助剂对铁基费托合成催化剂氧化行为的影响:H2O作用的解读

以纯Fe催化剂为研究对象,采用XRD、Raman和TPH等手段考察了催化剂的碳化程度、还原程度对H 2O氧化过程的影响,获得了H 2O氧化过程与催化剂中碳物种转变之间的相互影响规律;系统考察了典型的费托合成助剂K和SiO 2存在时对催化剂物化性质以及H 2O氧化行为的影响,发现催化剂的碳化程度越高,碳化铁的抗H 2O氧化能力越强,氧化过程使得碳物种的石墨化程度增加。适量K助剂可促进碳化铁和催化剂表面石墨碳的形成,提高了碳化铁在H 2O氧化过程中的稳定性;SiO 2助剂的加入显著抑制了催化剂的碳化,但可有效提高碳化铁以及碳物种的稳定性。

A first-principles study on elastic properties and stability of Ti_xV_(1-x)C multiple carbide

The structure,stability and elastic properties of di-transition-metal carbides TixV1-xC were investigated by using the first-principles with a pseudopotential plane-waves method.The results show that the equilibrium lattice constants of TixV1-xC show a nearly linear reduction with increasing addition of V.The elastic properties of TixV1-xC are varied by doping with V.The bulk modulus of Ti0.5V0.5C is larger than that of pure TiC,as well as Ti0.5V0.5C has the largest C44 among TixV1-xC（0≤x≤1）,indicating that Ti0.5V0.5C has higher hardness than pure TiC.However,Ti0.5V0.5C presents brittleness based on the analysis of ductile/brittle behavior.The Ti0.5V0.5C carbide has the lowest formation energy,indicating that Ti0.5V0.5C is more stable than all other alloys.

Catalytic oxidation of diesel soot particulates over Ag/LaCoO_3 perovskite oxides in air and NO_x

Ag/LaCoO3 perovskite catalysts for soot combustion were prepared by the impregnation method.The structure and physicochemical properties of the catalysts were characterized using X-ray diffraction,N2 adsorption-desorption,H2 temperature-programmed reduction,soot temperatureprogrammed reduction,and X-ray photoelectron spectroscopy.The catalytic activity of the catalysts for soot oxidation was tested by temperature-programmed oxidation in air and in a NOx atmosphere.Metallic Ag particles were the main Ag species.Part of the Ag migrated from the surface to the lattice of the LaCoO3 perovskite,to form La（1-x）AgxCoO3.This increased the amount of oxygen vacancies in the perovskite structure during thermal treatment.Compared with unmodified LaCoO3,the maximum soot oxidation rate temperature（Tp） decreased by 50-70 ℃ in air when LaCoO3 was partially modified by Ag,depending on the thermal treatment temperature.The Tp of the Ag/LaCoO3catalyst calcined at 400℃ in a NOx atmosphere decreased to about 140℃,compared with that of LaCoO3.Ag particles and oxygen vacancies in the catalysts contributed to their high catalytic activity for soot oxidation.The stable catalytic activity of the Ag/LaCoO3 catalyst calcined at 700℃ in a NOx atmosphere was related to its stable structure.

Overcoming coke formation in high-temperature CO_(2)electrolysis

High-temperature CO_(2)reduction reaction(HT-CO_(2)RR)in solid oxide electrochemical cells(SOECs)features near-unity selectivity,high energy efficiency,and industrial relevant current density for the production of CO,a widely-utilized“building block”in today’s chemical industry.Thus,it offers an intriguing and promising means to radically change the way of chemical manufacturing and achieve carbon neutrality using renewable energy sources,CO_(2),and water.Albeit with the great potential of HT-CO_(2)RR,this carbon utilization approach,unfortunately,has been suffering coke formation that is seriously detrimental to its energy efficiency and operating lifetime.In recent years,much effort has been added to understanding the mechanism of coke formation,managing reaction conditions to mitigate coke formation,and devising coke-formation-free electrode materials.These investigations have substantially advanced the HT-CO_(2)RR toward a practical industrial technology,but the resulting coke formation prevention strategies compromise activity and energy efficiency.Future research may target exploiting the control over both catalyst design and system design to gain selectivity,energy efficiency,and stability synchronously.Therefore,this perspective overviews the progress of research on coke formation in HT-CO_(2)RR,and elaborates on possible future directions that may accelerate its practical implementation at a large scale.

Comparative Studies of Thermal Stability of Coal Tar Pitches

In the present work, three medium softening point coal tar pitches were used for comparative thermal stability and under-storage stability investigation. Powders of the pitches were found to be different under storage： one of the pitches was caked and slumped after 7-day or longer storage. For thermal stability investigation the soft temperature treatment （265℃） of coal tar pitches was used. Detailed study of initial and treated pitches was carried out. Experimental results demonstrated that LMW-HC （high low-molecular-weight hydrocarbons） and oxygen content influence pitch quality characteristics in a negative way under long-term storage and lead to highest properties change after thermal stability treatment.

Experimental Study on Hydrocarbon Fuel Thermal Stability

The.thermal stability characteristics of kerosine-type fuels are examined using a heated-tube apparatus which allows independent control of fuel pressure,fuel temperature,tube-wall temperature and fuel flow rate.This method is identified simply as a“constant wall temperature method”.It is different from a previous widely used method,which is identified as a“constant heat flux method”.It is a single-pass system.Rate of deposition on the tube walls are measured by weighing the test tube before and after each test. For a fuel temperature of 250℃,it is found that deposition rates increase continuously with increase in tube- wall temperature.This finding contradicts the results of previous studies which had led to the conclusion that deposition rates increase with increase in wall temperature up to a certain value(around 650 K)beyond which any further increase in wall temperature causes the rate of deposition to decline. The present results show clearly that the constant wall temperature method is more suitable for assessing the thermal stability of gas turbine fuels.

S, N co-doped carbon nanotube-encapsulated core-shelled CoS2@Co nanoparticles： efficient and stable bifunctional catalysts for overall water splitting

Hydrogen, serving as a clean, sustainable energy source, may be mainly produced from electrolysis water. Herein, we report cobalt disulphide encapsulated in self-catalyzed carbon nanotubes （S, N-CNTs/ CoS2@Co） serving as a bifunctional catalyst, which exhibits excellent hydrogen evolution reaction perfor-mance （10.0 mAcm^-2 at 0.112 V, and low Tafel slope for 104.9 mV dec^-1 ） and oxygen evolution reaction performance （10.0 mAcm^-2 at 1.57 V, and low Tafel slope for 76.1 mV dec^-1）, meanwbile with a strong stability at various current densities. In-depth study reveals that the excellent catalytic properties can be mainly attributed to the increased catalytic sites induced by S, N co-doping, the improved electronic con-ductivity derived from the carbon nanotubes, and Mott-Schottky effect between the metal cobalt and semiconductive cobalt disulfide. Notably, when the bifunctional catalysts are applied to overall water splitting, a low potential of 1.633 V at the current density of 10.0 mAcm^-2 is achieved, which can com-pete with the precious metal catalyst benchmarks in alkaline media, demonstrating its promising prac-ticability in the realistic water splitting application. This work elucidates a practicable way to the design of transition metal and nano-carbon composite catalysts for a broad application in the fields of energy chemistry.

Effects of leaf age,elevation and light conditions on photosynthesis and leaf traits in saplings of two evergreen conifers,Abies veitchii and A.mariesii

Aims Subalpine coniferous species are distributed over a wide range of elevations in which they must contend with stressful conditions,such as high elevations and extended periods of darkness.Two evergreen coniferous species,Abies veitchii and Abies mariesii,dominate at low and high elevations,respectively,in the subalpine zone,central Japan.The aim of this study is to examine the effects of leaf age,elevation and light conditions on photosynthetic rates through changes in morphological and physiological leaf traits in the two species.Methods We here examined effects of leaf age,elevation and light conditions on photosynthesis,and leaf traits in A.veitchii and A.mariesii.Saplings of the two conifers were sampled in the understory and canopy gaps at their lower(1600 m)and upper(2300 m)distribution limits.Important Findings The two species showed similar responses to leaf age and different responses to elevation and light conditions in photosynthesis and leaf traits.The maximum photosynthetic rate of A.veitchii is correlated negatively with leaf mass per area(LMA)and non-structural carbohydrate(NSC)concentration.LMA increased at high elevations in the two species,whereas NSC concentrations increased only in A.veitchii.Therefore,the maximum photosynthetic rate of A.veitchii decreased at high elevations.Furthermore,maximum photosynthetic rates correlate positively with nitrogen concentration in both species.In the understory,leaf nitrogen concentrations decreased and increased in A.veitchii and A.mariesii,respectively.LMA decreased and the chlorophyll-to-nitrogen ratio increased in understory conditions only for A.mariesii,suggesting it has a higher light-capture efficiency in dark conditions than does A.veitchii.This study concluded that A.mariesii has more shade-tolerant photosynthetic and leaf traits and its photosynthetic rate is less affected by elevation compared with A.veitchii,allowing A.mariesii to survive in the understory and to dominate at high elevations.