Developing efficient and stable cathodes for low-temperature solid oxide fuel cells(LT-SOFCs) is of great importance for the practical commercialization.Herein,we propose a series of Sm-modified Bi_(0.7-x)Sm_xSr_(0.3)...Developing efficient and stable cathodes for low-temperature solid oxide fuel cells(LT-SOFCs) is of great importance for the practical commercialization.Herein,we propose a series of Sm-modified Bi_(0.7-x)Sm_xSr_(0.3)FeO_(3-δ) perovskites as highly-active catalysts for LT-SOFCs.Sm doping can significantly enhance the electrocata lytic activity and chemical stability of cathode.At 600℃,Bi_(0.675)Sm_(0.025)Sr_(0.3)FeO_(3-δ)(BSSF25) cathode has been found to be the optimum composition with a polarization resistance of 0.098 Ω cm^2,which is only around 22.8% of Bi_(0.7)Sr_(0.3)FeO_(3-δ)(BSF).A full cell utilizing BSSF25 displays an exceptional output density of 790 mW cm^(-2),which can operate continuously over100 h without obvious degradation.The remarkable electrochemical performance observed can be attributed to the improved O_(2) transport kinetics,superior surface oxygen adsorption capacity,as well as O_(2)p band centers in close proximity to the Fermi level.Moreover,larger average bonding energy(ABE) and the presence of highly acidic Bi,Sm,and Fe ions restrict the adsorption of CO_(2) on the cathode surface,resulting in excellent CO_(2) resistivity.This work provides valuable guidance for systematic design of efficient and durable catalysts for LT-SOFCs.展开更多
Iron‐based pyrophosphates are attractive cathodes for sodium‐ion batteries due to their large framework,cost‐effectiveness,and high energy density.However,the understanding of the crystal structure is scarce and on...Iron‐based pyrophosphates are attractive cathodes for sodium‐ion batteries due to their large framework,cost‐effectiveness,and high energy density.However,the understanding of the crystal structure is scarce and only a limited candidates have been reported so far.In this work,we found for the first time that a continuous solid solution,Na_(4−α)Fe_(2+α)_(2)(P_(2)O_(7))_(2)(0≤α≤1,could be obtained by mutual substitution of cations at center‐symmetric Na3 and Na4 sites while keeping the crystal building blocks of anionic P_(2)O_(7) unchanged.In particular,a novel off‐stoichiometric Na_(3)Fe(2.5)(P_(2)O_(7))_(2)is thus proposed,and its structure,energy storage mechanism,and electrochemical performance are extensively investigated to unveil the structure–function relationship.The as‐prepared off‐stoichiometric electrode delivers appealing performance with a reversible discharge capacity of 83 mAh g^(−1),a working voltage of 2.9 V(vs.Na^(+)/Na),the retention of 89.2%of the initial capacity after 500 cycles,and enhanced rate capability of 51 mAh g^(−1)at a current density of 1600 mA g^(−1).This research shows that sodium ferric pyrophosphate could form extended solid solution composition and promising phase is concealed in the range of Na_(4−α)Fe_(2+α)_(2)(P_(2)O_(7))_(2),offering more chances for exploration of new cathode materials for the construction of high‐performance SIBs.展开更多
Solid oxide electrolysis cells(SOECs),displaying high current density and energy efficiency,have been proven to be an effective technique to electrochemically reduce CO_(2)into CO.However,the insufficiency of cathode ...Solid oxide electrolysis cells(SOECs),displaying high current density and energy efficiency,have been proven to be an effective technique to electrochemically reduce CO_(2)into CO.However,the insufficiency of cathode activity and stability is a tricky problem to be addressed for SOECs.Hence,it is urgent to develop suitable cathode materials with excellent catalytic activity and stability for further practical application of SOECs.Herein,a reduced perovskite oxide,Pr_(0.35)Sr_(0.6)Fe_(0.7)Cu_(0.2)Mo_(0.1)O_(3-δ)(PSFCM0.35),is developed as SOECs cathode to electrolyze CO_(2).After reduction in 10%H_(2)/Ar,Cu and Fe nanoparticles are exsolved from the PSFCM0.35 lattice,resulting in a phase transformation from cubic perovskite to Ruddlesden-Popper(RP)perovskite with more oxygen vacancies.The exsolved metal nanoparticles are tightly attached to the perovskite substrate and afford more active sites to accelerate CO_(2)adsorption and dissociation on the cathode surface.The significantly strengthened CO_(2)adsorption capacity obtained after reduction is demonstrated by in situ Fourier transform-infrared(FT-IR)spectra.Symmetric cells with the reduced PSFCM0.35(R-PSFCM0.35)electrode exhibit a low polarization resistance of 0.43Ωcm^(2)at 850℃.Single electrolysis cells with the R-PSFCM0.35 cathode display an outstanding current density of 2947 mA cm^(-2)at 850℃and 1.6 V.In addition,the catalytic stability of the R-PSFCM0.35 cathode is also proved by operating at 800℃with an applied constant current density of 600 mA cm^(-2)for 100 h.展开更多
The insurmountable charge transfer impedance at the Li metal/solid polymer electrolytes(SPEs)interface at room temperature as well as the ascending risk of short circuits at the operating temperature higher than the m...The insurmountable charge transfer impedance at the Li metal/solid polymer electrolytes(SPEs)interface at room temperature as well as the ascending risk of short circuits at the operating temperature higher than the melting point,dominantly limits their applications in solid-state batteries(SSBs).Although the inorganic filler such as CeO_(2)nanoparticle content of composite solid polymer electrolytes(CSPEs)can significantly reduce the enormous charge transfer impedance at the Li metal/SPEs interface,we found that the required content of CeO_(2)nanoparticles in SPEs varies for achieving a decent interfacial charge transfer impedance and the bulk ionic conductivity in CSPEs.In this regard,a sandwich-type composited solid polymer electrolyte with a 10%CeO_(2)CSPEs interlayer sandwiched between two 50%CeO_(2)CSPEs thin layers(sandwiched CSPEs)is constructed to simultaneously achieve low charge transfer impedance and superior ionic conductivity at 30℃.The sandwiched CSPEs allow for stable cycling of Li plating and stripping for 1000 h with 129 mV polarized voltage at 0.1 mA cm^(-2)and 30℃.In addition,the LiFePO_(4)/Sandwiched CSPEs/Li cell also exhibits exceptional cycle performance at 30℃and even elevated120℃without short circuits.Constructing multi-layered CSPEs with optimized contents of the inorganic fillers can be an efficient method for developing all solid-state PEO-based batteries with high performance at a wide range of temperatures.展开更多
MgH_(2) and TiH_(2) have been extensively studied as potential anode materials due to their high theoretical specific capacities of 2036 and 1024 mAh/g,respectively.However,the large volume changes that these compound...MgH_(2) and TiH_(2) have been extensively studied as potential anode materials due to their high theoretical specific capacities of 2036 and 1024 mAh/g,respectively.However,the large volume changes that these compounds undergo during cycling affects their performance and limits practical applications.The present work demonstrates a novel approach to limiting the volume changes of active materials.This effect is based on mechanical support from an intimate interface generated in situ via the reaction between MgH_(2) and Ti within the electrode prior to lithiation to form Mg and TiH_(2).The resulting Mg can be transformed back to MgH_(2) by reaction with LiH during delithiation.In addition,the TiH_(2) improves the reaction kinetics of MgH_(2) and enhances electrochemical performance.The intimate interface produced in this manner is found to improve the electrochemical properties of a MgH_(2)-Ti-LiH electrode.An exceptional reversible capacity of 800 mAh/g is observed even after 200 cycles with a high current density of 1 mA/cm^(2) and a high proportion of active material(90 wt.%)at an operation temperature of 120℃.This study therefore showcases a new means of improving the performance of electrodes by limiting the volume changes of active materials.展开更多
Tungstated zirconia(WO_(3)/ZrO_(2))solid acid catalysts with different WO_(3) contents were prepared by a hydrothermal method and then used in the catalytic aquathermolysis of heavy oil from Xinjiang.The WO_(3)/ZrO_(2...Tungstated zirconia(WO_(3)/ZrO_(2))solid acid catalysts with different WO_(3) contents were prepared by a hydrothermal method and then used in the catalytic aquathermolysis of heavy oil from Xinjiang.The WO_(3)/ZrO_(2) solid acid catalyst was characterized by a range of characterization methods,including X-ray diffraction,NH3-temperature programmed desorption,and pyridine infrared spectroscopy.The WO_(3) content of the WO_(3)/ZrO_(2) catalysts had an important impact on the structure and property of the catalysts.When the WO_(3) mass fraction was 20%,it facilitated the formation of tetragonal zirconia,thereby enhancing the creation of robust acidic sites.Acidity is considered to have a strong impact on the catalytic performance of the aquathermolysis of heavy oil.When the catalyst containing 20%WO_(3) was used to catalyze the aquathermolysis of heavy oil under conditions of 14.5 MPa,340℃,and 24 h,the viscosity of heavy oil decreased from 47266 to 5398 mPa·s and the viscosity reduction rate reached 88.6%.The physicochemical properties of heavy oil before and after the aquathermolysis were analyzed using a saturates,aromatics,resins,and asphaltenes analysis,gas chromatography,elemental analysis,densimeter etc.After the aquathermolysis,the saturate and aromatic contents significantly increased from 43.3%to 48.35%and 19.47%to 21.88%,respectively,with large reductions in the content of resin and asphaltene from 28.22%to 25.06%and 5.36%to 2.03%,respectively.The sulfur and nitrogen contents,and the density of the oil were significantly decreased.These factors were likely the main reasons for promoting the viscosity reduction of heavy oil during the aquathermolysis over the WO_(3)/ZrO_(2) solid acid catalysts.展开更多
Changing the N content in the Ti_(3)AlC_(2−y)N_(y) MAX phase solid solutions allows for the fine-tuning of their properties.However,systematic studies on the synthesis and properties of Ti_(3)AlC_(2−y)N_(y) solid solu...Changing the N content in the Ti_(3)AlC_(2−y)N_(y) MAX phase solid solutions allows for the fine-tuning of their properties.However,systematic studies on the synthesis and properties of Ti_(3)AlC_(2−y)N_(y) solid solution bulks have not been reported thus far.Here,previously reported Ti_(3)AlC_(2−y)N_(y) solid solution bulks(y=0.3,0.5,0.8,and 1.0)were synthesized via hot pressing of their powder counterparts under optimized conditions.The prepared Ti_(3)AlC_(2−y)N_(y) bulks are dense and have a fine microstructure with grain sizes of 6–8μm.The influence of the N content on the mechanical properties,electrical conductivities,and coefficients of thermal expansion(CTEs)of the prepared Ti_(3)AlC_(2−y)N_(y) bulk materials was clarified.The flexural strength and Vickers hardness values increased with increasing N content,suggesting that solid solution strengthening effectively improved the mechanical properties of Ti_(3)AlC_(2−y)N_(y).Ti_(3)AlCN(y=1)had the highest Vickers hardness and flexural strength among the studied samples,reaching 5.54 GPa and 550 MPa,respectively.However,the electrical conductivity and CTEs of the Ti_(3)AlC_(2−y)N_(y) solid solutions decreased with increasing N content,from 8.93×10^(−6) to 7.69×10^(−6) K^(−1) and from 1.33×10^(6) to 0.95×10^(6) S/m,respectively.This work demonstrated the tunable properties of Ti_(3)AlC_(2−y)N_(y) solid solutions with varying N contents and widened the MAX phase family for fundamental studies and applications.展开更多
Physical vapor deposition(PVD)can be used to produce high-quality Gd_(2)O_(3)-doped CeO2(GDC)films.Among various PVD methods,reactive sputtering provides unique benefits,such as high deposition rates and easy upscalin...Physical vapor deposition(PVD)can be used to produce high-quality Gd_(2)O_(3)-doped CeO2(GDC)films.Among various PVD methods,reactive sputtering provides unique benefits,such as high deposition rates and easy upscaling for industrial applications.GDC thin films were successfully fabricated through reactive sputtering using a Gd_(0.2)Ce_(0.8)(at%)metallic target,and their application in solid oxide fuel cells,such as buffer layers between yttria-stabilized zirconia(YSZ)/La0.6Sr0.4Co0.2Fe0.8O_(3−δ)and as sublayers in the steel/coating system,was evaluated.First,the direct current(DC)reactive-sputtering behavior of the GdCe metallic target was determined.Then,the GDC films were deposited on NiO-YSZ/YSZ half-cells to investigate the influence of oxygen flow rate on the quality of annealed GDC films.The results demonstrated that reactive sputtering can be used to prepare thin and dense GDC buffer layers without high-temperature sintering.Furthermore,the cells with a sputtered GDC buffer layer showed better electrochemical performance than those with a screen-printed GDC buffer layer.In addition,the insertion of a GDC sublayer between the SUS441 interconnects and the Mn-Co spinel coatings contributed to the reduction of the oxidation rate for SUS441 at operating temperatures,according to the area-specific resistance tests.展开更多
The significant decrease of acid sites caused by alkali metal poisoning is the major factor in the deactivation of commercial V_(2)O_(5)-WO_(3)/TiO_(2)NH_(3)-SCR catalysts.In this work,the solid superacid SO_(4)^(2-)-...The significant decrease of acid sites caused by alkali metal poisoning is the major factor in the deactivation of commercial V_(2)O_(5)-WO_(3)/TiO_(2)NH_(3)-SCR catalysts.In this work,the solid superacid SO_(4)^(2-)-TiO_(2) modified by sulfate radicals,was selected as the catalyst support,which showed superior potassium resistance.The physicochemical properties and K-poisoning resistance of the V_(2)O_(5)-WO_(3)/SO_(4)^(2-)-TiO_(2)(VWSTi) catalyst were carried out by XRD,BET,H2-TPR,NH3-TPD,XPS,in situ DRIFTS and TG.The results pointed out that the introduction of SO_(4)^(2-)significantly increased the NH3-SCR catalytic activity at high temperatures,with an exceptionally high NO_(x) conversion over 90% between 275℃ and 500℃.When 0.5%(mass) K_(2)O was doped on the catalysts,the catalytic performance of the traditional V_(2)O_(5)-WO_(3)/TiO_(2)(VWTi) catalyst decreased significantly,while the VWSTi catalyst could still maintain a NOxconversion over 90%in the range of 300–500℃.The characterizations suggested that the support of SO_(4)^(2-)-TiO_(2) greatly increased the number of acidic sites,thereby enhancing the adsorption capacity of the reactant NH_(3).The results above demonstrated a potential approach to achieve superior potassium resistance for NH3-SCR catalysts using solid superacid.展开更多
基金supported by the National Natural Science Foundation of China(22279025,21773048)the Natural Science Foundation of Heilongjiang Province(LH2021A013)+1 种基金the Sichuan Science and Technology Program(2021YFSY0022)the Fundamental Research Funds for the Central Universities(2023FRFK06005,HIT.NSRIF202204)。
文摘Developing efficient and stable cathodes for low-temperature solid oxide fuel cells(LT-SOFCs) is of great importance for the practical commercialization.Herein,we propose a series of Sm-modified Bi_(0.7-x)Sm_xSr_(0.3)FeO_(3-δ) perovskites as highly-active catalysts for LT-SOFCs.Sm doping can significantly enhance the electrocata lytic activity and chemical stability of cathode.At 600℃,Bi_(0.675)Sm_(0.025)Sr_(0.3)FeO_(3-δ)(BSSF25) cathode has been found to be the optimum composition with a polarization resistance of 0.098 Ω cm^2,which is only around 22.8% of Bi_(0.7)Sr_(0.3)FeO_(3-δ)(BSF).A full cell utilizing BSSF25 displays an exceptional output density of 790 mW cm^(-2),which can operate continuously over100 h without obvious degradation.The remarkable electrochemical performance observed can be attributed to the improved O_(2) transport kinetics,superior surface oxygen adsorption capacity,as well as O_(2)p band centers in close proximity to the Fermi level.Moreover,larger average bonding energy(ABE) and the presence of highly acidic Bi,Sm,and Fe ions restrict the adsorption of CO_(2) on the cathode surface,resulting in excellent CO_(2) resistivity.This work provides valuable guidance for systematic design of efficient and durable catalysts for LT-SOFCs.
基金National Natural Science Foundation of China,Grant/Award Numbers:21972108,U20A20249,U22A20438Changzhou Science and Technology Bureau,Grant/Award Number:CM20223017Innovation and Technology Commission(ITC)of Hong Kong,The Innovation&Technology Fund(ITF)with Project No.ITS/126/21。
文摘Iron‐based pyrophosphates are attractive cathodes for sodium‐ion batteries due to their large framework,cost‐effectiveness,and high energy density.However,the understanding of the crystal structure is scarce and only a limited candidates have been reported so far.In this work,we found for the first time that a continuous solid solution,Na_(4−α)Fe_(2+α)_(2)(P_(2)O_(7))_(2)(0≤α≤1,could be obtained by mutual substitution of cations at center‐symmetric Na3 and Na4 sites while keeping the crystal building blocks of anionic P_(2)O_(7) unchanged.In particular,a novel off‐stoichiometric Na_(3)Fe(2.5)(P_(2)O_(7))_(2)is thus proposed,and its structure,energy storage mechanism,and electrochemical performance are extensively investigated to unveil the structure–function relationship.The as‐prepared off‐stoichiometric electrode delivers appealing performance with a reversible discharge capacity of 83 mAh g^(−1),a working voltage of 2.9 V(vs.Na^(+)/Na),the retention of 89.2%of the initial capacity after 500 cycles,and enhanced rate capability of 51 mAh g^(−1)at a current density of 1600 mA g^(−1).This research shows that sodium ferric pyrophosphate could form extended solid solution composition and promising phase is concealed in the range of Na_(4−α)Fe_(2+α)_(2)(P_(2)O_(7))_(2),offering more chances for exploration of new cathode materials for the construction of high‐performance SIBs.
基金supported by the National Natural Science Foundation of China(No.22278203,No.22279057)the support of the Inner Mongolia major science and technology project(2021ZD0042),Development of integrated technology for CO_(2)emission reduction in electric power metallurgy industry
文摘Solid oxide electrolysis cells(SOECs),displaying high current density and energy efficiency,have been proven to be an effective technique to electrochemically reduce CO_(2)into CO.However,the insufficiency of cathode activity and stability is a tricky problem to be addressed for SOECs.Hence,it is urgent to develop suitable cathode materials with excellent catalytic activity and stability for further practical application of SOECs.Herein,a reduced perovskite oxide,Pr_(0.35)Sr_(0.6)Fe_(0.7)Cu_(0.2)Mo_(0.1)O_(3-δ)(PSFCM0.35),is developed as SOECs cathode to electrolyze CO_(2).After reduction in 10%H_(2)/Ar,Cu and Fe nanoparticles are exsolved from the PSFCM0.35 lattice,resulting in a phase transformation from cubic perovskite to Ruddlesden-Popper(RP)perovskite with more oxygen vacancies.The exsolved metal nanoparticles are tightly attached to the perovskite substrate and afford more active sites to accelerate CO_(2)adsorption and dissociation on the cathode surface.The significantly strengthened CO_(2)adsorption capacity obtained after reduction is demonstrated by in situ Fourier transform-infrared(FT-IR)spectra.Symmetric cells with the reduced PSFCM0.35(R-PSFCM0.35)electrode exhibit a low polarization resistance of 0.43Ωcm^(2)at 850℃.Single electrolysis cells with the R-PSFCM0.35 cathode display an outstanding current density of 2947 mA cm^(-2)at 850℃and 1.6 V.In addition,the catalytic stability of the R-PSFCM0.35 cathode is also proved by operating at 800℃with an applied constant current density of 600 mA cm^(-2)for 100 h.
基金supported by the National Key R&D Program of China(2021YFB2400400)the National Natural Science Foundation of China(Grant No.22379120,22179085)+5 种基金the Key Research and Development Plan of Shanxi Province(China,Grant No.2018ZDXM-GY-135,2021JLM-36)the National Natural Science Foundation of China(Grant No.22108218)the“Young Talent Support Plan”of Xi’an Jiaotong University(71211201010723)the Qinchuangyuan Innovative Talent Project(QCYRCXM-2022-137)the“Young Talent Support Plan”of Xi’an Jiaotong University(HG6J003)the“1000-Plan program”of Shaanxi Province。
文摘The insurmountable charge transfer impedance at the Li metal/solid polymer electrolytes(SPEs)interface at room temperature as well as the ascending risk of short circuits at the operating temperature higher than the melting point,dominantly limits their applications in solid-state batteries(SSBs).Although the inorganic filler such as CeO_(2)nanoparticle content of composite solid polymer electrolytes(CSPEs)can significantly reduce the enormous charge transfer impedance at the Li metal/SPEs interface,we found that the required content of CeO_(2)nanoparticles in SPEs varies for achieving a decent interfacial charge transfer impedance and the bulk ionic conductivity in CSPEs.In this regard,a sandwich-type composited solid polymer electrolyte with a 10%CeO_(2)CSPEs interlayer sandwiched between two 50%CeO_(2)CSPEs thin layers(sandwiched CSPEs)is constructed to simultaneously achieve low charge transfer impedance and superior ionic conductivity at 30℃.The sandwiched CSPEs allow for stable cycling of Li plating and stripping for 1000 h with 129 mV polarized voltage at 0.1 mA cm^(-2)and 30℃.In addition,the LiFePO_(4)/Sandwiched CSPEs/Li cell also exhibits exceptional cycle performance at 30℃and even elevated120℃without short circuits.Constructing multi-layered CSPEs with optimized contents of the inorganic fillers can be an efficient method for developing all solid-state PEO-based batteries with high performance at a wide range of temperatures.
基金supported in part by JSPS KAKENHI grants (nos. JP21K05243 and JP22H04621grants-in-aid for Scientific Research on Innovative Areas “Interface Ionics”)+1 种基金by a JST grant (no. JPMJFS2132,for the establishment of university fellowships toward the creation of science technology innovation)by the Suzuki foundation
文摘MgH_(2) and TiH_(2) have been extensively studied as potential anode materials due to their high theoretical specific capacities of 2036 and 1024 mAh/g,respectively.However,the large volume changes that these compounds undergo during cycling affects their performance and limits practical applications.The present work demonstrates a novel approach to limiting the volume changes of active materials.This effect is based on mechanical support from an intimate interface generated in situ via the reaction between MgH_(2) and Ti within the electrode prior to lithiation to form Mg and TiH_(2).The resulting Mg can be transformed back to MgH_(2) by reaction with LiH during delithiation.In addition,the TiH_(2) improves the reaction kinetics of MgH_(2) and enhances electrochemical performance.The intimate interface produced in this manner is found to improve the electrochemical properties of a MgH_(2)-Ti-LiH electrode.An exceptional reversible capacity of 800 mAh/g is observed even after 200 cycles with a high current density of 1 mA/cm^(2) and a high proportion of active material(90 wt.%)at an operation temperature of 120℃.This study therefore showcases a new means of improving the performance of electrodes by limiting the volume changes of active materials.
基金the financial support from the Open Fund Project of the National Oil Shale Exploitation Research and Development Center,China(No.33550000-22-ZC0613-0255)the Graduate Student Innovation and Practical Ability Training Program of Xi’an Shiyou University(No.YCS23213098)+3 种基金the National Natural Science Foundation of China(No.52274039)the Natural Science Basic Research Plan in Shaanxi Province of China(Program No.2024JC-YBMS-085)the CNPC Innovation Found(No.2022DQ02-0402)The authors also thank the Modern Analysis and Test Center of Xi’an Shiyou University for their help with the characterization of catalysts and analysis of products.
文摘Tungstated zirconia(WO_(3)/ZrO_(2))solid acid catalysts with different WO_(3) contents were prepared by a hydrothermal method and then used in the catalytic aquathermolysis of heavy oil from Xinjiang.The WO_(3)/ZrO_(2) solid acid catalyst was characterized by a range of characterization methods,including X-ray diffraction,NH3-temperature programmed desorption,and pyridine infrared spectroscopy.The WO_(3) content of the WO_(3)/ZrO_(2) catalysts had an important impact on the structure and property of the catalysts.When the WO_(3) mass fraction was 20%,it facilitated the formation of tetragonal zirconia,thereby enhancing the creation of robust acidic sites.Acidity is considered to have a strong impact on the catalytic performance of the aquathermolysis of heavy oil.When the catalyst containing 20%WO_(3) was used to catalyze the aquathermolysis of heavy oil under conditions of 14.5 MPa,340℃,and 24 h,the viscosity of heavy oil decreased from 47266 to 5398 mPa·s and the viscosity reduction rate reached 88.6%.The physicochemical properties of heavy oil before and after the aquathermolysis were analyzed using a saturates,aromatics,resins,and asphaltenes analysis,gas chromatography,elemental analysis,densimeter etc.After the aquathermolysis,the saturate and aromatic contents significantly increased from 43.3%to 48.35%and 19.47%to 21.88%,respectively,with large reductions in the content of resin and asphaltene from 28.22%to 25.06%and 5.36%to 2.03%,respectively.The sulfur and nitrogen contents,and the density of the oil were significantly decreased.These factors were likely the main reasons for promoting the viscosity reduction of heavy oil during the aquathermolysis over the WO_(3)/ZrO_(2) solid acid catalysts.
基金supported by the Fundamental Research Funds for the Central Universities(Nos.2023YJS061 and 2023JBZY019).
文摘Changing the N content in the Ti_(3)AlC_(2−y)N_(y) MAX phase solid solutions allows for the fine-tuning of their properties.However,systematic studies on the synthesis and properties of Ti_(3)AlC_(2−y)N_(y) solid solution bulks have not been reported thus far.Here,previously reported Ti_(3)AlC_(2−y)N_(y) solid solution bulks(y=0.3,0.5,0.8,and 1.0)were synthesized via hot pressing of their powder counterparts under optimized conditions.The prepared Ti_(3)AlC_(2−y)N_(y) bulks are dense and have a fine microstructure with grain sizes of 6–8μm.The influence of the N content on the mechanical properties,electrical conductivities,and coefficients of thermal expansion(CTEs)of the prepared Ti_(3)AlC_(2−y)N_(y) bulk materials was clarified.The flexural strength and Vickers hardness values increased with increasing N content,suggesting that solid solution strengthening effectively improved the mechanical properties of Ti_(3)AlC_(2−y)N_(y).Ti_(3)AlCN(y=1)had the highest Vickers hardness and flexural strength among the studied samples,reaching 5.54 GPa and 550 MPa,respectively.However,the electrical conductivity and CTEs of the Ti_(3)AlC_(2−y)N_(y) solid solutions decreased with increasing N content,from 8.93×10^(−6) to 7.69×10^(−6) K^(−1) and from 1.33×10^(6) to 0.95×10^(6) S/m,respectively.This work demonstrated the tunable properties of Ti_(3)AlC_(2−y)N_(y) solid solutions with varying N contents and widened the MAX phase family for fundamental studies and applications.
基金financially supported by the National Key R&D Program of China (No. 2018YFB1502203-1)the Guangdong Basic and Applied Basic Research Foundation (No. 2021B1515120087)the Stable Supporting Fund of Shenzhen, China (No. GXWD20201230155427003-202007 28114835006)
文摘Physical vapor deposition(PVD)can be used to produce high-quality Gd_(2)O_(3)-doped CeO2(GDC)films.Among various PVD methods,reactive sputtering provides unique benefits,such as high deposition rates and easy upscaling for industrial applications.GDC thin films were successfully fabricated through reactive sputtering using a Gd_(0.2)Ce_(0.8)(at%)metallic target,and their application in solid oxide fuel cells,such as buffer layers between yttria-stabilized zirconia(YSZ)/La0.6Sr0.4Co0.2Fe0.8O_(3−δ)and as sublayers in the steel/coating system,was evaluated.First,the direct current(DC)reactive-sputtering behavior of the GdCe metallic target was determined.Then,the GDC films were deposited on NiO-YSZ/YSZ half-cells to investigate the influence of oxygen flow rate on the quality of annealed GDC films.The results demonstrated that reactive sputtering can be used to prepare thin and dense GDC buffer layers without high-temperature sintering.Furthermore,the cells with a sputtered GDC buffer layer showed better electrochemical performance than those with a screen-printed GDC buffer layer.In addition,the insertion of a GDC sublayer between the SUS441 interconnects and the Mn-Co spinel coatings contributed to the reduction of the oxidation rate for SUS441 at operating temperatures,according to the area-specific resistance tests.
基金supported by the National Natural Science Foundation of China (22108184)China Postdoctoral Science Foundation (2021TQ0221)+1 种基金the Sichuan Science and Technology Program (2021JDRC0117)Chengdu Science and Technology Program (2021-YF05-00378-SN)。
文摘The significant decrease of acid sites caused by alkali metal poisoning is the major factor in the deactivation of commercial V_(2)O_(5)-WO_(3)/TiO_(2)NH_(3)-SCR catalysts.In this work,the solid superacid SO_(4)^(2-)-TiO_(2) modified by sulfate radicals,was selected as the catalyst support,which showed superior potassium resistance.The physicochemical properties and K-poisoning resistance of the V_(2)O_(5)-WO_(3)/SO_(4)^(2-)-TiO_(2)(VWSTi) catalyst were carried out by XRD,BET,H2-TPR,NH3-TPD,XPS,in situ DRIFTS and TG.The results pointed out that the introduction of SO_(4)^(2-)significantly increased the NH3-SCR catalytic activity at high temperatures,with an exceptionally high NO_(x) conversion over 90% between 275℃ and 500℃.When 0.5%(mass) K_(2)O was doped on the catalysts,the catalytic performance of the traditional V_(2)O_(5)-WO_(3)/TiO_(2)(VWTi) catalyst decreased significantly,while the VWSTi catalyst could still maintain a NOxconversion over 90%in the range of 300–500℃.The characterizations suggested that the support of SO_(4)^(2-)-TiO_(2) greatly increased the number of acidic sites,thereby enhancing the adsorption capacity of the reactant NH_(3).The results above demonstrated a potential approach to achieve superior potassium resistance for NH3-SCR catalysts using solid superacid.