Chemical doping is a critical factor in the development of new superconductors or optimizing the superconducting transition temperature(T_(c))of the parent superconducting materials.Here,a new simple urea approach is ...Chemical doping is a critical factor in the development of new superconductors or optimizing the superconducting transition temperature(T_(c))of the parent superconducting materials.Here,a new simple urea approach is developed to synthesize the N-dopedα-Mo_(2)C.Benefiting from the simple urea method,a broad superconducting dome is found in the Mo_(2)C1−xNx(0≤x≤0.49)compositions.X-ray diffraction results show that the structure of𝛼α-Mo_(2)C remains unchanged and there is a variation of lattice parameters with nitrogen doping.Resistivity,magnetic susceptibility,and heat capacity measurement results confirm that T_(c)was strongly increased from 2.68K(x=0)to 7.05K(x=0.49).First-principles calculations and our analysis indicate that increasing nitrogen doping leads to a rise in the density of states at the Fermi level and doping-induced phonon softening,which enhances electron–phonon coupling.This results in an increase in𝑇T_(c)and a sharp rise in the upper critical field.Our findings provide a promising strategy for fabricating transition metal carbonitrides and provide a material platform for further study of the superconductivity of transition metal carbides.展开更多
Rational synthesis of robust layered double hydroxides(LDHs) nanosheets for high-energy supercapacitors is full of challenges.Herein,we reported an ultrasonication-assisted strategy to eco-friendly fabricate NiFe-LDHs...Rational synthesis of robust layered double hydroxides(LDHs) nanosheets for high-energy supercapacitors is full of challenges.Herein,we reported an ultrasonication-assisted strategy to eco-friendly fabricate NiFe-LDHs nanosheets for the enhanced capacitive behavior.The experimental results combined with different advanced characterization tools document that the utilization of ultrasonication has a profound effect on the morphology and thickness of the as-obtained NiFe-LDHs,alternatively affecting the capacitive behavior.It shows that NiFe-LDHs nanosheets prepared with 2-h ultrasonic treatments display the exceptional capacitive performance because of the synergetic effect of ultrathin thickness,large specific surface area,and high mesoporous volume.The maximum specific capacitance of Ni_(3) Fe_(1)-LDHs nanosheets with the thickness of 7.39 nm and the specific surface area of 77.16 m~2 g^(-1) reached 1923 F g^(-1),which is competitive with most previously reported values.In addition,the maximum specific energy of the assembled NiFe-LDHs//AC asymmetric supercapacitor achieved 49.13 Wh kg^(-1) at400 W kg^(-1).This work provides a green technology to fabricate LDHs nanosheets,and offers deep insights for understanding the relationship between the morphology/structure and capacitive behavior of LDHs nanosheets,which is helpful for achieving high-performance LDHs-based electrode materials.展开更多
We report a systematic investigation on the evolution of the structural and physical properties,including the charge density wave(CDW) and superconductivity of the polycrystalline CuIr_(2)Te_(4-x)Ix for 0.0 ≤x≤ 1.0....We report a systematic investigation on the evolution of the structural and physical properties,including the charge density wave(CDW) and superconductivity of the polycrystalline CuIr_(2)Te_(4-x)Ix for 0.0 ≤x≤ 1.0.Xray diffraction results indicate that both of a and c lattice parameters increase linearly when 0.0 ≤ x ≤ 1.0.The resistivity measurements indicate that the CDW is destabilized with slight x but reappears at x≥0.9 with very high TCDW.Meanwhile,the superconducting transition temperature Tc enhances as x increases and reaches a maximum value of around 2.95 K for the optimal composition CuIr_(2)Te_(1.9)I_(0.1) followed by a slight decrease with higher iodine doping content.The specific heat jump(ΔC/γTc) for the optimal composition CuIr_(2)Te_(3.9)I_(0.1) is approximately 1.46,which is close to the Bardeen-Cooper-Schrieffer value of 1.43,indicating that it is a bulk superconductor.The results of thermodynamic heat capacity measurements under different magnetic fields |Cp(T,H)],magnetization M(T,H) and magneto-transport ρ(T,H) measurements further suggest that CuIr_(2)Te_(4-x)Ix bulks are type-Ⅱ superconductors.Finally,an electronic phase diagram for this CuIr_(2)Te_(4-x)Ix system has been constructed.The present study provides a suitable material platform for further investigation of the interplay of the CDW and superconductivity.展开更多
The conductive metal-organic frameworks(MOFs)are suggested as the ideal electrocatalysts for hydrogen evolution reaction(HER)because of the high utilization of metal atoms.Rational design and facile synthesis of MOFs ...The conductive metal-organic frameworks(MOFs)are suggested as the ideal electrocatalysts for hydrogen evolution reaction(HER)because of the high utilization of metal atoms.Rational design and facile synthesis of MOFs with large specific surface area,proper metals as center,and tunable chemical components is still full of challenges.Herein,we report the facile synthesis three types of porous MOFs by regulating metal center using benzene-1,3,5-tricarboxylic acid(H3 BTC)as organic ligand and have successfully synthesized the rhombic octahedral Cu-BTC,rod-shaped Co-BTC and spherical Ni-BTC materials with large specific surface area ranged in 350-500 m^(2)g^(-1).These as-prepared MOFs materials exhibit high performance of HER in 0.5 M H_(2)SO_(4).Ni-BTC material exhibits the lowest overpotential of 53 mV at 10 mA cm-2 and the smallest Tafel slope of 62 mV dec^(-1)than those of Cu-BTC(270 mV,155 mV dec^(-1))and Co-BTC(123 mV,100 mV dec^(-1)),which are much superior to these previously reported MOFs catalysts.In addition,the fast catalytic kinetic of Ni-BTC was confirmed by the smaller charge transfer resistance(Rct)value of 0.9Ωand larger electrochemical active surface area(ECSA)of 35.5 cm^(2)than those of Cu-BTC(8.2Ω,22.5 cm^(2))and Co-BTC(1.9Ω,27.7 cm^(2)).Because of the structural advantage and large ECSA,the turnover frequency(TOF)value of Ni-BTC reaches up to 0.041 s-1 at 120 mV overpotential,which is 20.5 and 2.6 times greater than that of Cu-BTC(0.002 s-1)and Co-BTC(0.016 s-1).Besides,these three types of MOFs exhibited excellent durability over 12 h.This study unfolds diverse insights into the design and facile synthesis of MOFs for electrochemical energy conversion system.展开更多
Here we report a TiHfNbTa bulk medium-entropy alloy(MEA)superconductor crystallized in the body-centered cubic structure with the unit cell parameter a=3.35925?,which is synthesized by an arc melting method.Supercondu...Here we report a TiHfNbTa bulk medium-entropy alloy(MEA)superconductor crystallized in the body-centered cubic structure with the unit cell parameter a=3.35925?,which is synthesized by an arc melting method.Superconducting properties of the TiHfNbTa are studied by employing magnetic susceptibility,resistivity,and specific heat measurements.Experimental results show a bulk superconducting transition temperature(Tc)of around 6.75 K.The lower and upper critical fields for TiHfNbTa are45.8 m T and 10.46 T,respectively.First-principles calculations show that the d electrons of Ti,Hf,Nb,and Ta are the main contribution to the total density of states near the Fermi level.Our results indicate that the superconductivity is a conventional swave type with extremely strong coupling(△C_(el)/γ_(n)T_(c)=2.88,2△_(0)/k_(B)T_(c)=5.02,and λ_(ep)=2.77).The extremely strong coupling behavior in the s-wave type Ti Hf Nb Ta MEA superconductor is unusual because it generally happens in cuprates,pnictides,and other unconventional superconductors.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.12274471 and 11922415)Guangdong Basic and Applied Basic Research Foundation(Grant No.2022A1515011168)+3 种基金the Key Research&Development Program of Guangdong Province,China(Grant No.2019B110209003)the Guangdong Provincial Key Laboratory of Magnetoelectric Physics and Devices(Grant Nos.2022B1212010008)Lingyong Zeng was supported by the Postdoctoral Fellowship Program of CPSF(Grant Nos.GZC20233299)Fundamental Research Funds for the Central Universities,Sun Yat-Sen University(Grant Nos.29000-31610058)。
文摘Chemical doping is a critical factor in the development of new superconductors or optimizing the superconducting transition temperature(T_(c))of the parent superconducting materials.Here,a new simple urea approach is developed to synthesize the N-dopedα-Mo_(2)C.Benefiting from the simple urea method,a broad superconducting dome is found in the Mo_(2)C1−xNx(0≤x≤0.49)compositions.X-ray diffraction results show that the structure of𝛼α-Mo_(2)C remains unchanged and there is a variation of lattice parameters with nitrogen doping.Resistivity,magnetic susceptibility,and heat capacity measurement results confirm that T_(c)was strongly increased from 2.68K(x=0)to 7.05K(x=0.49).First-principles calculations and our analysis indicate that increasing nitrogen doping leads to a rise in the density of states at the Fermi level and doping-induced phonon softening,which enhances electron–phonon coupling.This results in an increase in𝑇T_(c)and a sharp rise in the upper critical field.Our findings provide a promising strategy for fabricating transition metal carbonitrides and provide a material platform for further study of the superconductivity of transition metal carbides.
基金the financial supports from KeyArea Research and Development Program of Guangdong Province (2019B110209003)Guangdong Basic and Applied Basic Research Foundation (2019B1515120058, 2020A1515011149)+3 种基金National Key R&D Program of China (2018YFD0800700)National Ten Thousand Talent Plan, National Natural Science Foundation of China (21776324)the Fundamental Research Funds for the Central Universities (19lgzd25)Hundred Talent Plan (201602) from Sun Yatsen University。
文摘Rational synthesis of robust layered double hydroxides(LDHs) nanosheets for high-energy supercapacitors is full of challenges.Herein,we reported an ultrasonication-assisted strategy to eco-friendly fabricate NiFe-LDHs nanosheets for the enhanced capacitive behavior.The experimental results combined with different advanced characterization tools document that the utilization of ultrasonication has a profound effect on the morphology and thickness of the as-obtained NiFe-LDHs,alternatively affecting the capacitive behavior.It shows that NiFe-LDHs nanosheets prepared with 2-h ultrasonic treatments display the exceptional capacitive performance because of the synergetic effect of ultrathin thickness,large specific surface area,and high mesoporous volume.The maximum specific capacitance of Ni_(3) Fe_(1)-LDHs nanosheets with the thickness of 7.39 nm and the specific surface area of 77.16 m~2 g^(-1) reached 1923 F g^(-1),which is competitive with most previously reported values.In addition,the maximum specific energy of the assembled NiFe-LDHs//AC asymmetric supercapacitor achieved 49.13 Wh kg^(-1) at400 W kg^(-1).This work provides a green technology to fabricate LDHs nanosheets,and offers deep insights for understanding the relationship between the morphology/structure and capacitive behavior of LDHs nanosheets,which is helpful for achieving high-performance LDHs-based electrode materials.
基金Supported by the National Natural Science Foundation of China(Grants No.11922415)the Guangdong Basic and Applied Basic Research Foundation(Grants No.2019A1515011718)+10 种基金the Fundamental Research Funds for the Central Universities(Grants No.19lgzd03)the Key R&D Program of Guangdong Province,China(Grants No.2019B110209003)the Pearl River Scholarship Program of Guangdong Province Universities and Colleges(Grants No.20191001)supported by the National Natural Science Foundation of China(Grant No.12004441)the Hundreds of Talents Program of Sun Yat-Sen Universitythe Fundamental Research Funds for the Central Universities(Grants No.20lgpy165)supported by the National Natural Science Foundation of China(Grant No.11974432)NKRDPC-2017YFA0206203,and NKRDPC-2018YFA0306001supported by the National Nature Science Foundation of China(11904414)the Natural Science Foundation of Guangdong(2018A030313055)National Key Research and Development Program of China(Grants No.2019YFA0705700)。
文摘We report a systematic investigation on the evolution of the structural and physical properties,including the charge density wave(CDW) and superconductivity of the polycrystalline CuIr_(2)Te_(4-x)Ix for 0.0 ≤x≤ 1.0.Xray diffraction results indicate that both of a and c lattice parameters increase linearly when 0.0 ≤ x ≤ 1.0.The resistivity measurements indicate that the CDW is destabilized with slight x but reappears at x≥0.9 with very high TCDW.Meanwhile,the superconducting transition temperature Tc enhances as x increases and reaches a maximum value of around 2.95 K for the optimal composition CuIr_(2)Te_(1.9)I_(0.1) followed by a slight decrease with higher iodine doping content.The specific heat jump(ΔC/γTc) for the optimal composition CuIr_(2)Te_(3.9)I_(0.1) is approximately 1.46,which is close to the Bardeen-Cooper-Schrieffer value of 1.43,indicating that it is a bulk superconductor.The results of thermodynamic heat capacity measurements under different magnetic fields |Cp(T,H)],magnetization M(T,H) and magneto-transport ρ(T,H) measurements further suggest that CuIr_(2)Te_(4-x)Ix bulks are type-Ⅱ superconductors.Finally,an electronic phase diagram for this CuIr_(2)Te_(4-x)Ix system has been constructed.The present study provides a suitable material platform for further investigation of the interplay of the CDW and superconductivity.
基金supported by the National Natural Science Foundation of China(Nos.11922415,22078374,21776324 and 21701197)the National Natural Science Foundation of China(Nos.11922415,21776324 and 21701197)+6 种基金Key-Area Research and Development Program of Guangdong Province(No.2019B110209003)the Guangdong Basic and Applied Basic Research Foundation(Nos.2019A1515011718,2019B1515120058 and 2020A1515011149)the National Key R&D Program of China(No.2018YFD0800700)the National Ten Thousand Talent Planthe Pearl River Scholarship Program of Guangdong Province Universities and Colleges(No.20191001)the Fundamental Research Funds for the Central Universities(Nos.19lgzd25 and 19lgzd03)the Hundred Talent Plan from Sun Yat-sen University。
文摘The conductive metal-organic frameworks(MOFs)are suggested as the ideal electrocatalysts for hydrogen evolution reaction(HER)because of the high utilization of metal atoms.Rational design and facile synthesis of MOFs with large specific surface area,proper metals as center,and tunable chemical components is still full of challenges.Herein,we report the facile synthesis three types of porous MOFs by regulating metal center using benzene-1,3,5-tricarboxylic acid(H3 BTC)as organic ligand and have successfully synthesized the rhombic octahedral Cu-BTC,rod-shaped Co-BTC and spherical Ni-BTC materials with large specific surface area ranged in 350-500 m^(2)g^(-1).These as-prepared MOFs materials exhibit high performance of HER in 0.5 M H_(2)SO_(4).Ni-BTC material exhibits the lowest overpotential of 53 mV at 10 mA cm-2 and the smallest Tafel slope of 62 mV dec^(-1)than those of Cu-BTC(270 mV,155 mV dec^(-1))and Co-BTC(123 mV,100 mV dec^(-1)),which are much superior to these previously reported MOFs catalysts.In addition,the fast catalytic kinetic of Ni-BTC was confirmed by the smaller charge transfer resistance(Rct)value of 0.9Ωand larger electrochemical active surface area(ECSA)of 35.5 cm^(2)than those of Cu-BTC(8.2Ω,22.5 cm^(2))and Co-BTC(1.9Ω,27.7 cm^(2)).Because of the structural advantage and large ECSA,the turnover frequency(TOF)value of Ni-BTC reaches up to 0.041 s-1 at 120 mV overpotential,which is 20.5 and 2.6 times greater than that of Cu-BTC(0.002 s-1)and Co-BTC(0.016 s-1).Besides,these three types of MOFs exhibited excellent durability over 12 h.This study unfolds diverse insights into the design and facile synthesis of MOFs for electrochemical energy conversion system.
基金supported by the National Natural Science Foundation of China(Grant Nos.12274471,and 11922415)the Guangdong Basic and Applied Basic Research Foundation(Grant Nos.2022A1515011168,and 2019A1515011718)+6 种基金the Key Research and Development Program of Guangdong Province,China(Grant No.2019B110209003)supported by the Foreign Young Talents Program of China(Grant No.22KW041C211)supported by the Key-Area Research and Development Program of Guangdong Province(Grant No.2020B0101340002)supported by the NKRDPC(Grant Nos.2022YFA1402802,and 2018YFA0306001)the National Natural Science Foundation of China(Grant Nos.11974432,and 92165204)the Leading Talent Program of Guangdong Special Projects(Grant No.201626003)the Shenzhen International Quantum Academy(Grant No.SIQA202102)。
文摘Here we report a TiHfNbTa bulk medium-entropy alloy(MEA)superconductor crystallized in the body-centered cubic structure with the unit cell parameter a=3.35925?,which is synthesized by an arc melting method.Superconducting properties of the TiHfNbTa are studied by employing magnetic susceptibility,resistivity,and specific heat measurements.Experimental results show a bulk superconducting transition temperature(Tc)of around 6.75 K.The lower and upper critical fields for TiHfNbTa are45.8 m T and 10.46 T,respectively.First-principles calculations show that the d electrons of Ti,Hf,Nb,and Ta are the main contribution to the total density of states near the Fermi level.Our results indicate that the superconductivity is a conventional swave type with extremely strong coupling(△C_(el)/γ_(n)T_(c)=2.88,2△_(0)/k_(B)T_(c)=5.02,and λ_(ep)=2.77).The extremely strong coupling behavior in the s-wave type Ti Hf Nb Ta MEA superconductor is unusual because it generally happens in cuprates,pnictides,and other unconventional superconductors.