The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic ...The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic material and renewable energy-generated electricity drive the conversion of carbon dioxide into high-value chemicals and carbon-neutral fuels.Over the past few years,single-atom catalysts have been intensively studied as they could provide near-unity atom utilization and unique catalytic performance.Single-atom catalysts have become one of the state-of-the-art catalyst materials for the electrochemical reduction of carbon dioxide into carbon monoxide.However,it remains a challenge for single-atom catalysts to facilitate the efficient conversion of carbon dioxide into products beyond carbon monoxide.In this review,we summarize and present important findings and critical insights from studies on the electrochemical carbon dioxide reduction reaction into hydrocarbons and oxygenates using single-atom catalysts.It is hoped that this review gives a thorough recapitulation and analysis of the science behind the catalysis of carbon dioxide into more reduced products through singleatom catalysts so that it can be a guide for future research and development on catalysts with industry-ready performance for the electrochemical reduction of carbon dioxide into high-value chemicals and carbon-neutral fuels.展开更多
In this work, we studied the catalytic activity of LaMnO3 and(La0.8A0.2)MnO3(A = Sr, K) perovskite catalysts for oxidation of NO and C10H22 and selective reduction of NO by C10H22. The catalytic per‐formances of thes...In this work, we studied the catalytic activity of LaMnO3 and(La0.8A0.2)MnO3(A = Sr, K) perovskite catalysts for oxidation of NO and C10H22 and selective reduction of NO by C10H22. The catalytic per‐formances of these perovskites were compared with that of a 2 wt% Pt/SiO2 catalyst. The La site substitution increased the catalytic properties for NO or C10H22 oxidation compared with the non‐substituted LaMnO3 sample. For the most efficient perovskite catalyst,(La0.8Sr0.2)MnO3, the results showed the presence of two temperature domains for NO adsorption:(1) a domain corre‐sponding to weakly adsorbed NO, desorbing at temperatures lower than 270 °C and(2) a second domain corresponding to NO adsorbed on the surface as nitrate species, desorbing at temperatures higher than 330 °C. For the Sr‐substituted perovskite, the maximum NO2 yield of 80% was observed in the intermediate temperature domain (around 285 °C). In the reactant mixture of NO/C10H22/O2/H2O/He,(La0.8Sr0.2)MnO3 perovskite showed better performance than the 2 wt% Pt/SiO2 catalyst: NO2 yields reaching 50% and 36% at 290 and 370 °C, respectively. This activity improvement was found to be because of atomic scale interactions between the A and B active sites, Sr2+ cation and Mn4+/Mn3+ redox couple. Thus,(La0.8Sr0.2)MnO3 perovskite could be an alternative free noble metal catalyst for exhaust gas after treatment.展开更多
A series of layered mixed oxides La 4BaCu 5-x Mn x O 13+λ ( x =0—5) was prepared, characterized and used as catalysts for NO+CO reaction. It was found that all the samples were single phase having a structure with f...A series of layered mixed oxides La 4BaCu 5-x Mn x O 13+λ ( x =0—5) was prepared, characterized and used as catalysts for NO+CO reaction. It was found that all the samples were single phase having a structure with five layered perovskite. La 4BaCu 2Mn 3O 13+λ showed the highest activity in the title reaction, this could be attributed to the synergetic effect between Cu and Mn. The results of TPR, TPD and excess oxygen investigations confirmed that the Cu ion would be the active center. The displacement of the Cu ion by Mn caused the Cu ion to be more easily reducible and more content of excess oxygen, and it was beneficial to the activity of the catalyst. The reaction mechanism was also proposed.展开更多
The presented work reports the selective catalytic reduction(SCR)of NO_(x) assisted by dielectric barrier discharge plasma via simulating marine diesel engine exhaust,and the experimental results demonstrate that the ...The presented work reports the selective catalytic reduction(SCR)of NO_(x) assisted by dielectric barrier discharge plasma via simulating marine diesel engine exhaust,and the experimental results demonstrate that the low-temperature activity of NH_(3)-SCR assisted by non-thermal plasma is enhanced significantly,particularly in the presence of a C_(3)H_(6) additive.Simultaneously,CeMnZrO_(x)@TiO_(2) exhibits strong tolerance to SO_(2) poisoning and superior catalytic stability.It is worthwhile to explore a new approach to remove NO_(x) from marine diesel engine exhaust,which is of vital significance for both academic research and practical applications.展开更多
To reduce CO_(2) emissions from coal-fired power plants,the development of low-carbon or carbon-free fuel combustion technologies has become urgent.As a new zero-carbon fuel,ammonia(NH_(3))can be used to address the s...To reduce CO_(2) emissions from coal-fired power plants,the development of low-carbon or carbon-free fuel combustion technologies has become urgent.As a new zero-carbon fuel,ammonia(NH_(3))can be used to address the storage and transportation issues of hydrogen energy.Since it is not feasible to completely replace coal with ammonia in the short term,the development of ammonia-coal co-combustion technology at the current stage is a fast and feasible approach to reduce CO_(2) emissions from coal-fired power plants.This study focuses on modifying the boiler and installing two layers of eight pure-ammonia burners in a 300-MW coal-fired power plant to achieve ammonia-coal co-combustion at proportions ranging from 20%to 10%(by heat ratio)at loads of 180-to 300-MW,respectively.The results show that,during ammonia-coal co-combustion in a 300-MW coal-fired power plant,there was a more significant change in NO_(x) emissions at the furnace outlet compared with that under pure-coal combustion as the boiler oxygen levels varied.Moreover,ammonia burners located in the middle part of the main combustion zone exhibited a better high-temperature reduction performance than those located in the upper part of the main combustion zone.Under all ammonia co-combustion conditions,the NH_(3) concentration at the furnace outlet remained below 1 parts per million(ppm).Compared with that under pure-coal conditions,the thermal efficiency of the boiler slightly decreased(by 0.12%-0.38%)under different loads when ammonia co-combustion reached 15 t·h^(-1).Ammonia co-combustion in coal-fired power plants is a potentially feasible technology route for carbon reduction.展开更多
Copper(Cu)provides a cost-effective means of producing value-added fuels through the electrochemical reduction of carbon dioxide(CO_(2)RR).However,we observed the production of hydrocarbons via CO_(2)RR on commercial ...Copper(Cu)provides a cost-effective means of producing value-added fuels through the electrochemical reduction of carbon dioxide(CO_(2)RR).However,we observed the production of hydrocarbons via CO_(2)RR on commercial Cu films is less efficient because of the surface impurities,i.e.,Fe.Carbon monoxide(CO),a reaction intermediate of CO_(2)RR to hydrocarbons,binds strongly to the Fe sites and interrupts the production of hydrocarbons,resulting in an active hydrogen evolution reaction(HER).Herein,we report a method of blocking the effect of Fe impurities on the Cu surface through the preferential growth of nano-sized metal-organic frameworks(MOFs)on Fe site.When zirconium(Zr)-based MOFs(UiO-66)forms a compensating layer on Cu film via the terephthalic acid(TPA)-Fe coordination bond,the Ui O-66 coated Cu film(UiO-66@Cu)presents significantly improved hydrocarbon Faradaic efficiency(FE)of 37.59%compared to 14.68%FE on commercial Cu film(99.9%purity)by suppressing HER.According to X-ray photoelectron spectroscopy(XPS)analysis,the UiO-66 ligand binds to entire metallic Fe site on the Cu surface,while metallic Cu is retained.Thus,UiO-66@Cu provides active sites of Cu for CO_(2)RR and leads to highly efficient and selective production of hydrocarbons.展开更多
Herein,we report the excellent De-NO_(x)performance of La0.7Sr0.3MnO3(LSM)perovskite-supported Pd catalysts(Pd-LSM)in alternating lean-burn/fuel-rich atmospheres using C3H6 as reductant and describe the in situ activa...Herein,we report the excellent De-NO_(x)performance of La0.7Sr0.3MnO3(LSM)perovskite-supported Pd catalysts(Pd-LSM)in alternating lean-burn/fuel-rich atmospheres using C3H6 as reductant and describe the in situ activation of the Pd catalysts via metal-support interaction(MSI)tuning.The NO_(x)reduction conversion of the Pd-LSM catalyst increased significantly from 56.1%to 90.1%and the production of N2O was suppressed.Our results demonstrated that this behavior was mainly attributed to the in situ transformation of Pd2+into Pd0 during the reaction.The generated Pd0 species could readily activate the C3H6 reductant and achieve an eight-fold higher turnover frequency than Pd2+for the reduction of NO_(x).Moreover,excessive MSIs inhibited the in situ generation of Pd0,and thereby,lowered the De-NO_(x)activity of the catalyst even at high Pd dispersion.In addition,the Pd-LSM catalysts exhibited much higher S tolerance than conventional Al_(2)O_(3)-supported catalysts.Our study provides a new approach for analyzing and designing highly active metal catalysts operated under dynamic alternating oxidizing/reducing atmospheric conditions.展开更多
In this study, we used a simple impregnation method to prepare Fe-Ce-O<sub> x </sub> catalysts and tested them regarding their low-temperature (200-300 °C) selective catalytic reduction (SCR) of ...In this study, we used a simple impregnation method to prepare Fe-Ce-O<sub> x </sub> catalysts and tested them regarding their low-temperature (200-300 °C) selective catalytic reduction (SCR) of NO using NH<sub>3</sub>. We investigated the effects of Fe/Ce molar ratio, the gas hourly space velocity (GHSV), the stability and SO<sub>2</sub>/H<sub>2</sub>O resistance of the catalysts. The results showed that the FeCe(1:6)O<sub> x </sub> (Ce/Fe molar ratio is 1:6) catalyst, which has some ordered parallel channels, exhibited good SCR performance. The FeCe(1:6)O<sub> x </sub> catalyst had the highest NO conversion with an activity of 94-99% at temperatures between 200 and 300 °C at a space velocity of 28,800 h<sup>−1</sup>. The NO conversion for the FeCe(1:6)O<sub> x </sub> catalyst also reached 80-98% between 200 and 300 °C at a space velocity of 204,000 h<sup>−1</sup>. In addition, the FeCe(1:6)O<sub> x </sub> catalyst demonstrated good stability in a 10-h SCR reaction at 200-300 °C. Even in the presence of SO<sub>2</sub> and H<sub>2</sub>O, the FeCe(1:6)O<sub> x </sub> catalyst exhibited good SCR performance.展开更多
The ultrafine alloy powders,CuRh,γ-Ni_(0.33)Fe_(0.66) and α-Fe_(0.66)Co_(0.33) of size less than 35 nm were prepared by reduction of complex metallic oxides under atmosphere of 15% H_2 and 85%Ar.
This study aims to improve a way for reducing backscattered radiation in an X-ray room. An iron steel grid, capable to absorb a significant portion of the backscattered radiation, was used. X-ray machine as a source f...This study aims to improve a way for reducing backscattered radiation in an X-ray room. An iron steel grid, capable to absorb a significant portion of the backscattered radiation, was used. X-ray machine as a source for radiation was directed normally on the phantom, and the backscattered radiation was measured by using ion chamber. The measurements were recorded at various applied voltages (60 kvp to 120 kvp) and the fabricated grid was designed from iron steel constructed of perpendicular parallel strips mounted on a base. The results indicated that the use of iron steel grid was very effective in the reduction of backscattered radiation in an X-ray room up to about 46% by using fabricated iron steel grid.展开更多
The synthesis of Sn-3.5Ag alloy nanosolder was investigated by chemical reduction method. In this method, chemical precipitation was achieved by using sodium NaBH4 as a reducing agent and PVP (poly-m-vinyl 2- pyrrolid...The synthesis of Sn-3.5Ag alloy nanosolder was investigated by chemical reduction method. In this method, chemical precipitation was achieved by using sodium NaBH4 as a reducing agent and PVP (poly-m-vinyl 2- pyrrolidone) as a stabilizer. The experimental results obtained with different amounts of NaBH4 and PVP were compared. X-ray diffraction (XRD) patterns revealed that Ag3Sn was formed due to the successful alloying process. Scanning Electron Microscopy (SEM) and Transmission Electron Microscopy (TEM) demonstrated a change in the morphology of Sn-3.5 Ag alloy nanosolder with increase in the PVP content in the bath. The size of the nanoparticles ranged from 300 to 700 nm. The nanosolder/nanoparticles were thus synthesized successfully under controlled and optimized chemical reduction process.展开更多
A photocatalyst composed of TiO 2 nanotube arrays（TNTs） and octahedral Cu2 O nanoparticles was fabricated,and its performance in the photocatalytic reduction of CO2 under visible and simulated solar irradiation was ...A photocatalyst composed of TiO 2 nanotube arrays（TNTs） and octahedral Cu2 O nanoparticles was fabricated,and its performance in the photocatalytic reduction of CO2 under visible and simulated solar irradiation was studied. The average nanotube diameter and length was 100 nm and 5 μm,respectively. The different amount of octahedral Cu2 O modified TNTs were obtained by varying electrochemical deposition time. TNTs modified with an optimized amount of Cu2 O nanoparticles exhibited high efficiency in the photocatalysis,and the predominant hydrocarbon product was methane. The methane yield increased with increasing Cu2 O content of the catalyst up to a certain deposition time,and decreased with further increase in Cu2 O deposition time. Insufficient deposition time（5 min） resulted in a small amount of Cu2 O nanoparticles on the TNTs,leading to the disadvantage of harvesting light. However,excess deposition time（45 min） gave rise to entire TNT surface being most covered with Cu2 O nanoparticles with large sizes,inconvenient for the transport of photo-generated carriers. The highest methane yield under simulated solar and visible light irradiation was observed for the catalysts prepared at a Cu2 O deposition time of 15 and 30 min respectively. The morphology,crystallization,photoresponse and electrochemical properties of the catalyst were characterized to understand the mechanism of its high photocatalytic activity. The TNT structure provided abundant active sites for the adsorption of reactants,and promoted the transport of photogenerated carriers that improved charge separation. Modifying the TNTs with octahedral Cu2 O nanoparticles promoted light absorption,and prevented the hydrocarbon product from oxidation. These factors provided the Cu2O-modified TNT photocatalyst with high efficiency in the reduction of CO2,without requiring co-catalysts or sacrificial agents.展开更多
The development of efficient single-atom catalysts(SACs) for the oxygen reduction reaction(ORR)remains a formidable challenge,primarily due to the symmetric charge distribution of metal singleatom sites(M-N_(4)).To ad...The development of efficient single-atom catalysts(SACs) for the oxygen reduction reaction(ORR)remains a formidable challenge,primarily due to the symmetric charge distribution of metal singleatom sites(M-N_(4)).To address such issue,herein,Fe-N_(x) sites coupled synergistic catalysts fabrication strategy is presented to break the uniform electronic distribution,thus enhancing the intrinsic catalytic activity.Precisely,atomically dispersed Fe-N_(x) sites supported on N/S-doped mesoporous carbon(NSC)coupled with FeS@C core-shell nanoparticles(FAS-NSC@950) is synthesized by a facile hydrothermal reaction and subsequent pyrolysis.Due to the presence of an in situ-grown conductive graphitic layer(shell),the FeS nanoparticles(core) effectively adjust the electronic structure of single-atom Fe sites and facilitate the ORR kinetics via short/long-range coupling interactions.Consequently,FAS-NSC@950displays a more positive half-wave potential(E_(1/2)) of 0.871 V with a significantly boosted ORR kinetics(Tafel slope=52.2 mV dec^(-1)),outpacing the commercial Pt/C(E_(1/2)=0.84 V and Tafel slope=54.6 mV dec^(-1)).As a bifunctional electrocatalyst,it displays a smaller bifunctional activity parameter(ΔE) of 0.673 V,surpassing the Pt/C-RuO_(2) combination(ΔE=0.724 V).Besides,the FAS-NSC@950-based zincair battery(ZAB) displays superior power density,specific capacity,and long-term cycling performance to the Pt/C-Ir/C-based ZAB.This work significantly contributes to the field by offering a promising strategy to enhance the catalytic activity of SACs for ORR,with potential implications for energy conversion and storage technologies.展开更多
MnO_(x)-Fe_(3)O_(4) nanomaterials were fabricated by using the innovative scheme of pyrolyzing manganesedoped iron-based metal organic framework in inert atmosphere and exhibited extraordinary performance of NO reduct...MnO_(x)-Fe_(3)O_(4) nanomaterials were fabricated by using the innovative scheme of pyrolyzing manganesedoped iron-based metal organic framework in inert atmosphere and exhibited extraordinary performance of NO reduction by CO(CO-SCR).Multi-technology characterizations were conducted to ascertain the properties of fabricated materials(e.g.,TGA,XRD,SEM,FT-IR,XPS,BET,H_(2)-TPR and O_(2)-TPD).Moreover,the interaction between reactants and catalysts was ascertained by in situ FT-IR.Experimental results demonstrated that Mn was an ideal promoter for iron oxides,resulting in decrease of crystallite size,improve reducibility property,enhance the mobility and the amount of lattice O^(2-) species,as well as strength the adsorption ability of active NO and CO to form multiple species(e.g.,nitrate and carbonate).The unprecedented enhancement of CO-SCR activity over Mn-Fe nanomaterials follows the Eley-Rideal(E-R)and Langmuir-Hinshelwood(L-H)reaction pathway.展开更多
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIP)(NRF,2021R1C1C1013953,2022K1A4A7A04094394,2022K1A4A7A04095890)。
文摘The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic material and renewable energy-generated electricity drive the conversion of carbon dioxide into high-value chemicals and carbon-neutral fuels.Over the past few years,single-atom catalysts have been intensively studied as they could provide near-unity atom utilization and unique catalytic performance.Single-atom catalysts have become one of the state-of-the-art catalyst materials for the electrochemical reduction of carbon dioxide into carbon monoxide.However,it remains a challenge for single-atom catalysts to facilitate the efficient conversion of carbon dioxide into products beyond carbon monoxide.In this review,we summarize and present important findings and critical insights from studies on the electrochemical carbon dioxide reduction reaction into hydrocarbons and oxygenates using single-atom catalysts.It is hoped that this review gives a thorough recapitulation and analysis of the science behind the catalysis of carbon dioxide into more reduced products through singleatom catalysts so that it can be a guide for future research and development on catalysts with industry-ready performance for the electrochemical reduction of carbon dioxide into high-value chemicals and carbon-neutral fuels.
基金Financial supports by national agency for research are gratefully acknowledged.
文摘In this work, we studied the catalytic activity of LaMnO3 and(La0.8A0.2)MnO3(A = Sr, K) perovskite catalysts for oxidation of NO and C10H22 and selective reduction of NO by C10H22. The catalytic per‐formances of these perovskites were compared with that of a 2 wt% Pt/SiO2 catalyst. The La site substitution increased the catalytic properties for NO or C10H22 oxidation compared with the non‐substituted LaMnO3 sample. For the most efficient perovskite catalyst,(La0.8Sr0.2)MnO3, the results showed the presence of two temperature domains for NO adsorption:(1) a domain corre‐sponding to weakly adsorbed NO, desorbing at temperatures lower than 270 °C and(2) a second domain corresponding to NO adsorbed on the surface as nitrate species, desorbing at temperatures higher than 330 °C. For the Sr‐substituted perovskite, the maximum NO2 yield of 80% was observed in the intermediate temperature domain (around 285 °C). In the reactant mixture of NO/C10H22/O2/H2O/He,(La0.8Sr0.2)MnO3 perovskite showed better performance than the 2 wt% Pt/SiO2 catalyst: NO2 yields reaching 50% and 36% at 290 and 370 °C, respectively. This activity improvement was found to be because of atomic scale interactions between the A and B active sites, Sr2+ cation and Mn4+/Mn3+ redox couple. Thus,(La0.8Sr0.2)MnO3 perovskite could be an alternative free noble metal catalyst for exhaust gas after treatment.
文摘A series of layered mixed oxides La 4BaCu 5-x Mn x O 13+λ ( x =0—5) was prepared, characterized and used as catalysts for NO+CO reaction. It was found that all the samples were single phase having a structure with five layered perovskite. La 4BaCu 2Mn 3O 13+λ showed the highest activity in the title reaction, this could be attributed to the synergetic effect between Cu and Mn. The results of TPR, TPD and excess oxygen investigations confirmed that the Cu ion would be the active center. The displacement of the Cu ion by Mn caused the Cu ion to be more easily reducible and more content of excess oxygen, and it was beneficial to the activity of the catalyst. The reaction mechanism was also proposed.
基金supported by National Key Research and Development Project of China(No.2019YFC1805503)National Engineering Laboratory for Mobile Source Emission Control Technology(No.NELMS2019A13)+1 种基金the Open Project Program of the State Key Laboratory of Petroleum Pollution Control(No.PPC2019013)Major Science and Technology Projects of Shanxi Province(No.20181102017)。
文摘The presented work reports the selective catalytic reduction(SCR)of NO_(x) assisted by dielectric barrier discharge plasma via simulating marine diesel engine exhaust,and the experimental results demonstrate that the low-temperature activity of NH_(3)-SCR assisted by non-thermal plasma is enhanced significantly,particularly in the presence of a C_(3)H_(6) additive.Simultaneously,CeMnZrO_(x)@TiO_(2) exhibits strong tolerance to SO_(2) poisoning and superior catalytic stability.It is worthwhile to explore a new approach to remove NO_(x) from marine diesel engine exhaust,which is of vital significance for both academic research and practical applications.
基金supported by the National Key Research and Development Program of China(2023YFB4005700,2023YFB4005705,and 2023YFB4005702-03)the Academy-Local Cooperation Project of the Chinese Academy of Engineering(2023-DFZD-01)+4 种基金the National Natural Science Foundation of China(52207151)the Natural Science Foundation of Anhui Province(2208085QA29)the University Synergy Innovation Program of Anhui Province(GXXT-2022025)the independent project of the Energy Research Institute of Hefei Comprehensive National Science Center(Anhui Energy Laboratory22KZZ525,23KZS402,22KZS301,and 22KZS304).
文摘To reduce CO_(2) emissions from coal-fired power plants,the development of low-carbon or carbon-free fuel combustion technologies has become urgent.As a new zero-carbon fuel,ammonia(NH_(3))can be used to address the storage and transportation issues of hydrogen energy.Since it is not feasible to completely replace coal with ammonia in the short term,the development of ammonia-coal co-combustion technology at the current stage is a fast and feasible approach to reduce CO_(2) emissions from coal-fired power plants.This study focuses on modifying the boiler and installing two layers of eight pure-ammonia burners in a 300-MW coal-fired power plant to achieve ammonia-coal co-combustion at proportions ranging from 20%to 10%(by heat ratio)at loads of 180-to 300-MW,respectively.The results show that,during ammonia-coal co-combustion in a 300-MW coal-fired power plant,there was a more significant change in NO_(x) emissions at the furnace outlet compared with that under pure-coal combustion as the boiler oxygen levels varied.Moreover,ammonia burners located in the middle part of the main combustion zone exhibited a better high-temperature reduction performance than those located in the upper part of the main combustion zone.Under all ammonia co-combustion conditions,the NH_(3) concentration at the furnace outlet remained below 1 parts per million(ppm).Compared with that under pure-coal conditions,the thermal efficiency of the boiler slightly decreased(by 0.12%-0.38%)under different loads when ammonia co-combustion reached 15 t·h^(-1).Ammonia co-combustion in coal-fired power plants is a potentially feasible technology route for carbon reduction.
基金supported by the Basic Science Research Program of the National Research Foundation of Korea(NRF2021R1A2C4001777,NRF-2021R1A2C2007823)the Carbon to X Project(NRF-2020M3H7A1098231)funded by the Ministry of Science and ICT,Republic of Koreasupported by the Technology Innovation Program(20013794,Center for Composite Materials and Concurrent Design)funded by the Ministry of Trade,Industry&Energy(MOTIE),Republic of Korea。
文摘Copper(Cu)provides a cost-effective means of producing value-added fuels through the electrochemical reduction of carbon dioxide(CO_(2)RR).However,we observed the production of hydrocarbons via CO_(2)RR on commercial Cu films is less efficient because of the surface impurities,i.e.,Fe.Carbon monoxide(CO),a reaction intermediate of CO_(2)RR to hydrocarbons,binds strongly to the Fe sites and interrupts the production of hydrocarbons,resulting in an active hydrogen evolution reaction(HER).Herein,we report a method of blocking the effect of Fe impurities on the Cu surface through the preferential growth of nano-sized metal-organic frameworks(MOFs)on Fe site.When zirconium(Zr)-based MOFs(UiO-66)forms a compensating layer on Cu film via the terephthalic acid(TPA)-Fe coordination bond,the Ui O-66 coated Cu film(UiO-66@Cu)presents significantly improved hydrocarbon Faradaic efficiency(FE)of 37.59%compared to 14.68%FE on commercial Cu film(99.9%purity)by suppressing HER.According to X-ray photoelectron spectroscopy(XPS)analysis,the UiO-66 ligand binds to entire metallic Fe site on the Cu surface,while metallic Cu is retained.Thus,UiO-66@Cu provides active sites of Cu for CO_(2)RR and leads to highly efficient and selective production of hydrocarbons.
文摘Herein,we report the excellent De-NO_(x)performance of La0.7Sr0.3MnO3(LSM)perovskite-supported Pd catalysts(Pd-LSM)in alternating lean-burn/fuel-rich atmospheres using C3H6 as reductant and describe the in situ activation of the Pd catalysts via metal-support interaction(MSI)tuning.The NO_(x)reduction conversion of the Pd-LSM catalyst increased significantly from 56.1%to 90.1%and the production of N2O was suppressed.Our results demonstrated that this behavior was mainly attributed to the in situ transformation of Pd2+into Pd0 during the reaction.The generated Pd0 species could readily activate the C3H6 reductant and achieve an eight-fold higher turnover frequency than Pd2+for the reduction of NO_(x).Moreover,excessive MSIs inhibited the in situ generation of Pd0,and thereby,lowered the De-NO_(x)activity of the catalyst even at high Pd dispersion.In addition,the Pd-LSM catalysts exhibited much higher S tolerance than conventional Al_(2)O_(3)-supported catalysts.Our study provides a new approach for analyzing and designing highly active metal catalysts operated under dynamic alternating oxidizing/reducing atmospheric conditions.
基金supported by the National Natural Science Foundation of China (No.21206108)Tianjin Municipal Science and Technology Commission (No.14JCYBJC21200)
文摘In this study, we used a simple impregnation method to prepare Fe-Ce-O<sub> x </sub> catalysts and tested them regarding their low-temperature (200-300 °C) selective catalytic reduction (SCR) of NO using NH<sub>3</sub>. We investigated the effects of Fe/Ce molar ratio, the gas hourly space velocity (GHSV), the stability and SO<sub>2</sub>/H<sub>2</sub>O resistance of the catalysts. The results showed that the FeCe(1:6)O<sub> x </sub> (Ce/Fe molar ratio is 1:6) catalyst, which has some ordered parallel channels, exhibited good SCR performance. The FeCe(1:6)O<sub> x </sub> catalyst had the highest NO conversion with an activity of 94-99% at temperatures between 200 and 300 °C at a space velocity of 28,800 h<sup>−1</sup>. The NO conversion for the FeCe(1:6)O<sub> x </sub> catalyst also reached 80-98% between 200 and 300 °C at a space velocity of 204,000 h<sup>−1</sup>. In addition, the FeCe(1:6)O<sub> x </sub> catalyst demonstrated good stability in a 10-h SCR reaction at 200-300 °C. Even in the presence of SO<sub>2</sub> and H<sub>2</sub>O, the FeCe(1:6)O<sub> x </sub> catalyst exhibited good SCR performance.
文摘The ultrafine alloy powders,CuRh,γ-Ni_(0.33)Fe_(0.66) and α-Fe_(0.66)Co_(0.33) of size less than 35 nm were prepared by reduction of complex metallic oxides under atmosphere of 15% H_2 and 85%Ar.
文摘This study aims to improve a way for reducing backscattered radiation in an X-ray room. An iron steel grid, capable to absorb a significant portion of the backscattered radiation, was used. X-ray machine as a source for radiation was directed normally on the phantom, and the backscattered radiation was measured by using ion chamber. The measurements were recorded at various applied voltages (60 kvp to 120 kvp) and the fabricated grid was designed from iron steel constructed of perpendicular parallel strips mounted on a base. The results indicated that the use of iron steel grid was very effective in the reduction of backscattered radiation in an X-ray room up to about 46% by using fabricated iron steel grid.
文摘The synthesis of Sn-3.5Ag alloy nanosolder was investigated by chemical reduction method. In this method, chemical precipitation was achieved by using sodium NaBH4 as a reducing agent and PVP (poly-m-vinyl 2- pyrrolidone) as a stabilizer. The experimental results obtained with different amounts of NaBH4 and PVP were compared. X-ray diffraction (XRD) patterns revealed that Ag3Sn was formed due to the successful alloying process. Scanning Electron Microscopy (SEM) and Transmission Electron Microscopy (TEM) demonstrated a change in the morphology of Sn-3.5 Ag alloy nanosolder with increase in the PVP content in the bath. The size of the nanoparticles ranged from 300 to 700 nm. The nanosolder/nanoparticles were thus synthesized successfully under controlled and optimized chemical reduction process.
基金supported by the National Natural Science Foundation of China(2137704421573085)+5 种基金the Key Project of Natural Science Foundation of Hubei Province(2015CFA037)Wuhan Planning Project of Science and Technology(2014010101010023)Self-determined Research Funds of CCNU from the Colleges’Basic Research and Operation of MOE(CCNU15ZD007CCNU15KFY005)China Postdoctoral Science Foundation(2015M572187)Hubei Provincial Department of Education(D20152702)~~
文摘A photocatalyst composed of TiO 2 nanotube arrays（TNTs） and octahedral Cu2 O nanoparticles was fabricated,and its performance in the photocatalytic reduction of CO2 under visible and simulated solar irradiation was studied. The average nanotube diameter and length was 100 nm and 5 μm,respectively. The different amount of octahedral Cu2 O modified TNTs were obtained by varying electrochemical deposition time. TNTs modified with an optimized amount of Cu2 O nanoparticles exhibited high efficiency in the photocatalysis,and the predominant hydrocarbon product was methane. The methane yield increased with increasing Cu2 O content of the catalyst up to a certain deposition time,and decreased with further increase in Cu2 O deposition time. Insufficient deposition time（5 min） resulted in a small amount of Cu2 O nanoparticles on the TNTs,leading to the disadvantage of harvesting light. However,excess deposition time（45 min） gave rise to entire TNT surface being most covered with Cu2 O nanoparticles with large sizes,inconvenient for the transport of photo-generated carriers. The highest methane yield under simulated solar and visible light irradiation was observed for the catalysts prepared at a Cu2 O deposition time of 15 and 30 min respectively. The morphology,crystallization,photoresponse and electrochemical properties of the catalyst were characterized to understand the mechanism of its high photocatalytic activity. The TNT structure provided abundant active sites for the adsorption of reactants,and promoted the transport of photogenerated carriers that improved charge separation. Modifying the TNTs with octahedral Cu2 O nanoparticles promoted light absorption,and prevented the hydrocarbon product from oxidation. These factors provided the Cu2O-modified TNT photocatalyst with high efficiency in the reduction of CO2,without requiring co-catalysts or sacrificial agents.
基金financially supported by the National Natural Science Foundation of China(21773024)the Natural Science Foundation of Sichuan Province of China(2023NSFC0084)the China Postdoctoral Science Foundation(2019M663469)。
文摘The development of efficient single-atom catalysts(SACs) for the oxygen reduction reaction(ORR)remains a formidable challenge,primarily due to the symmetric charge distribution of metal singleatom sites(M-N_(4)).To address such issue,herein,Fe-N_(x) sites coupled synergistic catalysts fabrication strategy is presented to break the uniform electronic distribution,thus enhancing the intrinsic catalytic activity.Precisely,atomically dispersed Fe-N_(x) sites supported on N/S-doped mesoporous carbon(NSC)coupled with FeS@C core-shell nanoparticles(FAS-NSC@950) is synthesized by a facile hydrothermal reaction and subsequent pyrolysis.Due to the presence of an in situ-grown conductive graphitic layer(shell),the FeS nanoparticles(core) effectively adjust the electronic structure of single-atom Fe sites and facilitate the ORR kinetics via short/long-range coupling interactions.Consequently,FAS-NSC@950displays a more positive half-wave potential(E_(1/2)) of 0.871 V with a significantly boosted ORR kinetics(Tafel slope=52.2 mV dec^(-1)),outpacing the commercial Pt/C(E_(1/2)=0.84 V and Tafel slope=54.6 mV dec^(-1)).As a bifunctional electrocatalyst,it displays a smaller bifunctional activity parameter(ΔE) of 0.673 V,surpassing the Pt/C-RuO_(2) combination(ΔE=0.724 V).Besides,the FAS-NSC@950-based zincair battery(ZAB) displays superior power density,specific capacity,and long-term cycling performance to the Pt/C-Ir/C-based ZAB.This work significantly contributes to the field by offering a promising strategy to enhance the catalytic activity of SACs for ORR,with potential implications for energy conversion and storage technologies.
基金We acknowledge the financial support of the National Natural Science Foundation of China(Nos.21866022,21567018)Inner Mongolia"Grassland talents"project,Inner Mongolia Key Laboratory of Environmental Pollution Control and Waste Resource Recycle,Key Laboratory of Ecology and Resource Use of the Mongolian Plateau and Collaborative Innovation Center for Grassland Ecological Security,Ministry of Education of China.
文摘MnO_(x)-Fe_(3)O_(4) nanomaterials were fabricated by using the innovative scheme of pyrolyzing manganesedoped iron-based metal organic framework in inert atmosphere and exhibited extraordinary performance of NO reduction by CO(CO-SCR).Multi-technology characterizations were conducted to ascertain the properties of fabricated materials(e.g.,TGA,XRD,SEM,FT-IR,XPS,BET,H_(2)-TPR and O_(2)-TPD).Moreover,the interaction between reactants and catalysts was ascertained by in situ FT-IR.Experimental results demonstrated that Mn was an ideal promoter for iron oxides,resulting in decrease of crystallite size,improve reducibility property,enhance the mobility and the amount of lattice O^(2-) species,as well as strength the adsorption ability of active NO and CO to form multiple species(e.g.,nitrate and carbonate).The unprecedented enhancement of CO-SCR activity over Mn-Fe nanomaterials follows the Eley-Rideal(E-R)and Langmuir-Hinshelwood(L-H)reaction pathway.
