Organic electrode materials are desirable for green and sustainable Li-ion batteries(LIBs) due to their light-weight, low cost, abundance and multi-electron transfer reactions during battery operation. However, the su...Organic electrode materials are desirable for green and sustainable Li-ion batteries(LIBs) due to their light-weight, low cost, abundance and multi-electron transfer reactions during battery operation. However, the successful utilization of organic electrodes is hindered by their poor electrical conductivity and low cyclic stability. Herein, a facile synthesis of π-conjugated N-containing heteroaromatic hexacarboxylate(Li6-HAT) compound and its electrochemical performance as an anode material in LIBs is reported.The as-synthesized Li6-HAT electrode renders an ultrahigh initial capacity of 1126.3 m Ah g^(-1) at the current density of 100 m A g^(-1). Moreover, π-conjugated N-containing heteroaromatic center provide excellent reversibility of(de)lithiation process, resulting in excellent capacity retention. Furthermore, a combination of density functional theory(DFT) calculations, in-situ Fourier transform infrared(FTIR) and ex-situ X-ray photoelectron spectroscopy(XPS) characterization reveal that the π-conjugated nitrogen and carboxyl oxygen act as electrochemically active sites during the charge/discharge process. The current work provides novel insights into the charge storage mechanism of organic electrodes and opens up avenues for further development and utilization of organic electrodes in Li-ion batteries.展开更多
Sodium-ion batteries(SIBs)have attracted considerable interest as an alternative to lithium-ion batteries owing to their similar electrochemical performance and superior long-term cycle stability.Organic materials are...Sodium-ion batteries(SIBs)have attracted considerable interest as an alternative to lithium-ion batteries owing to their similar electrochemical performance and superior long-term cycle stability.Organic materials are regarded as promising anode materials for constructing SIBs with high capacity and good retention.However,utilization of organic materials is rather limited by their low energy density and poor stability at high current densities.To overcome these limitations,we utilized a novel polymeric disodium phthalocyanines(pNaPc)as SIB anodes to provide stable coordination sites for Na ions as well as to enhance the stability at high current density.By varying the linker type during a one-pot cyclization and polymerization process,two pNaPc anodes with O-(O-pNaPc)and S-linkers(S-pNaPc)were prepared,and their structural and electrochemical properties were investigated.The O-pNaPc binds Na ions with a lower binding energy compared with S-pNaPc,which leads to more facile Na-ion coordination/dissociation when engaged as SIB anode.The use of O-pNaPc significantly improves the redox kinetics and cycle stability and allows the fabrication of a full cell against Na_(3)V_(2)(PO_(4))_(2)F_(3)/C cathode,which demonstrates its practical application with high energy density(288 Wh kg^(-1))and high power density(149 W kg^(-1)).展开更多
Future battery advances and economies of scale will help scrub CO2emissions from transportation and the grid.Economical energy storage lets battery-powered electric vehicles replace internal combustion engines in the ...Future battery advances and economies of scale will help scrub CO2emissions from transportation and the grid.Economical energy storage lets battery-powered electric vehicles replace internal combustion engines in the transportation sector,which now accounts for the plurality of CO2emissions.For grid-scale applications,the benefits of adding storage are many and well documented[1–2].Beyond increased penetration of intermittent renewable energy generated from such as solar panels展开更多
It is still challenging to obtain broadband emission covering visible light spectrum as much as possible with negligible angular dependence. In this work, we demonstrate a low driving voltage top-emitting white organi...It is still challenging to obtain broadband emission covering visible light spectrum as much as possible with negligible angular dependence. In this work, we demonstrate a low driving voltage top-emitting white organic light-emitting diode (TEWOLED) based on complementary blue and yellow phosphor emitters with negligible angular dependence. The bottom copper anode with medium reflectance, which is compatible with the standard complementary metal oxide semiconductor (CMOS) technology below 0.13 μm, and the semitransparent multi- layer Cs2CO3/AI/Cu cathode as a top electrode, are introduced to realize high-performance TEWOLED. Our TEWOLED achieves high efficiencies of 15.4callA and 12.1 1m/W at a practical brightness of lO00cd/m2 at low voltage of 4 V.展开更多
Rechargeable sodium-ion batteries usually suffer from accelerated electrode destruction at high temperatures and high synthesis costs of electrode materials.Therefore,it is highly desirable to explore novel organic el...Rechargeable sodium-ion batteries usually suffer from accelerated electrode destruction at high temperatures and high synthesis costs of electrode materials.Therefore,it is highly desirable to explore novel organic electrodes considering their cost-effectiveness and large adaptability to volume changes.Herein,natural biomass,pristine lignin,is employed as the sodium-ion battery anodes,and their sodium storage performance is investigated at room temperature and 60℃.The lignin anodes exhibit excellent high-temperature sodium-ion battery performance.This mainly results from the generation of abundant reactive sites(C=O)due to the high temperature-induced homogeneous cleavage of the C_(β)-O bond in the lignin macromolecule.This work can inspire researchers to explore other natural organic materials for large-scale applications and high-value utilization in advanced energy storage devices.展开更多
Polymer materials offer controllable structure-dependent performances in separation,catalysis and drug release.Their molecular structures can be precisely tailored to accept Li^(+)for energy storage applications.Here ...Polymer materials offer controllable structure-dependent performances in separation,catalysis and drug release.Their molecular structures can be precisely tailored to accept Li^(+)for energy storage applications.Here the design of sp^(2)carbon-based polyphenylene(PPH)with high lithium-ion uptakes and long-term stability is reported.Linear-PPH(L-PPH)exceeds the performance of crosslink-PPH(C-PPH),due to the fact that it has an ordered lamellar structure,promoting the Li^(+)intercalation/deintercalation channel.The L-PPH cell shows a clear charge and discharge plateau at 0.35 and 0.15 V vs.Li^(+)/Li,respectively,which is absent in the C-PPH cell.The Li^(+)storage capacity of L-PPH is five times that of the C-PPH.The reversible storage capacity is further improved to 261 m Ah g;by functionalizing the L-PPH with the–SO_(3)H groups.In addition,the Li-intercalated structures of C-PPH and L-PPH are investigated via near-edge X-ray absorption fine structure(NEXAFS),suggesting the high reversible Li^(+)–C=C bond interaction at L-PPH.This strategy,based on new insight into sp^(2)functional groups,is the first step toward a molecular understanding of the structure storage-capacity relationship in sp^(2)carbon-based polymer.展开更多
Inorganic/organic nanohybrids composed of arrayed TiO_2 nanotubes(Ti NTs)/porphyrin nanoparticles(NPs) have been fabricated via a wet chemical approach. The inorganic component, particularly the arrayed one-dimens...Inorganic/organic nanohybrids composed of arrayed TiO_2 nanotubes(Ti NTs)/porphyrin nanoparticles(NPs) have been fabricated via a wet chemical approach. The inorganic component, particularly the arrayed one-dimensional(1D) nanostructures, provides high charge-carrier mobility and rapid charge transport. The organic component exhibits extensive visible light absorption and good solution processability. Additionally, the geometric restraint by supramolecular assembly renders an improved photostability. A combination of these two components could thus allow for an efficient solar energy conversion. In this work, a colloid of porphyrin NPs prepared by a solvent exchange method is coated on anodic Ti NTs by means of a dip-coating treatment to form inorganic/organic hybrids. The hybrids exhibit an improvement on solar absorption and a significant enhancement on photocurrent generation at a small bias compared with individual component. Herein, the inorganic/organic nanohybrids are proved to be excellent photoanodes highly responsive to visible light and thus pave a way to discover new inorganic/organic assemblies for high-performance optoelectronic applications, as well as for device integration.展开更多
Organic anode materials have attracted considerable interest owing to their high tunability by adopting various active functional groups.However,the interaction mechanisms between the alkali metals and the active func...Organic anode materials have attracted considerable interest owing to their high tunability by adopting various active functional groups.However,the interaction mechanisms between the alkali metals and the active functional groups in host materials have been rarely studied systematically.Here,a widely used organic semiconductor of perylene-3,4,9,10-tetracarboxylic diimide(PTCDI)was selected as a model system to investigate how alkali metals interact with imide functional groups and induce changes in chemical and electronic structures of PTCDI.The interaction at the alkali/PTCDI interface was probed by in-situ X-ray photoelectron spectroscopy(XPS),ultraviolet photoelectron spectroscopy(UPS),synchrotron-based near edge X-ray absorption fine structure(NEXAFS),and corroborated by density functional theory(DFT)calculations.Our results indicate that the alkali metal replaces the hydrogen atoms in the imide group and interact with the imide nitrogen of PTCDI.Electron transfer induced gap states and downward band-bending like effects are identified on the alkali-deposited PTCDI surface.It was found that Na shows a stronger electron transfer effect than Li.Such a model study of alkali insertion/intercalation in PTCDI gives insights for the exploration of the potential host materials for alkali storage applications.展开更多
A simple, cost effective and rapid electrochemical method has been developed for the determination of micro level ortho nitrobenzaldehyde(ONB) based on outstanding properties of modified aluminum electrode tin nanor...A simple, cost effective and rapid electrochemical method has been developed for the determination of micro level ortho nitrobenzaldehyde(ONB) based on outstanding properties of modified aluminum electrode tin nanorods/anodic aluminum oxide/aluminum(SnNR/AAO/Al) for the first time. The SnNR/AAO/Al electrode was fabricated by a second step anodization, followed by electrodeposition and its electrochemical behavior was investigated in detail. The cyclic voltammetry results indicated that the SnNR/AAO/Al electrode exhibited efficient electrocatalytic activity toward reduction of ONB in the acidic solution. It provides an appreciable improvement of reduction peak for ONB at-0.721 V.Furthermore, various kinetic parameters such as transfer electron number, transfer proton number and standard heterogeneous rate constant were calculated from the scan rates.The electrocatalytic behavior was further exploited as a sensitive detection scheme for the ONB determination by differential pulse voltammetry. Under the optimized conditions, the concentration range and detection limit are 0.1-100 μmol/L and 0.05 μmol/L, respectively,for ONB. The analytical performance of this modified sensor has been evaluated for detection of real sample such as river water and recovery of ONB was achieved all-out up to102.3% under standard addition method.展开更多
基金financial support from the National Natural Science Foundation of China (51764048, 21961030 and 51474191)Yunnan Province Thousand Youth Talents Plan+1 种基金the Application Basis Research Project of Yunnan Province Science and Technology Department (2017FD144)the Key Natural Science Foundation of Yunnan Province China (2018FA28, 2019FY003023 and 2018FH001-007)。
文摘Organic electrode materials are desirable for green and sustainable Li-ion batteries(LIBs) due to their light-weight, low cost, abundance and multi-electron transfer reactions during battery operation. However, the successful utilization of organic electrodes is hindered by their poor electrical conductivity and low cyclic stability. Herein, a facile synthesis of π-conjugated N-containing heteroaromatic hexacarboxylate(Li6-HAT) compound and its electrochemical performance as an anode material in LIBs is reported.The as-synthesized Li6-HAT electrode renders an ultrahigh initial capacity of 1126.3 m Ah g^(-1) at the current density of 100 m A g^(-1). Moreover, π-conjugated N-containing heteroaromatic center provide excellent reversibility of(de)lithiation process, resulting in excellent capacity retention. Furthermore, a combination of density functional theory(DFT) calculations, in-situ Fourier transform infrared(FTIR) and ex-situ X-ray photoelectron spectroscopy(XPS) characterization reveal that the π-conjugated nitrogen and carboxyl oxygen act as electrochemically active sites during the charge/discharge process. The current work provides novel insights into the charge storage mechanism of organic electrodes and opens up avenues for further development and utilization of organic electrodes in Li-ion batteries.
基金financial supports from the Research Grants Council of the Hong Kong Special Administrative Region(Poly U15217521)the Hong Kong Polytechnic University(Q-CDA3)Initiative for fostering University of Research and Innovation Program of the National Research Foundation(NRF)funded by the Korean government(MSIT)(No.2020M3H1A1077095)
文摘Sodium-ion batteries(SIBs)have attracted considerable interest as an alternative to lithium-ion batteries owing to their similar electrochemical performance and superior long-term cycle stability.Organic materials are regarded as promising anode materials for constructing SIBs with high capacity and good retention.However,utilization of organic materials is rather limited by their low energy density and poor stability at high current densities.To overcome these limitations,we utilized a novel polymeric disodium phthalocyanines(pNaPc)as SIB anodes to provide stable coordination sites for Na ions as well as to enhance the stability at high current density.By varying the linker type during a one-pot cyclization and polymerization process,two pNaPc anodes with O-(O-pNaPc)and S-linkers(S-pNaPc)were prepared,and their structural and electrochemical properties were investigated.The O-pNaPc binds Na ions with a lower binding energy compared with S-pNaPc,which leads to more facile Na-ion coordination/dissociation when engaged as SIB anode.The use of O-pNaPc significantly improves the redox kinetics and cycle stability and allows the fabrication of a full cell against Na_(3)V_(2)(PO_(4))_(2)F_(3)/C cathode,which demonstrates its practical application with high energy density(288 Wh kg^(-1))and high power density(149 W kg^(-1)).
文摘Future battery advances and economies of scale will help scrub CO2emissions from transportation and the grid.Economical energy storage lets battery-powered electric vehicles replace internal combustion engines in the transportation sector,which now accounts for the plurality of CO2emissions.For grid-scale applications,the benefits of adding storage are many and well documented[1–2].Beyond increased penetration of intermittent renewable energy generated from such as solar panels
基金Supported by the National Basic Research Program of China under Grant No 2010CB327701the National Natural Science Foundation of China under Grant No 61275033
文摘It is still challenging to obtain broadband emission covering visible light spectrum as much as possible with negligible angular dependence. In this work, we demonstrate a low driving voltage top-emitting white organic light-emitting diode (TEWOLED) based on complementary blue and yellow phosphor emitters with negligible angular dependence. The bottom copper anode with medium reflectance, which is compatible with the standard complementary metal oxide semiconductor (CMOS) technology below 0.13 μm, and the semitransparent multi- layer Cs2CO3/AI/Cu cathode as a top electrode, are introduced to realize high-performance TEWOLED. Our TEWOLED achieves high efficiencies of 15.4callA and 12.1 1m/W at a practical brightness of lO00cd/m2 at low voltage of 4 V.
基金financialy supported by the National Natural Science Foundation of China(nos.22078069,22178069,51903254)
文摘Rechargeable sodium-ion batteries usually suffer from accelerated electrode destruction at high temperatures and high synthesis costs of electrode materials.Therefore,it is highly desirable to explore novel organic electrodes considering their cost-effectiveness and large adaptability to volume changes.Herein,natural biomass,pristine lignin,is employed as the sodium-ion battery anodes,and their sodium storage performance is investigated at room temperature and 60℃.The lignin anodes exhibit excellent high-temperature sodium-ion battery performance.This mainly results from the generation of abundant reactive sites(C=O)due to the high temperature-induced homogeneous cleavage of the C_(β)-O bond in the lignin macromolecule.This work can inspire researchers to explore other natural organic materials for large-scale applications and high-value utilization in advanced energy storage devices.
基金funded by the Engineering and Physical Sciences Research Council(EPSRC)(EP/P02467X/1 and EP/S018204/1)the Centre for Nature Inspired Chemical Engineering(EP K038656/1)。
文摘Polymer materials offer controllable structure-dependent performances in separation,catalysis and drug release.Their molecular structures can be precisely tailored to accept Li^(+)for energy storage applications.Here the design of sp^(2)carbon-based polyphenylene(PPH)with high lithium-ion uptakes and long-term stability is reported.Linear-PPH(L-PPH)exceeds the performance of crosslink-PPH(C-PPH),due to the fact that it has an ordered lamellar structure,promoting the Li^(+)intercalation/deintercalation channel.The L-PPH cell shows a clear charge and discharge plateau at 0.35 and 0.15 V vs.Li^(+)/Li,respectively,which is absent in the C-PPH cell.The Li^(+)storage capacity of L-PPH is five times that of the C-PPH.The reversible storage capacity is further improved to 261 m Ah g;by functionalizing the L-PPH with the–SO_(3)H groups.In addition,the Li-intercalated structures of C-PPH and L-PPH are investigated via near-edge X-ray absorption fine structure(NEXAFS),suggesting the high reversible Li^(+)–C=C bond interaction at L-PPH.This strategy,based on new insight into sp^(2)functional groups,is the first step toward a molecular understanding of the structure storage-capacity relationship in sp^(2)carbon-based polymer.
基金the National Natural Science Foundation of China (Nos. 51503014 and 51501008)the Beijing Higher Education Young Elite Teacher Project (No. YETP0419)
文摘Inorganic/organic nanohybrids composed of arrayed TiO_2 nanotubes(Ti NTs)/porphyrin nanoparticles(NPs) have been fabricated via a wet chemical approach. The inorganic component, particularly the arrayed one-dimensional(1D) nanostructures, provides high charge-carrier mobility and rapid charge transport. The organic component exhibits extensive visible light absorption and good solution processability. Additionally, the geometric restraint by supramolecular assembly renders an improved photostability. A combination of these two components could thus allow for an efficient solar energy conversion. In this work, a colloid of porphyrin NPs prepared by a solvent exchange method is coated on anodic Ti NTs by means of a dip-coating treatment to form inorganic/organic hybrids. The hybrids exhibit an improvement on solar absorption and a significant enhancement on photocurrent generation at a small bias compared with individual component. Herein, the inorganic/organic nanohybrids are proved to be excellent photoanodes highly responsive to visible light and thus pave a way to discover new inorganic/organic assemblies for high-performance optoelectronic applications, as well as for device integration.
基金The authors acknowledge the financial support from Singapore MOE Tier II grant R143-000-A29-112,Academic Research Fund Tie I grant RG104/18,and the National Research Foundation under the grant of NRF2017NRF-NSFC001-007the computing resources from National Supercomputing Centre Singapore.
文摘Organic anode materials have attracted considerable interest owing to their high tunability by adopting various active functional groups.However,the interaction mechanisms between the alkali metals and the active functional groups in host materials have been rarely studied systematically.Here,a widely used organic semiconductor of perylene-3,4,9,10-tetracarboxylic diimide(PTCDI)was selected as a model system to investigate how alkali metals interact with imide functional groups and induce changes in chemical and electronic structures of PTCDI.The interaction at the alkali/PTCDI interface was probed by in-situ X-ray photoelectron spectroscopy(XPS),ultraviolet photoelectron spectroscopy(UPS),synchrotron-based near edge X-ray absorption fine structure(NEXAFS),and corroborated by density functional theory(DFT)calculations.Our results indicate that the alkali metal replaces the hydrogen atoms in the imide group and interact with the imide nitrogen of PTCDI.Electron transfer induced gap states and downward band-bending like effects are identified on the alkali-deposited PTCDI surface.It was found that Na shows a stronger electron transfer effect than Li.Such a model study of alkali insertion/intercalation in PTCDI gives insights for the exploration of the potential host materials for alkali storage applications.
基金CSIR (09/0810 (0021)/ 2012-EMR-I), Periyar University for providing fundUGC networking resource center for providing visiting fellowship
文摘A simple, cost effective and rapid electrochemical method has been developed for the determination of micro level ortho nitrobenzaldehyde(ONB) based on outstanding properties of modified aluminum electrode tin nanorods/anodic aluminum oxide/aluminum(SnNR/AAO/Al) for the first time. The SnNR/AAO/Al electrode was fabricated by a second step anodization, followed by electrodeposition and its electrochemical behavior was investigated in detail. The cyclic voltammetry results indicated that the SnNR/AAO/Al electrode exhibited efficient electrocatalytic activity toward reduction of ONB in the acidic solution. It provides an appreciable improvement of reduction peak for ONB at-0.721 V.Furthermore, various kinetic parameters such as transfer electron number, transfer proton number and standard heterogeneous rate constant were calculated from the scan rates.The electrocatalytic behavior was further exploited as a sensitive detection scheme for the ONB determination by differential pulse voltammetry. Under the optimized conditions, the concentration range and detection limit are 0.1-100 μmol/L and 0.05 μmol/L, respectively,for ONB. The analytical performance of this modified sensor has been evaluated for detection of real sample such as river water and recovery of ONB was achieved all-out up to102.3% under standard addition method.