Metal oxide charge transport materials are preferable for realizing long-term stable and potentially low-cost perovskite solar cells(PSCs).However,due to some technical difficulties(e.g.,intricate fabrication protocol...Metal oxide charge transport materials are preferable for realizing long-term stable and potentially low-cost perovskite solar cells(PSCs).However,due to some technical difficulties(e.g.,intricate fabrication protocols,high-temperature heating process,incompatible solvents,etc.),it is still challenging to achieve efficient and reliable all-metal-oxide-based devices.Here,we developed efficient inverted PSCs(IPSCs)based on solution-processed nickel oxide(NiO_(x))and tin oxide(SnO_(2))nanoparticles,working as hole and electron transport materials respectively,enabling a fast and balanced charge transfer for photogenerated charge carriers.Through further understanding and optimizing the perovskite/metal oxide interfaces,we have realized an outstanding power conversion efficiency(PCE)of 23.5%(the bandgap of the perovskite is 1.62 eV),which is the highest efficiency among IPSCs based on all-metal-oxide charge transport materials.Thanks to these stable metal oxides and improved interface properties,ambient stability(retaining 95%of initial PCE after 1 month),thermal stability(retaining 80%of initial PCE after 2 weeks)and light stability(retaining 90%of initial PCE after 1000 hours aging)of resultant devices are enhanced significantly.In addition,owing to the low-temperature fabrication procedures of the entire device,we have obtained a PCE of over 21%for flexible IPSCs with enhanced operational stability.展开更多
In this study,Ni catalysts supported on Pr-doped Ce O_(2) are studied for the CO_(2) methanation reaction and the effect of Pr doping on the physicochemical properties and the catalytic performance is thoroughly evalu...In this study,Ni catalysts supported on Pr-doped Ce O_(2) are studied for the CO_(2) methanation reaction and the effect of Pr doping on the physicochemical properties and the catalytic performance is thoroughly evaluated.It is shown,that Pr^(3+)ions can substitute Ce^(4+)ones in the support lattice,thereby introducing a high population of oxygen vacancies,which act as active sites for CO_(2) chemisorption.Pr doping can also act to reduce the crystallite size of metallic Ni,thus promoting the active metal dispersion.Catalytic performance evaluation evidences the promoting effect of low Pr loadings(5 at%and 10 at%)towards a higher catalytic activity and lower CO_(2) activation energy.On the other hand,higher Pr contents negate the positive effects on the catalytic activity by decreasing the oxygen vacancy population,thereby creating a volcano-type trend towards an optimum amount of aliovalent substitution.展开更多
Heat treatment of metal-organic frameworks(MOFs)has provided a wide variety of functional carbons coordinated with metal compounds.In this study,two kinds of zinc-based MOF(ZMOF),C_(16)H_(10)O_(4)Zn(ZMOF1)and C_(8)H_(...Heat treatment of metal-organic frameworks(MOFs)has provided a wide variety of functional carbons coordinated with metal compounds.In this study,two kinds of zinc-based MOF(ZMOF),C_(16)H_(10)O_(4)Zn(ZMOF1)and C_(8)H_(4)O_(4)Zn(ZMOF2),were prepared.ZMOF1 and ZMOF2 were carbonized at 1000℃,forming CZMOF1 and CZMOF2,respectively.The specific surface area(S_(BET))of CZMOF2 was~2700 m^(2)g^(−1),much higher than that of CZMOF1(~1300 m^(2)g^(−1)).A supercapacitor electrode based on CZMOF2 achieved specific capacitances of 360,278,and 221 F g^(−1)at 50,250,and 1000 mA g^(−1)in an aqueous electrolyte(H2SO_(4)),respectively,the highest values reported to date for ZMOF-derived electrodes under identical conditions.The practical applicability of the CZMOF-based supercapacitor was verified in non-aqueous electrolytes.The initial capacitance retention was 78%after 100000 charge/discharge cycles at 10 A g^(−1).Crucially,the high capacitance of CZMOF2 arises from pore generation during carbonization.Below 1000℃,pore generation is dominated by the Zn/C ratio of ZMOFs,as carbon atoms reduce the zinc oxides formed during carbonization.Above 1000℃,a high O/C ratio becomes essential for pore generation because the oxygen functional groups are pyrolyzed.These findings will provide insightful information for other metal-based MOFderived multifunctional carbons.展开更多
Thermoelectrics are a promising solution to the recovery of some of the 60%of the worldwide energy wasted as heat.However,their conversion efficiency is low and the best performing materials are brittle,toxic,and made...Thermoelectrics are a promising solution to the recovery of some of the 60%of the worldwide energy wasted as heat.However,their conversion efficiency is low and the best performing materials are brittle,toxic,and made of expensive ceramics.The challenge in developing better performing materials is in disrupting the electrical vs thermal conductivity correlation,to achieve low thermal conductivity simultaneously with a high electrical conductivity.Carbon nanotubes allow for the decoupling of the electronic density of states from the phonon density of states and this paper shows that flexible,thin films of double-walled carbon nanotube(DWCNT)can form effective n-and p-doped semiconductors that can achieve a combined Seebeck coefficient of 157.6µV K^(−1),the highest reported for a single DWCNT device to date.This is achieved through selected surfactant doping,whose role is correlated with the length of the hydrocarbon chain of the hydrophobic tail group of the surfactant’s molecules.CNTs functionalized with Triton X-405 show the highest output power consisting of a single junction of p-and n-type thermoelectric elements,reaching as high as 67 nW for a 45 K temperature gradient.Thus enabling flexible,cheaper,and more efficient thermoelectric generators through the use of functionalized CNTs.展开更多
One of the major problems limiting the applications of electric double-layer(EDLC)supercapacitor devices is their inability to maintain their cell voltage over a significant period.Self-discharge is a spontaneous deca...One of the major problems limiting the applications of electric double-layer(EDLC)supercapacitor devices is their inability to maintain their cell voltage over a significant period.Self-discharge is a spontaneous decay in charged energy,often resulting in fully depleted devices in a matter of hours.Here,a new method for suppressing this self-discharge phenomenon is proposed by using directionally polarized piezoelectric electrospun nanofiber films as separator materials.Tailored engineering of polyvinylidene fluoride(PVDF)nanofiber films containing a small concentration of sodium dodecyl sulfate(SDS)results in a high proportion of polarβphases,reaching 380.5%of the total material.Inducing polarity into the separator material provides a reverse-diode mechanism in the device,such that it drops from an initial voltage of 1.6 down to 1 V after 10 h,as opposed to 0.3 V with a nonpolarized,commercial separator material.Thus,the energy retained for the polarized separator is 37%and 4%for the nonpolarized separator,making supercapacitors a more attractive solution for long-term energy storage.展开更多
基金UK Engineering and Physical Sciences Research Council(EPSRC)New Investigator Award(2018,EP/R043272/1)Newton Advanced Fellowship(192097)for financial support+3 种基金the Royal Society,the Engineering and Physical Sciences Research Council(EPSRC,EP/R023980/1,EP/V027131/1)the European Research Council(ERC)under the European Union's Horizon 2020 research and innovation program(HYPERION,Grant Agreement Number 756962)the Royal Society and Tata Group(UF150033)EPSRC SPECIFIC IKC(EP/N020863/1)
文摘Metal oxide charge transport materials are preferable for realizing long-term stable and potentially low-cost perovskite solar cells(PSCs).However,due to some technical difficulties(e.g.,intricate fabrication protocols,high-temperature heating process,incompatible solvents,etc.),it is still challenging to achieve efficient and reliable all-metal-oxide-based devices.Here,we developed efficient inverted PSCs(IPSCs)based on solution-processed nickel oxide(NiO_(x))and tin oxide(SnO_(2))nanoparticles,working as hole and electron transport materials respectively,enabling a fast and balanced charge transfer for photogenerated charge carriers.Through further understanding and optimizing the perovskite/metal oxide interfaces,we have realized an outstanding power conversion efficiency(PCE)of 23.5%(the bandgap of the perovskite is 1.62 eV),which is the highest efficiency among IPSCs based on all-metal-oxide charge transport materials.Thanks to these stable metal oxides and improved interface properties,ambient stability(retaining 95%of initial PCE after 1 month),thermal stability(retaining 80%of initial PCE after 2 weeks)and light stability(retaining 90%of initial PCE after 1000 hours aging)of resultant devices are enhanced significantly.In addition,owing to the low-temperature fabrication procedures of the entire device,we have obtained a PCE of over 21%for flexible IPSCs with enhanced operational stability.
基金support of this work by the project“Development of new innovative low carbon energy technologies to improve excellence in the Region of Western Macedonia”(MIS 5047197)which is implemented under the Action“Reinforcement of the Research and Innovation Infrastructure”funded by the Operational Program“Competitiveness,Entrepreneurship and Innovation”(NSRF 2014-2020)co-financed by Greece and the European Union(European Regional Development Fund)。
文摘In this study,Ni catalysts supported on Pr-doped Ce O_(2) are studied for the CO_(2) methanation reaction and the effect of Pr doping on the physicochemical properties and the catalytic performance is thoroughly evaluated.It is shown,that Pr^(3+)ions can substitute Ce^(4+)ones in the support lattice,thereby introducing a high population of oxygen vacancies,which act as active sites for CO_(2) chemisorption.Pr doping can also act to reduce the crystallite size of metallic Ni,thus promoting the active metal dispersion.Catalytic performance evaluation evidences the promoting effect of low Pr loadings(5 at%and 10 at%)towards a higher catalytic activity and lower CO_(2) activation energy.On the other hand,higher Pr contents negate the positive effects on the catalytic activity by decreasing the oxygen vacancy population,thereby creating a volcano-type trend towards an optimum amount of aliovalent substitution.
基金partially supported by a Grant-in-Aid for Scientific Research(KAKENHI)from the Japan Society for the Promotion of Science(JSPS)(grant number 19H05332)。
文摘Heat treatment of metal-organic frameworks(MOFs)has provided a wide variety of functional carbons coordinated with metal compounds.In this study,two kinds of zinc-based MOF(ZMOF),C_(16)H_(10)O_(4)Zn(ZMOF1)and C_(8)H_(4)O_(4)Zn(ZMOF2),were prepared.ZMOF1 and ZMOF2 were carbonized at 1000℃,forming CZMOF1 and CZMOF2,respectively.The specific surface area(S_(BET))of CZMOF2 was~2700 m^(2)g^(−1),much higher than that of CZMOF1(~1300 m^(2)g^(−1)).A supercapacitor electrode based on CZMOF2 achieved specific capacitances of 360,278,and 221 F g^(−1)at 50,250,and 1000 mA g^(−1)in an aqueous electrolyte(H2SO_(4)),respectively,the highest values reported to date for ZMOF-derived electrodes under identical conditions.The practical applicability of the CZMOF-based supercapacitor was verified in non-aqueous electrolytes.The initial capacitance retention was 78%after 100000 charge/discharge cycles at 10 A g^(−1).Crucially,the high capacitance of CZMOF2 arises from pore generation during carbonization.Below 1000℃,pore generation is dominated by the Zn/C ratio of ZMOFs,as carbon atoms reduce the zinc oxides formed during carbonization.Above 1000℃,a high O/C ratio becomes essential for pore generation because the oxygen functional groups are pyrolyzed.These findings will provide insightful information for other metal-based MOFderived multifunctional carbons.
文摘Thermoelectrics are a promising solution to the recovery of some of the 60%of the worldwide energy wasted as heat.However,their conversion efficiency is low and the best performing materials are brittle,toxic,and made of expensive ceramics.The challenge in developing better performing materials is in disrupting the electrical vs thermal conductivity correlation,to achieve low thermal conductivity simultaneously with a high electrical conductivity.Carbon nanotubes allow for the decoupling of the electronic density of states from the phonon density of states and this paper shows that flexible,thin films of double-walled carbon nanotube(DWCNT)can form effective n-and p-doped semiconductors that can achieve a combined Seebeck coefficient of 157.6µV K^(−1),the highest reported for a single DWCNT device to date.This is achieved through selected surfactant doping,whose role is correlated with the length of the hydrocarbon chain of the hydrophobic tail group of the surfactant’s molecules.CNTs functionalized with Triton X-405 show the highest output power consisting of a single junction of p-and n-type thermoelectric elements,reaching as high as 67 nW for a 45 K temperature gradient.Thus enabling flexible,cheaper,and more efficient thermoelectric generators through the use of functionalized CNTs.
基金the UK Engineering and Physical Sciences Research Council(EPSRC)for funding this work under the Doctoral Training Partnership(DTP)award(EP/N509772/1).
文摘One of the major problems limiting the applications of electric double-layer(EDLC)supercapacitor devices is their inability to maintain their cell voltage over a significant period.Self-discharge is a spontaneous decay in charged energy,often resulting in fully depleted devices in a matter of hours.Here,a new method for suppressing this self-discharge phenomenon is proposed by using directionally polarized piezoelectric electrospun nanofiber films as separator materials.Tailored engineering of polyvinylidene fluoride(PVDF)nanofiber films containing a small concentration of sodium dodecyl sulfate(SDS)results in a high proportion of polarβphases,reaching 380.5%of the total material.Inducing polarity into the separator material provides a reverse-diode mechanism in the device,such that it drops from an initial voltage of 1.6 down to 1 V after 10 h,as opposed to 0.3 V with a nonpolarized,commercial separator material.Thus,the energy retained for the polarized separator is 37%and 4%for the nonpolarized separator,making supercapacitors a more attractive solution for long-term energy storage.