NiFe(oxy)hydroxides nanosheets were synthesized on nickel foams via co-precipitation and electrochemical activation. It is found that the phosphate precursors(Na_(3)PO_(4), Na_(2)HPO_(4)and NaH_(2)PO_(4)) have diverse...NiFe(oxy)hydroxides nanosheets were synthesized on nickel foams via co-precipitation and electrochemical activation. It is found that the phosphate precursors(Na_(3)PO_(4), Na_(2)HPO_(4)and NaH_(2)PO_(4)) have diverse effects on the morphology and thus the oxygen evolution reaction activity of the formed final catalysts. The resulting NiFe(oxy)hydroxides nanosheets prepared with Na_(2)HPO_(4)demonstrate a low overpotential of 205 m V to achieve a current density of 50 mA/cm^(2) with a Tafel slope down to 30 mV/dec in 1 mol/L KOH, and remain stable for 20 h during stability test.展开更多
Developing highly active and cost-effective electrocatalysts for enhancing the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is a significant challenge for overall water splitting.Sulfur-incorporat...Developing highly active and cost-effective electrocatalysts for enhancing the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is a significant challenge for overall water splitting.Sulfur-incorporated nickel iron(oxy)hydroxide(S-NiFeOOH)nanosheets were directly grown on commercial nickel foam using a galvanic corrosion method and a hydrothermal method.The incorporation of sulfur into NiFeOOH enhanced the catalytic activity for the HER and OER in 1 M KOH electrolyte.The enhanced catalytic activity is attributed to the change in the local structure and chemical states due to the incorporation of sulfur.High performance for overall water splitting was achieved with an alkaline water electrolyzer.This was realized by employing S-NiFeOOH as a bifunctional electrocatalyst,thereby outperforming a water electrolyzer that requires the usage of precious metal electrocatalysts(i.e.,Pt/C as the HER electrocatalyst and IrO_(2) as the OER electrocatalyst).Moreover,when driven by a commercial silicon solar cell,an alkaline water electrolyzer that uses S-NiFeOOH as a bifunctional electrocatalyst generated hydrogen under natural illumination.This study shows that S-NiFeOOH is a promising candidate for a large-scale industrial implementation of hydrogen production for overall water splitting because of its low cost,high activity,and durability.In addition,the solar-driven water electrolyzer using S-NiFeOOH as a bifunctional electrocatalyst affords the opportunity for developing effective and feasible solar power systems in the future.展开更多
The title compound N-((3-(2-nitrophenyl) propanoyl)oxy)-N-phenylbenzamide(C22H18N2O5,Mr = 390.38) was synthesized with nitrobenzene as the starting materials and structurally characterized by 1H NMR,13 C NMR,I...The title compound N-((3-(2-nitrophenyl) propanoyl)oxy)-N-phenylbenzamide(C22H18N2O5,Mr = 390.38) was synthesized with nitrobenzene as the starting materials and structurally characterized by 1H NMR,13 C NMR,IR,H RMS(E-SI) and single-crystal X-ray diffraction.The crystalline structure of the title compound was studied in detail.The single-crystal X-ray diffraction revealed that the compound crystallizes in monoclinic,space group P21/n,with a = 14.4481(7),b = 8.0089(5),c = 16.6808(9) A,α = 90.00(5),β = 100.069(5),γ = 90.00(5)°,Mr = 390.38,V = 1900.46(18) A^3,Z = 4,Dc = 1.364 g/cm^-3,μ = 0.098,F(000) = 816.0,the final R = 0.0530 and w R = 0.1141 for 2525 observed reflections(I 〉 2σ(I)),R(all data) = 0.0813,w R(all data) = 0.1335,completeness to theta of 26.020 is 99.8% and GOF = 1.085.The crystal structure contains three branched chains with its center placed at the midpoint of N.The phenyl ring(C(8)~C(13)) makes a dihedral angle of 83.5(1) ℃ with the phenyl ring(C(1)~C(6)),and 80.5(1) ℃with the nitro-substituted benzene ring(C(17)~C(22)),indicating that the three rings are not coplanar.Hydrogen bonds(C(10)–H(10)···O(3)),(C(15)–H(15B)···O(4) and C(16)–H(16B)···O(4)) together with π-π stacking interactions stabilize the structure of the molecule.The preliminary biological test shows that the title compound has good antitumor activity against A549 in vitro with the IC50 value of 3.17 μmol.展开更多
In this work,a facile chelation-mediated route was developed to fabricate ultrathin cobalt(oxy)hydroxides(CoOOH)nanosheets on hematite photoanode(Fe_(2)O_(3)).The route contains two steps of the adsorption of[Co-EDTA]...In this work,a facile chelation-mediated route was developed to fabricate ultrathin cobalt(oxy)hydroxides(CoOOH)nanosheets on hematite photoanode(Fe_(2)O_(3)).The route contains two steps of the adsorption of[Co-EDTA]^(2-)species on Fe_(2)O_(3) nanorod array followed by the hydrolysis in alkaline solution.The resulting CoOOH/Fe_(2)O_(3) exhibits a remarkably improved photocurrent density of 2.10 mA cm^(-2) at 1.23 V vs.RHE,which is ca.2.8 times that of bare Fe_(2)O_(3).In addition,a negative shift of onset potential ca.200 mV is achieved.The structural characterizations reveal the chelate EDTA plays important roles that enhance the adsorption of Co species and the formation of contact between CoOOH and Fe_(2)O_(3).(Photo)electrochemical analysis suggests,besides providing active sites for water oxidation,CoOOH at large extent promotes the charge separation and the charge transfer via passivating surface states and suppressing charge recombination.It also found CoOOH possesses some oxygen vacancies,which could act as trapping centers for photogenerated holes and facilitate the charge separation.Intensity modulated photocurrent spectroscopy(IMPS)shows that,under low applied potential the water oxidation mainly occurs on CoOOH,while under high applied potential the water oxidation could occur on both CoOOH and Fe_(2)O_(3).The findings not only provide an efficient strategy for designing ultrathin(oxy)hydroxides on semiconductors for PEC applications but also put forward a new insight on the role of CoOOH during water oxidation.展开更多
Oxy fuel combustion and conventional cycle(currently working cycle) in Kazeroon plant are modeled using commercial thermodynamic modeling software. Economic evaluation of the two models regarding the resources of tran...Oxy fuel combustion and conventional cycle(currently working cycle) in Kazeroon plant are modeled using commercial thermodynamic modeling software. Economic evaluation of the two models regarding the resources of transport and injection of carbon dioxide into oil fields at Gachsaran for enhanced oil recovery in the various oil price indices is conducted and indices net present value(NPV) and internal rate of return on investment(IRR) are calculated. The results of the two models reveal that gross efficiency of the oxy fuel cycle is more than reference cycle(62% compared to 49.03%), but the net efficiency is less(41.85% compared to 47.92%) because of the high-energy consumption of the components, particularly air separation unit(ASU) in the oxy fuel cycle. In this model, pure carbon dioxide with pressure of 20×105 Pa and purity of 96.84% was captured. NOX emissions also decrease by 4289.7 tons per year due to separation of nitrogen in ASU. In this model, none of the components of oxy fuel cycle is a major engineering challenge. With increasing oil price, economic justification of oxy fuel combustion model increases. With the price of oil at $ 80 per barrel in mind and $ 31 per ton fines for emissions of carbon dioxide in the atmosphere, IRR is the same for both models.展开更多
High-entropy materials(HEMs)have attracted extensive attention in the field of electrochemical catal-ysis due to their unique properties.However,the preparation of high-entropy catalysts typically relies on high-tempe...High-entropy materials(HEMs)have attracted extensive attention in the field of electrochemical catal-ysis due to their unique properties.However,the preparation of high-entropy catalysts typically relies on high-temperature,energy-intensive,and time-consuming synthesis methods due to their compositional complexity.In this study,a facile low-temperature electrochemical reconstruction approach is adopted to synthesize Ag-decorated septenary Co-Cu-Fe-Mo-Zn-Ag-Ru high-entropy(oxy)hydroxide electro-catalysts for oxygen evolution reaction(OER).By introducing Ag and Ru elements and implanting Ag nanoparticles to co-regulate the electronic structure of the catalysts,the as-prepared catalyst achieves remarkable OER performance with a low overpotential of 298 mV at 100 mA/cm^(2)and a small Tafel slope of 30.1 mV/dec in 1 mol/L KOH.This work offers a valuable strategy for developing high-performance high-entropy OER electrocatalysts.展开更多
Single crystals of two 1,3-phenylenebis(oxy)diacetic acid(C10H10O8) compounds 1 and 2 were obtained via slow evaporation.The compounds were characterized by elemental analysis,IR and single-crystal X-ray diffracti...Single crystals of two 1,3-phenylenebis(oxy)diacetic acid(C10H10O8) compounds 1 and 2 were obtained via slow evaporation.The compounds were characterized by elemental analysis,IR and single-crystal X-ray diffraction.Compound 1(C10H14O8) crystallizes in the triclinic system,space group P1 with a = 6.3751(6),b = 8.5311(8),c = 11.4510(11)A,α = 93.3650(10),β = 105.3190(10),γ = 97.2140(10)°,V = 593.15(10) A^3,Z = 2,Mr = 262.21,Dc = 1.468 g/cm^3,F(000) = 276,GOOF = 1.005,° = 0.129 mm^-1,the final R = 0.0361 and w R = 0.0802 for 1854 observed reflections with I 〉 2σ(I).Compound 2(C30H28N2O12) crystallizes in the triclinic system,space group P1 with a = 9.7416(13),b = 11.839(2),c = 12.9828(13) A,α = 74.191(4),β = 77.953(2),γ = 74.726(3)°,V = 1374.5(3) A^3,Z = 2,Mr = 608.54,Dc = 1.470 g/cm^3,F(000) = 636,GOOF = 1.061,° = 0.115 mm^-1,the final R = 0.0500 and w R = 0.1221 for 3966 observed reflections with I 〉 2σ(I).Both compounds 1 and 2 exhibit 3D supramolecular structures under hydrogen bonding interactions.The results of preliminary antibacterial activity show that the title compounds display moderate antibacterial activities against the tested gram positive bacteria(S.aureus,C.albicans and B.subtilis) and gram negative bacteria(E.coli and P.aeruginosa).展开更多
The contraction of isolated rat and rabbit uteri induced by oxytocin and PGF2α was markedly inhibited by chlorpheniramine (Chl) and astemizolum (Ast) , both of which also decreased the resting tension of uteri, and t...The contraction of isolated rat and rabbit uteri induced by oxytocin and PGF2α was markedly inhibited by chlorpheniramine (Chl) and astemizolum (Ast) , both of which also decreased the resting tension of uteri, and their spontaneous contraction. The inhibitory effects of both drugs were dose-dependent. At high concentrations , Chl 7. 4 × 10-4 mol/L and Ast 10-4 mol/L could counteract the contraction of the uteri induced by Oxy and PGF2α, and their spontaneous contraction as well. They decreased the resting tension to the lower level. The mechanism of their non-special relaxed action on uteri could not be completely explained only by their H1-receptor blocking action. Whether they act by blocking calcium channel or by inhibiting calmodulin (CaM) remains to be further explored.展开更多
The inversion reaction of hydroxy lamine was investigated by using the ab initiointrinsic reaction coordinate(IRC)method with 4-31G basis set.Our results indicate that the ∠H_1NO changes arastically in the vicinity o...The inversion reaction of hydroxy lamine was investigated by using the ab initiointrinsic reaction coordinate(IRC)method with 4-31G basis set.Our results indicate that the ∠H_1NO changes arastically in the vicinity of the transition state while the other bo-nd angles and bond lengths change little throughout the reaction process.展开更多
The compound N-phenyl-N-[(o-nitrophenylacetyl)oxy]benzamide (C21HI6N2Os, Mr = 376) has been synthesized by the reaction of N-hydroxy-N-phenylbenzamide with 2-(2-nitro- phenyl)acetyl chloride in dichlorom-ethane ...The compound N-phenyl-N-[(o-nitrophenylacetyl)oxy]benzamide (C21HI6N2Os, Mr = 376) has been synthesized by the reaction of N-hydroxy-N-phenylbenzamide with 2-(2-nitro- phenyl)acetyl chloride in dichlorom-ethane and its structure Was characterized by 1H NMR, 13C NMR, IR, H RMS(ESI) and single-crystal X-ray diffraction. The crystal of the title compound belongs to monoclinic, space group C2/c with a = 32.30(2), b = 8.400(5), c = 15.099(9) A, fl = 114.256(10)°, V = 3735(4) A3, Z = 8, D, = 1.339 g/cm3, F(000) = 1568, p = 0.097 mm-1, the final R = 0.0506 and wR = 0.1176 for 2318 observed reflections (1 〉 2a(/)). The title molecule contains three branched chains with its center placed at the midpoint of N. The phenyl ring (C(1)'-C(6)) makes a dihedral angle of 70.3(1)° with the phenyl ring (C(10)-C(15)) of benzoyl group, and 14.3(1)° with the phenyl ring (C(16) - C(21)), Hydrogen bonds C(5)-H(5)...O(1) and C(12)-H(12)...O(3) together with it-Jr stacking interactions contribute to the stability of the structure.展开更多
New compounds were synthesized,which belong to 3 types of pyrimidinyl(triazinyl)oxy substituted carboxylic derivatives respectively.In bioassay,the effects of the structural factors on the herbicidal activity were inv...New compounds were synthesized,which belong to 3 types of pyrimidinyl(triazinyl)oxy substituted carboxylic derivatives respectively.In bioassay,the effects of the structural factors on the herbicidal activity were investigated,in which the stereochemistry has a strong influence on the activity.展开更多
FeOOH have received considerable attention due to their natural abundance and cost-effectiveness.Despite the significant progress achieved,the one-step synthesis of integrated FeOOH is still a major challenge.Meanwhil...FeOOH have received considerable attention due to their natural abundance and cost-effectiveness.Despite the significant progress achieved,the one-step synthesis of integrated FeOOH is still a major challenge.Meanwhile,the current research on FeOOH catalyst still suffers from the unclear mechanism of controlling morphology.Here,density functional theory(DFT)calculations and X-ray photoelectron spectroscopy(XPS)demonstrated the strong electron-capturing and hydrogen absorption ability of Co in FeOOH,which further promotes the formation and stabilization of FeOOH.We used a one-step electrodeposition method to synthesize Co introduced FeOOH integrated electrocatalyst and propose to introduce ions with different valence states to regulate the morphology of FeOOH by precise modulation of electric double layer(EDL)composition and thickness.The prepared Co-FeOOH-K^(+)has a larger electrochemically active surface area(ECSA)(325 cm^(2))and turnover frequency(TOF)value(0.75 s^(-1)).In the electrochemical experiments of an alkaline anion exchange membrane electrolyzer,Co-FeOOH-K^(+)shows better oxygen evolution performance than commercial RuO_(2) under industrial production conditions and has good industrial application prospects.展开更多
Although Fe-Ni combination performs well in transition metal-based oxygen evolution reaction(OER)electrocatalysts,there are lack of clear and general regulations mechanism to fully play the synergistic catalytic effec...Although Fe-Ni combination performs well in transition metal-based oxygen evolution reaction(OER)electrocatalysts,there are lack of clear and general regulations mechanism to fully play the synergistic catalytic effect.Here,we made the utmost of the interaction of Fe–Ni heteroatomic pair to obtain a highly active Fe-Ni(oxy)hydroxide catalytic layer on iron foam(IF)and nickel foam(NF)by in-situ electrochemical deposition and rapid surface reconstruction,which only required 327 and 351 mV overpotential to provide a large current of 1,000 mA·cm^(−2),respectively.The results confirm that the moderate Ni-rich heteroatomic bonding(Ni–O–Fe–O–Ni)formed by adjusting the Ni/Fe ratio on the catalyst surface is important to offer predominant OER performance.Fe is a key component that enhances OER activity of Ni(O)OH,but Fe-rich structural surface formed by Fe–O–Ni–O–Fe bonding is not ideal.Finally,the remarkable oxygen evolution performance of the prepared Ni2Fe(O)OH/IF and FeNi2(O)OH/NF can be chalked up to the optimized electronic structure of Fe–Ni heteroatomic bonding,the efficient gas spillover,the fast electron transport,and nanosheet clusters morphology.In summary,our work suggests a comprehensive regulation mechanism for the construction of efficient Fe-Ni(oxy)hydroxide catalytic layer on inexpensive,stable,and self-supporting metallic material surface.展开更多
The 2,2'-((sulfonylbis(4,1-phenylene))bis(oxy))diacetic acid(H2L) and 4,4'-bipyridine(4,4'-bipy) are employed as organic ligands to react with metal salts to obtain two new metal-organic frameworks(MOFs), ...The 2,2'-((sulfonylbis(4,1-phenylene))bis(oxy))diacetic acid(H2L) and 4,4'-bipyridine(4,4'-bipy) are employed as organic ligands to react with metal salts to obtain two new metal-organic frameworks(MOFs), namely [M2L2(4,4'-bipy)](M = Zn(1), Cu(2)). They have been successfully synthesized under hydrothermal conditions. Single-crystal X-ray diffraction reveals that two complexes are isostructural and crystallize in orthorhombic system with space group Pbcn. All L^(2-) ligands bridge metal ions to form an infinite 1D Z-shaped chain along the a axis. Then through 4,4'-bipy, contiguous Z-shaped chains are linked to form a 2D layer structure. The luminescent studies of the H2L ligand and complex 1 in the solid state and thermogravimetric analyses(TGA) of two complexes are investigated.展开更多
基金supported by the National Natural Science Foundation of China (Nos. 11904411, 52072308)the Fundamental Research Funds for the Central Universities, China (Nos. 3102021MS0404, 3102019JC001)。
文摘NiFe(oxy)hydroxides nanosheets were synthesized on nickel foams via co-precipitation and electrochemical activation. It is found that the phosphate precursors(Na_(3)PO_(4), Na_(2)HPO_(4)and NaH_(2)PO_(4)) have diverse effects on the morphology and thus the oxygen evolution reaction activity of the formed final catalysts. The resulting NiFe(oxy)hydroxides nanosheets prepared with Na_(2)HPO_(4)demonstrate a low overpotential of 205 m V to achieve a current density of 50 mA/cm^(2) with a Tafel slope down to 30 mV/dec in 1 mol/L KOH, and remain stable for 20 h during stability test.
基金supported by the Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(No.NRF-2016R1D1A3B04935101).
文摘Developing highly active and cost-effective electrocatalysts for enhancing the hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)is a significant challenge for overall water splitting.Sulfur-incorporated nickel iron(oxy)hydroxide(S-NiFeOOH)nanosheets were directly grown on commercial nickel foam using a galvanic corrosion method and a hydrothermal method.The incorporation of sulfur into NiFeOOH enhanced the catalytic activity for the HER and OER in 1 M KOH electrolyte.The enhanced catalytic activity is attributed to the change in the local structure and chemical states due to the incorporation of sulfur.High performance for overall water splitting was achieved with an alkaline water electrolyzer.This was realized by employing S-NiFeOOH as a bifunctional electrocatalyst,thereby outperforming a water electrolyzer that requires the usage of precious metal electrocatalysts(i.e.,Pt/C as the HER electrocatalyst and IrO_(2) as the OER electrocatalyst).Moreover,when driven by a commercial silicon solar cell,an alkaline water electrolyzer that uses S-NiFeOOH as a bifunctional electrocatalyst generated hydrogen under natural illumination.This study shows that S-NiFeOOH is a promising candidate for a large-scale industrial implementation of hydrogen production for overall water splitting because of its low cost,high activity,and durability.In addition,the solar-driven water electrolyzer using S-NiFeOOH as a bifunctional electrocatalyst affords the opportunity for developing effective and feasible solar power systems in the future.
基金Supported by the Lanzhou Science and Technology Bureau Program Funds(2013-4-79,2014-1-174,2014-1-214)
文摘The title compound N-((3-(2-nitrophenyl) propanoyl)oxy)-N-phenylbenzamide(C22H18N2O5,Mr = 390.38) was synthesized with nitrobenzene as the starting materials and structurally characterized by 1H NMR,13 C NMR,IR,H RMS(E-SI) and single-crystal X-ray diffraction.The crystalline structure of the title compound was studied in detail.The single-crystal X-ray diffraction revealed that the compound crystallizes in monoclinic,space group P21/n,with a = 14.4481(7),b = 8.0089(5),c = 16.6808(9) A,α = 90.00(5),β = 100.069(5),γ = 90.00(5)°,Mr = 390.38,V = 1900.46(18) A^3,Z = 4,Dc = 1.364 g/cm^-3,μ = 0.098,F(000) = 816.0,the final R = 0.0530 and w R = 0.1141 for 2525 observed reflections(I 〉 2σ(I)),R(all data) = 0.0813,w R(all data) = 0.1335,completeness to theta of 26.020 is 99.8% and GOF = 1.085.The crystal structure contains three branched chains with its center placed at the midpoint of N.The phenyl ring(C(8)~C(13)) makes a dihedral angle of 83.5(1) ℃ with the phenyl ring(C(1)~C(6)),and 80.5(1) ℃with the nitro-substituted benzene ring(C(17)~C(22)),indicating that the three rings are not coplanar.Hydrogen bonds(C(10)–H(10)···O(3)),(C(15)–H(15B)···O(4) and C(16)–H(16B)···O(4)) together with π-π stacking interactions stabilize the structure of the molecule.The preliminary biological test shows that the title compound has good antitumor activity against A549 in vitro with the IC50 value of 3.17 μmol.
基金supported by the National Natural Science Foundation of China(51502078)the Major Project of Science and Technology,Education Department of Henan Province(19A150019 and 19A150018)+2 种基金the Science and Technology Research Project of Henan Province(192102310490 and 182102410090)the program for Science&Technology Innovation Team in Universities of Henan Province(19IRTSTHN029)supported by the U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences,Chemical Sciences,Geosciences,and Biosciences Division,Catalysis Science program。
文摘In this work,a facile chelation-mediated route was developed to fabricate ultrathin cobalt(oxy)hydroxides(CoOOH)nanosheets on hematite photoanode(Fe_(2)O_(3)).The route contains two steps of the adsorption of[Co-EDTA]^(2-)species on Fe_(2)O_(3) nanorod array followed by the hydrolysis in alkaline solution.The resulting CoOOH/Fe_(2)O_(3) exhibits a remarkably improved photocurrent density of 2.10 mA cm^(-2) at 1.23 V vs.RHE,which is ca.2.8 times that of bare Fe_(2)O_(3).In addition,a negative shift of onset potential ca.200 mV is achieved.The structural characterizations reveal the chelate EDTA plays important roles that enhance the adsorption of Co species and the formation of contact between CoOOH and Fe_(2)O_(3).(Photo)electrochemical analysis suggests,besides providing active sites for water oxidation,CoOOH at large extent promotes the charge separation and the charge transfer via passivating surface states and suppressing charge recombination.It also found CoOOH possesses some oxygen vacancies,which could act as trapping centers for photogenerated holes and facilitate the charge separation.Intensity modulated photocurrent spectroscopy(IMPS)shows that,under low applied potential the water oxidation mainly occurs on CoOOH,while under high applied potential the water oxidation could occur on both CoOOH and Fe_(2)O_(3).The findings not only provide an efficient strategy for designing ultrathin(oxy)hydroxides on semiconductors for PEC applications but also put forward a new insight on the role of CoOOH during water oxidation.
文摘Oxy fuel combustion and conventional cycle(currently working cycle) in Kazeroon plant are modeled using commercial thermodynamic modeling software. Economic evaluation of the two models regarding the resources of transport and injection of carbon dioxide into oil fields at Gachsaran for enhanced oil recovery in the various oil price indices is conducted and indices net present value(NPV) and internal rate of return on investment(IRR) are calculated. The results of the two models reveal that gross efficiency of the oxy fuel cycle is more than reference cycle(62% compared to 49.03%), but the net efficiency is less(41.85% compared to 47.92%) because of the high-energy consumption of the components, particularly air separation unit(ASU) in the oxy fuel cycle. In this model, pure carbon dioxide with pressure of 20×105 Pa and purity of 96.84% was captured. NOX emissions also decrease by 4289.7 tons per year due to separation of nitrogen in ASU. In this model, none of the components of oxy fuel cycle is a major engineering challenge. With increasing oil price, economic justification of oxy fuel combustion model increases. With the price of oil at $ 80 per barrel in mind and $ 31 per ton fines for emissions of carbon dioxide in the atmosphere, IRR is the same for both models.
基金supported by the National Key Research and Development Program of China[grant number 2020YFE0100100]the National Natural Science Foundation of China[grant number 52222103]the Fundamental Research Funds for the Central Universities and the Key Research and Development Program of Sichuan Province(Scientific and Technological Cooperation of Sichuan Province with Institutes and Universities)[grant number 2020YFSY0001].
文摘High-entropy materials(HEMs)have attracted extensive attention in the field of electrochemical catal-ysis due to their unique properties.However,the preparation of high-entropy catalysts typically relies on high-temperature,energy-intensive,and time-consuming synthesis methods due to their compositional complexity.In this study,a facile low-temperature electrochemical reconstruction approach is adopted to synthesize Ag-decorated septenary Co-Cu-Fe-Mo-Zn-Ag-Ru high-entropy(oxy)hydroxide electro-catalysts for oxygen evolution reaction(OER).By introducing Ag and Ru elements and implanting Ag nanoparticles to co-regulate the electronic structure of the catalysts,the as-prepared catalyst achieves remarkable OER performance with a low overpotential of 298 mV at 100 mA/cm^(2)and a small Tafel slope of 30.1 mV/dec in 1 mol/L KOH.This work offers a valuable strategy for developing high-performance high-entropy OER electrocatalysts.
基金Supported by the National Natural Science Foundation of China(No.21264011,20961007)the Aviation Fund(No.2014ZF56020)
文摘Single crystals of two 1,3-phenylenebis(oxy)diacetic acid(C10H10O8) compounds 1 and 2 were obtained via slow evaporation.The compounds were characterized by elemental analysis,IR and single-crystal X-ray diffraction.Compound 1(C10H14O8) crystallizes in the triclinic system,space group P1 with a = 6.3751(6),b = 8.5311(8),c = 11.4510(11)A,α = 93.3650(10),β = 105.3190(10),γ = 97.2140(10)°,V = 593.15(10) A^3,Z = 2,Mr = 262.21,Dc = 1.468 g/cm^3,F(000) = 276,GOOF = 1.005,° = 0.129 mm^-1,the final R = 0.0361 and w R = 0.0802 for 1854 observed reflections with I 〉 2σ(I).Compound 2(C30H28N2O12) crystallizes in the triclinic system,space group P1 with a = 9.7416(13),b = 11.839(2),c = 12.9828(13) A,α = 74.191(4),β = 77.953(2),γ = 74.726(3)°,V = 1374.5(3) A^3,Z = 2,Mr = 608.54,Dc = 1.470 g/cm^3,F(000) = 636,GOOF = 1.061,° = 0.115 mm^-1,the final R = 0.0500 and w R = 0.1221 for 3966 observed reflections with I 〉 2σ(I).Both compounds 1 and 2 exhibit 3D supramolecular structures under hydrogen bonding interactions.The results of preliminary antibacterial activity show that the title compounds display moderate antibacterial activities against the tested gram positive bacteria(S.aureus,C.albicans and B.subtilis) and gram negative bacteria(E.coli and P.aeruginosa).
文摘The contraction of isolated rat and rabbit uteri induced by oxytocin and PGF2α was markedly inhibited by chlorpheniramine (Chl) and astemizolum (Ast) , both of which also decreased the resting tension of uteri, and their spontaneous contraction. The inhibitory effects of both drugs were dose-dependent. At high concentrations , Chl 7. 4 × 10-4 mol/L and Ast 10-4 mol/L could counteract the contraction of the uteri induced by Oxy and PGF2α, and their spontaneous contraction as well. They decreased the resting tension to the lower level. The mechanism of their non-special relaxed action on uteri could not be completely explained only by their H1-receptor blocking action. Whether they act by blocking calcium channel or by inhibiting calmodulin (CaM) remains to be further explored.
文摘The inversion reaction of hydroxy lamine was investigated by using the ab initiointrinsic reaction coordinate(IRC)method with 4-31G basis set.Our results indicate that the ∠H_1NO changes arastically in the vicinity of the transition state while the other bo-nd angles and bond lengths change little throughout the reaction process.
基金supported by the Fundamental Research Funds for the Central Universities(lzujbky-2010-137)
文摘The compound N-phenyl-N-[(o-nitrophenylacetyl)oxy]benzamide (C21HI6N2Os, Mr = 376) has been synthesized by the reaction of N-hydroxy-N-phenylbenzamide with 2-(2-nitro- phenyl)acetyl chloride in dichlorom-ethane and its structure Was characterized by 1H NMR, 13C NMR, IR, H RMS(ESI) and single-crystal X-ray diffraction. The crystal of the title compound belongs to monoclinic, space group C2/c with a = 32.30(2), b = 8.400(5), c = 15.099(9) A, fl = 114.256(10)°, V = 3735(4) A3, Z = 8, D, = 1.339 g/cm3, F(000) = 1568, p = 0.097 mm-1, the final R = 0.0506 and wR = 0.1176 for 2318 observed reflections (1 〉 2a(/)). The title molecule contains three branched chains with its center placed at the midpoint of N. The phenyl ring (C(1)'-C(6)) makes a dihedral angle of 70.3(1)° with the phenyl ring (C(10)-C(15)) of benzoyl group, and 14.3(1)° with the phenyl ring (C(16) - C(21)), Hydrogen bonds C(5)-H(5)...O(1) and C(12)-H(12)...O(3) together with it-Jr stacking interactions contribute to the stability of the structure.
文摘New compounds were synthesized,which belong to 3 types of pyrimidinyl(triazinyl)oxy substituted carboxylic derivatives respectively.In bioassay,the effects of the structural factors on the herbicidal activity were investigated,in which the stereochemistry has a strong influence on the activity.
基金supported by the National Natural Science Foundation of China(Nos.22001143,52072197)the Youth Innovation and Technology Foundation of Shandong Higher Education Institutions,China(No.2019KJC004)+4 种基金the Outstanding Youth Foundation of Shandong Province,China(No.ZR2019JQ14)the Taishan Scholar Young Talent Program(Nos.tsqn201909114,tsqn201909123)the Natural Science Foundation of Shandong Province(No.ZR2020YQ34)the Major Scientific and Technological Innovation Project(No.2019JZZY020405)the Major Basic Research Program of Natural Science Foundation of Shandong Province under Grant No.ZR2020ZD09.
文摘FeOOH have received considerable attention due to their natural abundance and cost-effectiveness.Despite the significant progress achieved,the one-step synthesis of integrated FeOOH is still a major challenge.Meanwhile,the current research on FeOOH catalyst still suffers from the unclear mechanism of controlling morphology.Here,density functional theory(DFT)calculations and X-ray photoelectron spectroscopy(XPS)demonstrated the strong electron-capturing and hydrogen absorption ability of Co in FeOOH,which further promotes the formation and stabilization of FeOOH.We used a one-step electrodeposition method to synthesize Co introduced FeOOH integrated electrocatalyst and propose to introduce ions with different valence states to regulate the morphology of FeOOH by precise modulation of electric double layer(EDL)composition and thickness.The prepared Co-FeOOH-K^(+)has a larger electrochemically active surface area(ECSA)(325 cm^(2))and turnover frequency(TOF)value(0.75 s^(-1)).In the electrochemical experiments of an alkaline anion exchange membrane electrolyzer,Co-FeOOH-K^(+)shows better oxygen evolution performance than commercial RuO_(2) under industrial production conditions and has good industrial application prospects.
基金the National Natural Science Foundation of China(No.52174283)the Shandong Provincial Natural Science Foundation(No.ZR2020MB044)Postgraduate Innovation Engineering Project of China University of Petroleum(East China)(No.YCX2021147).
文摘Although Fe-Ni combination performs well in transition metal-based oxygen evolution reaction(OER)electrocatalysts,there are lack of clear and general regulations mechanism to fully play the synergistic catalytic effect.Here,we made the utmost of the interaction of Fe–Ni heteroatomic pair to obtain a highly active Fe-Ni(oxy)hydroxide catalytic layer on iron foam(IF)and nickel foam(NF)by in-situ electrochemical deposition and rapid surface reconstruction,which only required 327 and 351 mV overpotential to provide a large current of 1,000 mA·cm^(−2),respectively.The results confirm that the moderate Ni-rich heteroatomic bonding(Ni–O–Fe–O–Ni)formed by adjusting the Ni/Fe ratio on the catalyst surface is important to offer predominant OER performance.Fe is a key component that enhances OER activity of Ni(O)OH,but Fe-rich structural surface formed by Fe–O–Ni–O–Fe bonding is not ideal.Finally,the remarkable oxygen evolution performance of the prepared Ni2Fe(O)OH/IF and FeNi2(O)OH/NF can be chalked up to the optimized electronic structure of Fe–Ni heteroatomic bonding,the efficient gas spillover,the fast electron transport,and nanosheet clusters morphology.In summary,our work suggests a comprehensive regulation mechanism for the construction of efficient Fe-Ni(oxy)hydroxide catalytic layer on inexpensive,stable,and self-supporting metallic material surface.
基金supported by the Natural Science Foundation of Zhejiang Province(No.Y12B010003)。
文摘The 2,2'-((sulfonylbis(4,1-phenylene))bis(oxy))diacetic acid(H2L) and 4,4'-bipyridine(4,4'-bipy) are employed as organic ligands to react with metal salts to obtain two new metal-organic frameworks(MOFs), namely [M2L2(4,4'-bipy)](M = Zn(1), Cu(2)). They have been successfully synthesized under hydrothermal conditions. Single-crystal X-ray diffraction reveals that two complexes are isostructural and crystallize in orthorhombic system with space group Pbcn. All L^(2-) ligands bridge metal ions to form an infinite 1D Z-shaped chain along the a axis. Then through 4,4'-bipy, contiguous Z-shaped chains are linked to form a 2D layer structure. The luminescent studies of the H2L ligand and complex 1 in the solid state and thermogravimetric analyses(TGA) of two complexes are investigated.