Multivalent-ion(such as Zn^(2+),Mg^(2+),Al^(3+))batteries are considered as a prospective alternative for large-scale energy storage.However,the main problem of cathode materials for multivalent-ion batteries is the s...Multivalent-ion(such as Zn^(2+),Mg^(2+),Al^(3+))batteries are considered as a prospective alternative for large-scale energy storage.However,the main problem of cathode materials for multivalent-ion batteries is the sluggish diffusion of multivalent ions.Many cathode materials will self-adjust under electrochemical conditions to achieve the optimal state for multivalent-ion storage.In this review,the significant role of electrochemical in situ structural reconstruction of cathode materials is suggested.The types,basic characteristics,and formation mechanisms of reconstructed phases have been systematically discussed and commented.The most important insight we pointed out is that the cathode materials with loose structures after in situ electrochemical activation are conducive to the reversible diffusion of multivalent ions.Moreover,several crucial issues of electrochemical activation and reconstruction were further analyzed and discussed.The challenges and future perspectives are presented in the final section.展开更多
Facilitating sulfur reduction reaction(SRR)is a promising pathway to tackle the polysulfide shuttle effect and enhance the electrochemical performance of lithium-sulfur(Li-S)batteries.Catalysts with a solo active site...Facilitating sulfur reduction reaction(SRR)is a promising pathway to tackle the polysulfide shuttle effect and enhance the electrochemical performance of lithium-sulfur(Li-S)batteries.Catalysts with a solo active site can reduce a reaction barrier of a certain transition-intermediate,but the linear scaling relationship between multi-intermediates still obstructs overall SRR.Herein,we construct tandem Co–O dual sites with accelerating SRR kinetics by loading highly dispersed cobalt sulfide clusters on halloysite.This catalyst features Co with upshifted d-orbital and O with downshifted p-orbital,which cooperatively adsorb long-chain polysulfide and dissociate an S–S bond,thus achieving both optimal adsorption–desorption strength and reduced conversion energy barrier of multi-intermediates in SRR.The Li-S coin batteries using the electrocatalyst endows a high specific capacity of 1224.3 m Ah g^(-1)at 0.2 C after 200cycles,and enhances cycling stability with a low-capacity decay rate of 0.03%per cycle at 1 C after1000 cycles.Moreover,the strategy of the tandem Co–O dual sites is further verified in a practical Li-S pouch battery that realizes 1014.1 m Ah g^(-1)for 100 cycles,which opens up a novel avenue for designing electrocatalysts to accelerate multi-step reactions.展开更多
Sodium metal has shown great potential as an inexpensive anode for rechargeable batteries. However, the growth of sodium dendrites continues to hinder the commercialization of Na metal batteries. Herein, an effective ...Sodium metal has shown great potential as an inexpensive anode for rechargeable batteries. However, the growth of sodium dendrites continues to hinder the commercialization of Na metal batteries. Herein, an effective strategy using anion-anchoring halloysite nanotube(HNT) coating was proven to prevent the diffusion of anions and trigger uniform Na deposition. Through theoretical calculation, a model of active site of fixed anions exposed from HNTs after acid activation was established for the first time, revealing that Si–Al sites are effective active site of acid-activated HNTs. Furthermore, HNTs with strong and effective adsorption capacity for anions were obtained by controlling the structure of HNTs to regulate the exposure of Si–Al sites. The strong interaction between sites of acid-activated HNTs and the SO_(3)CF_(3)^(-) anion effectively promotes the dissociation of sodium salts, the release of Na^(+) and subsequent migration. As a result, HNTs acid activation for 4 h shows a steady sodium deposition process and displays high Coulombic efficiency in half cell, long cycle life in symmetric cell and full cell. This work provides a basic theoretical basis for the design of nanoclay with abundant and effective active site to fix anions for dendritic free metal batteries.展开更多
An innovative cancer therapy strategy regarding the interface engineering of kaolinite has been designed. The exposed silanol group facilitates more guest species with high dispersion on the supports. Mn_3O_4 magnetic...An innovative cancer therapy strategy regarding the interface engineering of kaolinite has been designed. The exposed silanol group facilitates more guest species with high dispersion on the supports. Mn_3O_4 magnetic nanoparticles are uniformly distributed on external surfaces of the Kaolin_(C12N)with the Al–O–Mn bond for the detection of the tumor microenvironment by T1-MRI; Doxorubicin(DOX) are loaded in the interlayer space with the electrostatic interaction for chemo-treating; and KI is coated on the outer layer of the nanocomposites based on the electrostatic interaction for thyroid cancer targeting. The synergetic effects and the treatment mechanism enhanced by the interface engineering, KI@DOX-Mn_3O_4-Kaolin_(C12N)can cause remarkably low cell viability(57%, 200 μg/mL), tumor shrinking(75%, 20 μg/kg), and accumulation into the tumor tissues. The novel kaolinite based drug delivery system is expected to incorporate imaging diagnosis, targeted therapy and drug delivery into one single system for postoperative residual thyroid cancer treatment and observation for metastasis of focal area.展开更多
基金This work was supported by the National Natural Science Foundation of China (Grant no.51774330,52072411,51932011)the Natural Science Foundation of Hunan Province (Grant no.2021JJ20060)The science and technology innovation Program of Hunan Province (Grant no.2021RC3001).
文摘Multivalent-ion(such as Zn^(2+),Mg^(2+),Al^(3+))batteries are considered as a prospective alternative for large-scale energy storage.However,the main problem of cathode materials for multivalent-ion batteries is the sluggish diffusion of multivalent ions.Many cathode materials will self-adjust under electrochemical conditions to achieve the optimal state for multivalent-ion storage.In this review,the significant role of electrochemical in situ structural reconstruction of cathode materials is suggested.The types,basic characteristics,and formation mechanisms of reconstructed phases have been systematically discussed and commented.The most important insight we pointed out is that the cathode materials with loose structures after in situ electrochemical activation are conducive to the reversible diffusion of multivalent ions.Moreover,several crucial issues of electrochemical activation and reconstruction were further analyzed and discussed.The challenges and future perspectives are presented in the final section.
基金supported by the National Science Fund for Distinguished Young Scholars(51225403)the National Natural Science Foundation of China(52042403)+3 种基金the National Postdoctoral Program for Innovative Talents(BX2021276)the China Postdoctoral Science Foundation(2020M682519)the Strategic Priority Research Program of Central South University(ZLXD2017005)the“CUG Scholar"Scientific Research Funds at China University of Geosciences(Wuhan)(Project No.20222020110)。
文摘Facilitating sulfur reduction reaction(SRR)is a promising pathway to tackle the polysulfide shuttle effect and enhance the electrochemical performance of lithium-sulfur(Li-S)batteries.Catalysts with a solo active site can reduce a reaction barrier of a certain transition-intermediate,but the linear scaling relationship between multi-intermediates still obstructs overall SRR.Herein,we construct tandem Co–O dual sites with accelerating SRR kinetics by loading highly dispersed cobalt sulfide clusters on halloysite.This catalyst features Co with upshifted d-orbital and O with downshifted p-orbital,which cooperatively adsorb long-chain polysulfide and dissociate an S–S bond,thus achieving both optimal adsorption–desorption strength and reduced conversion energy barrier of multi-intermediates in SRR.The Li-S coin batteries using the electrocatalyst endows a high specific capacity of 1224.3 m Ah g^(-1)at 0.2 C after 200cycles,and enhances cycling stability with a low-capacity decay rate of 0.03%per cycle at 1 C after1000 cycles.Moreover,the strategy of the tandem Co–O dual sites is further verified in a practical Li-S pouch battery that realizes 1014.1 m Ah g^(-1)for 100 cycles,which opens up a novel avenue for designing electrocatalysts to accelerate multi-step reactions.
基金Projects(51774330, 52072411) supported by the National Natural Science Foundation of ChinaProject(2015) supported by the Teacher Research Foundation of Central South University,China+2 种基金Project(2022ZZTS0422) supported by the Fundamental Research Funds for the Central Universities,ChinaProject(2021JJ20060) supported by the Natural Science Foundation of Hunan Province,ChinaProject(2021RC3001) supported by the Science and Technology Innovation Program of Hunan Province,China。
基金supported by the National Key R&D Program of China (2022YFE0201300)the China Postdoctoral Science Foundation (2022M712948)+2 种基金the CUG Scholar Scientific Research Funds at China University of Geosciences (Wuhan) (2019152)the Fundamental Research Funds for the Central Universities at China University of Geosciences (Wuhan)the National Science Fund for Distinguished Young Scholars (51225403)。
文摘Sodium metal has shown great potential as an inexpensive anode for rechargeable batteries. However, the growth of sodium dendrites continues to hinder the commercialization of Na metal batteries. Herein, an effective strategy using anion-anchoring halloysite nanotube(HNT) coating was proven to prevent the diffusion of anions and trigger uniform Na deposition. Through theoretical calculation, a model of active site of fixed anions exposed from HNTs after acid activation was established for the first time, revealing that Si–Al sites are effective active site of acid-activated HNTs. Furthermore, HNTs with strong and effective adsorption capacity for anions were obtained by controlling the structure of HNTs to regulate the exposure of Si–Al sites. The strong interaction between sites of acid-activated HNTs and the SO_(3)CF_(3)^(-) anion effectively promotes the dissociation of sodium salts, the release of Na^(+) and subsequent migration. As a result, HNTs acid activation for 4 h shows a steady sodium deposition process and displays high Coulombic efficiency in half cell, long cycle life in symmetric cell and full cell. This work provides a basic theoretical basis for the design of nanoclay with abundant and effective active site to fix anions for dendritic free metal batteries.
基金This work was supported by the National Natural Science Foundation of China （Nos. 51225403 and 41572036）, the Hunan Provincial Science and Technology Project （Nos. 2016RS2004 and 2015TP1006）, the Postdoctoral Science Foundation of Central South University （No. 155219） and the China Postdoctoral Science Foundation （No. 2015M582346）.
基金supported by the National Natural Science Foundation of China(21878341,51804343,41572036,51225403)the Strategic Priority Research Program of Central South University(ZLXD2017005)+2 种基金the Natural Science Foundation of Hunan Province(2018JJ3670)the Key R&D Program of Hunan Province(2017GK2251)Hunan Provincial Science and Technology Project(2016RS2004,2015TP1006)
文摘An innovative cancer therapy strategy regarding the interface engineering of kaolinite has been designed. The exposed silanol group facilitates more guest species with high dispersion on the supports. Mn_3O_4 magnetic nanoparticles are uniformly distributed on external surfaces of the Kaolin_(C12N)with the Al–O–Mn bond for the detection of the tumor microenvironment by T1-MRI; Doxorubicin(DOX) are loaded in the interlayer space with the electrostatic interaction for chemo-treating; and KI is coated on the outer layer of the nanocomposites based on the electrostatic interaction for thyroid cancer targeting. The synergetic effects and the treatment mechanism enhanced by the interface engineering, KI@DOX-Mn_3O_4-Kaolin_(C12N)can cause remarkably low cell viability(57%, 200 μg/mL), tumor shrinking(75%, 20 μg/kg), and accumulation into the tumor tissues. The novel kaolinite based drug delivery system is expected to incorporate imaging diagnosis, targeted therapy and drug delivery into one single system for postoperative residual thyroid cancer treatment and observation for metastasis of focal area.
