Violet phosphorus,a recently explored layered elemental semiconductor,has attracted much attention due to its unique photoelectric,mechanical properties,and high hole mobility.Herein,violet arsenic phosphorus has for ...Violet phosphorus,a recently explored layered elemental semiconductor,has attracted much attention due to its unique photoelectric,mechanical properties,and high hole mobility.Herein,violet arsenic phosphorus has for the first time been synthesized by a molten lead method.The crystal structure of violet arsenic phosphorus(P^(83.4)As_(0.6),CSD-2408761)was determined by single crystal X-ray diffraction to have similar structure as that of violet phosphorus,where P12 is occupied by arsenic/phosphorus(As/P)atoms as mixed occupancy sites As1/P12.The arsenic substitution has been demonstrated to tune the band structure of violet phosphorus,switching p-type of violet phosphorus to high-performance n-type violet arsenic phosphorus.The effective electron mass along the<010>direction is significantly reduced from 1.792 to 0.515 m_(0)by arsenic substitution,resulting in an extremely high electron mobility of 2622.503 cm^(2)V^(-1)s^(-1).The field effect transistor built with P_(83.4)As_(0.6)nanosheets was measured to have a high electron mobility(137.06 cm^(2)V^(-1)s^(-1),61.2 nm),even under ambient conditions for 5 h,much higher than the hole mobility of violet phosphorene nanosheets(4.07 cm^(2)V^(-1)s^(-1),73.3 nm).This work provides a new idea for designing phosphorus-based materials for field effect transistors,giving significant potential in complementary metal-oxide-semiconductor applications.展开更多
Benzoic acid containing fluorine atom at ortho-,meta-,and para-position are employed as self-assembled monolayers to modify the buried interface in perovskite solar cells(PSCs).It is demonstrated that the position of ...Benzoic acid containing fluorine atom at ortho-,meta-,and para-position are employed as self-assembled monolayers to modify the buried interface in perovskite solar cells(PSCs).It is demonstrated that the position of fluorine atom influences the passivation effect and para-fluorinated one provided the most substantial performance enhancement mainly originating from ameliorated contact and energy band alignment between NiOx and perovskite,improved perovskite quality and defect healing.Resultantly,PSC with a power conversion efficiency of 24%can be achieved.Meanwhile,which can maintain 96.8%of the initial PCE after a 1000 h storage,presenting enhanced durability.This work highlights the critical role of molecular functionality and conformation in the buried interface modification of PSCs,providing valuable insights for future developments.展开更多
The Kagome metal CsV3Sb5 transitions from a weakly correlated state to a strongly correlated state upon Cr substitution;however,the mechanism driving this enhancement remains an open question.Here,we employed a combin...The Kagome metal CsV3Sb5 transitions from a weakly correlated state to a strongly correlated state upon Cr substitution;however,the mechanism driving this enhancement remains an open question.Here,we employed a combination of density functional theory and dynamical mean-field theory(DFT+DMFT)to systematically investigate the evolution of electronic correlations in the CsV_(3−x)Cr_(x)Sb_(5)(x=0,1,and 3)series.Our calculations revealed that Cr doping drives the system into a strongly correlated Hund’s metal phase,which is characterized by significant and orbital-dependent enhancements in the quasiparticle effective masses and electronic scattering rates.We trace the origin of this transition to the doping-induced shift from low-to high-spin atomic configurations.This preference for high-spin states,which is promoted by near-half-filling of the Cr-d orbitals,induces a pronounced orbital blocking effect that strengthens the correlations.Our findings establish that Hund’s coupling is the decisive factor governing the rich correlation physics in the CsV_(3−x)Cr_(x)Sb_(5) family,providing a tunable platform for exploring Hund’s metallicity.展开更多
The n-octanol/water partition coefficients （lgKow） of 18 substituted anilines were determined at 25 ℃ by shake-flask method. The geometrical optimization of substituted anilines has been performed at B3LYP/6-311G^...The n-octanol/water partition coefficients （lgKow） of 18 substituted anilines were determined at 25 ℃ by shake-flask method. The geometrical optimization of substituted anilines has been performed at B3LYP/6-311G^＊＊ level with Gaussian98 program, and the molecular surface areas of substituted anilines were calculated using ChemOffice 2004 program. The calculated structural parameters of substituted anilines were used as theoretical descriptors and the two-parameter （molecular surface area （MA） and the energy of the highest occupied molecular orbital （EaoMo）） quantitative structure-property relationship （QSPR） model of lgKow for substituted aniline with molecular structural parameters was developed by multi-linear regression method. The regression coefficient square （r^2） is 0.990 and the standard deviation SE 0.109. The model was validated by variance inflation factors （VIF） and t-test, and the results show that there exists small self-correlation between variables of the model with perfect stability. The model gives results in good qualitative agreement with experimental data. At last, the model was applied to predict lgKow values of five substituted anilines whose lgKow values have not been determined experimentally.展开更多
Boron for aluminum substitution in the cordierite structure has been examined by sol-gel preparation of different samples along the compositional junction Mg2Al4-xBxSi5O18 with x=0,0.5,1,1.5.By increasing the x value ...Boron for aluminum substitution in the cordierite structure has been examined by sol-gel preparation of different samples along the compositional junction Mg2Al4-xBxSi5O18 with x=0,0.5,1,1.5.By increasing the x value from 0 to 1.5 the crystallization behavior changed accordingly.Proper amount B2O3 doping can promote the sintering of amorphous cordierite gel,effectively restrain the precipitation ofμ-cordierite and enhance the crystallization ofα-cordierite.The substitution of B3+for Al3+in cordierite crystal structure can effectively improve the near-infrared spectral emissivity of this cordierite based glass-ceramics.展开更多
Metal-organic frameworks(MOFs)and MOF-derived materials have attracted great attention as alternatives to noble-metal based electrocatalysts owing to their intriguing structure properties,especially for high efficienc...Metal-organic frameworks(MOFs)and MOF-derived materials have attracted great attention as alternatives to noble-metal based electrocatalysts owing to their intriguing structure properties,especially for high efficiency and stable oxygen reduction reaction(ORR).Herein,we employed a one-pot reaction to make a multimetal(Fe,Co,Cu,and Zn)mixed zeolitic imidazolate framework(MM-ZIF)via adopting a simple in situ redox reaction.Further pyrolysis of the target MM-ZIF,a highly porous carbon polyhedron(FC-C@NC)grafted with abundant carbon nanotubes was obtained,in which ultrasmall Co nanoparticles with partial lattice sites substituted by Fe and Cu were embedded.The obtained FC-C@NC possessed large surface area,highly porous structure,widely-spread metal active sites,and conductive carbon frameworks,contributing to outstanding ORR activity and long-term stability.It displayed superior tolerance to methanol crossover and exceeded the commercial Pt/C catalyst and most previously reported non-noble-metal catalysts.Impressively,the as-produced FC-C@NC-based zinc-air battery afforded an open-circuit potential of 1.466 V,a large specific capacity of 659.5 mAh/g,and a high gravimetric energy density of 784.3 Wh/kgZn,significantly outperforming the Pt/C-based cathode.展开更多
The polymerization of acrylamide (AAM)in H_2O/DMF or in H_2O/CH_3CN mixed solvent initiated with ceric ion (Ce^(4+) )/N-(substituted phenyl)-acetamide systems have been studied. The redox polymerization was revealed b...The polymerization of acrylamide (AAM)in H_2O/DMF or in H_2O/CH_3CN mixed solvent initiated with ceric ion (Ce^(4+) )/N-(substituted phenyl)-acetamide systems have been studied. The redox polymerization was revealed by the low value of overall activation energy (E_α) of AAM polymerization using ceric ion/N-(substituted phenyl) acetamide system as an initiator. The end group of polymer formed was detected by IR spectrum analysis method, it revealed the presence of N-(m-acetoxy-methylphenyl) acetamide (m-AAe) moiety end group in the polymer obtained with ceric ion/m-AAe initiation system.展开更多
An efficient methodology for the synthesis of 2,3-disubstituted 3H-quinazolin-4-ones is described via one-pot three component reaction from anthranilic acid using T3 P as catalyst. Mild reaction conditions,short react...An efficient methodology for the synthesis of 2,3-disubstituted 3H-quinazolin-4-ones is described via one-pot three component reaction from anthranilic acid using T3 P as catalyst. Mild reaction conditions,short reaction time, broad functional group tolerance, easy isolation of products and good yields are main advantages of this protocol.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.22175136)the State Key Laboratory of Electrical Insulation and Power Equipment(Grant No.EIPE23127)the Fundamental Research Funds for the Central Universities(xtr052024009,xtr052025002).
文摘Violet phosphorus,a recently explored layered elemental semiconductor,has attracted much attention due to its unique photoelectric,mechanical properties,and high hole mobility.Herein,violet arsenic phosphorus has for the first time been synthesized by a molten lead method.The crystal structure of violet arsenic phosphorus(P^(83.4)As_(0.6),CSD-2408761)was determined by single crystal X-ray diffraction to have similar structure as that of violet phosphorus,where P12 is occupied by arsenic/phosphorus(As/P)atoms as mixed occupancy sites As1/P12.The arsenic substitution has been demonstrated to tune the band structure of violet phosphorus,switching p-type of violet phosphorus to high-performance n-type violet arsenic phosphorus.The effective electron mass along the<010>direction is significantly reduced from 1.792 to 0.515 m_(0)by arsenic substitution,resulting in an extremely high electron mobility of 2622.503 cm^(2)V^(-1)s^(-1).The field effect transistor built with P_(83.4)As_(0.6)nanosheets was measured to have a high electron mobility(137.06 cm^(2)V^(-1)s^(-1),61.2 nm),even under ambient conditions for 5 h,much higher than the hole mobility of violet phosphorene nanosheets(4.07 cm^(2)V^(-1)s^(-1),73.3 nm).This work provides a new idea for designing phosphorus-based materials for field effect transistors,giving significant potential in complementary metal-oxide-semiconductor applications.
基金the Key project of Nature Science Foundation of Tianjin(22JCZDJC00120)the 111 Project(B16027)for financial support.
文摘Benzoic acid containing fluorine atom at ortho-,meta-,and para-position are employed as self-assembled monolayers to modify the buried interface in perovskite solar cells(PSCs).It is demonstrated that the position of fluorine atom influences the passivation effect and para-fluorinated one provided the most substantial performance enhancement mainly originating from ameliorated contact and energy band alignment between NiOx and perovskite,improved perovskite quality and defect healing.Resultantly,PSC with a power conversion efficiency of 24%can be achieved.Meanwhile,which can maintain 96.8%of the initial PCE after a 1000 h storage,presenting enhanced durability.This work highlights the critical role of molecular functionality and conformation in the buried interface modification of PSCs,providing valuable insights for future developments.
基金supported by the Development Program of China and the National Key Research (Grant Nos.2023YFA1406200 and 2022YFA1402304)the National Natural Science Foundation of China (Grant Nos.12274169 and 12122405)+3 种基金the Fundamental Research Funds for the Central Universitiesthe Innovation Team for Functional Materials and Devices for Informatics at Anhui Higher Education Institutes (Grant No.2024AH010024)the Natural Science Research Project of Education Department of Anhui Province (Grant No.2025AHGXZK31203)the PHD Research Startup Foundation of Fuyang Normal University (Grant No.2025KYQD0072)。
文摘The Kagome metal CsV3Sb5 transitions from a weakly correlated state to a strongly correlated state upon Cr substitution;however,the mechanism driving this enhancement remains an open question.Here,we employed a combination of density functional theory and dynamical mean-field theory(DFT+DMFT)to systematically investigate the evolution of electronic correlations in the CsV_(3−x)Cr_(x)Sb_(5)(x=0,1,and 3)series.Our calculations revealed that Cr doping drives the system into a strongly correlated Hund’s metal phase,which is characterized by significant and orbital-dependent enhancements in the quasiparticle effective masses and electronic scattering rates.We trace the origin of this transition to the doping-induced shift from low-to high-spin atomic configurations.This preference for high-spin states,which is promoted by near-half-filling of the Cr-d orbitals,induces a pronounced orbital blocking effect that strengthens the correlations.Our findings establish that Hund’s coupling is the decisive factor governing the rich correlation physics in the CsV_(3−x)Cr_(x)Sb_(5) family,providing a tunable platform for exploring Hund’s metallicity.
基金This work was supported by the National Natural Science Foundation of China (No. 20737001)
文摘The n-octanol/water partition coefficients （lgKow） of 18 substituted anilines were determined at 25 ℃ by shake-flask method. The geometrical optimization of substituted anilines has been performed at B3LYP/6-311G^＊＊ level with Gaussian98 program, and the molecular surface areas of substituted anilines were calculated using ChemOffice 2004 program. The calculated structural parameters of substituted anilines were used as theoretical descriptors and the two-parameter （molecular surface area （MA） and the energy of the highest occupied molecular orbital （EaoMo）） quantitative structure-property relationship （QSPR） model of lgKow for substituted aniline with molecular structural parameters was developed by multi-linear regression method. The regression coefficient square （r^2） is 0.990 and the standard deviation SE 0.109. The model was validated by variance inflation factors （VIF） and t-test, and the results show that there exists small self-correlation between variables of the model with perfect stability. The model gives results in good qualitative agreement with experimental data. At last, the model was applied to predict lgKow values of five substituted anilines whose lgKow values have not been determined experimentally.
基金supported by the National Nature Science Foundation of China(No.50771014)
文摘Boron for aluminum substitution in the cordierite structure has been examined by sol-gel preparation of different samples along the compositional junction Mg2Al4-xBxSi5O18 with x=0,0.5,1,1.5.By increasing the x value from 0 to 1.5 the crystallization behavior changed accordingly.Proper amount B2O3 doping can promote the sintering of amorphous cordierite gel,effectively restrain the precipitation ofμ-cordierite and enhance the crystallization ofα-cordierite.The substitution of B3+for Al3+in cordierite crystal structure can effectively improve the near-infrared spectral emissivity of this cordierite based glass-ceramics.
基金This study was financially supported by the Natural Science Foundation of China(Grant no.51825201 and 51772008)the National Key Research and Development Program of China(Grant no.2017YFA0206701)National Program for Support of Top-notch Young Professionals,and Changjiang Scholar Program.
文摘Metal-organic frameworks(MOFs)and MOF-derived materials have attracted great attention as alternatives to noble-metal based electrocatalysts owing to their intriguing structure properties,especially for high efficiency and stable oxygen reduction reaction(ORR).Herein,we employed a one-pot reaction to make a multimetal(Fe,Co,Cu,and Zn)mixed zeolitic imidazolate framework(MM-ZIF)via adopting a simple in situ redox reaction.Further pyrolysis of the target MM-ZIF,a highly porous carbon polyhedron(FC-C@NC)grafted with abundant carbon nanotubes was obtained,in which ultrasmall Co nanoparticles with partial lattice sites substituted by Fe and Cu were embedded.The obtained FC-C@NC possessed large surface area,highly porous structure,widely-spread metal active sites,and conductive carbon frameworks,contributing to outstanding ORR activity and long-term stability.It displayed superior tolerance to methanol crossover and exceeded the commercial Pt/C catalyst and most previously reported non-noble-metal catalysts.Impressively,the as-produced FC-C@NC-based zinc-air battery afforded an open-circuit potential of 1.466 V,a large specific capacity of 659.5 mAh/g,and a high gravimetric energy density of 784.3 Wh/kgZn,significantly outperforming the Pt/C-based cathode.
基金The project supported by the National Natural Science Foundation of China
文摘The polymerization of acrylamide (AAM)in H_2O/DMF or in H_2O/CH_3CN mixed solvent initiated with ceric ion (Ce^(4+) )/N-(substituted phenyl)-acetamide systems have been studied. The redox polymerization was revealed by the low value of overall activation energy (E_α) of AAM polymerization using ceric ion/N-(substituted phenyl) acetamide system as an initiator. The end group of polymer formed was detected by IR spectrum analysis method, it revealed the presence of N-(m-acetoxy-methylphenyl) acetamide (m-AAe) moiety end group in the polymer obtained with ceric ion/m-AAe initiation system.
基金Financial support from DST-Fast track,New Delhi(No.SERB/F/2013-14)
文摘An efficient methodology for the synthesis of 2,3-disubstituted 3H-quinazolin-4-ones is described via one-pot three component reaction from anthranilic acid using T3 P as catalyst. Mild reaction conditions,short reaction time, broad functional group tolerance, easy isolation of products and good yields are main advantages of this protocol.
