The unstable zinc(Zn)/electrolyte interfaces formed by undesired dendrites and parasitic side reactions greatly hinder the development of aqueous zinc ion batteries.Herein,the hydroxy-rich sorbitol was used as an addi...The unstable zinc(Zn)/electrolyte interfaces formed by undesired dendrites and parasitic side reactions greatly hinder the development of aqueous zinc ion batteries.Herein,the hydroxy-rich sorbitol was used as an additive to reshape the solvation structure and modulate the interface chemistry.The strong interactions among sorbitol and both water molecules and Zn electrode can reduce the free water activity,optimize the solvation shell of water and Zn^(2+)ions,and regulate the formation of local water(H_(2)O)-poor environment on the surface of Zn electrode,which effectively inhibit the decomposition of water molecules,and thus,achieve the thermodynamically stable and highly reversible Zn electrochemistry.As a result,the assembled Zn/Zn symmetric cells with the sorbitol additive realized an excellent cycling life of 2000 h at 1 mA·cm^(-2)and 1 mAh·cm^(-2),and over 250 h at 5 mA.cm^(-2)and 5 mAh.cm^(-2).Moreover,the Zn/Cu asymmetric cells with the sorbitol additive achieved a high Coulombic efficiency of 99.6%,obtaining a better performance than that with a pure 2 mol-L^(-1)ZnSO_(4)electrolyte.And the constructed Zn/poly1,5-naphthalenediamine(PNDA)batteries could be stably discharged for 2300 cycles at 1 A g^(-1)with an excellent capacity retention rate.This result indicates that the addition of 1 mol-L^(-1)non-toxic sorbitol into a conventional ZnSO_(4)electrolyte can successfully protect the Zn anode interface by improving the electrochemical properties of Zn reversible deposition/decomposition,which greatly promotes its cycle performance,providing a new approach in future development of high performance aqueous Zn ion batteries.展开更多
Zinc-ion capacitors(ZICs),which consist of a capacitor-type electrode and a battery-type electrode,not only possess the high power density of supercapacitors and the high energy density of batteries,but also have othe...Zinc-ion capacitors(ZICs),which consist of a capacitor-type electrode and a battery-type electrode,not only possess the high power density of supercapacitors and the high energy density of batteries,but also have other advantages such as abundant resources,high safety and environmental friendliness.However,they still face problems such as insufficient specific capacitance,a short cycling life,and narrow operating voltage and temperature ranges,which are hindering their practical use.We provide a comprehensive overview of the fundamental theory of carbon-based ZICs and summarize recent research progress from three perspectives:the carbon cathode,electrolyte and zinc anode.The influence of the structure and surface chemical properties of the carbon materials on the capacitive performance of ZICs is considered together with theoretical guidance for advancing their development and practical use.展开更多
Rechargeable lithium-oxygen(Li-O_(2))batteries have attracted wide attention due to their high energy density.However,the sluggish cathode kinetics results in high overvoltage and poor cycling performance.Ruthenium(Ru...Rechargeable lithium-oxygen(Li-O_(2))batteries have attracted wide attention due to their high energy density.However,the sluggish cathode kinetics results in high overvoltage and poor cycling performance.Ruthenium(Ru)-based electrocatalysts have been demonstrated to be promising cathode catalysts to promote oxygen evolution reaction(OER).It facilitates decomposition of lithium peroxide(Li_(2)O_(2))by adjusting Li_(2)O_(2) morphologies,which is due to the strong interaction between Ru-based catalyst and superoxide anion(O_(2))intermediate.In this review,the design strategies of Ru-based electrocatalysts are introduced to enhance their OER catalytic kinetics in Li-O_(2) batteries.Different configurations of Ru-based catalysts,including metal particles(Ru metal and alloys),single-atom catalysts,and Ru-loaded compounds with various substrates(carbon materials,metal oxides/sulfides),have been summarized to regulate the electronic structure and the matrix architecture of the Ru-based electrocatalysts.The structure-property relationship of Ru-based catalysts is discussed for a better understanding of the Li_(2)O_(2) decomposition mechanism at the cathode interface.Finally,the challenges of Ru-based electrocatalysts are proposed for the future development of Li-O_(2) batteries.展开更多
Research on two-dimensional(2D) materials has been explosively increasing in last seventeen years in varying subjects including condensed matter physics, electronic engineering, materials science, and chemistry since ...Research on two-dimensional(2D) materials has been explosively increasing in last seventeen years in varying subjects including condensed matter physics, electronic engineering, materials science, and chemistry since the mechanical exfoliation of graphene in 2004. Starting from graphene, 2D materials now have become a big family with numerous members and diverse categories. The unique structural features and physicochemical properties of 2D materials make them one class of the most appealing candidates for a wide range of potential applications. In particular, we have seen some major breakthroughs made in the field of 2D materials in last five years not only in developing novel synthetic methods and exploring new structures/properties but also in identifying innovative applications and pushing forward commercialisation. In this review, we provide a critical summary on the recent progress made in the field of 2D materials with a particular focus on last five years. After a brief backgroundintroduction, we first discuss the major synthetic methods for 2D materials, including the mechanical exfoliation, liquid exfoliation, vapor phase deposition, and wet-chemical synthesis as well as phase engineering of 2D materials belonging to the field of phase engineering of nanomaterials(PEN). We then introduce the superconducting/optical/magnetic properties and chirality of 2D materials along with newly emerging magic angle 2D superlattices. Following that, the promising applications of 2D materials in electronics, optoelectronics, catalysis, energy storage, solar cells, biomedicine, sensors, environments, etc. are described sequentially. Thereafter, we present the theoretic calculations and simulations of 2D materials. Finally, after concluding the current progress, we provide some personal discussions on the existing challenges and future outlooks in this rapidly developing field.展开更多
Development of robust electrocatalyst for oxygen reduction reaction(ORR)in a seawater electrolyte is the key to realize seawater electrolyte-based zinc-air batteries(SZABs).Herein,constructing a local electric field c...Development of robust electrocatalyst for oxygen reduction reaction(ORR)in a seawater electrolyte is the key to realize seawater electrolyte-based zinc-air batteries(SZABs).Herein,constructing a local electric field coupled with chloride ions(Cl-)fixation strategy in dual single-atom catalysts(DSACs)was proposed,and the resultant catalyst delivered considerable ORR performance in a seawater electrolyte,with a high half-wave potential(E_(1/2))of 0.868 V and a good maximum power density(Pmax)of 182 mW·cm^(−2)in the assembled SZABs,much higher than those of the Pt/C catalyst(E_(1/2):0.846 V;Pmax:150 mW·cm^(−2)).The in-situ characterization and theoretical calculations revealed that the Fe sites have a higher Cl^(−)adsorption affinity than the Co sites,and preferentially adsorbs Cl^(−)in a seawater electrolyte during the ORR process,and thus constructs a low-concentration Cl^(−)local microenvironment through the common-ion exclusion effect,which prevents Cl^(−)adsorption and corrosion in the Co active centers,achieving impressive catalytic stability.In addition,the directional charge movement between Fe and Co atomic pairs establishes a local electric field,optimizing the adsorption energy of Co sites for oxygen-containing intermediates,and further improving the ORR activity.展开更多
基金supported by the National Natural Science Foundation of China(22279063,52001170)Tianjin Natural Science Foundation(22JCYBJC00590)the Fundamental Research Funds for the Central Universities.We thank the Haihe Laboratoryof Sustainable Chemical Transformations for financial support.
文摘The unstable zinc(Zn)/electrolyte interfaces formed by undesired dendrites and parasitic side reactions greatly hinder the development of aqueous zinc ion batteries.Herein,the hydroxy-rich sorbitol was used as an additive to reshape the solvation structure and modulate the interface chemistry.The strong interactions among sorbitol and both water molecules and Zn electrode can reduce the free water activity,optimize the solvation shell of water and Zn^(2+)ions,and regulate the formation of local water(H_(2)O)-poor environment on the surface of Zn electrode,which effectively inhibit the decomposition of water molecules,and thus,achieve the thermodynamically stable and highly reversible Zn electrochemistry.As a result,the assembled Zn/Zn symmetric cells with the sorbitol additive realized an excellent cycling life of 2000 h at 1 mA·cm^(-2)and 1 mAh·cm^(-2),and over 250 h at 5 mA.cm^(-2)and 5 mAh.cm^(-2).Moreover,the Zn/Cu asymmetric cells with the sorbitol additive achieved a high Coulombic efficiency of 99.6%,obtaining a better performance than that with a pure 2 mol-L^(-1)ZnSO_(4)electrolyte.And the constructed Zn/poly1,5-naphthalenediamine(PNDA)batteries could be stably discharged for 2300 cycles at 1 A g^(-1)with an excellent capacity retention rate.This result indicates that the addition of 1 mol-L^(-1)non-toxic sorbitol into a conventional ZnSO_(4)electrolyte can successfully protect the Zn anode interface by improving the electrochemical properties of Zn reversible deposition/decomposition,which greatly promotes its cycle performance,providing a new approach in future development of high performance aqueous Zn ion batteries.
文摘Zinc-ion capacitors(ZICs),which consist of a capacitor-type electrode and a battery-type electrode,not only possess the high power density of supercapacitors and the high energy density of batteries,but also have other advantages such as abundant resources,high safety and environmental friendliness.However,they still face problems such as insufficient specific capacitance,a short cycling life,and narrow operating voltage and temperature ranges,which are hindering their practical use.We provide a comprehensive overview of the fundamental theory of carbon-based ZICs and summarize recent research progress from three perspectives:the carbon cathode,electrolyte and zinc anode.The influence of the structure and surface chemical properties of the carbon materials on the capacitive performance of ZICs is considered together with theoretical guidance for advancing their development and practical use.
基金the National Natural Science Foundation of China(22325902 and 51671107)Haihe Laboratory of Sustainable Chemical Transformations.
文摘Rechargeable lithium-oxygen(Li-O_(2))batteries have attracted wide attention due to their high energy density.However,the sluggish cathode kinetics results in high overvoltage and poor cycling performance.Ruthenium(Ru)-based electrocatalysts have been demonstrated to be promising cathode catalysts to promote oxygen evolution reaction(OER).It facilitates decomposition of lithium peroxide(Li_(2)O_(2))by adjusting Li_(2)O_(2) morphologies,which is due to the strong interaction between Ru-based catalyst and superoxide anion(O_(2))intermediate.In this review,the design strategies of Ru-based electrocatalysts are introduced to enhance their OER catalytic kinetics in Li-O_(2) batteries.Different configurations of Ru-based catalysts,including metal particles(Ru metal and alloys),single-atom catalysts,and Ru-loaded compounds with various substrates(carbon materials,metal oxides/sulfides),have been summarized to regulate the electronic structure and the matrix architecture of the Ru-based electrocatalysts.The structure-property relationship of Ru-based catalysts is discussed for a better understanding of the Li_(2)O_(2) decomposition mechanism at the cathode interface.Finally,the challenges of Ru-based electrocatalysts are proposed for the future development of Li-O_(2) batteries.
文摘Research on two-dimensional(2D) materials has been explosively increasing in last seventeen years in varying subjects including condensed matter physics, electronic engineering, materials science, and chemistry since the mechanical exfoliation of graphene in 2004. Starting from graphene, 2D materials now have become a big family with numerous members and diverse categories. The unique structural features and physicochemical properties of 2D materials make them one class of the most appealing candidates for a wide range of potential applications. In particular, we have seen some major breakthroughs made in the field of 2D materials in last five years not only in developing novel synthetic methods and exploring new structures/properties but also in identifying innovative applications and pushing forward commercialisation. In this review, we provide a critical summary on the recent progress made in the field of 2D materials with a particular focus on last five years. After a brief backgroundintroduction, we first discuss the major synthetic methods for 2D materials, including the mechanical exfoliation, liquid exfoliation, vapor phase deposition, and wet-chemical synthesis as well as phase engineering of 2D materials belonging to the field of phase engineering of nanomaterials(PEN). We then introduce the superconducting/optical/magnetic properties and chirality of 2D materials along with newly emerging magic angle 2D superlattices. Following that, the promising applications of 2D materials in electronics, optoelectronics, catalysis, energy storage, solar cells, biomedicine, sensors, environments, etc. are described sequentially. Thereafter, we present the theoretic calculations and simulations of 2D materials. Finally, after concluding the current progress, we provide some personal discussions on the existing challenges and future outlooks in this rapidly developing field.
基金supported by the National Natural Science Foundation of China(52164028,52274297)the Start-up Research Foundation of Hainan University(KYQD(ZR)20008,KYQD(ZR)21125,KYQD(ZR)23169))+1 种基金Collaborative Innovation Center of Marine Science and Technology of Hainan University(XTCX2022HYC14)Innovative Research Project for Postgraduate Students in Hainan Province(Qhyb2024-95).
文摘Development of robust electrocatalyst for oxygen reduction reaction(ORR)in a seawater electrolyte is the key to realize seawater electrolyte-based zinc-air batteries(SZABs).Herein,constructing a local electric field coupled with chloride ions(Cl-)fixation strategy in dual single-atom catalysts(DSACs)was proposed,and the resultant catalyst delivered considerable ORR performance in a seawater electrolyte,with a high half-wave potential(E_(1/2))of 0.868 V and a good maximum power density(Pmax)of 182 mW·cm^(−2)in the assembled SZABs,much higher than those of the Pt/C catalyst(E_(1/2):0.846 V;Pmax:150 mW·cm^(−2)).The in-situ characterization and theoretical calculations revealed that the Fe sites have a higher Cl^(−)adsorption affinity than the Co sites,and preferentially adsorbs Cl^(−)in a seawater electrolyte during the ORR process,and thus constructs a low-concentration Cl^(−)local microenvironment through the common-ion exclusion effect,which prevents Cl^(−)adsorption and corrosion in the Co active centers,achieving impressive catalytic stability.In addition,the directional charge movement between Fe and Co atomic pairs establishes a local electric field,optimizing the adsorption energy of Co sites for oxygen-containing intermediates,and further improving the ORR activity.
