Understanding how nitrogen(N) availability interacts with soil acidity and phosphorus(P) availability to affect soil-atmosphere exchanges in CO_2, CH_4 and N_2O in forest ecosystems is important for understanding ...Understanding how nitrogen(N) availability interacts with soil acidity and phosphorus(P) availability to affect soil-atmosphere exchanges in CO_2, CH_4 and N_2O in forest ecosystems is important for understanding the mechanisms driving ecosystem responses to enhanced N deposition. Here, we conducted an experiment with N, P and acid(H) addition in a mixed forest in subtropical China to investigate how acid and P addition affects CO_2, CH_4 and N_2O exchange under N addition. Our results showed that soil NH4^+-N and NO3^--N increased after N addition, but CO_2 emissions in N addition plots remained unaffected. CH_4 uptake in N–, P–, NP–, NH– and NPH–addition plots were reduced by 21.1%, 15.7%, 39.1%, 26.6%, and 28.4%, respectively. CH_4 uptake in NP–addition plots were lower compared to N–addition and P–addition plots, indicating that N and P addition had an additive effect on inhibiting CH_4 uptake. N_2O emission in N–, NP–, NH– and NPH–addition plots increased by 158.6%, 176.0%, 117.2%, and 91.8%, respectively. N_2O emissions in NPH–addition plots were lower compared to NP–addition plots while showed no difference between N–addition and NH–addition plots. This suggests that only under P rich conditions, acid addition would greatly mitigate N_2O emissions under N addition. Our results demonstrate that for N and P co-limited forest ecosystems with acidic soils, low P availability constrains the inhibition of soil CH_4 uptake by N deposition. When P availability is low, a weak soil acidation induced by N deposition may have less influence on the stimulation of N_2O emissions by N deposition.展开更多
Mg-air batteries have attracted tremendous attention as a potential next-generation power source for portable electronics and e-transportation due to their remarkable high theoretical volumetric energy density,environ...Mg-air batteries have attracted tremendous attention as a potential next-generation power source for portable electronics and e-transportation due to their remarkable high theoretical volumetric energy density,environmental sustainability,and cost-effectiveness.However,the fast hydrogen evolution reaction(HER)in NaCl-based aqueous electrolytes impairs the performance of Mg-air batteries and leads to poor specific capacity,low energy density,and low utilization.Thus,the conventionally used NaCl solute was proposed to be replaced by NaNO_(3)and acetic acid additive as a corrosion inhibitor,therefore an electrolyte engineering for long-life time Mg-air batteries is reported.The resulting Mg-air batteries based on this optimized electrolyte demonstrate an improved discharge voltage reaching~1.8 V for initial 5 h at a current density of 0.5 mA/cm^(2) and significantly prolonged cells'operational lifetime to over 360 h,in contrast to only~17 h observed in NaCl electrolyte.X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry were employed to analyse the composition of surface film and scanning electron microscopy combined with transmission electron microscopy to clarify the morphology changes of the surface layer as a function of acetic acid addition.The thorough studies of chemical composition and morphology of corrosion products have allowed us to elucidate the working mechanism of Mg anode in this optimized electrolyte for Mg-air batteries.展开更多
Zinc-ion batteries are promising for large-scale electrochemical energy storage systems,which still suffer from interfacial issues,e.g.,hydrogen evolution side reaction(HER),self-corrosion,and uncontrollable dendritic...Zinc-ion batteries are promising for large-scale electrochemical energy storage systems,which still suffer from interfacial issues,e.g.,hydrogen evolution side reaction(HER),self-corrosion,and uncontrollable dendritic Zn electrodeposition.Although the regulation of electric double layer(EDL)has been verified for interfacial issues,the principle to select the additive as the regulator is still misted.Here,several typical amino acids with different characteristics were examined to reveal the interfacial behaviors in regulated EDL on the Zn anode.Negative charged acidic polarity(NCAP)has been unveiled as the guideline for selecting additive to reconstruct EDL with an inner zincophilic H_(2)O-poor layer and to replace H_(2)O molecules of hydrated Zn^(2+)with NCAP glutamate.Taking the synergistic effects of EDL regulation,the uncontrollable interface is significantly stabilized from the suppressed HER and anti-self-corrosion with uniform electrodeposition.Consequently,by adding NCAP glutamate,a high average Coulombic efficiency of 99.83%of Zn metal is achieved in Zn|Cu asymmetrical cell for over 2000 cycles,and NH4V4O10|Zn full cell exhibits a high-capacity retention of 82.1%after 3000 cycles at 2 A g^(-1).Recapitulating,the NCAP principle posted here can quicken the design of trailblazing electrolyte additives for aqueous Zn-based electrochemical energy storage systems.展开更多
Recent reports have demonstrated that the new commercially available immobilized-type chiral stationary phases(CSPs) containing amylose tris(3-chloro-5-methylphenylcarbamate)(ACMPC) as a selector exhibit not onl...Recent reports have demonstrated that the new commercially available immobilized-type chiral stationary phases(CSPs) containing amylose tris(3-chloro-5-methylphenylcarbamate)(ACMPC) as a selector exhibit not only an exceptionally high enantioselectivity in high-performance liquid chromatography(HPLC) but they are also applicable to a wide range of chiral analytes. Herein, we report the results obtained in the HPLC analysis of omeprazole and its impurities B and E on the ACMPC-based Chiralpak IG-3 CSP(CSP) under polar organic conditions. A systematic evaluation of the retention characteristics of the selected benzimidazole chiral probes was carried out by changing the composition of the mobile phase and the column temperature. It is worth emphasizing that the high affinity of both enantiomers of all analytes recorded in pure methanol mode dramatically decreased incorporating small volumes of either basic or acid additives in the mobile phase. Unspecified sites of the IG-3 CSP presumably involved in strong and non-stereoselective H-bonding contacts with chiral analytes are assumed responsible for the unproductive retention process.展开更多
The β-aminocarboxylic acid derivatives were synthesized by Michael addition reaction of alkyl amine and α,β-unsaturated carbonyl compounds in the presence of potassium fluoride on alumina.
Various acidic components(MOx:phosphate,sulfate,tungstate and niobate) were loaded on Ce0.75 Zr0.25 O2 powders by an impregnation method.The as-prepared catalysts were hydrothermally treated at 760 oC for 48 h in a...Various acidic components(MOx:phosphate,sulfate,tungstate and niobate) were loaded on Ce0.75 Zr0.25 O2 powders by an impregnation method.The as-prepared catalysts were hydrothermally treated at 760 oC for 48 h in air containing 10 vol.% H2 O to obtain the aged catalysts.The catalysts were characterized by X-ray diffraction,Fourier transform infrared spectroscopy,H2 programmed-reduction,NH3 adsorption and deNOx activity measurements.The results showed that,among the catalysts investigated,the phosphated Ce0.75 Zr0.25 O2 catalyst showed the highest hydrothermal stability.The remained high acidity of the phosphated catalyst with moderate redox property helped to maintain the excellent NH3-SCR activity of hydrothermally aged catalyst.Cerium tungstate led to the poor redox property of the tungstated catalyst although the acidity of catalyst was still high.The decomposition of sulfates at temperatures higher than 600 °C restrained the usage of sulfated catalysts in high temperature conditions.The overall dehydration of niobate to niobium oxides led to the low acidity of hydrothermally aged Nb2 O5-Ce0.75 Zr0.25 O2 catalyst.展开更多
基金Natural Sciences Foundation of China(No.31290221)
文摘Understanding how nitrogen(N) availability interacts with soil acidity and phosphorus(P) availability to affect soil-atmosphere exchanges in CO_2, CH_4 and N_2O in forest ecosystems is important for understanding the mechanisms driving ecosystem responses to enhanced N deposition. Here, we conducted an experiment with N, P and acid(H) addition in a mixed forest in subtropical China to investigate how acid and P addition affects CO_2, CH_4 and N_2O exchange under N addition. Our results showed that soil NH4^+-N and NO3^--N increased after N addition, but CO_2 emissions in N addition plots remained unaffected. CH_4 uptake in N–, P–, NP–, NH– and NPH–addition plots were reduced by 21.1%, 15.7%, 39.1%, 26.6%, and 28.4%, respectively. CH_4 uptake in NP–addition plots were lower compared to N–addition and P–addition plots, indicating that N and P addition had an additive effect on inhibiting CH_4 uptake. N_2O emission in N–, NP–, NH– and NPH–addition plots increased by 158.6%, 176.0%, 117.2%, and 91.8%, respectively. N_2O emissions in NPH–addition plots were lower compared to NP–addition plots while showed no difference between N–addition and NH–addition plots. This suggests that only under P rich conditions, acid addition would greatly mitigate N_2O emissions under N addition. Our results demonstrate that for N and P co-limited forest ecosystems with acidic soils, low P availability constrains the inhibition of soil CH_4 uptake by N deposition. When P availability is low, a weak soil acidation induced by N deposition may have less influence on the stimulation of N_2O emissions by N deposition.
基金the China Scholarship Council(CSC)for funding(no.201806310116)。
文摘Mg-air batteries have attracted tremendous attention as a potential next-generation power source for portable electronics and e-transportation due to their remarkable high theoretical volumetric energy density,environmental sustainability,and cost-effectiveness.However,the fast hydrogen evolution reaction(HER)in NaCl-based aqueous electrolytes impairs the performance of Mg-air batteries and leads to poor specific capacity,low energy density,and low utilization.Thus,the conventionally used NaCl solute was proposed to be replaced by NaNO_(3)and acetic acid additive as a corrosion inhibitor,therefore an electrolyte engineering for long-life time Mg-air batteries is reported.The resulting Mg-air batteries based on this optimized electrolyte demonstrate an improved discharge voltage reaching~1.8 V for initial 5 h at a current density of 0.5 mA/cm^(2) and significantly prolonged cells'operational lifetime to over 360 h,in contrast to only~17 h observed in NaCl electrolyte.X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry were employed to analyse the composition of surface film and scanning electron microscopy combined with transmission electron microscopy to clarify the morphology changes of the surface layer as a function of acetic acid addition.The thorough studies of chemical composition and morphology of corrosion products have allowed us to elucidate the working mechanism of Mg anode in this optimized electrolyte for Mg-air batteries.
基金funded by the National Natural Science Foundation of China(U21B2057,12102328,and 52372252)the Newly Introduced Scientific Research Start-up Funds for Hightech Talents(DD11409024).
文摘Zinc-ion batteries are promising for large-scale electrochemical energy storage systems,which still suffer from interfacial issues,e.g.,hydrogen evolution side reaction(HER),self-corrosion,and uncontrollable dendritic Zn electrodeposition.Although the regulation of electric double layer(EDL)has been verified for interfacial issues,the principle to select the additive as the regulator is still misted.Here,several typical amino acids with different characteristics were examined to reveal the interfacial behaviors in regulated EDL on the Zn anode.Negative charged acidic polarity(NCAP)has been unveiled as the guideline for selecting additive to reconstruct EDL with an inner zincophilic H_(2)O-poor layer and to replace H_(2)O molecules of hydrated Zn^(2+)with NCAP glutamate.Taking the synergistic effects of EDL regulation,the uncontrollable interface is significantly stabilized from the suppressed HER and anti-self-corrosion with uniform electrodeposition.Consequently,by adding NCAP glutamate,a high average Coulombic efficiency of 99.83%of Zn metal is achieved in Zn|Cu asymmetrical cell for over 2000 cycles,and NH4V4O10|Zn full cell exhibits a high-capacity retention of 82.1%after 3000 cycles at 2 A g^(-1).Recapitulating,the NCAP principle posted here can quicken the design of trailblazing electrolyte additives for aqueous Zn-based electrochemical energy storage systems.
基金funding from the European Community's Seventh Framework Programme under the grant agreement 602051 (Project HERACLES: Humancystic Echinococcosis Rese Arch in Centra L and Eastern Societies http://www.Heracles-fp7.eu/)
文摘Recent reports have demonstrated that the new commercially available immobilized-type chiral stationary phases(CSPs) containing amylose tris(3-chloro-5-methylphenylcarbamate)(ACMPC) as a selector exhibit not only an exceptionally high enantioselectivity in high-performance liquid chromatography(HPLC) but they are also applicable to a wide range of chiral analytes. Herein, we report the results obtained in the HPLC analysis of omeprazole and its impurities B and E on the ACMPC-based Chiralpak IG-3 CSP(CSP) under polar organic conditions. A systematic evaluation of the retention characteristics of the selected benzimidazole chiral probes was carried out by changing the composition of the mobile phase and the column temperature. It is worth emphasizing that the high affinity of both enantiomers of all analytes recorded in pure methanol mode dramatically decreased incorporating small volumes of either basic or acid additives in the mobile phase. Unspecified sites of the IG-3 CSP presumably involved in strong and non-stereoselective H-bonding contacts with chiral analytes are assumed responsible for the unproductive retention process.
文摘The β-aminocarboxylic acid derivatives were synthesized by Michael addition reaction of alkyl amine and α,β-unsaturated carbonyl compounds in the presence of potassium fluoride on alumina.
基金supported by National Natural Science Foundation of China(51202126)Strategic Emerging Industry Development Funds of Shenzhen(JCYJ20120619152738634)
文摘Various acidic components(MOx:phosphate,sulfate,tungstate and niobate) were loaded on Ce0.75 Zr0.25 O2 powders by an impregnation method.The as-prepared catalysts were hydrothermally treated at 760 oC for 48 h in air containing 10 vol.% H2 O to obtain the aged catalysts.The catalysts were characterized by X-ray diffraction,Fourier transform infrared spectroscopy,H2 programmed-reduction,NH3 adsorption and deNOx activity measurements.The results showed that,among the catalysts investigated,the phosphated Ce0.75 Zr0.25 O2 catalyst showed the highest hydrothermal stability.The remained high acidity of the phosphated catalyst with moderate redox property helped to maintain the excellent NH3-SCR activity of hydrothermally aged catalyst.Cerium tungstate led to the poor redox property of the tungstated catalyst although the acidity of catalyst was still high.The decomposition of sulfates at temperatures higher than 600 °C restrained the usage of sulfated catalysts in high temperature conditions.The overall dehydration of niobate to niobium oxides led to the low acidity of hydrothermally aged Nb2 O5-Ce0.75 Zr0.25 O2 catalyst.