The dissolution kinetics of diatomite in alkaline solution is the theoretical basis for the process optimization of alkali-diatomite reaction and its applications.In this study,the dissolution kinetics of diatomite in...The dissolution kinetics of diatomite in alkaline solution is the theoretical basis for the process optimization of alkali-diatomite reaction and its applications.In this study,the dissolution kinetics of diatomite in NaOH solution is investigated.The results indicate that the dissolution reaction fits well the unreacted shrinking core model for solid-liquid heterogeneous reactions.The apparent reaction order for NaOH is 2 and the apparent activation energy for the reaction(Ea) is 28.06 kJ·mol-1.The intra-particle diffusion through the sodium silicate layer is the rate-controlling step.When the dissolution reaction occurs at the interface of unreacted diatomite solid core,the diffusion in the trans-layer(the liquid film around the wetted particle) reduces the rate of whole dissolution process.展开更多
A hydrophobic complex of Cu2＋[bis-salicylic aldehyde-o-phenylenediamine], Cu-SPA, was prepared and used as a heterogeneous photocatalyst to degrade organic pollutants in water under visible irradiation （λ≥420 nm）...A hydrophobic complex of Cu2＋[bis-salicylic aldehyde-o-phenylenediamine], Cu-SPA, was prepared and used as a heterogeneous photocatalyst to degrade organic pollutants in water under visible irradiation （λ≥420 nm） at neutral pH. The structure of complex was characterized by using nuclear magnetic resonance （NMR）, elemental analysis, IR and UV-vis spectrometries. Degradation of Rhodamine B （RhB）, Sulforhodamine B （SRB） and Benzoic acid （BA） in water were used as model reactions to evaluate the photocatalytic activities of Cu-SPA. The results indicated that RhB and SRB were easily adsorbed on the hydrophobic surface of Cu-SPA from aqueous solution （the maximum adsorption amount： Qmax = 11.09 and 8.05 μmol/g, respectively）. Under visible irradiation, RhB and SRB were decolorized completely after 210 and 240 min, respectively, and BA was removed completely after 5 h. The efficiency of H202 was 〉 95%, in contrast to that of the reaction without catalyst or light （〈 20%）. In water soluble medium, the hydrophobic Cu-SPA can be used more than 6 cycles. ESR results and the behavior of cy- clic voltammetry showed that, in the reaction process, Cu2＋-SPA was reduced to intermediate state Cu＋-SPA firstly, which was extremely unstable and reacted rapidly with H2O2, leading to high reactive oxygen species （.OH radical ） to degrade the substrate.展开更多
Developing highly efficient,cost-effective,and stable electrocatalysts for hydrogen evolution reaction(HER)is of considerable importance but remains challenging.Herein,we report the fabrication of a robust Ru-based el...Developing highly efficient,cost-effective,and stable electrocatalysts for hydrogen evolution reaction(HER)is of considerable importance but remains challenging.Herein,we report the fabrication of a robust Ru-based electrocatalyst,which comprises heterostructured Ru-Ru_(2)P nanoparticles that are embedded in the N,P-codoped carbon nanofibers(CNFs),through a synthetic strategy involving electrospinning and temperature-controlled pyrolysis treatment.The as-prepared Ru-Ru_(2)P catalyst(Ru-Ru_(2)P@CNFs)shows excellent HER catalytic activities with low overpotentials of 11 and 14 mV in acidic and alkaline media,respectively,to achieve a current density of 10 mA cm^(−2),which are superior to the individual components of pure Ru and Ru_(2)P catalysts.Density functional theory calculations demonstrate the existence of electronic coupling effect between Ru and Ru_(2)P at the heterointerfaces,leading to a well-modulated electronic structure with optimized hydrogen adsorption strength and enhanced electrical conductivity for efficient HER electrocatalysis.In addition,the overall synthetic strategy can be generalized for the synthesis of a series of transitional metal phosphide-based nanofibers,thereby holding a remarkable capacity for various potential applications.展开更多
基金Supported by the National lqatural Science Foundation of China （50674080）.
文摘The dissolution kinetics of diatomite in alkaline solution is the theoretical basis for the process optimization of alkali-diatomite reaction and its applications.In this study,the dissolution kinetics of diatomite in NaOH solution is investigated.The results indicate that the dissolution reaction fits well the unreacted shrinking core model for solid-liquid heterogeneous reactions.The apparent reaction order for NaOH is 2 and the apparent activation energy for the reaction(Ea) is 28.06 kJ·mol-1.The intra-particle diffusion through the sodium silicate layer is the rate-controlling step.When the dissolution reaction occurs at the interface of unreacted diatomite solid core,the diffusion in the trans-layer(the liquid film around the wetted particle) reduces the rate of whole dissolution process.
基金supported by the National Natural Science Foundation of China(21207079,21307073,21177072,21377067)
文摘A hydrophobic complex of Cu2＋[bis-salicylic aldehyde-o-phenylenediamine], Cu-SPA, was prepared and used as a heterogeneous photocatalyst to degrade organic pollutants in water under visible irradiation （λ≥420 nm） at neutral pH. The structure of complex was characterized by using nuclear magnetic resonance （NMR）, elemental analysis, IR and UV-vis spectrometries. Degradation of Rhodamine B （RhB）, Sulforhodamine B （SRB） and Benzoic acid （BA） in water were used as model reactions to evaluate the photocatalytic activities of Cu-SPA. The results indicated that RhB and SRB were easily adsorbed on the hydrophobic surface of Cu-SPA from aqueous solution （the maximum adsorption amount： Qmax = 11.09 and 8.05 μmol/g, respectively）. Under visible irradiation, RhB and SRB were decolorized completely after 210 and 240 min, respectively, and BA was removed completely after 5 h. The efficiency of H202 was 〉 95%, in contrast to that of the reaction without catalyst or light （〈 20%）. In water soluble medium, the hydrophobic Cu-SPA can be used more than 6 cycles. ESR results and the behavior of cy- clic voltammetry showed that, in the reaction process, Cu2＋-SPA was reduced to intermediate state Cu＋-SPA firstly, which was extremely unstable and reacted rapidly with H2O2, leading to high reactive oxygen species （.OH radical ） to degrade the substrate.
基金financially supported by the Natural Science Foundation of Zhejiang Province (LQ20B030001 and LY20E020002)China Postdoctoral Science Foundation (2021M702305)。
文摘Developing highly efficient,cost-effective,and stable electrocatalysts for hydrogen evolution reaction(HER)is of considerable importance but remains challenging.Herein,we report the fabrication of a robust Ru-based electrocatalyst,which comprises heterostructured Ru-Ru_(2)P nanoparticles that are embedded in the N,P-codoped carbon nanofibers(CNFs),through a synthetic strategy involving electrospinning and temperature-controlled pyrolysis treatment.The as-prepared Ru-Ru_(2)P catalyst(Ru-Ru_(2)P@CNFs)shows excellent HER catalytic activities with low overpotentials of 11 and 14 mV in acidic and alkaline media,respectively,to achieve a current density of 10 mA cm^(−2),which are superior to the individual components of pure Ru and Ru_(2)P catalysts.Density functional theory calculations demonstrate the existence of electronic coupling effect between Ru and Ru_(2)P at the heterointerfaces,leading to a well-modulated electronic structure with optimized hydrogen adsorption strength and enhanced electrical conductivity for efficient HER electrocatalysis.In addition,the overall synthetic strategy can be generalized for the synthesis of a series of transitional metal phosphide-based nanofibers,thereby holding a remarkable capacity for various potential applications.
