Using Object-oriented design and a new programming language JAVA, a physically-based model was built to simulate the hydrological, alkalization/de-alkalization and salinization/desalinization processes in soil. Furthe...Using Object-oriented design and a new programming language JAVA, a physically-based model was built to simulate the hydrological, alkalization/de-alkalization and salinization/desalinization processes in soil. Furthermore, a process-based model was built to evaluate the dynamics of four herbaceous ecosystems (including dynamics of above-ground biomass, below-ground biomass, and litter biomass), each dominated by Aneurolepidium chinense (Trin.) Kitag., Chloris virgata Sw., Puccinellia tenuiflora (Turcz.) Scribn. et Merr. and Suaeda glauca Bunge. This model is a daily-time step model, suitable for simulating hydrological, alkalization/de-alkalization and salinization/desalinization processes of heterogeneous soil, and growth dynamics of different grassland communities. With climatic data and experimental data of Changling Experimental Site in Jilin Province, the soil moisture content (in 1991, 1996, 1997 and 1998), soil salt concentration, exchangeable cation percentage and pH in soil and growth dynamics of these four sorts of grassland communities (in 1991) were simulated and the results were verified to be in accord with observed data.展开更多
Ethanol conversion to high-value-added products has attracted considerable attention in both academic research and industrial fields.In this study,we synthesized a series of tunable acid–base bifunctional Zn-Zr-Al me...Ethanol conversion to high-value-added products has attracted considerable attention in both academic research and industrial fields.In this study,we synthesized a series of tunable acid–base bifunctional Zn-Zr-Al metal oxides(represented as Zn2ZrxAl-MMO)in light of the structural topotactic transformation of Zn2ZrxAl-hydrotalcite precursors(Zn2ZrxAl-LDH).The resulting Zn2ZrxAl-MMO catalysts were employed in the conversion of ethanol to diethyl carbonate.The Zr^4+ ion content of the LDH precursor plays a key role in modulating the acid-base properties and determining catalytic performance:the Zn2Zr0.1Al-MMO sample exhibits the optimal catalytic behavior with a diethyl carbonate(DEC)yield of 42.1%,which is the highest reported for metal oxide catalysts.Structure-property correlation investigations revealed that the synergic catalysis between medium-strong basic sites and weak acid sites plays a predominant role in the catalytic behavior.Furthermore,in situ Fourier transform infrared measurements showed that the weak acidic site promotes activation adsorption of the reactant(urea)and the intermediate product(ethyl carbamate),while the medium-strong basic site accelerates ethanol activation.Moreover,the Zn2Zr0.1Al-MMO catalyst has the advantages of cost effectiveness,good stability,and reusability.Therefore,the acid-base bifunctional catalysts developed in this work can be employed as promising candidates in acid-base catalytic reactions such as ethanol conversion.展开更多
Acid-catalyzed dehydration of alcohols has been widely employed for the synthesis of alkenes. However, activated alcohols when employed as substrates in dehydration reactions are often pla-gued by the lack of alkene s...Acid-catalyzed dehydration of alcohols has been widely employed for the synthesis of alkenes. However, activated alcohols when employed as substrates in dehydration reactions are often pla-gued by the lack of alkene selectivity. In this work, the reaction system can be significantly improved through enhancing the performance of Lewis acid catalysts in the dehydration of activated alcohols by combining with a Lewis base. Observations of the reaction mechanism revealed that the Lewis base component might have changed the reaction rate order. Although both the principal and side reaction rates decreased, the effect was markedly more observed on the latter reaction. Therefore, the selectivity of the dehydration reaction was improved. On the basis of this observation, a new route to synthesize 2-cinnamyl-1,3-dicarbonyl compounds was developed by using 2-aryl-3,4- di-hydropyran as a starting substrate in the presence of a Lewis acid/Lewis base combined catalyst system.展开更多
Efficient,stable,and noble‐metal‐free electrocatalysts for both the oxygen evolution reaction and the hydrogen evolution reaction are highly imperative for the realization of low‐cost commercial water‐splitting el...Efficient,stable,and noble‐metal‐free electrocatalysts for both the oxygen evolution reaction and the hydrogen evolution reaction are highly imperative for the realization of low‐cost commercial water‐splitting electrolyzers.Herein,a cost‐effective and ecofriendly strategy is reported to fabricate coral‐like FeNi(OH)x/Ni as a bifunctional electrocatalyst for overall water splitting in alkaline media.With the assistance of mild corrosion of Ni by Fe(NO3)3,in situ generated FeNi(OH)x nanosheets are intimately attached on metallic coral‐like Ni.Integration of these nanosheets with the electrodeposited coral‐like Ni skeleton and the supermacroporous Ni foam substrate forms a binder‐free hierarchical electrode,which is beneficial for exposing catalytic active sites,accelerating mass transport,and facilitating the release of gaseous species.In 1.0 mol L^-1 KOH solution,a symmetric electrolyzer constructed with FeNi(OH)x/Ni as both the anode and the cathode exhibits an excellent activity with an applied potential difference of 1.52 V at 10 mA cm^-2,which is superior to that of an asymmetric electrolyzer constructed with the state‐of‐the‐art RuO2‐PtC couple(applied potential difference of 1.55 V at 10 mA cm^-2).This work contributes a facile and reliable strategy for manufacturing affordable,practical,and promising water‐splitting devices.展开更多
Supercritical water has been focused on as an environmentally attractive reaction media, in which organic materials can be decomposed into smaller molecules. The reaction behavior of pyrrole as a simple model compound...Supercritical water has been focused on as an environmentally attractive reaction media, in which organic materials can be decomposed into smaller molecules. The reaction behavior of pyrrole as a simple model compound of nonbasic nitrogen compounds found in petroleum residua was studied in supercritical water with a batch type reactor. The reaction was carried out at temperatures of 698-748 K and at various pressures under an argon atmosphere. The chemical species in the aqueous products were identified by GCMS （gas chromatography mass spectrometry） and quantified using GC-FID （gas chromatography flame ionization detector）. The effect of temperature and reaction time on the conversion process of pyrrole is presented. Under supercritical water conditions, pyrrole underwent successful decomposition in water into its derived compounds. The conversion of pyrrole could approach 81.12 wt% at 723 K and 40 MPa within 240 min of reaction time. The decomposition process was accelerated with the existence of water at the same temperature. Ultimate analysis of solid products was also conducted using a CHN analyzer. The process investigated in this study may form the basis for an efficient method of nitrogen compound decomposition in future.展开更多
Electrochemical oxidation of 5-hydroxymethylfurfural(HMF)has shown promising prospects in producing highly valuable chemicals.Herein,we report the synthesis of ultrasmall Ag nanoclusters anchored on NiColayered double...Electrochemical oxidation of 5-hydroxymethylfurfural(HMF)has shown promising prospects in producing highly valuable chemicals.Herein,we report the synthesis of ultrasmall Ag nanoclusters anchored on NiColayered double hydroxide(NiCo-LDH)nanosheet arrays(Agn@NiCo-LDH)via a facile electrodeposition strategy.The prepared Agn@NiCo-LDH nanosheet arrays exhibit excellent electrocatalytic HMF oxidation performance with a current density of 10 mA cm^(−2) at 1.29 VRHE and the Faraday efficiency of nearly 100%for 2,5-furandicarboxylic acid production.This study offers an effective approach to rationally design nanoclusters to achieve high catalytic activity for sustainable energy conversion and production.展开更多
文摘Using Object-oriented design and a new programming language JAVA, a physically-based model was built to simulate the hydrological, alkalization/de-alkalization and salinization/desalinization processes in soil. Furthermore, a process-based model was built to evaluate the dynamics of four herbaceous ecosystems (including dynamics of above-ground biomass, below-ground biomass, and litter biomass), each dominated by Aneurolepidium chinense (Trin.) Kitag., Chloris virgata Sw., Puccinellia tenuiflora (Turcz.) Scribn. et Merr. and Suaeda glauca Bunge. This model is a daily-time step model, suitable for simulating hydrological, alkalization/de-alkalization and salinization/desalinization processes of heterogeneous soil, and growth dynamics of different grassland communities. With climatic data and experimental data of Changling Experimental Site in Jilin Province, the soil moisture content (in 1991, 1996, 1997 and 1998), soil salt concentration, exchangeable cation percentage and pH in soil and growth dynamics of these four sorts of grassland communities (in 1991) were simulated and the results were verified to be in accord with observed data.
基金supported by the National Key R&D Program(2017YFA0206804)the National Natural Science Foundation of China(21871021,21521005)the Fundamental Research Funds for the Central Universities(buctylkxj01,XK1802-6)~~
文摘Ethanol conversion to high-value-added products has attracted considerable attention in both academic research and industrial fields.In this study,we synthesized a series of tunable acid–base bifunctional Zn-Zr-Al metal oxides(represented as Zn2ZrxAl-MMO)in light of the structural topotactic transformation of Zn2ZrxAl-hydrotalcite precursors(Zn2ZrxAl-LDH).The resulting Zn2ZrxAl-MMO catalysts were employed in the conversion of ethanol to diethyl carbonate.The Zr^4+ ion content of the LDH precursor plays a key role in modulating the acid-base properties and determining catalytic performance:the Zn2Zr0.1Al-MMO sample exhibits the optimal catalytic behavior with a diethyl carbonate(DEC)yield of 42.1%,which is the highest reported for metal oxide catalysts.Structure-property correlation investigations revealed that the synergic catalysis between medium-strong basic sites and weak acid sites plays a predominant role in the catalytic behavior.Furthermore,in situ Fourier transform infrared measurements showed that the weak acidic site promotes activation adsorption of the reactant(urea)and the intermediate product(ethyl carbamate),while the medium-strong basic site accelerates ethanol activation.Moreover,the Zn2Zr0.1Al-MMO catalyst has the advantages of cost effectiveness,good stability,and reusability.Therefore,the acid-base bifunctional catalysts developed in this work can be employed as promising candidates in acid-base catalytic reactions such as ethanol conversion.
基金supported by the National Natural Science Foundation of China (21173089 and 21373093)the Fundamental Research Funds for the Central Universities of China (2014ZZGH019)the Cooperative Innovation Center of Hubei Province
文摘Acid-catalyzed dehydration of alcohols has been widely employed for the synthesis of alkenes. However, activated alcohols when employed as substrates in dehydration reactions are often pla-gued by the lack of alkene selectivity. In this work, the reaction system can be significantly improved through enhancing the performance of Lewis acid catalysts in the dehydration of activated alcohols by combining with a Lewis base. Observations of the reaction mechanism revealed that the Lewis base component might have changed the reaction rate order. Although both the principal and side reaction rates decreased, the effect was markedly more observed on the latter reaction. Therefore, the selectivity of the dehydration reaction was improved. On the basis of this observation, a new route to synthesize 2-cinnamyl-1,3-dicarbonyl compounds was developed by using 2-aryl-3,4- di-hydropyran as a starting substrate in the presence of a Lewis acid/Lewis base combined catalyst system.
文摘Efficient,stable,and noble‐metal‐free electrocatalysts for both the oxygen evolution reaction and the hydrogen evolution reaction are highly imperative for the realization of low‐cost commercial water‐splitting electrolyzers.Herein,a cost‐effective and ecofriendly strategy is reported to fabricate coral‐like FeNi(OH)x/Ni as a bifunctional electrocatalyst for overall water splitting in alkaline media.With the assistance of mild corrosion of Ni by Fe(NO3)3,in situ generated FeNi(OH)x nanosheets are intimately attached on metallic coral‐like Ni.Integration of these nanosheets with the electrodeposited coral‐like Ni skeleton and the supermacroporous Ni foam substrate forms a binder‐free hierarchical electrode,which is beneficial for exposing catalytic active sites,accelerating mass transport,and facilitating the release of gaseous species.In 1.0 mol L^-1 KOH solution,a symmetric electrolyzer constructed with FeNi(OH)x/Ni as both the anode and the cathode exhibits an excellent activity with an applied potential difference of 1.52 V at 10 mA cm^-2,which is superior to that of an asymmetric electrolyzer constructed with the state‐of‐the‐art RuO2‐PtC couple(applied potential difference of 1.55 V at 10 mA cm^-2).This work contributes a facile and reliable strategy for manufacturing affordable,practical,and promising water‐splitting devices.
文摘Supercritical water has been focused on as an environmentally attractive reaction media, in which organic materials can be decomposed into smaller molecules. The reaction behavior of pyrrole as a simple model compound of nonbasic nitrogen compounds found in petroleum residua was studied in supercritical water with a batch type reactor. The reaction was carried out at temperatures of 698-748 K and at various pressures under an argon atmosphere. The chemical species in the aqueous products were identified by GCMS （gas chromatography mass spectrometry） and quantified using GC-FID （gas chromatography flame ionization detector）. The effect of temperature and reaction time on the conversion process of pyrrole is presented. Under supercritical water conditions, pyrrole underwent successful decomposition in water into its derived compounds. The conversion of pyrrole could approach 81.12 wt% at 723 K and 40 MPa within 240 min of reaction time. The decomposition process was accelerated with the existence of water at the same temperature. Ultimate analysis of solid products was also conducted using a CHN analyzer. The process investigated in this study may form the basis for an efficient method of nitrogen compound decomposition in future.
基金financially supported by the National Natural Science Foundation of China (21975013)the Fundamental Research Funds for the Central Universities。
文摘Electrochemical oxidation of 5-hydroxymethylfurfural(HMF)has shown promising prospects in producing highly valuable chemicals.Herein,we report the synthesis of ultrasmall Ag nanoclusters anchored on NiColayered double hydroxide(NiCo-LDH)nanosheet arrays(Agn@NiCo-LDH)via a facile electrodeposition strategy.The prepared Agn@NiCo-LDH nanosheet arrays exhibit excellent electrocatalytic HMF oxidation performance with a current density of 10 mA cm^(−2) at 1.29 VRHE and the Faraday efficiency of nearly 100%for 2,5-furandicarboxylic acid production.This study offers an effective approach to rationally design nanoclusters to achieve high catalytic activity for sustainable energy conversion and production.
