Methanol oxidation reaction （MOR） at Pt and Pt electrode surface deposited with various amounts of Ru （denoted as PtxRuy, nominal coverage y is 0.17, 0.27, and 0.44 ML） in 0.1 mol/L HClO4＋0.5 mol/L MeOH has been ...Methanol oxidation reaction （MOR） at Pt and Pt electrode surface deposited with various amounts of Ru （denoted as PtxRuy, nominal coverage y is 0.17, 0.27, and 0.44 ML） in 0.1 mol/L HClO4＋0.5 mol/L MeOH has been studied under potentiostatic conditions by in situ FTIR spectroscopy in attenuated-total-reflection con guration and di erential electro-chemical mass spectrometry under controlled flow conditions. Results reveal that （i） CO is the only methanol-related adsorbate observed by IR spectroscopy at all the Pt and PtRu electrodes examined at potentials from 0.3 V to 0.6 V （vs. RHE）; （ii） at Pt0.56Ru0.44, two IR bands, one from CO adsorbed at Ru islands and the other from COL at Pt substrate are detected, while at other electrodes, only a single band for COL adsorbed at Pt is observed; （iii） MOR activity decreases in the order of Pt0.73Ru0.27〉Pt0.56Ru0.44〉Pt0.83Ru0.17〉Pt; （iv） at 0.5 V, MOR at Pt0.73Ru0.27 reaches a current e ciency of 50% for CO2 production, the turn-over frequency from CH3OH to CO2 is ca. 0.1 molecule/（site sec）. Suggestions for further improving of PtRu catalysts for MOR are provided.展开更多
The effects of O2 and the supported Pt nano-particles on the mechanisms and kinetics of the carbon support corrosion are investigated by monitoring the CO2 production using differential electrochemical mass spectromet...The effects of O2 and the supported Pt nano-particles on the mechanisms and kinetics of the carbon support corrosion are investigated by monitoring the CO2 production using differential electrochemical mass spectrometry in a dual-thin layer flow cell. Carbon can be oxidized in different distinct potential regimes; O2 accelerates carbon oxidation, the rates of CO2 production from carbon oxidation in O2 saturated solution are two times of that in N2 saturated solution at the same potential; Pt can catalyze the carbon oxidation, with supported Pt nanoparticles, the overpotential for carbon oxidation is much smaller than that without loading in the carbon electrode. The mechanism for the enhanced carbon oxidation by Pt and O2 are discussed.展开更多
A fog monitor, hotplate total precipitation sensor, weather identifier and visibility sensor, ultrasonic wind speed meter,an icing gradient observation frame, and an automated weather station were involved in the obse...A fog monitor, hotplate total precipitation sensor, weather identifier and visibility sensor, ultrasonic wind speed meter,an icing gradient observation frame, and an automated weather station were involved in the observations at the Lushan Meteorological Bureau of Jiangxi Province, China. In this study, for the icing process under a cold surge from 20–25 January2016, the duration, frequency, and spectrum distribution of agglomerate fog were analyzed. The effects of rain, snow, and supercooled fog on icing growth were studied and the icing and meteorological conditions at two heights(10 m and 1.5 m)were compared. There were 218 agglomerate fogs in this icing process, of which agglomerate fogs with durations less than and greater than 10 min accounted for 91.3% and 8.7%, respectively. The average time interval was 10.3 min. The fog droplet number concentration for sizes 2–15 μm and 30–50 μm increased during rainfall, and that for 2–27 μm decreased during snowfall. Icing grew rapidly(1.3 mm h-1) in the freezing rain phase but slowly(0.1 mm h-1) during the dry snow phase. Intensive supercooled fog, lower temperatures and increased wind speed all favored icing growth during dry snow(0.5 mm h-1). There were significant differences in the thickness, duration, density, and growth mechanism of icing at the heights of 10 m and 1.5 m. Differences in temperature and wind speed between the two heights were the main reasons for the differences in icing conditions, which indicated that icing was strongly affected by height.展开更多
Bimetallic catalysts can improve CO2 reduction efficiency via the combined properties of two metals.CuPd shows enhanced CO2 reduction activity compared to copper alone.Using differential electrochemical mass spectrome...Bimetallic catalysts can improve CO2 reduction efficiency via the combined properties of two metals.CuPd shows enhanced CO2 reduction activity compared to copper alone.Using differential electrochemical mass spectrometry(DEMS)and electrochemical infrared(IR)spectroscopy,volatile products and adsorbed intermediates were measured during CO2 and CO reduction on Cu and CuPd.The IR band corresponding to adsorbed CO appears 300 mV more positive on CuPd than that on Cu,indicating acceleration of CO2 reduction to CO.Electrochemical IR spectroscopy measurements in CO-saturated solutions reveal similar potentials for CO adsorption and CO3^2-desorption on CuPd and Cu,indicating that CO adsorption is controlled by desorption of CO3^2-.DEMS measurements carried out during CO reduction at both electrodes showed that the onset potential for reduction of CO to CH4 and CH3OH on CuPd is about 200 mV more positive than that on Cu.We attribute these improvements to interaction of Cu and Pd,which shifts the d-band center of the Cu sites.展开更多
The present study theoretically explored the feasibility of the capillary method for measuring near-infrared (NIR) spectra of liquid or solution samples with microlitre volume, which was proposed in our previous studi...The present study theoretically explored the feasibility of the capillary method for measuring near-infrared (NIR) spectra of liquid or solution samples with microlitre volume, which was proposed in our previous studies. Lambert-Beer absorb- ance rule was applied to establish a model for the integral absorbance of capillary, which was then implemented in numerical analyses of the effects of capillary on various spectral features and dynamic range of absorption measurement. The theoretical speculations indicated that the capillary method might be used in NIR spectroscopy, which was further supported by the empirical data collected from our experiments by comparison between capillary NIR spectra of several organic solvents and cuvette cell NIR spectra.展开更多
The elemental composition,heat expansibility and breaking characteristics of limestone have been investigated with the use of an energy spectrum analyzer,a SEM,an optical microscope and an experimental heat swelling p...The elemental composition,heat expansibility and breaking characteristics of limestone have been investigated with the use of an energy spectrum analyzer,a SEM,an optical microscope and an experimental heat swelling power system.The results show that 1) the heat expansibility of limestone has anisotropic properties,and 2) the heat expansion rate in the direction perpendicular to stratification is eight times greater than the rate parallel to stratification.The changes in heat expansibility as a function of heating temperature is essentially coincident with that of swelling and breaking of mineral particles and the appearance of cracks,indicating that the reason for causing the heat expansion of rock are the structural changes of limestone caused by thermal stress,crystal transformation and mineral decomposition.The apparent destruction of limestone under high temperatures is largely characterized by rock stratification breaks.When the limestone is heated beyond a certain limit,the rock destroys into crazed cracks.展开更多
Single-walled carbon nanotubes （SWCNTs） illuminated by white light should appear colored due to resonance Rayleigh scattering. However, true-color imaging of SWCNTs on substrates has not been reported, because of th...Single-walled carbon nanotubes （SWCNTs） illuminated by white light should appear colored due to resonance Rayleigh scattering. However, true-color imaging of SWCNTs on substrates has not been reported, because of the extremely low scattering intensity of SWCNTs and the strong substrate scattering. Here we show that Rayleigh scattering can be greatly enhanced by the interface dipole enhancement effect. Consequently colorful SWCNTs on substrates can be directly imaged under an optical microscope by wide field supercontinuum laser illumination, which facilitates high throughput chirality assignment of individual SWCNTs. This approach, termed ＂Rayleigh imaging microscopy＂, is not restricted to SWCNTs, but widely applicable to a variety of nanomaterials, which enables the colorful nanoworld to be explored under optical microscopes.展开更多
文摘Methanol oxidation reaction （MOR） at Pt and Pt electrode surface deposited with various amounts of Ru （denoted as PtxRuy, nominal coverage y is 0.17, 0.27, and 0.44 ML） in 0.1 mol/L HClO4＋0.5 mol/L MeOH has been studied under potentiostatic conditions by in situ FTIR spectroscopy in attenuated-total-reflection con guration and di erential electro-chemical mass spectrometry under controlled flow conditions. Results reveal that （i） CO is the only methanol-related adsorbate observed by IR spectroscopy at all the Pt and PtRu electrodes examined at potentials from 0.3 V to 0.6 V （vs. RHE）; （ii） at Pt0.56Ru0.44, two IR bands, one from CO adsorbed at Ru islands and the other from COL at Pt substrate are detected, while at other electrodes, only a single band for COL adsorbed at Pt is observed; （iii） MOR activity decreases in the order of Pt0.73Ru0.27〉Pt0.56Ru0.44〉Pt0.83Ru0.17〉Pt; （iv） at 0.5 V, MOR at Pt0.73Ru0.27 reaches a current e ciency of 50% for CO2 production, the turn-over frequency from CH3OH to CO2 is ca. 0.1 molecule/（site sec）. Suggestions for further improving of PtRu catalysts for MOR are provided.
基金ACKNOWLEDGMENTS This work was supported by the National Natural Science Foundation of China （No.20773116）, the one hundred Talents＇ Program Sciences, and the National China （No.2010CB923302） of the Chinese Academy of Basic Research Program of
文摘The effects of O2 and the supported Pt nano-particles on the mechanisms and kinetics of the carbon support corrosion are investigated by monitoring the CO2 production using differential electrochemical mass spectrometry in a dual-thin layer flow cell. Carbon can be oxidized in different distinct potential regimes; O2 accelerates carbon oxidation, the rates of CO2 production from carbon oxidation in O2 saturated solution are two times of that in N2 saturated solution at the same potential; Pt can catalyze the carbon oxidation, with supported Pt nanoparticles, the overpotential for carbon oxidation is much smaller than that without loading in the carbon electrode. The mechanism for the enhanced carbon oxidation by Pt and O2 are discussed.
基金supported by the National Natural Science Foundation of China (Grant Nos.41775134,41375138,41505121,41675132 and 41675136)Graduate Student Innovation Plan for the Universities of Jiangsu Province (KYCX18 1010)
文摘A fog monitor, hotplate total precipitation sensor, weather identifier and visibility sensor, ultrasonic wind speed meter,an icing gradient observation frame, and an automated weather station were involved in the observations at the Lushan Meteorological Bureau of Jiangxi Province, China. In this study, for the icing process under a cold surge from 20–25 January2016, the duration, frequency, and spectrum distribution of agglomerate fog were analyzed. The effects of rain, snow, and supercooled fog on icing growth were studied and the icing and meteorological conditions at two heights(10 m and 1.5 m)were compared. There were 218 agglomerate fogs in this icing process, of which agglomerate fogs with durations less than and greater than 10 min accounted for 91.3% and 8.7%, respectively. The average time interval was 10.3 min. The fog droplet number concentration for sizes 2–15 μm and 30–50 μm increased during rainfall, and that for 2–27 μm decreased during snowfall. Icing grew rapidly(1.3 mm h-1) in the freezing rain phase but slowly(0.1 mm h-1) during the dry snow phase. Intensive supercooled fog, lower temperatures and increased wind speed all favored icing growth during dry snow(0.5 mm h-1). There were significant differences in the thickness, duration, density, and growth mechanism of icing at the heights of 10 m and 1.5 m. Differences in temperature and wind speed between the two heights were the main reasons for the differences in icing conditions, which indicated that icing was strongly affected by height.
基金supported by the National Natural Science Foundation of China(No.91545124 and No.21750110437)supported by the Chinese Academy of Sciences President’s International Fellowship Initiative(No.2017PM0049)。
文摘Bimetallic catalysts can improve CO2 reduction efficiency via the combined properties of two metals.CuPd shows enhanced CO2 reduction activity compared to copper alone.Using differential electrochemical mass spectrometry(DEMS)and electrochemical infrared(IR)spectroscopy,volatile products and adsorbed intermediates were measured during CO2 and CO reduction on Cu and CuPd.The IR band corresponding to adsorbed CO appears 300 mV more positive on CuPd than that on Cu,indicating acceleration of CO2 reduction to CO.Electrochemical IR spectroscopy measurements in CO-saturated solutions reveal similar potentials for CO adsorption and CO3^2-desorption on CuPd and Cu,indicating that CO adsorption is controlled by desorption of CO3^2-.DEMS measurements carried out during CO reduction at both electrodes showed that the onset potential for reduction of CO to CH4 and CH3OH on CuPd is about 200 mV more positive than that on Cu.We attribute these improvements to interaction of Cu and Pd,which shifts the d-band center of the Cu sites.
文摘The present study theoretically explored the feasibility of the capillary method for measuring near-infrared (NIR) spectra of liquid or solution samples with microlitre volume, which was proposed in our previous studies. Lambert-Beer absorb- ance rule was applied to establish a model for the integral absorbance of capillary, which was then implemented in numerical analyses of the effects of capillary on various spectral features and dynamic range of absorption measurement. The theoretical speculations indicated that the capillary method might be used in NIR spectroscopy, which was further supported by the empirical data collected from our experiments by comparison between capillary NIR spectra of several organic solvents and cuvette cell NIR spectra.
基金Project 50574037 supported by the National Natural Science Foundation of China
文摘The elemental composition,heat expansibility and breaking characteristics of limestone have been investigated with the use of an energy spectrum analyzer,a SEM,an optical microscope and an experimental heat swelling power system.The results show that 1) the heat expansibility of limestone has anisotropic properties,and 2) the heat expansion rate in the direction perpendicular to stratification is eight times greater than the rate parallel to stratification.The changes in heat expansibility as a function of heating temperature is essentially coincident with that of swelling and breaking of mineral particles and the appearance of cracks,indicating that the reason for causing the heat expansion of rock are the structural changes of limestone caused by thermal stress,crystal transformation and mineral decomposition.The apparent destruction of limestone under high temperatures is largely characterized by rock stratification breaks.When the limestone is heated beyond a certain limit,the rock destroys into crazed cracks.
基金The authors would like to thank Prof. Feng Wang, Prof. Xuedong Bai, and Prof. Kaihui Liu for helpful discussions. This work was supported by the National Basic Research Program of China （No. 2012CB932301） and the National Natural Science Foundation of China （Nos. 90921012, 11321091, 51102144, 11274190, and 51102147）.
文摘Single-walled carbon nanotubes （SWCNTs） illuminated by white light should appear colored due to resonance Rayleigh scattering. However, true-color imaging of SWCNTs on substrates has not been reported, because of the extremely low scattering intensity of SWCNTs and the strong substrate scattering. Here we show that Rayleigh scattering can be greatly enhanced by the interface dipole enhancement effect. Consequently colorful SWCNTs on substrates can be directly imaged under an optical microscope by wide field supercontinuum laser illumination, which facilitates high throughput chirality assignment of individual SWCNTs. This approach, termed ＂Rayleigh imaging microscopy＂, is not restricted to SWCNTs, but widely applicable to a variety of nanomaterials, which enables the colorful nanoworld to be explored under optical microscopes.
