Electrocatalysis is key to improving energy efficiency,reducing carbon emissions,and providing a sustainable way of meeting global energy needs.Therefore,elucidating electrochemical reaction mechanisms at the electrol...Electrocatalysis is key to improving energy efficiency,reducing carbon emissions,and providing a sustainable way of meeting global energy needs.Therefore,elucidating electrochemical reaction mechanisms at the electrolyte/electrode interfaces is essential for developing advanced renewable energy technologies.However,the direct probing of real-time interfacial changes,i.e.,the surface intermediates,chemical environment,and electronic structure,under operating conditions is challenging and necessitates the use of in situ methods.Herein,we present a new lab-based instrument commissioned to perform in situ chemical analysis at liquid/solid interfaces using ambient pressure X-ray photoelectron spectroscopy(APXPS).This setup takes advantage of a chromium source of tender X-rays and is designed to study liquid/solid interfaces by the“dip and pull”method.Each of the main components was carefully described,and the results of performance tests are presented.Using a three-electrode setup,the system can probe the intermediate species and potential shifts across the liquid electrolyte/solid electrode interface.In addition,we demonstrate how this system allows the study of interfacial changes at gas/solid interfaces using a case study:a sodium–oxygen model battery.However,the use of APXPS in electrochemical studies is still in the early stages,so we summarize the current challenges and some developmental frontiers.Despite the challenges,we expect that joint efforts to improve instruments and the electrochemical setup will enable us to obtain a better understanding of the composition–reactivity relationship at electrochemical interfaces under realistic reaction conditions.展开更多
The limited CO_(2)content in aqueous solution and low adsorption amount of CO_(2)on catalyst surface lead to poor photocatalytic CO_(2)reduction activity and selectivity.Herein,the design and fabrication of a novel ph...The limited CO_(2)content in aqueous solution and low adsorption amount of CO_(2)on catalyst surface lead to poor photocatalytic CO_(2)reduction activity and selectivity.Herein,the design and fabrication of a novel photocatalytic architecture is reported,accomplished via chemical vapor deposition of polymeric carbon nitride on carbon paper.The as-obtained samples with a hydrophobic surface exhibit excellent CO_(2)transport and adsorption ability,as well as the building of triphase air-liquid-solid(CO_(2)-H_(2)O-catalyst)joint interfaces,eventually resulting in the inhibition of H2 evolution and great promotion of CO_(2)reduction with a selectivity of 78.6%.The addition of phosphate to reaction environment makes further improvement of CO_(2)photoreduction into carbon fuels with a selectivity of 93.8%and an apparent quantum yield of 0.4%.This work provides new insight for constructing efficient photocatalytic architecture of CO_(2)photoreduction in aqueous solution and demonstrates that phosphate could play a key role in this process.展开更多
Slag movement on SiO2-based prism refractories in different slag systems was observed. The cross section shape evolution mechanism was discussed. Two types of shape evolution appear. For PbO-SiO2 slag whose surface te...Slag movement on SiO2-based prism refractories in different slag systems was observed. The cross section shape evolution mechanism was discussed. Two types of shape evolution appear. For PbO-SiO2 slag whose surface tension improves with SiO2 concentration, slag film flows up along four edges under axial Marangoni shear force and wettability. Then, it flows down along four lateral faces under gravity. Corrosion rate at edges is larger than that on lateral faces due to different SiO2 solubilities of ascending and descending flow. Prism cross section shape changes from square to round. For FetO-SiO2 slag whose surface tension reduces with the increase of SiO2 concentration, slag film flows up under the inflence of wettability. Then, it flows down under Marangoni shear force and gravity. Compared to four edges, slag is mainly up and down on four lateral faces due to larger surface tension and size. So, prism cross section shape keeps square.展开更多
An theoretical investigation was conducted to detect the gas-solid interface effect on laminar flow characteristics for gas flowing through micropassages. In the wall-adjacent region, the change in viscosity of fluid ...An theoretical investigation was conducted to detect the gas-solid interface effect on laminar flow characteristics for gas flowing through micropassages. In the wall-adjacent region, the change in viscosity of fluid vs the distance from the wall surface, as derived from the kinetic theory of gases result in significallt influence on the flow characteristics in micropassages. A model was proposed to account for the wall effect. Analytical expressions for velocity profiles and pressure drop were derived, respectively,for laminar fiow of gases in microtubes and in extremely narrow parallel plates. The Knudsen number,Kn, as a criterion, that the fiow can be treated reasonably as flow in macrochannels, is discussed.展开更多
文摘Electrocatalysis is key to improving energy efficiency,reducing carbon emissions,and providing a sustainable way of meeting global energy needs.Therefore,elucidating electrochemical reaction mechanisms at the electrolyte/electrode interfaces is essential for developing advanced renewable energy technologies.However,the direct probing of real-time interfacial changes,i.e.,the surface intermediates,chemical environment,and electronic structure,under operating conditions is challenging and necessitates the use of in situ methods.Herein,we present a new lab-based instrument commissioned to perform in situ chemical analysis at liquid/solid interfaces using ambient pressure X-ray photoelectron spectroscopy(APXPS).This setup takes advantage of a chromium source of tender X-rays and is designed to study liquid/solid interfaces by the“dip and pull”method.Each of the main components was carefully described,and the results of performance tests are presented.Using a three-electrode setup,the system can probe the intermediate species and potential shifts across the liquid electrolyte/solid electrode interface.In addition,we demonstrate how this system allows the study of interfacial changes at gas/solid interfaces using a case study:a sodium–oxygen model battery.However,the use of APXPS in electrochemical studies is still in the early stages,so we summarize the current challenges and some developmental frontiers.Despite the challenges,we expect that joint efforts to improve instruments and the electrochemical setup will enable us to obtain a better understanding of the composition–reactivity relationship at electrochemical interfaces under realistic reaction conditions.
文摘The limited CO_(2)content in aqueous solution and low adsorption amount of CO_(2)on catalyst surface lead to poor photocatalytic CO_(2)reduction activity and selectivity.Herein,the design and fabrication of a novel photocatalytic architecture is reported,accomplished via chemical vapor deposition of polymeric carbon nitride on carbon paper.The as-obtained samples with a hydrophobic surface exhibit excellent CO_(2)transport and adsorption ability,as well as the building of triphase air-liquid-solid(CO_(2)-H_(2)O-catalyst)joint interfaces,eventually resulting in the inhibition of H2 evolution and great promotion of CO_(2)reduction with a selectivity of 78.6%.The addition of phosphate to reaction environment makes further improvement of CO_(2)photoreduction into carbon fuels with a selectivity of 93.8%and an apparent quantum yield of 0.4%.This work provides new insight for constructing efficient photocatalytic architecture of CO_(2)photoreduction in aqueous solution and demonstrates that phosphate could play a key role in this process.
基金Projects(U1738101,51804023)supported by the National Natural Science Foundation of ChinaProjects(FRF-TP-18-007A1,FRF-MP-18-007)supported by Fundamental Research Funds for the Central Universities,ChinaProject(2019M650489)supported by China Postdoctoral Science Foundation
文摘Slag movement on SiO2-based prism refractories in different slag systems was observed. The cross section shape evolution mechanism was discussed. Two types of shape evolution appear. For PbO-SiO2 slag whose surface tension improves with SiO2 concentration, slag film flows up along four edges under axial Marangoni shear force and wettability. Then, it flows down along four lateral faces under gravity. Corrosion rate at edges is larger than that on lateral faces due to different SiO2 solubilities of ascending and descending flow. Prism cross section shape changes from square to round. For FetO-SiO2 slag whose surface tension reduces with the increase of SiO2 concentration, slag film flows up under the inflence of wettability. Then, it flows down under Marangoni shear force and gravity. Compared to four edges, slag is mainly up and down on four lateral faces due to larger surface tension and size. So, prism cross section shape keeps square.
文摘An theoretical investigation was conducted to detect the gas-solid interface effect on laminar flow characteristics for gas flowing through micropassages. In the wall-adjacent region, the change in viscosity of fluid vs the distance from the wall surface, as derived from the kinetic theory of gases result in significallt influence on the flow characteristics in micropassages. A model was proposed to account for the wall effect. Analytical expressions for velocity profiles and pressure drop were derived, respectively,for laminar fiow of gases in microtubes and in extremely narrow parallel plates. The Knudsen number,Kn, as a criterion, that the fiow can be treated reasonably as flow in macrochannels, is discussed.
