Magnesium hydride has attracted great attention because of its high theoretical capacity and outstanding reversibility, nevertheless, its practical applications have been restricted by the disadvantages of the sluggis...Magnesium hydride has attracted great attention because of its high theoretical capacity and outstanding reversibility, nevertheless, its practical applications have been restricted by the disadvantages of the sluggish kinetics and high thermodynamic stability. In this work, an unexpected high reversible hydrogen capacity over 8.0 wt% has been achieved from MgH2 metal hydride composited with small amounts of LiBH4 and Li3AlH6 complex hydrides, which begins to release hydrogen at 276 ℃ and then completely dehydrogenates at 360 ℃. The dehydrogenated MgH2+LiBH4/Li3AlH6 composite can fully reabsorb hydrogen below 300 ℃ with an excellent cycling stability. The composite exhibits a significant reduction of dehydrogenation activation energy from 279.7 kJ/mol(primitive MgH2) to 139.3 kJ/mol(MgH2+LiBH4/Li3AlH6),as well as a remarkable reduction of dehydrogenation enthalpy change from 75.1 k J/mol H2(primitive MgH2) to 62.8 kJ/mol H2(MgH2+LiBH4/Li3AlH6). The additives of LiBH4 and Li3AlH6 not only enhance the cycling hydrogen capacity, but also simultaneously improve the reversible de/rehydrogenation kinetics, as well as the dehydrogenation thermodynamics. This notable improvement on the hydrogen absorption/desorption behaviors of the MgH2+LiBH4/Li3AlH6 composite could be attributed to the dehydrogenated products including Li3Mg7, Mg17Al12 and MgAlB4, which play a key role on reducing the dehydrogenation activation energy and increasing diffusion rate of hydrogen. Meanwhile, the LiBH4 and Li3AlH6 effectively destabilize MgH2 with a remarkable reduction on dehydrogenation enthalpy change in terms of thermodynamics. In particular, the Li3Mg7, Mg17Al12 and MgAlB4 phases can reversibly transform into MgH2, Li3AlH6 and LiBH4 after rehydrogenation, which contribute to maintain a high cycling capacity.This constructing strategy can further promote the development of high reversible capacity Mg-based materials with suitable de/rehydrogenation properties.展开更多
MgH_(2),as one of the typical solid-state hydrogen storage materials,has attracted extensive attention.However,the slow kinetics and poor cycle stability limit its application.In this work,LiBH_(4) and YNi_(5) alloy w...MgH_(2),as one of the typical solid-state hydrogen storage materials,has attracted extensive attention.However,the slow kinetics and poor cycle stability limit its application.In this work,LiBH_(4) and YNi_(5) alloy were co-added as additives to MgH_(2) via ball milling,thereby realizing an excellent dehydrogenation per-formance and good cycle stability at 300 ℃.The MgH_(2)-0.04LiBH_(4)-0.01YNi_(5) composite can release 7 wt.%of hydrogen in around 10 min at 300 ℃ and still have a reversible hydrogen storage capacity of 6.42 wt.%after 110 cycles,with a capacity retention rate as high as 90.3%based on the second dehydrogenation capacity.The FTIR results show that LiBH_(4) can reversibly absorb and desorb hydrogen throughout the hydrogen ab/desorption process,which contributes a portion of the reversible hydrogen storage capacity to the MgH_(2)-0.04LiBH_(4)-0.01YNi_(5) composite.Due to the small amount of LiBH_(4) and YNi_(5),the dehydro-genation activation energy of MgH_(2) did not decrease significantly,nor did the dehydrogenation enthalpy(△H)change.However,the MgNi3B2 and in-situ formed YH3 during the hydrogen absorption/desorption cycles is not only beneficial to the improvement of the kinetics performance for MgH_(2) but also improves its cycle stability.This work provides a straightforward method for developing high reversible hydrogen capacity on Mg-based hydrogen storage materials with moderate kinetic performance.展开更多
Biomass-derived carbon materials for lithiumion batteries emerge as one of the most promising anodes from sustainable perspective.However,improving the reversible capacity and cycling performance remains a long-standi...Biomass-derived carbon materials for lithiumion batteries emerge as one of the most promising anodes from sustainable perspective.However,improving the reversible capacity and cycling performance remains a long-standing challenge.By combining the benefits of K2CO_(3) activation and KMnO_(4) hydrothermal treatment,this work proposes a two-step activation method to load MnO_(2) charge transfer onto biomass-derived carbon(KAC@MnO_(2)).Comprehensive analysis reveals that KAC@MnO_(2) has a micro-mesoporous coexistence structure and uniform surface distribution of MnO_(2),thus providing an improved electrochemical performance.Specifically,KAC@MnO_(2) exhibits an initial chargedischarge capacity of 847.3/1813.2 mAh·g^(-1) at 0.2 A·g^(-1),which is significantly higher than that of direct pyrolysis carbon and K2CO_(3) activated carbon,respectively.Furthermore,the KAC@MnO_(2) maintains a reversible capacity of 652.6 mAh·g^(-1) after 100 cycles.Even at a high current density of 1.0 A·g^(-1),KAC@MnO_(2) still exhibits excellent long-term cycling stability and maintains a stable reversible capacity of 306.7 mAh·g^(-1) after 500 cycles.Compared with reported biochar anode materials,the KAC@MnO_(2) prepared in this work shows superior reversible capacity and cycling performance.Additionally,the Li+insertion and de-insertion mechanisms are verified by ex situ X-ray diffraction analysis during the chargedischarge process,helping us better understand the energy storage mechanism of KAC@MnO_(2).展开更多
On account of the high theoretical capacity, high corrosion resistance, environmental benignity, abundant availability and low cost, the research on a-Fe_2O_3 has been gradually fastened on as promising anodes materia...On account of the high theoretical capacity, high corrosion resistance, environmental benignity, abundant availability and low cost, the research on a-Fe_2O_3 has been gradually fastened on as promising anodes materials toward lithium-ion batteries(LIBs). A high-performance anode for LIBs based on α-Fe_2O_3 nanoplates have been selectively prepared. The α-Fe_2O_3 nanoplates can be synthesized with iron ionbased ionic liquid as iron source and template. The α-Fe_2O_3 nanoplates as the anode of LIBs can display high capacity of around1950 mAh g^(-1) at 0.5 A g^(-1) which have exceeded the theoretical capacity of α-Fe_2O_3. On account of unique nanoplate structures and gum arabic as binder, the α-Fe_2O_3 nanoplates also exhibit high rate capability and excellent cycling performance.展开更多
Sodium-ion batteries(SIBs)are expected to offer affordability and high energy density for large-scale energy storage system.However,the commercial application of SIBs is hurdled by low initial coulombic efficiency(ICE...Sodium-ion batteries(SIBs)are expected to offer affordability and high energy density for large-scale energy storage system.However,the commercial application of SIBs is hurdled by low initial coulombic efficiency(ICE),continuous Na loss during long-term operation,and low sodium-content of cathode materials.In this scenario,presodiation strategy by introducing an external sodium reservoir has been rationally proposed,which could supplement additional sodium ions into the system and thereby markedly improve both the cycling performance and energy density of SIBs.In this review,the significance of presodiation is initially introduced,followed by comprehensive interpretation on technological properties,underlying principles,and associated approaches,as well as our perspectives on present inferiorities and future research directions.Overall,this contribution outlines a distinct pathway towards the presodiation methodology,of significance but still in its nascent phase,which may inspire the targeted guidelines to explore new chemistry in this field.展开更多
With a high reversible capacity exceeding 1000 mAh g^(-1),rechargeable sodium-chlorine(Na-Cl_(2))batteries offer a compelling alternative to conventional lithium-ion batteries(e.g.,LiFePO_(4)offers a capacity of less ...With a high reversible capacity exceeding 1000 mAh g^(-1),rechargeable sodium-chlorine(Na-Cl_(2))batteries offer a compelling alternative to conventional lithium-ion batteries(e.g.,LiFePO_(4)offers a capacity of less than 200 mAh g^(-1)),leveraging the abundance and low cost of sodium/chlorine resources[1,2].However,the commercial viability of these batteries has been significantly hindered by the severe corrosivity of the conventional thionyl chloride(SOCl_(2))-based electrolytes.展开更多
基金the financial supports for this research from the National Basic Research Program of China(2019YFB1505103)the National Natural Science Foundation of China(51571179 and 51671173)the Open Fund of the Guangdong Provincial Key Laboratory of Advance Energy Storage Materials。
文摘Magnesium hydride has attracted great attention because of its high theoretical capacity and outstanding reversibility, nevertheless, its practical applications have been restricted by the disadvantages of the sluggish kinetics and high thermodynamic stability. In this work, an unexpected high reversible hydrogen capacity over 8.0 wt% has been achieved from MgH2 metal hydride composited with small amounts of LiBH4 and Li3AlH6 complex hydrides, which begins to release hydrogen at 276 ℃ and then completely dehydrogenates at 360 ℃. The dehydrogenated MgH2+LiBH4/Li3AlH6 composite can fully reabsorb hydrogen below 300 ℃ with an excellent cycling stability. The composite exhibits a significant reduction of dehydrogenation activation energy from 279.7 kJ/mol(primitive MgH2) to 139.3 kJ/mol(MgH2+LiBH4/Li3AlH6),as well as a remarkable reduction of dehydrogenation enthalpy change from 75.1 k J/mol H2(primitive MgH2) to 62.8 kJ/mol H2(MgH2+LiBH4/Li3AlH6). The additives of LiBH4 and Li3AlH6 not only enhance the cycling hydrogen capacity, but also simultaneously improve the reversible de/rehydrogenation kinetics, as well as the dehydrogenation thermodynamics. This notable improvement on the hydrogen absorption/desorption behaviors of the MgH2+LiBH4/Li3AlH6 composite could be attributed to the dehydrogenated products including Li3Mg7, Mg17Al12 and MgAlB4, which play a key role on reducing the dehydrogenation activation energy and increasing diffusion rate of hydrogen. Meanwhile, the LiBH4 and Li3AlH6 effectively destabilize MgH2 with a remarkable reduction on dehydrogenation enthalpy change in terms of thermodynamics. In particular, the Li3Mg7, Mg17Al12 and MgAlB4 phases can reversibly transform into MgH2, Li3AlH6 and LiBH4 after rehydrogenation, which contribute to maintain a high cycling capacity.This constructing strategy can further promote the development of high reversible capacity Mg-based materials with suitable de/rehydrogenation properties.
基金National Natural Science Foundation of China(Nos.52271213 and 52271221).
文摘MgH_(2),as one of the typical solid-state hydrogen storage materials,has attracted extensive attention.However,the slow kinetics and poor cycle stability limit its application.In this work,LiBH_(4) and YNi_(5) alloy were co-added as additives to MgH_(2) via ball milling,thereby realizing an excellent dehydrogenation per-formance and good cycle stability at 300 ℃.The MgH_(2)-0.04LiBH_(4)-0.01YNi_(5) composite can release 7 wt.%of hydrogen in around 10 min at 300 ℃ and still have a reversible hydrogen storage capacity of 6.42 wt.%after 110 cycles,with a capacity retention rate as high as 90.3%based on the second dehydrogenation capacity.The FTIR results show that LiBH_(4) can reversibly absorb and desorb hydrogen throughout the hydrogen ab/desorption process,which contributes a portion of the reversible hydrogen storage capacity to the MgH_(2)-0.04LiBH_(4)-0.01YNi_(5) composite.Due to the small amount of LiBH_(4) and YNi_(5),the dehydro-genation activation energy of MgH_(2) did not decrease significantly,nor did the dehydrogenation enthalpy(△H)change.However,the MgNi3B2 and in-situ formed YH3 during the hydrogen absorption/desorption cycles is not only beneficial to the improvement of the kinetics performance for MgH_(2) but also improves its cycle stability.This work provides a straightforward method for developing high reversible hydrogen capacity on Mg-based hydrogen storage materials with moderate kinetic performance.
基金supported by the National Natural Science Foundation of China(Grant No.22078278)Hunan Innovative Talent Project(Grant No.2022RC1111)+1 种基金the Key project of Hunan Provincial Education Department(Grant No.22A0131)the State Key Laboratory of Clean Energy Utilization(Open Fund Project No.ZJUCEU2021009).
文摘Biomass-derived carbon materials for lithiumion batteries emerge as one of the most promising anodes from sustainable perspective.However,improving the reversible capacity and cycling performance remains a long-standing challenge.By combining the benefits of K2CO_(3) activation and KMnO_(4) hydrothermal treatment,this work proposes a two-step activation method to load MnO_(2) charge transfer onto biomass-derived carbon(KAC@MnO_(2)).Comprehensive analysis reveals that KAC@MnO_(2) has a micro-mesoporous coexistence structure and uniform surface distribution of MnO_(2),thus providing an improved electrochemical performance.Specifically,KAC@MnO_(2) exhibits an initial chargedischarge capacity of 847.3/1813.2 mAh·g^(-1) at 0.2 A·g^(-1),which is significantly higher than that of direct pyrolysis carbon and K2CO_(3) activated carbon,respectively.Furthermore,the KAC@MnO_(2) maintains a reversible capacity of 652.6 mAh·g^(-1) after 100 cycles.Even at a high current density of 1.0 A·g^(-1),KAC@MnO_(2) still exhibits excellent long-term cycling stability and maintains a stable reversible capacity of 306.7 mAh·g^(-1) after 500 cycles.Compared with reported biochar anode materials,the KAC@MnO_(2) prepared in this work shows superior reversible capacity and cycling performance.Additionally,the Li+insertion and de-insertion mechanisms are verified by ex situ X-ray diffraction analysis during the chargedischarge process,helping us better understand the energy storage mechanism of KAC@MnO_(2).
基金financially supported by the National Natural Science Foundation of China (No.21506081,21506077)Jiangsu University Scientific Research Funding (15JDG048)+1 种基金Chinese Postdoctoral Foundation (2016M590420)Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions
文摘On account of the high theoretical capacity, high corrosion resistance, environmental benignity, abundant availability and low cost, the research on a-Fe_2O_3 has been gradually fastened on as promising anodes materials toward lithium-ion batteries(LIBs). A high-performance anode for LIBs based on α-Fe_2O_3 nanoplates have been selectively prepared. The α-Fe_2O_3 nanoplates can be synthesized with iron ionbased ionic liquid as iron source and template. The α-Fe_2O_3 nanoplates as the anode of LIBs can display high capacity of around1950 mAh g^(-1) at 0.5 A g^(-1) which have exceeded the theoretical capacity of α-Fe_2O_3. On account of unique nanoplate structures and gum arabic as binder, the α-Fe_2O_3 nanoplates also exhibit high rate capability and excellent cycling performance.
基金the financial support from the National Nature Science Foundation of China(No.U20A20249)the National Key Research and Development Program of China(2021YFB3800300)the Shenzhen Science and Technology Innovation Commission(KCXST20221021111216037)。
文摘Sodium-ion batteries(SIBs)are expected to offer affordability and high energy density for large-scale energy storage system.However,the commercial application of SIBs is hurdled by low initial coulombic efficiency(ICE),continuous Na loss during long-term operation,and low sodium-content of cathode materials.In this scenario,presodiation strategy by introducing an external sodium reservoir has been rationally proposed,which could supplement additional sodium ions into the system and thereby markedly improve both the cycling performance and energy density of SIBs.In this review,the significance of presodiation is initially introduced,followed by comprehensive interpretation on technological properties,underlying principles,and associated approaches,as well as our perspectives on present inferiorities and future research directions.Overall,this contribution outlines a distinct pathway towards the presodiation methodology,of significance but still in its nascent phase,which may inspire the targeted guidelines to explore new chemistry in this field.
文摘With a high reversible capacity exceeding 1000 mAh g^(-1),rechargeable sodium-chlorine(Na-Cl_(2))batteries offer a compelling alternative to conventional lithium-ion batteries(e.g.,LiFePO_(4)offers a capacity of less than 200 mAh g^(-1)),leveraging the abundance and low cost of sodium/chlorine resources[1,2].However,the commercial viability of these batteries has been significantly hindered by the severe corrosivity of the conventional thionyl chloride(SOCl_(2))-based electrolytes.
