CZTSSe solar cells.The introduction of O reduces the non-radiative recombination and increases the carrier concentration of the CdS films.Furthermore,the defect density of the CdS film has been reduced from 8.24×10^(16)to2.91×10^(16)cm^(-3)by the O-doping.The results indicate that the electron transport is effectively promoted due to the decreased conduction band offset(CBO)at the heterojunction interface.As a result,the champion flexible CZTSSe solar cell achieves a power conversion efficiency(PCE)of 11.21%,with a significantly improved short circuit current density.The study for improving the CZTSSe/CdS heterojunction through O-doping treatment provides a new insight for enhancing the PCE of the flexible CZTSSe solar cells.
基金the financial support of the National Natural Science Foundation of China (51902089)the Educational Department of Jilin Province, China (JJKH20230587KJ)the Science and Technology Department of Jilin Province, China (20220101071JC)。
文摘As a promising candidate electrode material in both Li-and Na-ion batteries(L/SIBs),the application of Co_(9)S_(8) is being hindered by its unsatisfactory electrochemical performance caused by the sluggish ion diffusion kinetics and drastic volume expansion.Herein,a hybrid material composed of Co_(9)S_(8-x),N-doped carbon foam that seeded with Co nanoparticles(Co_(9)S_(8-x)@Co-NC) is constructed.Particularly,theoretical and experimental results imply that a built-in electric field at the interface of Co and NC is observed due to the variation of Fermi levels,forming rich Mott-Schottky-like heterointerfaces,which can significantly enhance the charge transfer capability between the active materials of Co_(9)S_(8) and conductive NC skeleton.Moreover,the sulfur defects in Co_(9)S_(8-x)can not only effectively lower the energy barrier of the ion diffusion and charge transfer processes,but also endow the target sample with more storage/adsorption/active sites for Li^(+)/Na^(+) ions,thus improving the rate performance of the Co_(9)S_(8-x)@Co-NC composite.As a result,the Co_(9)S_(8-x)@Co-NC exhibits fast surface-controlled redox kinetics and robust cycling stability.For instance,the Co_(9)S_(8-x)@Co-NC displays impressive Li-storage properties in both half and full cells with a high reversible capacity of 1007.4 mA h g^(-1)at 0.1 A g^(-1)after 100 cycles and superior rate capability up to 5 A g^(-1).Moreover,based on these comprehensive merits,the Co_(9)S_(8-x)@Co-NC composite shows decent electrochemical performance(472.2 and 311.1 mA h g^(-1)at 0.1 and 10 A g^(-1),respectively) as an anode for SIBs.This work presents an effective strategy for the construction of Mott-Schottky-like heterointerfaces in Co_(9)S_(8) based materials and provides specific inspiration for future works designing high-performance electrodes via interfacial engineering.
基金supported by the National Natural Science Foundation of China(52072196)the Major Basic Research Program of the Natural Science Foundation of Shandong Province(ZR2020ZD09)。
文摘MoS_(2)is a promising electrocatalyst because of its natural abundance and outstanding electrochemical stability.However,the poor conductivity and low activity limit its catalytic performance;furthermore,MoS_(2)is unable to satisfy the requirements of most industrial applications.In this study,to obtain a P-doped MoS_(2)catalyst with S vacancy defects,P is inserted into the MoS_(2)matrix via a solid phase ion exchange at room temperature.The optimal P-doping amount is 11.4 wt%,and the resultant catalyst delivers excellent electrocatalytic properties for the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)with the corresponding overpotentials of 93 and 316 mV at 10 mA cm^(-2) in an alkaline solution;these values surpass the overpotentials of most previously reported MoS_(2)-based materials.Theoretical calculations and results demonstrate that the synergistic effect of the doped P,which forms active centers in the basal plane of MoS_(2),and S vacancy defects caused by P doping intensifies the intrinsic electronic conductivity and electrocatalytic activity of the catalyst.Density functional theory calculations demonstrate that P optimizes the free energy of the MoS_(2)matrix for hydrogen adsorption,thereby considerably increasing the intrinsic activity of the doped catalyst for the HER compared with that observed from pristine MoS_(2).The enhanced catalytic activity of P-doped MoS_(2)for the OER is attributed to the ability of the doped P which facilitates the adsorption of hydroxyl and hydroperoxy intermediates and reduces the reaction energy barrier.This study provides a new environmentally friendly and convenient solid-phase ion exchange method to improve the electrocatalytic capability of two-dimensional transition-metal dichalcogenides in largescale applications.
