Thanks to its abundant reserves,relatively high energy density,and low reduction potential,potassium ion batteries(PIBs)have a high potential for large-scale energy storage applications.Due to the large radius of pota...Thanks to its abundant reserves,relatively high energy density,and low reduction potential,potassium ion batteries(PIBs)have a high potential for large-scale energy storage applications.Due to the large radius of potassium ions,most conventional anode materials undergo severe volume expansion,making it difficult to achieve stable and reversible energy storage.Therefore,developing high-performance anode materials is one of the critical factors in developing PIBs.In this sense,antimony(Sb)-based anode materials with high theoretical capacity and safe reaction potentials have a broad potential for application in PIBs.However,overcoming the rapid capacity decay induced by the large radius of potassium ions is still an issue that needs to be focused on.This paper reviews the latest research on different types of Sb-based anode materials and provides an in-depth analysis of their optimization strategies.We focus on material selection,structural design,and storage mechanisms to develop a detailed description of the material.In addition,the current challenges still faced by Sb-based anode materials are summarized,and some further optimization strategies have been added.We hope to provide some insights for researchers developing Sb-based anode materials for next-generation advanced PIBs.展开更多
Finding suitable strategies to effectively enhance the optical properties of materials are the goal being pursued by researchers.Herein,cation-anion synergetic interactions strategy was proposed to develop two novel o...Finding suitable strategies to effectively enhance the optical properties of materials are the goal being pursued by researchers.Herein,cation-anion synergetic interactions strategy was proposed to develop two novel organic-inorganic hybrid antimony-based optical materials,(C_(3)H_(5)N_(2))Sb F_(2)SO_(4)(I)and(C_(5)H_(6)N)Sb F_(2)SO_(4)(Ⅱ),which were obtained by introducing Sb^(3+)cation containing stereochemically active lone-pair(SCALP)and organicπ-conjugated cations into sulphate system.The synergistic interactions of the organicπ-conjugated cations,the inorganic[SbO_(2)F_(2)]^(3-)seesaw anions and the[SO_(4)]^(2-)distorted tetrahedra anions make their ultraviolet(UV)absorption edges approach 297 and 283 nm,respectively,and raise their birefringence up to 0.193@546 nm and 0.179@546 nm,respectively.Interestingly,although the two compounds have the same stoichiometric ratio and similar one-dimensional(1D)chain structure,they show opposite macroscopic symmetry,where the NCS compound(Ⅱ)exhibits a large secondharmonic generation(SHG)response(1.6 times that of KH_(2)PO_(4)).The two reported compounds are found to be promising UV optical materials in the experimental tests.展开更多
Chiral zero-dimensional(0D)hybrid metal halides,merging chirality with exceptional emission properties,are highly promising for circularly polarized luminescence(CPL).For CPL applications,it is difficult to simultaneo...Chiral zero-dimensional(0D)hybrid metal halides,merging chirality with exceptional emission properties,are highly promising for circularly polarized luminescence(CPL).For CPL applications,it is difficult to simultaneously achieve large dissymmetry factor(g_(lum))and photoluminescence quantum yield(PLQY).Herein,we propose a chemical design strategy to systematically control the g_(lum) and PLQY.We take achiral or chiral organic cations,to partially substitute the original A-site in A_(3)SbCl_(6)(A=(R/S)-morpholin-2-ylmethanol,R/S-MOR),to form ordered chiral-achiral halides(A)_(2)(B)SbCl_(6)(B=ethylammonium,isopropylammonium,2-chloroethylammonium,n-propylammonium,n-butylammonium),and ordered mixed chiral-chiral halides(A)_(2)(C)SbCl_(6)(C=(R/S)-1-amino-2-propanol),respectively.The introduction of different natures of cations not only systematically alters the PLQY(up to 86.0%)by increasing the Sb···Sb distances and[SbCl_(6)]^(3-)octahedral distortion,but also significantly amplifies the chirality with enhanced g_(lum).Among them,the mixed chiral-chiral material achieves the largest g_(lum) value(~9×10^(-3))with a high PLQY of 71.6%.The added dimension of a different chiral source reinforces the chirality and suppresses the inorganic octahedra vibration via hydrogen bonding interactions between the hydroxyl group and[SbCl_(6)]^(3-)octahedra.This work showcases an effective strategy to enhance the chiroptic properties and unlocks a large variety of new functional hybrid halides with ordered chiral/achiral cation combinations.展开更多
Low-dimensional hybrid halide perovskites represent a promising class of materials in optoelectronic applications because of strong broad self-trapped exciton(STE)emissions.However,there exists a limitation in designi...Low-dimensional hybrid halide perovskites represent a promising class of materials in optoelectronic applications because of strong broad self-trapped exciton(STE)emissions.However,there exists a limitation in designing the ideal A-site cation that makes the material satisfy the structure tolerance and exhibit STE emission raised by the appropriate electron–phonon coupling effect.To overcome this dilemma,we developed an inorganic metal-organic dimethyl sulfoxide(DMSO)coordinating strategy to synthesize a series of zero-dimensional(0D)Sb-based halide perovskites including Na_(3)SbBr_(6)·DMSO_(6)(1),AlSbBr_(6)·DMSO_(6)(2),AlSbCl_(6)·DMSO_(6)(3),GaSbCl_(6)·DMSO_(6)(4),Mn_(2)Sb_(2)Br10·DMSO_(13)(5)and MgSbBr_(5)·DMSO_(7)(6),in which the distinctive coordinating A-site cation[Am-DMSO_(6)]n+efficiently separate the[SbXz]polyhedrons.Advantageously,these materials all exhibit broadband-emissions with full widths at half maxima(FWHM)of 95–184 nm,and the highest photoluminescent quantum yield(PLQY)of 3 reaches 92%.Notably,compounds 2–4 are able to remain stable after storage of more than 120 d.First-principles calculations indicate that the origin of the efficient STE emission can be attribted to the localized distortion in[SbXz]polyhedron upon optical excitation.Experimental and calculational results demonstrate that the proposed coordinating strategy provides a way to efficiently expand the variety of novel high-performance STE emitters and continuously regulate their emission behaviors.展开更多
基金financially supported by the National Natural Science Foundation of China(No.22209057)the Guangzhou Basic and Applied Basic Research Foundation(No.2024A04J0839)。
文摘Thanks to its abundant reserves,relatively high energy density,and low reduction potential,potassium ion batteries(PIBs)have a high potential for large-scale energy storage applications.Due to the large radius of potassium ions,most conventional anode materials undergo severe volume expansion,making it difficult to achieve stable and reversible energy storage.Therefore,developing high-performance anode materials is one of the critical factors in developing PIBs.In this sense,antimony(Sb)-based anode materials with high theoretical capacity and safe reaction potentials have a broad potential for application in PIBs.However,overcoming the rapid capacity decay induced by the large radius of potassium ions is still an issue that needs to be focused on.This paper reviews the latest research on different types of Sb-based anode materials and provides an in-depth analysis of their optimization strategies.We focus on material selection,structural design,and storage mechanisms to develop a detailed description of the material.In addition,the current challenges still faced by Sb-based anode materials are summarized,and some further optimization strategies have been added.We hope to provide some insights for researchers developing Sb-based anode materials for next-generation advanced PIBs.
基金supported by the National Natural Science Foundation of China(Nos.22122106,22071158,21971171,22305166)the Fundamental Research Funds from Sichuan University(No.2021SCUNL101)the Natural Science Foundation of Sichuan Province(No.2023NSFC1066)。
文摘Finding suitable strategies to effectively enhance the optical properties of materials are the goal being pursued by researchers.Herein,cation-anion synergetic interactions strategy was proposed to develop two novel organic-inorganic hybrid antimony-based optical materials,(C_(3)H_(5)N_(2))Sb F_(2)SO_(4)(I)and(C_(5)H_(6)N)Sb F_(2)SO_(4)(Ⅱ),which were obtained by introducing Sb^(3+)cation containing stereochemically active lone-pair(SCALP)and organicπ-conjugated cations into sulphate system.The synergistic interactions of the organicπ-conjugated cations,the inorganic[SbO_(2)F_(2)]^(3-)seesaw anions and the[SO_(4)]^(2-)distorted tetrahedra anions make their ultraviolet(UV)absorption edges approach 297 and 283 nm,respectively,and raise their birefringence up to 0.193@546 nm and 0.179@546 nm,respectively.Interestingly,although the two compounds have the same stoichiometric ratio and similar one-dimensional(1D)chain structure,they show opposite macroscopic symmetry,where the NCS compound(Ⅱ)exhibits a large secondharmonic generation(SHG)response(1.6 times that of KH_(2)PO_(4)).The two reported compounds are found to be promising UV optical materials in the experimental tests.
基金supported by the Research and Development Fund of Inner Mongolia University(21300-5187174)the Program of Higher-Level Talents of Inner Mongolia University(10000-23112101/105)the National Natural Science Foundation of China(22275077,22461160285 and 22401161).
文摘Chiral zero-dimensional(0D)hybrid metal halides,merging chirality with exceptional emission properties,are highly promising for circularly polarized luminescence(CPL).For CPL applications,it is difficult to simultaneously achieve large dissymmetry factor(g_(lum))and photoluminescence quantum yield(PLQY).Herein,we propose a chemical design strategy to systematically control the g_(lum) and PLQY.We take achiral or chiral organic cations,to partially substitute the original A-site in A_(3)SbCl_(6)(A=(R/S)-morpholin-2-ylmethanol,R/S-MOR),to form ordered chiral-achiral halides(A)_(2)(B)SbCl_(6)(B=ethylammonium,isopropylammonium,2-chloroethylammonium,n-propylammonium,n-butylammonium),and ordered mixed chiral-chiral halides(A)_(2)(C)SbCl_(6)(C=(R/S)-1-amino-2-propanol),respectively.The introduction of different natures of cations not only systematically alters the PLQY(up to 86.0%)by increasing the Sb···Sb distances and[SbCl_(6)]^(3-)octahedral distortion,but also significantly amplifies the chirality with enhanced g_(lum).Among them,the mixed chiral-chiral material achieves the largest g_(lum) value(~9×10^(-3))with a high PLQY of 71.6%.The added dimension of a different chiral source reinforces the chirality and suppresses the inorganic octahedra vibration via hydrogen bonding interactions between the hydroxyl group and[SbCl_(6)]^(3-)octahedra.This work showcases an effective strategy to enhance the chiroptic properties and unlocks a large variety of new functional hybrid halides with ordered chiral/achiral cation combinations.
基金supported by the National Natural Science Foundation of China(Nos.21821004 and U21A2082).
文摘Low-dimensional hybrid halide perovskites represent a promising class of materials in optoelectronic applications because of strong broad self-trapped exciton(STE)emissions.However,there exists a limitation in designing the ideal A-site cation that makes the material satisfy the structure tolerance and exhibit STE emission raised by the appropriate electron–phonon coupling effect.To overcome this dilemma,we developed an inorganic metal-organic dimethyl sulfoxide(DMSO)coordinating strategy to synthesize a series of zero-dimensional(0D)Sb-based halide perovskites including Na_(3)SbBr_(6)·DMSO_(6)(1),AlSbBr_(6)·DMSO_(6)(2),AlSbCl_(6)·DMSO_(6)(3),GaSbCl_(6)·DMSO_(6)(4),Mn_(2)Sb_(2)Br10·DMSO_(13)(5)and MgSbBr_(5)·DMSO_(7)(6),in which the distinctive coordinating A-site cation[Am-DMSO_(6)]n+efficiently separate the[SbXz]polyhedrons.Advantageously,these materials all exhibit broadband-emissions with full widths at half maxima(FWHM)of 95–184 nm,and the highest photoluminescent quantum yield(PLQY)of 3 reaches 92%.Notably,compounds 2–4 are able to remain stable after storage of more than 120 d.First-principles calculations indicate that the origin of the efficient STE emission can be attribted to the localized distortion in[SbXz]polyhedron upon optical excitation.Experimental and calculational results demonstrate that the proposed coordinating strategy provides a way to efficiently expand the variety of novel high-performance STE emitters and continuously regulate their emission behaviors.
