Surface functionalization of Cu-based catalysts has demonstrated promising potential for enhancing the electrochemical CO_(2)reduction reaction(CO_(2)RR)toward multi-carbon(C2+)products,primarily by suppressing the pa...Surface functionalization of Cu-based catalysts has demonstrated promising potential for enhancing the electrochemical CO_(2)reduction reaction(CO_(2)RR)toward multi-carbon(C2+)products,primarily by suppressing the parasitic hydrogen evolution reaction and facilitating a localized CO_(2)/CO concentration at the electrode.Building upon this approach,we developed surface-functionalized catalysts with exceptional activity and selectivity for electrocatalytic CO_(2)RR to C_(2+)in a neutral electrolyte.Employing CuO nanoparticles coated with hexaethynylbenzene organic molecules(HEB-CuO NPs),a remarkable C_(2+)Faradaic efficiency of nearly 90%was achieved at an unprecedented current density of 300 mA cm^(-2),and a high FE(>80%)was maintained at a wide range of current densities(100-600 mA cm^(-2))in neutral environments using a flow cell.Furthermore,in a membrane electrode assembly(MEA)electrolyzer,86.14%FEC2+was achieved at a partial current density of 387.6 mA cm^(-2)while maintaining continuous operation for over 50 h at a current density of 200 mA cm^(-2).In-situ spectroscopy studies and molecular dynamics simulations reveal that reducing the coverage of coordinated K⋅H2O water increased the probability of intermediate reactants(CO)interacting with the surface,thereby promoting efficient C-C coupling and enhancing the yield of C_(2+)products.This advancement offers significant potential for optimizing local micro-environments for sustainable and highly efficient C_(2+)production.展开更多
The present paper renders a modeling and a 2D numerical simulation for the removal of CO_2from CO_2/CH_4gaseous stream utilizing sodium hydroxide(NaOH),monoethanolamine(MEA)and triethanolamine(TEA)liquid absorbents in...The present paper renders a modeling and a 2D numerical simulation for the removal of CO_2from CO_2/CH_4gaseous stream utilizing sodium hydroxide(NaOH),monoethanolamine(MEA)and triethanolamine(TEA)liquid absorbents inside the hollow fiber membrane contactor.Counter-current arrangement of absorbing agents and CO_2/CH_4gaseous mixture flows are implemented in the modeling and numerical simulation.Non-wetting and partial wetting modes of operation are considered where in the partial wetting mode,CO_2/CH_4gaseous mixture and liquid absorbents fill the membrane pores.The deteriorated removal of CO_2in the partial wetting mode of operation is mainly due to the mass transfer resistance imposed by the liquid in the pores of membrane.The validation of numerical simulation is done based on the comparison of simulation results of CO_2removal using Na OH and experimental data under non-wetting mode of operation.The comparison illustrates a desirable agreement with an average deviation of less than 5%.According to the results,MEA provides higher efficiency for CO_2removal in comparison with the other liquid absorbents.The order for CO_2removal performance is MEAN Na OHN TEA.The influence of non-wetting and partial wetting modes of operation on CO_2removal are evaluated in this article as one of the novelties.Besides,the percentage of CO_2sequestration as a function of gas velocity for various percentages of membrane pores wetting ranging from 0(non-wetting mode of operation)to 100%(complete wetting mode of operation)is studied in this research paper,which can be proposed as the other novelty.The results indicate that increase in some operational parameters such as module length,membrane porosity and absorbents concentration encourage the removal percentage of CO_2from CO_2/CH_4gaseous mixture while increasing in membrane tortuosity,gas velocity and initial CO_2concentration has unfavorable influence on the separation efficiency of CO_2.展开更多
Objective To investigate the photocatalytic degradation of gaseous ammonia in static state by using nano-TiO2 as photoeatalyst supported on latex paint film under UV-irradiation. Methods Experiments were conducted to ...Objective To investigate the photocatalytic degradation of gaseous ammonia in static state by using nano-TiO2 as photoeatalyst supported on latex paint film under UV-irradiation. Methods Experiments were conducted to study the relationship between the initial concentration of ammonia and the degradation products competing to be adsorbed on catalyst surface. Degradation of ammonia and its products were detected by spectrophotometry and catalytic kinetic spectrophotometry, respectively. Results On the one hand, TiO2 catalyst was excellent for degradation of ammonia, and the crystal phase of TiO2, anatase or ruffle, had little effect on degradation of ammonia, but the conversion of ammonia grew with the increase of catalyst content. On the other hand, apparent rate constant and conversion of ammonia decreased with the increase of initial concentration of ammonia, and the photocatalytic degradation reaction followed a pseudo-first-order expression due to-the evidence of linear correlation between -lnC/C0 vs. irradiation time t, but the relationship between initial concentration and the degradation products was not linear in low initial concentration. Conclusion Whether the photocatalytic degradation of ammonia in static state follows a first-order reaction depends on the initial ammonia concentration due to competition in adsorption between reactant and the degradation products.展开更多
The paper presented the results regarding the decomposition of gaseous CF_2ClB_r by cold plasma method.After two minutes discharge,the maximum decomposition rate of 2660 Pa CF_2ClB_r pure and 2660 Pa CF_2ClBr plus 798...The paper presented the results regarding the decomposition of gaseous CF_2ClB_r by cold plasma method.After two minutes discharge,the maximum decomposition rate of 2660 Pa CF_2ClB_r pure and 2660 Pa CF_2ClBr plus 7980 Pa O_2 reached 60% and 80%,respectively.The pa- per also studied the cold plasma gas phase chemistry reaction mechanism of CF_2ClBr at low pres- sure,and the pressure effects of CF_2ClBr and added gas(He,N_2,O_2 and dry air)on the CF_2ClBr decomposition respectively by cold plasma method.These studies will be helpful to application of cold plasma method in the treatment of hazardous gaseous wastes.展开更多
A method combining theoretical analysis with experiment is adopted and the flowing process of Ti-48A1-2Cr-2Nb alloy melt poured in a permanent mould during the centrifugal casting process has been analyzed. A mathemat...A method combining theoretical analysis with experiment is adopted and the flowing process of Ti-48A1-2Cr-2Nb alloy melt poured in a permanent mould during the centrifugal casting process has been analyzed. A mathematical model of the filling process is established and the forming mechanism of internal gaseous defect is summarized. The results of calculation show that the melt fills the mould with varying cross-section area and inclined angle. The filling speed of the cross-section is a function of filling time. The cross-section area is directly proportional to the filling speed and the inclined angle is inversely proportional to the filling speed at a given rotating speed of the platform. Both of them changes more obvious near the mould entrance. The gaseous defect can be formed in several ways and the centrifugal field has an important influence on the formation of the defect. In addition, the filling process in centrifugal field has been verified by wax experiments and the theoretical analysis are consistent with experimental results.展开更多
Measurements of gaseous pollutants （03, NOx, SO2, and CO） were conducted at Dinghushan background station in southern China from January to December 2013. The levels and variations of O3, NOx, SO2, and CO were analy...Measurements of gaseous pollutants （03, NOx, SO2, and CO） were conducted at Dinghushan background station in southern China from January to December 2013. The levels and variations of O3, NOx, SO2, and CO were analyzed and their possible causes discussed. The annual average concentrations of 03, NOx, SO2, and CO were 24.6 ± 23.9, 12.8 ± 10.2, 4.0 ± 4.8, and 348 ± 185 ppbv, respectively. The observed levels of the gaseous pollutants are comparable to those at other background sites in China. The most obvious diurnal variation of 03 was observed in autumn, with minima in the early morning and maxima in the afternoon. The diurnal variations of SO2 showed high values during the day. The diurnal cycles of NOx showed higher values in the morning and lower values during the night. Higher CO concentrations were observed in spring followed by winter, autumn, and summer. Biomass burning, in combination with the transport of regional pollution, is an important source of CO, SO2, and NOx in spring and winter. Backward trajectories were calculated and analyzed together with corresponding pollutant concentrations. The results indicate that air masses passing over polluted areas are responsible for the high concentrations of gaseous pollutants at the Dinghushan background station.展开更多
Experimental evidences of occurrence of gaseous diatomic sulfur produced in the low temperature catalytic decomposition of hydrogen sulfide 2 H2S ←→ 2 H2 ＋ S2 （g） are summarized. The S2 molecule is suggested to b...Experimental evidences of occurrence of gaseous diatomic sulfur produced in the low temperature catalytic decomposition of hydrogen sulfide 2 H2S ←→ 2 H2 ＋ S2 （g） are summarized. The S2 molecule is suggested to be in the ground triplet state. Analysis of literature data allows concluding that the S2 metastable singlet state is realized in the thermal dissociation of hydrogen sulfide and solid sulfur. Arguments in favor of the hypothesis are been discussed.展开更多
In this study,precise control over the thickness and termination of Ti3C2TX MXene flakes is achieved to enhance their electrical properties,environmental stability,and gas-sensing performance.Utilizing a hybrid method...In this study,precise control over the thickness and termination of Ti3C2TX MXene flakes is achieved to enhance their electrical properties,environmental stability,and gas-sensing performance.Utilizing a hybrid method involving high-pressure processing,stirring,and immiscible solutions,sub-100 nm MXene flake thickness is achieved within the MXene film on the Si-wafer.Functionalization control is achieved by defunctionalizing MXene at 650℃ under vacuum and H2 gas in a CVD furnace,followed by refunctionalization with iodine and bromine vaporization from a bubbler attached to the CVD.Notably,the introduction of iodine,which has a larger atomic size,lower electronegativity,reduce shielding effect,and lower hydrophilicity(contact angle:99°),profoundly affecting MXene.It improves the surface area(36.2 cm^(2) g^(-1)),oxidation stability in aqueous/ambient environments(21 days/80 days),and film conductivity(749 S m^(-1)).Additionally,it significantly enhances the gas-sensing performance,including the sensitivity(0.1119Ωppm^(-1)),response(0.2% and 23%to 50 ppb and 200 ppm NO_(2)),and response/recovery times(90/100 s).The reduced shielding effect of the–I-terminals and the metallic characteristics of MXene enhance the selectivity of I-MXene toward NO2.This approach paves the way for the development of stable and high-performance gas-sensing two-dimensional materials with promising prospects for future studies.展开更多
This paper investigates the possibility of using the free expansion of gaseous CO2 in portable air-cooling systems. The cooling capacity of the gaseous CO2 free jet expansion was calculated using three different appro...This paper investigates the possibility of using the free expansion of gaseous CO2 in portable air-cooling systems. The cooling capacity of the gaseous CO2 free jet expansion was calculated using three different approaches and the results showed that the simplified calculations would give approximated cooling values with an 11.6% maximum error. The mass flow rate, upstream pressure and cooling capacity of the gaseous CO2 decreased with time. A maximum 48.5 watts of cooling was recorded at minute 4 and a minimum value of 10.4 watts at the end of the test. The drop in cooling capacity is due to the evaporation of the liquid CO2 inside the small cylinder which cools the two-phase CO2 mixture and causes a pressure drop (from 6 MPa to 2.97 MPa), which also affects the mass flow rate of gaseous CO2 exiting the orifice (from 0.56 g/s to 0.24 g/s). If this cooling technique is to be considered in portable compact-cooling systems, the mass, pressure and cooling capacity drop with time must be solved. One of the solutions could be to cover the cylinder with a heating coat to compensate for the heat absorbed by the evaporation of the liquid CO2.展开更多
基金supported by the National Natural Science Foundation of China(22101182)the Shenzhen Science and Technology Program(Nos.JCYJ20210324095202006,JCYJ20220531095813031,and JCYJ20230807140700001)Guangdong Basic and Applied Basic Research Foundation(2022A1515010318).
文摘Surface functionalization of Cu-based catalysts has demonstrated promising potential for enhancing the electrochemical CO_(2)reduction reaction(CO_(2)RR)toward multi-carbon(C2+)products,primarily by suppressing the parasitic hydrogen evolution reaction and facilitating a localized CO_(2)/CO concentration at the electrode.Building upon this approach,we developed surface-functionalized catalysts with exceptional activity and selectivity for electrocatalytic CO_(2)RR to C_(2+)in a neutral electrolyte.Employing CuO nanoparticles coated with hexaethynylbenzene organic molecules(HEB-CuO NPs),a remarkable C_(2+)Faradaic efficiency of nearly 90%was achieved at an unprecedented current density of 300 mA cm^(-2),and a high FE(>80%)was maintained at a wide range of current densities(100-600 mA cm^(-2))in neutral environments using a flow cell.Furthermore,in a membrane electrode assembly(MEA)electrolyzer,86.14%FEC2+was achieved at a partial current density of 387.6 mA cm^(-2)while maintaining continuous operation for over 50 h at a current density of 200 mA cm^(-2).In-situ spectroscopy studies and molecular dynamics simulations reveal that reducing the coverage of coordinated K⋅H2O water increased the probability of intermediate reactants(CO)interacting with the surface,thereby promoting efficient C-C coupling and enhancing the yield of C_(2+)products.This advancement offers significant potential for optimizing local micro-environments for sustainable and highly efficient C_(2+)production.
文摘The present paper renders a modeling and a 2D numerical simulation for the removal of CO_2from CO_2/CH_4gaseous stream utilizing sodium hydroxide(NaOH),monoethanolamine(MEA)and triethanolamine(TEA)liquid absorbents inside the hollow fiber membrane contactor.Counter-current arrangement of absorbing agents and CO_2/CH_4gaseous mixture flows are implemented in the modeling and numerical simulation.Non-wetting and partial wetting modes of operation are considered where in the partial wetting mode,CO_2/CH_4gaseous mixture and liquid absorbents fill the membrane pores.The deteriorated removal of CO_2in the partial wetting mode of operation is mainly due to the mass transfer resistance imposed by the liquid in the pores of membrane.The validation of numerical simulation is done based on the comparison of simulation results of CO_2removal using Na OH and experimental data under non-wetting mode of operation.The comparison illustrates a desirable agreement with an average deviation of less than 5%.According to the results,MEA provides higher efficiency for CO_2removal in comparison with the other liquid absorbents.The order for CO_2removal performance is MEAN Na OHN TEA.The influence of non-wetting and partial wetting modes of operation on CO_2removal are evaluated in this article as one of the novelties.Besides,the percentage of CO_2sequestration as a function of gas velocity for various percentages of membrane pores wetting ranging from 0(non-wetting mode of operation)to 100%(complete wetting mode of operation)is studied in this research paper,which can be proposed as the other novelty.The results indicate that increase in some operational parameters such as module length,membrane porosity and absorbents concentration encourage the removal percentage of CO_2from CO_2/CH_4gaseous mixture while increasing in membrane tortuosity,gas velocity and initial CO_2concentration has unfavorable influence on the separation efficiency of CO_2.
基金This work has been supported by Shandong Provincial Scientific Council, People’s Republic of China (Grant No. Z2000B01)
文摘Objective To investigate the photocatalytic degradation of gaseous ammonia in static state by using nano-TiO2 as photoeatalyst supported on latex paint film under UV-irradiation. Methods Experiments were conducted to study the relationship between the initial concentration of ammonia and the degradation products competing to be adsorbed on catalyst surface. Degradation of ammonia and its products were detected by spectrophotometry and catalytic kinetic spectrophotometry, respectively. Results On the one hand, TiO2 catalyst was excellent for degradation of ammonia, and the crystal phase of TiO2, anatase or ruffle, had little effect on degradation of ammonia, but the conversion of ammonia grew with the increase of catalyst content. On the other hand, apparent rate constant and conversion of ammonia decreased with the increase of initial concentration of ammonia, and the photocatalytic degradation reaction followed a pseudo-first-order expression due to-the evidence of linear correlation between -lnC/C0 vs. irradiation time t, but the relationship between initial concentration and the degradation products was not linear in low initial concentration. Conclusion Whether the photocatalytic degradation of ammonia in static state follows a first-order reaction depends on the initial ammonia concentration due to competition in adsorption between reactant and the degradation products.
文摘The paper presented the results regarding the decomposition of gaseous CF_2ClB_r by cold plasma method.After two minutes discharge,the maximum decomposition rate of 2660 Pa CF_2ClB_r pure and 2660 Pa CF_2ClBr plus 7980 Pa O_2 reached 60% and 80%,respectively.The pa- per also studied the cold plasma gas phase chemistry reaction mechanism of CF_2ClBr at low pres- sure,and the pressure effects of CF_2ClBr and added gas(He,N_2,O_2 and dry air)on the CF_2ClBr decomposition respectively by cold plasma method.These studies will be helpful to application of cold plasma method in the treatment of hazardous gaseous wastes.
文摘A method combining theoretical analysis with experiment is adopted and the flowing process of Ti-48A1-2Cr-2Nb alloy melt poured in a permanent mould during the centrifugal casting process has been analyzed. A mathematical model of the filling process is established and the forming mechanism of internal gaseous defect is summarized. The results of calculation show that the melt fills the mould with varying cross-section area and inclined angle. The filling speed of the cross-section is a function of filling time. The cross-section area is directly proportional to the filling speed and the inclined angle is inversely proportional to the filling speed at a given rotating speed of the platform. Both of them changes more obvious near the mould entrance. The gaseous defect can be formed in several ways and the centrifugal field has an important influence on the formation of the defect. In addition, the filling process in centrifugal field has been verified by wax experiments and the theoretical analysis are consistent with experimental results.
基金supported by Strategic Priority Research Program of the Chinese Academy of Sciences (Grant No.XDA05100100)
文摘Measurements of gaseous pollutants （03, NOx, SO2, and CO） were conducted at Dinghushan background station in southern China from January to December 2013. The levels and variations of O3, NOx, SO2, and CO were analyzed and their possible causes discussed. The annual average concentrations of 03, NOx, SO2, and CO were 24.6 ± 23.9, 12.8 ± 10.2, 4.0 ± 4.8, and 348 ± 185 ppbv, respectively. The observed levels of the gaseous pollutants are comparable to those at other background sites in China. The most obvious diurnal variation of 03 was observed in autumn, with minima in the early morning and maxima in the afternoon. The diurnal variations of SO2 showed high values during the day. The diurnal cycles of NOx showed higher values in the morning and lower values during the night. Higher CO concentrations were observed in spring followed by winter, autumn, and summer. Biomass burning, in combination with the transport of regional pollution, is an important source of CO, SO2, and NOx in spring and winter. Backward trajectories were calculated and analyzed together with corresponding pollutant concentrations. The results indicate that air masses passing over polluted areas are responsible for the high concentrations of gaseous pollutants at the Dinghushan background station.
文摘Experimental evidences of occurrence of gaseous diatomic sulfur produced in the low temperature catalytic decomposition of hydrogen sulfide 2 H2S ←→ 2 H2 ＋ S2 （g） are summarized. The S2 molecule is suggested to be in the ground triplet state. Analysis of literature data allows concluding that the S2 metastable singlet state is realized in the thermal dissociation of hydrogen sulfide and solid sulfur. Arguments in favor of the hypothesis are been discussed.
基金supported by the National Research Foundation of Korea (NRF) grant funded by the Korean government (MSIT)(No. 2021R1I1A1A0105621313, No. 2022R1F1A1074441, No. 2022K1A3A1A20014496, and No. 2022R1F1A1074083)supported by the Ministry of Education Funding (No. RIS 2021-004)supported by the Brain Pool program funded by the Ministry of Science and ICT through the National Research Foundation of Korea (RS-2023-00284318).
文摘In this study,precise control over the thickness and termination of Ti3C2TX MXene flakes is achieved to enhance their electrical properties,environmental stability,and gas-sensing performance.Utilizing a hybrid method involving high-pressure processing,stirring,and immiscible solutions,sub-100 nm MXene flake thickness is achieved within the MXene film on the Si-wafer.Functionalization control is achieved by defunctionalizing MXene at 650℃ under vacuum and H2 gas in a CVD furnace,followed by refunctionalization with iodine and bromine vaporization from a bubbler attached to the CVD.Notably,the introduction of iodine,which has a larger atomic size,lower electronegativity,reduce shielding effect,and lower hydrophilicity(contact angle:99°),profoundly affecting MXene.It improves the surface area(36.2 cm^(2) g^(-1)),oxidation stability in aqueous/ambient environments(21 days/80 days),and film conductivity(749 S m^(-1)).Additionally,it significantly enhances the gas-sensing performance,including the sensitivity(0.1119Ωppm^(-1)),response(0.2% and 23%to 50 ppb and 200 ppm NO_(2)),and response/recovery times(90/100 s).The reduced shielding effect of the–I-terminals and the metallic characteristics of MXene enhance the selectivity of I-MXene toward NO2.This approach paves the way for the development of stable and high-performance gas-sensing two-dimensional materials with promising prospects for future studies.
文摘This paper investigates the possibility of using the free expansion of gaseous CO2 in portable air-cooling systems. The cooling capacity of the gaseous CO2 free jet expansion was calculated using three different approaches and the results showed that the simplified calculations would give approximated cooling values with an 11.6% maximum error. The mass flow rate, upstream pressure and cooling capacity of the gaseous CO2 decreased with time. A maximum 48.5 watts of cooling was recorded at minute 4 and a minimum value of 10.4 watts at the end of the test. The drop in cooling capacity is due to the evaporation of the liquid CO2 inside the small cylinder which cools the two-phase CO2 mixture and causes a pressure drop (from 6 MPa to 2.97 MPa), which also affects the mass flow rate of gaseous CO2 exiting the orifice (from 0.56 g/s to 0.24 g/s). If this cooling technique is to be considered in portable compact-cooling systems, the mass, pressure and cooling capacity drop with time must be solved. One of the solutions could be to cover the cylinder with a heating coat to compensate for the heat absorbed by the evaporation of the liquid CO2.
