Formaldehyde(FA),as an important chemical raw material,has been widely used in many fields.However,the discharge of a large amount of FA-containing wastewater poses a serious threat to the environment and human health...Formaldehyde(FA),as an important chemical raw material,has been widely used in many fields.However,the discharge of a large amount of FA-containing wastewater poses a serious threat to the environment and human health.Recently,the in-situ hydrogen energy release technology of hydrogen-containing stable liquid has been extensively explored due to its safe storage.Exploring a robust method to achieve FA removal and synchronous in-situ hydrogen release from FA containing wastewater is of great significant for environmental protection and energy crisis alleviation.Here,we have innovatively introduced peroxymonosulfate(PMS)activation technology into FA removal and hydrogen production simultaneously.The composite of nitrogen doped carbon coating Co_(9)S_(8)nanotubes(Co_(9)S_(8)@N-C)is employed as a proof of concept for FA decomposition and simultaneously hydrogen production based on PMS activation system.As expected,the Co_(9)S_(8)@N-C/PMS system presents much superior hydrogen production efficiency and satisfactory FA removal rate towards FA wastewater than those of common catalysis,photocatalysis and Fenton reaction in the basic condition in a wide range of FA concentration.The hydrogen yield reaches a value as high as 471μmol within 60 min,corresponding to a FA degradation rate of 30%with an initial FA concentration of 0.722 mol L^(-1).Characterizations and density functional theory(DFT)calculations suggest that the free radical process dominated by superoxide radical(O_(2)·^(-))and nonradical process dominated by singlet oxygen(^(1)O_(2)),which are induced by Co_(9)S_(8)@N-C/PMS system,are responsible for highly efficient hydrogen production via FA degradation.These generated O_(2)·^(-)and ^(1)O_(2)can extract·H from FA to form·OOH intermediate,which can further combine with the·H from water to produce hydrogen.This study provides an applicable technique for environmental purification and new energy development based on FA containing wastewater.展开更多
Effective design of nanoheterostructure anode with high ion/electron migration kinetics can give electrode with superior electrochemical performance.However,the design and preparation of nanoheterostructure composites...Effective design of nanoheterostructure anode with high ion/electron migration kinetics can give electrode with superior electrochemical performance.However,the design and preparation of nanoheterostructure composites with high-capacity and long cycling life in half and pouch full cells remain a big challenge.Here,a novel micro-pore MnS/Mn_(2)SnS_(4)heterostructure nanowire were in situ encapsulated into the N and S elements co-doped amorphous carbon tubes(abbreviated as(MnS/Mn_(2)SnS_(4))@N,S-ACTs)and showed superior energy storage properties in Na-/Li-ion half cells and pouch full cells.The Na-/Li-storage capabilities improvement are attribute to the strong synergistic effect between MnS/Mn_(2)SnS_(4)heterostructure and N,S-ACTs protective layer,the former induces an local built-in electric field between Mn_(2)Sn S_(4)and MnS during charging/discharging,accelerating interfacial ion/electron diffusion dynamics,the latter effective maintains the morphology and volume evolution during Na~+/Li~+charging/discharging,achieving a long-term cycling stability(e.g.,high discharge capacity of 79.2 mAh/g with the capacity retention of 79.3%can be gained after 2200 cycles at 3 C in(Mn S/Mn_(2)Sn S_(4))@N,S-ACTs//LiFePO_(4)pouch full cells;a high capacity of~34 mAh/g at 10 C can be got with a Coulombic efficiency of 100%after 1000 cycles in pouch(Mn S/Mn_(2)Sn S_(4))@N,S-ACTs//Na_(3)V_(2)(PO_(4))_(2)O_(2)F full cells.展开更多
本文设计制备了一种新型的氮掺杂碳包覆镍钴双金属磷化物中空核壳结构纳米立方体(Ni1.2Co0.8P@N-C)作为钠离子电池负极材料.该材料以镍钴类普鲁士蓝(PBA)纳米粒子为模板,先后经水热法、磷化法和高温碳化处理后合成.将其作为活性材料应...本文设计制备了一种新型的氮掺杂碳包覆镍钴双金属磷化物中空核壳结构纳米立方体(Ni1.2Co0.8P@N-C)作为钠离子电池负极材料.该材料以镍钴类普鲁士蓝(PBA)纳米粒子为模板,先后经水热法、磷化法和高温碳化处理后合成.将其作为活性材料应用在钠离子电池中,该材料展现出优异的循环稳定性,当以100 m A·g^-1的电流密度循环至200圈时,该材料的库仑效率保持在99.3%.进一步通过对不同电位下Ni1.2Co0.8P@N-C材料中的氮掺杂碳进行原位拉曼光谱测试,结果显示钠离子在氮掺杂的碳壳中的脱嵌行为具有较大程度的可逆性,研究结果对钠离子电池充放电过程的后续电化学研究提供了有价值的信息.展开更多
Rational design of hybrid carbon host with high electrical conductivity and strong adsorption toward soluble lithium polysulfides is the main challenge for achieving high-performance lithium-sulfur batteries(LSBs).Her...Rational design of hybrid carbon host with high electrical conductivity and strong adsorption toward soluble lithium polysulfides is the main challenge for achieving high-performance lithium-sulfur batteries(LSBs).Herein,novel binder-free Ni@N-doped carbon nanospheres(N-CNSs)films as sulfur host are firstly synthesized via a facile combined hydrothermal-atomic layer deposition method.The cross-linked multilayer N-CNSs films can effectively enhance the electrical conductivity of electrode and provide physical blocking“dams”toward the soluble long-chain polysulfides.Moreover,the doped N heteroatoms and superficial NiO layer on Ni layer can work synergistically to suppress the shuttle of lithium polysulfides by effective chemical interaction/adsorption.In virtue of the unique composite architecture and reinforced dual physical and chemical adsorption to the soluble polysulfides,the obtained Ni@N-CNSs/S electrode is demonstrated with enhanced rate performance(816 mAh g?1 at 2 C)and excellent long cycling life(87%after 200 cycles at 0.1 C),much better than N-CNSs/S electrode and other carbon/S counterparts.Our proposed design strategy offers a promising prospect for construction of advanced sulfur cathodes for applications in LSBs and other energy storage systems.展开更多
基金the National Natural Science Foundation of China(Nos.21975193 and 51602237)the Fundamental Research Funds for the Central Universities,China(WUT:2021Ⅲ034JC)。
文摘Formaldehyde(FA),as an important chemical raw material,has been widely used in many fields.However,the discharge of a large amount of FA-containing wastewater poses a serious threat to the environment and human health.Recently,the in-situ hydrogen energy release technology of hydrogen-containing stable liquid has been extensively explored due to its safe storage.Exploring a robust method to achieve FA removal and synchronous in-situ hydrogen release from FA containing wastewater is of great significant for environmental protection and energy crisis alleviation.Here,we have innovatively introduced peroxymonosulfate(PMS)activation technology into FA removal and hydrogen production simultaneously.The composite of nitrogen doped carbon coating Co_(9)S_(8)nanotubes(Co_(9)S_(8)@N-C)is employed as a proof of concept for FA decomposition and simultaneously hydrogen production based on PMS activation system.As expected,the Co_(9)S_(8)@N-C/PMS system presents much superior hydrogen production efficiency and satisfactory FA removal rate towards FA wastewater than those of common catalysis,photocatalysis and Fenton reaction in the basic condition in a wide range of FA concentration.The hydrogen yield reaches a value as high as 471μmol within 60 min,corresponding to a FA degradation rate of 30%with an initial FA concentration of 0.722 mol L^(-1).Characterizations and density functional theory(DFT)calculations suggest that the free radical process dominated by superoxide radical(O_(2)·^(-))and nonradical process dominated by singlet oxygen(^(1)O_(2)),which are induced by Co_(9)S_(8)@N-C/PMS system,are responsible for highly efficient hydrogen production via FA degradation.These generated O_(2)·^(-)and ^(1)O_(2)can extract·H from FA to form·OOH intermediate,which can further combine with the·H from water to produce hydrogen.This study provides an applicable technique for environmental purification and new energy development based on FA containing wastewater.
基金financial support from the project funded by National Natural Science Foundation of China(Nos.52372188,51902090)2023 Introduction of studying abroad talent program,Science Technology Program of Jilin Province(No.20220508141RC)+5 种基金the 111 Project(No.B13013)China Postdoctoral Science Foundation(No.2019M652546)Henan Province Postdoctoral Start-Up Foundation(No.1901017)Henan Normal University Doctoral Start-Up Project Foundation,“111”project(No.D17007)Henan Center for Outstanding Overseas Scientists(No.GZS2018003)the Dalian Revitalization Talents Program(No.2022RG01)。
文摘Effective design of nanoheterostructure anode with high ion/electron migration kinetics can give electrode with superior electrochemical performance.However,the design and preparation of nanoheterostructure composites with high-capacity and long cycling life in half and pouch full cells remain a big challenge.Here,a novel micro-pore MnS/Mn_(2)SnS_(4)heterostructure nanowire were in situ encapsulated into the N and S elements co-doped amorphous carbon tubes(abbreviated as(MnS/Mn_(2)SnS_(4))@N,S-ACTs)and showed superior energy storage properties in Na-/Li-ion half cells and pouch full cells.The Na-/Li-storage capabilities improvement are attribute to the strong synergistic effect between MnS/Mn_(2)SnS_(4)heterostructure and N,S-ACTs protective layer,the former induces an local built-in electric field between Mn_(2)Sn S_(4)and MnS during charging/discharging,accelerating interfacial ion/electron diffusion dynamics,the latter effective maintains the morphology and volume evolution during Na~+/Li~+charging/discharging,achieving a long-term cycling stability(e.g.,high discharge capacity of 79.2 mAh/g with the capacity retention of 79.3%can be gained after 2200 cycles at 3 C in(Mn S/Mn_(2)Sn S_(4))@N,S-ACTs//LiFePO_(4)pouch full cells;a high capacity of~34 mAh/g at 10 C can be got with a Coulombic efficiency of 100%after 1000 cycles in pouch(Mn S/Mn_(2)Sn S_(4))@N,S-ACTs//Na_(3)V_(2)(PO_(4))_(2)O_(2)F full cells.
文摘本文设计制备了一种新型的氮掺杂碳包覆镍钴双金属磷化物中空核壳结构纳米立方体(Ni1.2Co0.8P@N-C)作为钠离子电池负极材料.该材料以镍钴类普鲁士蓝(PBA)纳米粒子为模板,先后经水热法、磷化法和高温碳化处理后合成.将其作为活性材料应用在钠离子电池中,该材料展现出优异的循环稳定性,当以100 m A·g^-1的电流密度循环至200圈时,该材料的库仑效率保持在99.3%.进一步通过对不同电位下Ni1.2Co0.8P@N-C材料中的氮掺杂碳进行原位拉曼光谱测试,结果显示钠离子在氮掺杂的碳壳中的脱嵌行为具有较大程度的可逆性,研究结果对钠离子电池充放电过程的后续电化学研究提供了有价值的信息.
基金supported by National Natural Science Foundation of China(Nos.51772272 and 51728204)Fundamental Research Funds for the Central Universities(No.2018QNA4011)+3 种基金Science and Technology Program of Guangdong Province of China(No.2016A010104020)Pearl River S&T Nova Program of Guangzhou(No.201610010116)Qianjiang Talents Plan D(QJD1602029)Startup Foundation for Hundred-Talent Program of Zhejiang University.
文摘Rational design of hybrid carbon host with high electrical conductivity and strong adsorption toward soluble lithium polysulfides is the main challenge for achieving high-performance lithium-sulfur batteries(LSBs).Herein,novel binder-free Ni@N-doped carbon nanospheres(N-CNSs)films as sulfur host are firstly synthesized via a facile combined hydrothermal-atomic layer deposition method.The cross-linked multilayer N-CNSs films can effectively enhance the electrical conductivity of electrode and provide physical blocking“dams”toward the soluble long-chain polysulfides.Moreover,the doped N heteroatoms and superficial NiO layer on Ni layer can work synergistically to suppress the shuttle of lithium polysulfides by effective chemical interaction/adsorption.In virtue of the unique composite architecture and reinforced dual physical and chemical adsorption to the soluble polysulfides,the obtained Ni@N-CNSs/S electrode is demonstrated with enhanced rate performance(816 mAh g?1 at 2 C)and excellent long cycling life(87%after 200 cycles at 0.1 C),much better than N-CNSs/S electrode and other carbon/S counterparts.Our proposed design strategy offers a promising prospect for construction of advanced sulfur cathodes for applications in LSBs and other energy storage systems.
