Water-saving irrigation strategies can successfully alleviate methane emissions from rice fields,but significantly stimulate nitrous oxide(N_(2)O)emissions because of variations in soil oxygen level and redox potentia...Water-saving irrigation strategies can successfully alleviate methane emissions from rice fields,but significantly stimulate nitrous oxide(N_(2)O)emissions because of variations in soil oxygen level and redox potential.However,the relationship linking soil N_(2)O emissions to nitrogen functional genes during various fertilization treatments in water-saving paddy fields has rarely been investigated.Furthermore,the mitigation potential of organic fertilizer substitution on N_(2)O emissions and the microbial mechanism in rice fields must be further elucidated.Our study examined how soil N_(2)O emissions were affected by related functional microorganisms(ammonia-oxidizing archaea(AOA),ammonia-oxidizing bacteria(AOB),nirS,nirK and nosZ)to various fertilization treatments in a rice field in southeast China over two years.In this study,three fertilization regimes were applied to rice cultivation:a no nitrogen(N)(Control),an inorganic N(Ni),and an inorganic N with partial N substitution with organic manure(N_(i)+N_(o)).Over two rice-growing seasons,cumulative N_(2)O emissions averaged 0.47,4.62 and 4.08 kg ha^(−1)for the Control,Ni and N_(i)+N_(o)treatments,respectively.In comparison to the Ni treatment,the N_(i)+N_(o)fertilization regime considerably reduced soil N_(2)O emissions by 11.6%while maintaining rice yield,with a lower N_(2)O emission factor(EF)from fertilizer N of 0.95%.Nitrogen fertilization considerably raised the AOB,nirS,nirK and nosZ gene abundances,in comparison to the Control treatment.Moreover,the substitution of organic manure for inorganic N fertilizer significantly decreased AOB and nirS gene abundances and increased nosZ gene abundance.The AOB responded to N fertilization more sensitively than the AOA.Total N_(2)O emissions significantly correlated positively with AOB and nirS gene abundances while having a negative correlation with nosZ gene abundance and the nosZ/nirS ratio across N-fertilized plots.In summary,we conclude that organic manure substitution for inorganic N fertilizer decreased soil N_(2)O emissions primarily by changing the soil NO_(3)^(−)-N,pH and DOC levels,thus inhibiting the activities of ammonia oxidation in nitrification and nitrite reduction in denitrification,and strengthening N_(2)O reduction in denitrification from water-saving rice paddies.展开更多
It is a challenge to coordinate carrier-kinetics performance and the redox capacity of photogenerated charges synchronously at the atomic level for boosting photocatalytic activity.Herein,the atomic Ni was introduced ...It is a challenge to coordinate carrier-kinetics performance and the redox capacity of photogenerated charges synchronously at the atomic level for boosting photocatalytic activity.Herein,the atomic Ni was introduced into the lattice of hexagonal ZnIn_(2)S_(4) nanosheets(Ni/ZnIn_(2)S_(4))via directionalsubstituting Zn atom with the facile hydrothermal method.The electronic structure calculations indicate that the introduction of Ni atom effectively extracts more electrons and acts as active site for subsequent reduction reaction.Besides the optimized light absorption range,the elevation of Efand ECBendows Ni/ZnIn_(2)S_(4) photocatalyst with the increased electron concentration and the enhanced reduction ability for surface reaction.Moreover,ultrafast transient absorption spectroscopy,as well as a series of electrochemical tests,demonstrates that Ni/ZnIn_(2)S_(4) possesses 2.15 times longer lifetime of the excited charge carriers and an order of magnitude increase for carrier mobility and separation efficiency compared with pristine ZnIn_(2)S_(4).These efficient kinetics performances of charge carriers and enhanced redox capacity synergistically boost photocatalytic activity,in which a 3-times higher conversion efficiency of nitrobenzene reduction was achieved upon Ni/ZnIn_(2)S_(4).Our study not only provides in-depth insights into the effect of atomic directional-substitution on the kinetic behavior of photogenerated charges,but also opens an avenue to the synchronous optimization of redox capacity and carrier-kinetics performance for efficient solar energy conversion.展开更多
Na-doped Li1.05Mn2O4 cathodes were synthesized using a sol-gel process.The samples were characterized by X-ray diffractometry(XRD),cyclic voltammetry(CV),electrochemical impedance spectroscopy(EIS)and charge-discharge...Na-doped Li1.05Mn2O4 cathodes were synthesized using a sol-gel process.The samples were characterized by X-ray diffractometry(XRD),cyclic voltammetry(CV),electrochemical impedance spectroscopy(EIS)and charge-discharge measurements. The results show that all the samples exhibit the same cubic spinel phase structure without impurity.The lattice constant and unit cell volume decrease with increasing the sodium dopant amount.As the molar ratio of sodium to manganese(x=n(Na)/n(Mn))increases from 0 to 0.03,the initial discharge capacity of the Li1.05Mn2O4 cathodes decreases from 119.2 to 107.9 mA·h/g,and the discharge capability at large current rate and the storage performance decline dramatically,while cycling performance at room temperature and 55℃are improved.The CV and EIS studies indicate that reversibility of Li1.05Mn2O4 cathodes decreases and the electrochemical impedance increases with increasing the sodium dopant amount.展开更多
MXene-based materials have gained considerable attention for lithium-sulfur(Li-S)batteries cathode materials due to their superior electric conductivity and high affinitive to polysulfides.However,there are still chal...MXene-based materials have gained considerable attention for lithium-sulfur(Li-S)batteries cathode materials due to their superior electric conductivity and high affinitive to polysulfides.However,there are still challenges in modifying the surface functional groups of MXene to further improve the electrochemical performance and increase the structure variety for MXene-based sulfur host.Herein,we report an efficient and flexible nucleophilic substitution(S_(N))strategy to modify the Ti_(3)C_(2)T_(x) surface terminations and purposefully designed Magnolol-modified Ti_(3)C_(2)T_(x)(M-Ti_(3)C_(2)T_(x))as powerful cathode host materials.Benefiting from more C-Ti-O bonds forming and diallyl groups terminations reducing after the dehalogenation and nucleophilic addition reactions,the given M-Ti_(3)C_(2)T_(x) electrode could effectively suppress the lithium polysulfides shuttling via chemisorption and C—S covalent bond formation.Besides,the Magnolol-modified Ti_(3)C_(2)T_(x) significantly accelerates polysulfide redox reaction and reduces the activation energy of Li_(2) S decomposition.As a result,the as-prepared M-Ti_(3)C_(2)T_(x) electrode displays an excellent rate capability and a high reversible capacity of 7.68 mAh cm^(-2)even under 7.2 mg cm^(-2)S-loaded with a low decay rate of 0.07%(from 2 nd cycle).This flexible surface-modified strategy for MXene terminations is expected to be extended to other diverse MXene applications.展开更多
Magnesium ion batteries(MIBs)are a potential field for the energy storage of the future but are restricted by insufficient rate capability and rapid capacity degradation.Magnesium-sodium hybrid ion batteries(MSHBs)are...Magnesium ion batteries(MIBs)are a potential field for the energy storage of the future but are restricted by insufficient rate capability and rapid capacity degradation.Magnesium-sodium hybrid ion batteries(MSHBs)are an effective way to address these problems.Here,we report a new type of MSHBs that use layered sodium vanadate((Na,Mn)V_(8)O_(20)·5H_(2)O,Mn-NVO)cathodes coupled with an organic 3,4,9,10-perylenetetracarboxylic diimide(PTCDI)anode in Mg^(2+)/Na^(+)hybrid electrolytes.During electrochemical cycling,Mg^(2+)and Na^(+)co-participate in the cathode reactions,and the introduction of Na^(+)promotes the structural stability of the Mn-NVO cathode,as cleared by several ex-situ characterizations.Consequently,the Mn-NVO cathode presents great specific capacity(249.9 mA h g^(−1)at 300 mA g^(−1))and cycling(1500 cycles at 1500 mA g^(−1))in the Mg^(2+)/Na^(+)hybrid electrolytes.Besides,full battery displays long lifespan with 10,000 cycles at 1000 mA g^(−1).The rate performance and cycling stability of MSHBs have been improved by an economical and scalable method,and the mechanism for these improvements is discussed.展开更多
Polycrystalline particles of Ca3-xErxCo2O6 (x=0.0, 0.15, 0.3, 0.45 and 0.6) were synthesized using sol-gel method combined with Low Temperature Sintering procedure (LTS) to evaluate the effect of Er substitution o...Polycrystalline particles of Ca3-xErxCo2O6 (x=0.0, 0.15, 0.3, 0.45 and 0.6) were synthesized using sol-gel method combined with Low Temperature Sintering procedure (LTS) to evaluate the effect of Er substitution on the thermoelectric properties of Ca3Co2O6. The crystal structure and microstructure were investigated using X-ray diffraction, infrared spectroscopy and scanning electron microscope. The electrical conductivity and Seebeck coefficient of the complex oxides were measured from 300 to 1073 K. The results showed that all the sampies were p-type semiconductors. The electrical conductivity increased with the increase in temperature. Er substitutions at Ca site affected carrier concentrations and carder mobility, resulting an increase in Seebeck coefficient and decrease in electrical conductivity. The power factor of Ca2.85Er0.15Co2O6 reached 10.66 μw/mK^2 at 1073 K.展开更多
The environmentally friendly Cu_(2)ZnSn(S,Se)_(4)(CZTSSe) compounds are promising direct bandgap materials for application in thin film solar cells, but the spontaneous surface defects disordering would lead to large ...The environmentally friendly Cu_(2)ZnSn(S,Se)_(4)(CZTSSe) compounds are promising direct bandgap materials for application in thin film solar cells, but the spontaneous surface defects disordering would lead to large open-circuit voltage deficit(V_(oc,deficit)) and significantly limit kesterite photovoltaics performance,primarily arising from the generated more recombination centers and insufficient p to n conversion at p-n junction. Herein, we establish a surface defects ordering structure in CZTSSe system via local substitution of Cu by Ag to suppress disordered Cu_(Zn) defects and generate benign n-type Zn_(Ag) donors. Taking advantage of the decreased annealing temperature of Ag F post deposition treatment(PDT), the high concentration of Ag incorporated into surface absorber facilitates the formation of surface ordered defect environment similar to that of efficient CIGS PV. The manipulation of highly doped surface structure could effectively reduce recombination centers, increase depletion region width and enlarge the band bending near p-n junction. As a result, the Ag F-PDT device finally achieves maximum efficiency of 12.34% with enhanced V_(oc) of 0.496 V. These results offer a new solution route in surface defects and energy-level engineering, and open the way to build up high quality p-n junction for future development of kesterite technology.展开更多
Layered P2–Na_(2/3)Ni_(1/3)Mn_(2/3)O_2 is a promising cathode material. It exhibits a high capacity and suitable operating voltage and undergoes a phase transition from P2 to O2 during charge/discharge.Researchers ha...Layered P2–Na_(2/3)Ni_(1/3)Mn_(2/3)O_2 is a promising cathode material. It exhibits a high capacity and suitable operating voltage and undergoes a phase transition from P2 to O2 during charge/discharge.Researchers have used Ti substitution to improve the cathode, yet the chemical principles that underpin elemental substitution and functional improvement remain unclear. To clarify these principles, we used in situ Raman spectroscopy to monitor chemical changes in P2–Na2/3 Ni1/3 Mn1/3 Ti1/3 O2 and P2–Na_(2/3)Ni_(1/3)Mn_(2/3)O_2 during charge/discharge. Based on the change in the A_(1g) and E_g peaks during charge/discharge, we concluded that Ti substitution compressed the transition metal layer and expanded the planar oxygen layer in the unit cell. Titanium stabilized the P2 phase structure, which improved the cycling stability of P2–NaNMT. Our results provide clear theoretical support for future research on modifying electrodes by elemental substitution.展开更多
The kesterite Cu2ZnSn(S,Se)4 (CZTSSe) solar cells have yielded a prospective conversion efficiency among all thin- film photovoltaic technology. However, its further development is still hindered by the lower open...The kesterite Cu2ZnSn(S,Se)4 (CZTSSe) solar cells have yielded a prospective conversion efficiency among all thin- film photovoltaic technology. However, its further development is still hindered by the lower open-circuit voltage (Voc), and the non-ideal bandgap of the absorber is an important factor affecting this issue. The substitution of Sn with Ge provides a unique ability to engineer the bandgap of the absorber film. Herein, a simple precursor solution approach was successfully developed to fabricate Cu2Zn(SnyGel_y)(SxSe~ x)4 (CZTGSSe) solar cells. By precisely adjusting the Ge content in a small range, the Voc and Jsc are enhanced simultaneously. Benefitting from the optimized bandgap and the maintained spike structure and light absorption, the 10% Ge/(Ge+Sn) content device with a bandgap of approximately 1.1 eV yields the highest efficiency of 9.36%. This further indicates that a precisely controlled Ge content could further improve the cell performance for efficient CZTGSSe solar cells.展开更多
The major histocompatibility complex (MHC) is a fundamental part of the immune system in nearly all vertebrates. DQA2 is a member of the MHC complex and an important candidate gene involved in susceptibility/resistanc...The major histocompatibility complex (MHC) is a fundamental part of the immune system in nearly all vertebrates. DQA2 is a member of the MHC complex and an important candidate gene involved in susceptibility/resistance to various diseases. Therefore, the present study aimed at investigating computationally molecular genetic variation of DQA2 gene of cattle, sheep and goats especially on its evolution and differentiation within and among species as well as the attendant effects of the polymorphism on the function of DQA2 gene. A total of thirty three DQA2 nucleotide sequences comprising cattle (10), sheep (12) and goats (11) were retrieved from the GenBank. Forty seven amino acid substitutions of the wild type alleles located in the putative peptide coding region of caprine DQA2 alleles were obtained from the alignment of deduced amino acid sequences of goats. Out of these, eleven amino acid substitutions (H14L, H14R, L34M, E35L, G56S, G56R, 161V, A62E, D69Q, T72N and T72G) were returned neutral;an indication that they did not impair protein function. The Expected Accuracy (EA) ranged from 53% - 87%. For sheep, sixteen amino acid substitutions (A11P, A11T, A11G, A11M, L14S, L14T, V27L, V27S, G35S, S46T, D55E, L57T, L57A, L57G, K65Q and V68I) appeared beneficial while the rest forty seven appeared harmful (EA ranged from 53% - 93%). Twenty four amino acid substitutions did not impair the function of protein while seventy seven substitutions appeared to have a negative effect on the function of protein of cattle (EA ranged from 53% - 94%). The phylogeny based on nucleotide and amino acid sequences of DQA2 gene revealed the close relatedness of the caprine, ovine and bovine species. The present knowledge would be relevant for performing further genotype-phenotype research as well as pharmacogenetics studies in order to show association between caprine, ovine and bovine DQA2 allelic variation and the clinical progression of infectious diseases especially in a developing country such as Nigeria.展开更多
A temperature stable Li2Zn0.95(SrxCa1-x)0.05Ti3O8(0≤x≤1)ceramics were fabricated using a conventional solid-state route sintered at 1100℃for 4 h.The XRD results indicate that the main phase Li2ZnTi3O8 and secondary...A temperature stable Li2Zn0.95(SrxCa1-x)0.05Ti3O8(0≤x≤1)ceramics were fabricated using a conventional solid-state route sintered at 1100℃for 4 h.The XRD results indicate that the main phase Li2ZnTi3O8 and secondary phase including SrxCa1-xTiO3(0≤x≤1)solid solution and TiO2 co-exist in composite and form a stable composite system when the(CaxSr1-x)(0≤x≤1)substitutes for Zn of Li2ZnTi3O8 ceramic.As x is increased from 0 to 1,the relative permittivity(εr)increases from 26.65 to 27.12,and the quality factor(Q×f)increases from 63300 to 66600 GHz.With the increased of x,the temperature coefficient of resonant frequency(τf)increases from 0.27 to 8.23 ppm/℃,and then decreases to 3.51 ppm/℃.On the whole,the Li2Zn0.95(SrxCa1-x)0.05Ti3O8(0≤x≤1)ceramics show excellent comprehensive properties of middleεr=25-27,higher Q×f≥60000 GHz andτf≤±8.5 ppm/℃.展开更多
Introduction The electrochemical reduction of O;was investigated widely during the past two decades. O;can react with various organic compounds. O;as a new synthesis reagent has been being explored.
Our previous research showed that aliphatic amines were put in order of high reactivity as “ethylamine > ammonia > t-butylamine > diethylamine” on the aromatic nucleophilic substitution of 1-dimetylamino-2,...Our previous research showed that aliphatic amines were put in order of high reactivity as “ethylamine > ammonia > t-butylamine > diethylamine” on the aromatic nucleophilic substitution of 1-dimetylamino-2,4-bis(trifluoroacetyl)-naphthalene 1 in acetonitrile. The DFT calculation study (B3LYP/6-31G* with solvation model) for the reactions of 1 with above four amines rationally explained the difference of each amines reactivity based on the energies of their Meisenheimer complexes 3 which are assumed to formed as the reaction intermediates in the course of the reaction giving the corresponding N-N exchange products 2. Intramolecular hydrogen bond between amino proton in 1-amino group and carbonyl oxygen in 2-trifluoroacetyl group stabilizes Meisenheimer complexes 3 effectively, and accelerates the substitution reaction from 1 to 2. Our calculation results also predicted that the above order of amines is also true if less polar toluene is used as a solvent instead of acetonitrile even though more enhanced conditions are required.展开更多
基金supported by the National Key Research and Development Program of China(2022YFD2300300)the National Natural Science Foundation of China(41907072)+1 种基金the Scientific Research Foundation of Zhejiang A&F University,China(2022LFR003)the Jiangsu Agriculture Science and Technology Innovation Fund,China(CX(21)3007).
文摘Water-saving irrigation strategies can successfully alleviate methane emissions from rice fields,but significantly stimulate nitrous oxide(N_(2)O)emissions because of variations in soil oxygen level and redox potential.However,the relationship linking soil N_(2)O emissions to nitrogen functional genes during various fertilization treatments in water-saving paddy fields has rarely been investigated.Furthermore,the mitigation potential of organic fertilizer substitution on N_(2)O emissions and the microbial mechanism in rice fields must be further elucidated.Our study examined how soil N_(2)O emissions were affected by related functional microorganisms(ammonia-oxidizing archaea(AOA),ammonia-oxidizing bacteria(AOB),nirS,nirK and nosZ)to various fertilization treatments in a rice field in southeast China over two years.In this study,three fertilization regimes were applied to rice cultivation:a no nitrogen(N)(Control),an inorganic N(Ni),and an inorganic N with partial N substitution with organic manure(N_(i)+N_(o)).Over two rice-growing seasons,cumulative N_(2)O emissions averaged 0.47,4.62 and 4.08 kg ha^(−1)for the Control,Ni and N_(i)+N_(o)treatments,respectively.In comparison to the Ni treatment,the N_(i)+N_(o)fertilization regime considerably reduced soil N_(2)O emissions by 11.6%while maintaining rice yield,with a lower N_(2)O emission factor(EF)from fertilizer N of 0.95%.Nitrogen fertilization considerably raised the AOB,nirS,nirK and nosZ gene abundances,in comparison to the Control treatment.Moreover,the substitution of organic manure for inorganic N fertilizer significantly decreased AOB and nirS gene abundances and increased nosZ gene abundance.The AOB responded to N fertilization more sensitively than the AOA.Total N_(2)O emissions significantly correlated positively with AOB and nirS gene abundances while having a negative correlation with nosZ gene abundance and the nosZ/nirS ratio across N-fertilized plots.In summary,we conclude that organic manure substitution for inorganic N fertilizer decreased soil N_(2)O emissions primarily by changing the soil NO_(3)^(−)-N,pH and DOC levels,thus inhibiting the activities of ammonia oxidation in nitrification and nitrite reduction in denitrification,and strengthening N_(2)O reduction in denitrification from water-saving rice paddies.
基金the National Natural Science Foundation of China (22209091)the Natural Science Foundation of Shandong Province (ZR2020QB057)+1 种基金the Key Program of National Natural Science Foundation of China (22133006)the Yankuang Group 2019 Science and Technology Program (YKKJ2019AJ05JG-R60)。
文摘It is a challenge to coordinate carrier-kinetics performance and the redox capacity of photogenerated charges synchronously at the atomic level for boosting photocatalytic activity.Herein,the atomic Ni was introduced into the lattice of hexagonal ZnIn_(2)S_(4) nanosheets(Ni/ZnIn_(2)S_(4))via directionalsubstituting Zn atom with the facile hydrothermal method.The electronic structure calculations indicate that the introduction of Ni atom effectively extracts more electrons and acts as active site for subsequent reduction reaction.Besides the optimized light absorption range,the elevation of Efand ECBendows Ni/ZnIn_(2)S_(4) photocatalyst with the increased electron concentration and the enhanced reduction ability for surface reaction.Moreover,ultrafast transient absorption spectroscopy,as well as a series of electrochemical tests,demonstrates that Ni/ZnIn_(2)S_(4) possesses 2.15 times longer lifetime of the excited charge carriers and an order of magnitude increase for carrier mobility and separation efficiency compared with pristine ZnIn_(2)S_(4).These efficient kinetics performances of charge carriers and enhanced redox capacity synergistically boost photocatalytic activity,in which a 3-times higher conversion efficiency of nitrobenzene reduction was achieved upon Ni/ZnIn_(2)S_(4).Our study not only provides in-depth insights into the effect of atomic directional-substitution on the kinetic behavior of photogenerated charges,but also opens an avenue to the synchronous optimization of redox capacity and carrier-kinetics performance for efficient solar energy conversion.
基金Project(2007CB613607) supported by the National Basic Research Program of ChinaProjects(2009FJ1002, 2009CK3062) supported by the Science and Technology Program of Hunan Province, China
文摘Na-doped Li1.05Mn2O4 cathodes were synthesized using a sol-gel process.The samples were characterized by X-ray diffractometry(XRD),cyclic voltammetry(CV),electrochemical impedance spectroscopy(EIS)and charge-discharge measurements. The results show that all the samples exhibit the same cubic spinel phase structure without impurity.The lattice constant and unit cell volume decrease with increasing the sodium dopant amount.As the molar ratio of sodium to manganese(x=n(Na)/n(Mn))increases from 0 to 0.03,the initial discharge capacity of the Li1.05Mn2O4 cathodes decreases from 119.2 to 107.9 mA·h/g,and the discharge capability at large current rate and the storage performance decline dramatically,while cycling performance at room temperature and 55℃are improved.The CV and EIS studies indicate that reversibility of Li1.05Mn2O4 cathodes decreases and the electrochemical impedance increases with increasing the sodium dopant amount.
基金the support from CNPC Innovation Found(2021DQ02-1001)Liao Ning Revitalization Talents Program(XLYC1907144)Xinghai Talent Cultivation Plan(X20200303)。
文摘MXene-based materials have gained considerable attention for lithium-sulfur(Li-S)batteries cathode materials due to their superior electric conductivity and high affinitive to polysulfides.However,there are still challenges in modifying the surface functional groups of MXene to further improve the electrochemical performance and increase the structure variety for MXene-based sulfur host.Herein,we report an efficient and flexible nucleophilic substitution(S_(N))strategy to modify the Ti_(3)C_(2)T_(x) surface terminations and purposefully designed Magnolol-modified Ti_(3)C_(2)T_(x)(M-Ti_(3)C_(2)T_(x))as powerful cathode host materials.Benefiting from more C-Ti-O bonds forming and diallyl groups terminations reducing after the dehalogenation and nucleophilic addition reactions,the given M-Ti_(3)C_(2)T_(x) electrode could effectively suppress the lithium polysulfides shuttling via chemisorption and C—S covalent bond formation.Besides,the Magnolol-modified Ti_(3)C_(2)T_(x) significantly accelerates polysulfide redox reaction and reduces the activation energy of Li_(2) S decomposition.As a result,the as-prepared M-Ti_(3)C_(2)T_(x) electrode displays an excellent rate capability and a high reversible capacity of 7.68 mAh cm^(-2)even under 7.2 mg cm^(-2)S-loaded with a low decay rate of 0.07%(from 2 nd cycle).This flexible surface-modified strategy for MXene terminations is expected to be extended to other diverse MXene applications.
基金the financial support from the National Natural Science Foundation of China, China (22005207, 52261160384)the Guangdong Basic and Applied Basic Research Foundation, Guangdong Province, China (2019A1515011819)+2 种基金the Outstanding Youth Basic Research Project of Shenzhen, Shenzhen, China (RCYX20221008092934093)the Joint Funds of the National Natural Science Foundation of China, China (U22A20140)the Science and Technology Development Fund, Macao SAR (0090/2021/A2 and 0049/2021/AGJ)
文摘Magnesium ion batteries(MIBs)are a potential field for the energy storage of the future but are restricted by insufficient rate capability and rapid capacity degradation.Magnesium-sodium hybrid ion batteries(MSHBs)are an effective way to address these problems.Here,we report a new type of MSHBs that use layered sodium vanadate((Na,Mn)V_(8)O_(20)·5H_(2)O,Mn-NVO)cathodes coupled with an organic 3,4,9,10-perylenetetracarboxylic diimide(PTCDI)anode in Mg^(2+)/Na^(+)hybrid electrolytes.During electrochemical cycling,Mg^(2+)and Na^(+)co-participate in the cathode reactions,and the introduction of Na^(+)promotes the structural stability of the Mn-NVO cathode,as cleared by several ex-situ characterizations.Consequently,the Mn-NVO cathode presents great specific capacity(249.9 mA h g^(−1)at 300 mA g^(−1))and cycling(1500 cycles at 1500 mA g^(−1))in the Mg^(2+)/Na^(+)hybrid electrolytes.Besides,full battery displays long lifespan with 10,000 cycles at 1000 mA g^(−1).The rate performance and cycling stability of MSHBs have been improved by an economical and scalable method,and the mechanism for these improvements is discussed.
基金the National Natural Science Foundation of China (20571019)Scientific Research Foundation for the Returned Overseas Chinese Scholars, Heilongjiang (LC06C130)Program of Harbin Subject Chief Scientist
文摘Polycrystalline particles of Ca3-xErxCo2O6 (x=0.0, 0.15, 0.3, 0.45 and 0.6) were synthesized using sol-gel method combined with Low Temperature Sintering procedure (LTS) to evaluate the effect of Er substitution on the thermoelectric properties of Ca3Co2O6. The crystal structure and microstructure were investigated using X-ray diffraction, infrared spectroscopy and scanning electron microscope. The electrical conductivity and Seebeck coefficient of the complex oxides were measured from 300 to 1073 K. The results showed that all the sampies were p-type semiconductors. The electrical conductivity increased with the increase in temperature. Er substitutions at Ca site affected carrier concentrations and carder mobility, resulting an increase in Seebeck coefficient and decrease in electrical conductivity. The power factor of Ca2.85Er0.15Co2O6 reached 10.66 μw/mK^2 at 1073 K.
基金supported by the National Natural Science Foundation of China(61874159,62074052,61974173,52072327,51702085 and 51802081)the Joint Talent Cultivation Funds of NSFC-HN(U1704151 and U1904192)+1 种基金the Zhongyuan Thousand Talents(Zhongyuan Scholars)Program of Henan Province(202101510004)the Science and Technology Innovation Talents in Universities of Henan Province(21HASTIT023)。
文摘The environmentally friendly Cu_(2)ZnSn(S,Se)_(4)(CZTSSe) compounds are promising direct bandgap materials for application in thin film solar cells, but the spontaneous surface defects disordering would lead to large open-circuit voltage deficit(V_(oc,deficit)) and significantly limit kesterite photovoltaics performance,primarily arising from the generated more recombination centers and insufficient p to n conversion at p-n junction. Herein, we establish a surface defects ordering structure in CZTSSe system via local substitution of Cu by Ag to suppress disordered Cu_(Zn) defects and generate benign n-type Zn_(Ag) donors. Taking advantage of the decreased annealing temperature of Ag F post deposition treatment(PDT), the high concentration of Ag incorporated into surface absorber facilitates the formation of surface ordered defect environment similar to that of efficient CIGS PV. The manipulation of highly doped surface structure could effectively reduce recombination centers, increase depletion region width and enlarge the band bending near p-n junction. As a result, the Ag F-PDT device finally achieves maximum efficiency of 12.34% with enhanced V_(oc) of 0.496 V. These results offer a new solution route in surface defects and energy-level engineering, and open the way to build up high quality p-n junction for future development of kesterite technology.
基金supported by the NSFC (21905239, 21925404, and 21775127)the Natural Science Foundation of Shanxi Province of China (201901D211265)the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi (2019L0609)。
文摘Layered P2–Na_(2/3)Ni_(1/3)Mn_(2/3)O_2 is a promising cathode material. It exhibits a high capacity and suitable operating voltage and undergoes a phase transition from P2 to O2 during charge/discharge.Researchers have used Ti substitution to improve the cathode, yet the chemical principles that underpin elemental substitution and functional improvement remain unclear. To clarify these principles, we used in situ Raman spectroscopy to monitor chemical changes in P2–Na2/3 Ni1/3 Mn1/3 Ti1/3 O2 and P2–Na_(2/3)Ni_(1/3)Mn_(2/3)O_2 during charge/discharge. Based on the change in the A_(1g) and E_g peaks during charge/discharge, we concluded that Ti substitution compressed the transition metal layer and expanded the planar oxygen layer in the unit cell. Titanium stabilized the P2 phase structure, which improved the cycling stability of P2–NaNMT. Our results provide clear theoretical support for future research on modifying electrodes by elemental substitution.
基金Project supported by the Joint Talent Cultivation Funds of NSFC-HN(Grant No.U1604138)the National Natural Science Foundation of China(Grant Nos.21603058 and 51702085)+2 种基金the Innovation Research Team of Science and Technology in Henan Province,China(Grant No.17IRTSTHN028)the Science and Technology Innovation Talents in Universities of Henan Province,China(Grant No.18HASTIT016)the Young Key Teacher Foundation of Universities of Henan Province,China(Grant No.2015GGJS-022)
文摘The kesterite Cu2ZnSn(S,Se)4 (CZTSSe) solar cells have yielded a prospective conversion efficiency among all thin- film photovoltaic technology. However, its further development is still hindered by the lower open-circuit voltage (Voc), and the non-ideal bandgap of the absorber is an important factor affecting this issue. The substitution of Sn with Ge provides a unique ability to engineer the bandgap of the absorber film. Herein, a simple precursor solution approach was successfully developed to fabricate Cu2Zn(SnyGel_y)(SxSe~ x)4 (CZTGSSe) solar cells. By precisely adjusting the Ge content in a small range, the Voc and Jsc are enhanced simultaneously. Benefitting from the optimized bandgap and the maintained spike structure and light absorption, the 10% Ge/(Ge+Sn) content device with a bandgap of approximately 1.1 eV yields the highest efficiency of 9.36%. This further indicates that a precisely controlled Ge content could further improve the cell performance for efficient CZTGSSe solar cells.
文摘The major histocompatibility complex (MHC) is a fundamental part of the immune system in nearly all vertebrates. DQA2 is a member of the MHC complex and an important candidate gene involved in susceptibility/resistance to various diseases. Therefore, the present study aimed at investigating computationally molecular genetic variation of DQA2 gene of cattle, sheep and goats especially on its evolution and differentiation within and among species as well as the attendant effects of the polymorphism on the function of DQA2 gene. A total of thirty three DQA2 nucleotide sequences comprising cattle (10), sheep (12) and goats (11) were retrieved from the GenBank. Forty seven amino acid substitutions of the wild type alleles located in the putative peptide coding region of caprine DQA2 alleles were obtained from the alignment of deduced amino acid sequences of goats. Out of these, eleven amino acid substitutions (H14L, H14R, L34M, E35L, G56S, G56R, 161V, A62E, D69Q, T72N and T72G) were returned neutral;an indication that they did not impair protein function. The Expected Accuracy (EA) ranged from 53% - 87%. For sheep, sixteen amino acid substitutions (A11P, A11T, A11G, A11M, L14S, L14T, V27L, V27S, G35S, S46T, D55E, L57T, L57A, L57G, K65Q and V68I) appeared beneficial while the rest forty seven appeared harmful (EA ranged from 53% - 93%). Twenty four amino acid substitutions did not impair the function of protein while seventy seven substitutions appeared to have a negative effect on the function of protein of cattle (EA ranged from 53% - 94%). The phylogeny based on nucleotide and amino acid sequences of DQA2 gene revealed the close relatedness of the caprine, ovine and bovine species. The present knowledge would be relevant for performing further genotype-phenotype research as well as pharmacogenetics studies in order to show association between caprine, ovine and bovine DQA2 allelic variation and the clinical progression of infectious diseases especially in a developing country such as Nigeria.
基金Funded by the Open Project Program of Key Laboratory of Inorganic Functional Materials and Devices,Chinese Academy of Sciences(No.KLIFMD201606)the Open Fund of National Innovation Platform(No.2017YJ163)+1 种基金the National Natural Science Foundation of China(Nos.51502220,51521001,and 51672197)the Open Foundation of Hubei Key Laboratory of Theory and Application of Advanced Materials Mechanics(Wuhan University of Technology)(No.TAM201802)。
文摘A temperature stable Li2Zn0.95(SrxCa1-x)0.05Ti3O8(0≤x≤1)ceramics were fabricated using a conventional solid-state route sintered at 1100℃for 4 h.The XRD results indicate that the main phase Li2ZnTi3O8 and secondary phase including SrxCa1-xTiO3(0≤x≤1)solid solution and TiO2 co-exist in composite and form a stable composite system when the(CaxSr1-x)(0≤x≤1)substitutes for Zn of Li2ZnTi3O8 ceramic.As x is increased from 0 to 1,the relative permittivity(εr)increases from 26.65 to 27.12,and the quality factor(Q×f)increases from 63300 to 66600 GHz.With the increased of x,the temperature coefficient of resonant frequency(τf)increases from 0.27 to 8.23 ppm/℃,and then decreases to 3.51 ppm/℃.On the whole,the Li2Zn0.95(SrxCa1-x)0.05Ti3O8(0≤x≤1)ceramics show excellent comprehensive properties of middleεr=25-27,higher Q×f≥60000 GHz andτf≤±8.5 ppm/℃.
基金Supported by the National Natural Science Foundation of China
文摘Introduction The electrochemical reduction of O;was investigated widely during the past two decades. O;can react with various organic compounds. O;as a new synthesis reagent has been being explored.
文摘Our previous research showed that aliphatic amines were put in order of high reactivity as “ethylamine > ammonia > t-butylamine > diethylamine” on the aromatic nucleophilic substitution of 1-dimetylamino-2,4-bis(trifluoroacetyl)-naphthalene 1 in acetonitrile. The DFT calculation study (B3LYP/6-31G* with solvation model) for the reactions of 1 with above four amines rationally explained the difference of each amines reactivity based on the energies of their Meisenheimer complexes 3 which are assumed to formed as the reaction intermediates in the course of the reaction giving the corresponding N-N exchange products 2. Intramolecular hydrogen bond between amino proton in 1-amino group and carbonyl oxygen in 2-trifluoroacetyl group stabilizes Meisenheimer complexes 3 effectively, and accelerates the substitution reaction from 1 to 2. Our calculation results also predicted that the above order of amines is also true if less polar toluene is used as a solvent instead of acetonitrile even though more enhanced conditions are required.