Kinetics insights into size effects of carbon nanotubes'growth and their supported platinum catalysts for 4,6-dinitroresorcinol hydrogenation

Size effects are a well-documented phenomenon in heterogeneous catalysis,typically attributed to alterations in geometric and electronic properties.In this study,we investigate the influence of catalyst size in the preparation of carbon nanotube(CNT)and the hydrogenation of 4,6-dinitroresorcinol(DNR)using Fe_(2)O_(3)and Pt catalysts,respectively.Various Fe_(2)O_(3)/Al_(2)O_(3)catalysts were synthesized for CNT growth through catalytic chemical vapor deposition.Our findings reveal a significant influence of Fe_(2)O_(3)nanoparticle size on the structure and yield of CNT.Specifically,CNT produced with Fe_(2)O_(3)/Al_(2)O_(3)containing 28%(mass)Fe loading exhibits abundant surface defects,an increased area for metal-particle immobilization,and a high carbon yield.This makes it a promising candidate for DNR hydrogenation.Utilizing this catalyst support,we further investigate the size effects of Pt nanoparticles on DNR hydrogenation.Larger Pt catalysts demonstrate a preference for 4,6-diaminoresorcinol generation at(100)sites,whereas smaller Pt catalysts are more susceptible to electronic properties.The kinetics insights obtained from this study have the potential to pave the way for the development of more efficient catalysts for both CNT synthesis and DNR hydrogenation.

Towards a molecular understanding of the electronic metal-support interaction(EMSI)in heterogeneous catalysis

Tailoring the electronic metal-support interaction(EMSI)has attracted considerable interests as one of the most efficient approaches to improve both the activity and stability of metal catalysts in heterogeneous catalysis.In this viewpoint,we illustrate the methodology and relevant fundamentals on the disentanglement,characterization,and interpretation of EMSI.Under the choice of monometallic catalyst over inert support,a combination of optimal experiment design,multimodal techniques,in situ characterization,with a comprehensive understanding of the underlying measurement protocols is highly desirable for a reliable determination of EMSI.Accordingly,not only the d-band filling but also d-band energy within the EMSI should be taken into consideration for providing general principles to guide the electron-promoting catalytic reaction.

Natural and Socioeconomic Factors and Their Interactive Effects on House Collapse Caused by Typhoon Mangkhut

Typhoons are an environmental threat that mainly affects coastal regions worldwide.The interactive effects of natural and socioeconomic factors on the losses caused by typhoon disasters need further examination.In this study,GeoDetector was used to quantify the determinant powers of natural and socioeconomic factors and their interactive effects on the rate of house collapse in Guangdong and Guangxi Provinces of southeast China caused by Typhoon Mangkhut in 2018.We further identify the dominant factors that influenced the disaster losses.The local indicators of spatial association method was then introduced to explain the spatial heterogeneity of the disaster losses under the influence of the dominant factor.The results indicate that both natural and socioeconomic factors significantly affected the house collapse rate.The maximum precipitation was the dominant factor,with a q value of 0.21,followed by slope and elevation,with q values of 0.17 and 0.13,respectively.Population density and per capita gross domestic product had q values of 0.15 and0.13,respectively.Among all of the interactive effects of the influencing factors,the interactive effect of elevation and the ratio of brick-wood houses had the greatest influence(q=0.63)on the house collapse rate.These results can contribute to the formulation of more specific safety and property protection policies.

Engineering electronic platinum-carbon support interaction to tame carbon monoxide activation

CO oxidation has been studied for more than a century;however,molecular-level understanding of its activation protocol and related intermediates remains elusive.Here,we present a unified mechanistic and kinetic picture of various electronic metal-support interactions within platinum-carbon catalysts via in situ spectroscopic/kinetic analyses and multi-scale simulations.Transient kinetic analysis and molecular dynamics simulations with a reactive force field provided a quantitative description of the competition between the oxygen association and oxygen dissociation mechanisms tuned by the interfacial charge distribution and CO coverage.Steady-state isotopic transient kinetic analysis and density functional theory calculations revealed a simultaneous shift in the rate-determining step(RDS)from O_(2)^(*)dissociation to O^(*)and CO^(*)and O_(2)^(*)and CO^(*)association.A de novo strategy from the interfacial charge distribution to the reaction mechanism,kinetics/thermodynamics of RDS,and,ultimately,catalytic performance was developed to quantitatively map the above CO activation mechanism with an order-of-magnitude increase in reactivity.The proposed catalytic picture and de novo strategy are expected to prompt the development of theories and methodologies for heterogeneous catalysis.