Anodic oxygen evolution reaction(OER)is the key bottleneck for water electrolysis technique owing to its sluggish reaction kinetics.Interfacial engineering on the rationally designed heterostructure can regulate the e...Anodic oxygen evolution reaction(OER)is the key bottleneck for water electrolysis technique owing to its sluggish reaction kinetics.Interfacial engineering on the rationally designed heterostructure can regulate the electronic states efficiently for intrinsic activity improvement.Here,we report a co-phosphorization approach to construct a VPO_(4)-Ni_(2)P heterostructure on nickel foam with strongly chemical binding,wherein phosphate acts as electronic modifier for Ni_(2)P electrocatalyst.Profiting from the interfacial interaction,it is uncovered that electron shifts from Ni_(2)P to VPO_(4)to render valence increment in Ni species.Such an electronic manipulation rationalizes the chemical affinities of various oxygen intermediates in OER pathway,giving a substantially reduced energy barrier.As a result,the advanced VPO_(4)-Ni_(2)P heterostructure only requires an overpotential of 289 mV to deliver a high current density of 350 mA/cm^(2)for OER in alkaline electrolyte,together with a Tafel slope as low as 28 mV/dec.This work brings fresh insights into interfacial engineering for advanced electrocatalyst design.展开更多
Excessive Fe^(3+) ion concentrations in wastewater pose a long-standing threat to human health.Achieving low-cost,high-efficiency quantification of Fe^(3+) ion concentration in unknown solutions can guide environmenta...Excessive Fe^(3+) ion concentrations in wastewater pose a long-standing threat to human health.Achieving low-cost,high-efficiency quantification of Fe^(3+) ion concentration in unknown solutions can guide environmental management decisions and optimize water treatment processes.In this study,by leveraging the rapid,real-time detection capabilities of nanopores and the specific chemical binding affinity of tannic acid to Fe^(3+),a linear relationship between the ion current and Fe^(3+) ion concentration was established.Utilizing this linear relationship,quantification of Fe^(3+) ion concentration in unknown solutions was achieved.Furthermore,ethylenediaminetetraacetic acid disodium salt was employed to displace Fe^(3+) from the nanopores,allowing them to be restored to their initial conditions and reused for Fe^(3+) ion quantification.The reusable bioinspired nanopores remain functional over 330 days of storage.This recycling capability and the long-term stability of the nanopores contribute to a significant reduction in costs.This study provides a strategy for the quantification of unknown Fe^(3+) concentration using nanopores,with potential applications in environmental assessment,health monitoring,and so forth.展开更多
A low-viscosity emulsion of crude oil in water can be believed to be the bulk of a flow regime in a pipeline.To differentiate which crude oil would and which would not counter the blockage of flow due to gas hydrate f...A low-viscosity emulsion of crude oil in water can be believed to be the bulk of a flow regime in a pipeline.To differentiate which crude oil would and which would not counter the blockage of flow due to gas hydrate formation in flow channels,varying amount of crude oil in water emulsion without any other extraneous additives has undergone methane gas hydrate formation in an autoclave cell.Crude oil was able to thermodynamically inhibit the gas hydrate formation as observed from its hydrate stability zone.The normalized rate of hydrate formation in the emulsion has been calculated from an illustrative chemical affinity model,which showed a decrease in the methane consumption（decreased normalized rate constant） with an increase in the oil content in the emulsion.Fourier transform infrared spectroscopy（FTIR） of the emulsion and characteristic properties of the crude oil have been used to find the chemical component that could be pivotal in selfinhibitory characteristic of the crude oil collected from Ankleshwar,India,against a situation of clogged flow due to formation of gas hydrate and establish flow assurance.展开更多
Hydrogen isotope separation is a challenging task due to their similar properties.Herein,based on the chemical affinity quantum sieve(CAQS)effect,the D_(2)/H_(2)separation performance of M_(2)(m-dobdc)(M=Co,Ni,Mg,Mn;m...Hydrogen isotope separation is a challenging task due to their similar properties.Herein,based on the chemical affinity quantum sieve(CAQS)effect,the D_(2)/H_(2)separation performance of M_(2)(m-dobdc)(M=Co,Ni,Mg,Mn;m-dobdc^(4-)=4,6-dioxido-1,3-benzenedicarboxylate),a series of honeycomb-shaped MOFs with high stability and abundant open metal sites,are studied by gases sorption and breakthrough experiments,in which two critical factors,gas uptake and adsorption enthalpy,are taken into consideration.Among these MOFs,Co_(2)(m-dobdc)exhibits the longest D_(2)retention time of 180 min/g(H_(2)/D_(2)/Ne:1/1/98)at 77 K because of its second-highest adsorption enthalpy(10.7 kJ/mol for H_(2)and 11.8 kJ/mol for D_(2))and the best sorption capacity(5.22 mmol/g for H_(2)and 5.49 mmol/g for D_(2))under low pressure of 1 kPa and 77 K,which make it a promising material for industrial hydrogen isotope separation.Moreover,the results indicate that H_(2)and D_(2)capacities under low pressure(about 1 kPa)dominate the final D_(2)/H_(2)separation property of MOFs.展开更多
Spectroscopic measurements of pharmaceutical compound 5-fluorouracil(5-FU)drug was achieved in solvents with different polarity.The drug gave clear absorption peak at 259,269,270 and 266 nm in hexane,dimethyl sulfoxid...Spectroscopic measurements of pharmaceutical compound 5-fluorouracil(5-FU)drug was achieved in solvents with different polarity.The drug gave clear absorption peak at 259,269,270 and 266 nm in hexane,dimethyl sulfoxide(DMSO),N,N-dimethylformamide(DMF)and ethanol,as well as phosphate buffer respectively,which was consistent with the standard values in literatures.The results of extension coefficient(ε)and wave length(λmax)showed reduction in polar medium as compared to non-polar medium.The calibration curve of 5-FU drug was achieved by using serials solutions dis–6–4 solved in phosphate buffer(pH=7.4 and T=37℃)within the range of 1×10^(-6)~1×10^(-4) M.The sta–5 bility of 5-FU drug was studied in phosphate buffer at pH=5,6,7,7.4 and 8 with 1×10^(-5) M and T=37℃,according to the equation of first-order reaction.The hydrolysis of 5-FU disappeared at alkaline solution,but had noticeable hydrolysis in acidic solutions with the rate constant 25,14 and 20 at pH of 5,6 and 7 respectively.The calculation of molar extension coefficient and half-life(t_(1/2))showed same sequence of 5-FU hydrolysis.Then,rearrangement of obtained results offered complicated reversible equilibrium state by the combination between thermodynamic and kinetic behaviors of 5-FU hydrolysis;with Keq=8.46,6.11 and 142.8 at pH of 5,6 and 7 respectively.The acidic hydrolysis of 5-FU occurred spontaneously within free energy(ΔG)did not exceed 10 kJ/mol,which meant the electro motive forces of interactions were weak,notable to release energy such as Van der Waals forces or hydrogen bonding.展开更多
基金financially supported in part by National Key R&D Program of China(Nos.2020YFA0406103,2017YFA0207301)National Natural Science Foundation of China(Nos.21725102,91961106,U1832156,22075267,21803002)+4 种基金Science and Technological Fund of Anhui Province for Outstanding Youth(No.2008085J05)Youth Innovation Promotion Association of CAS(No.2019444)Young Elite Scientist Sponsorship Program by CAST,MOST(No.2018YFA0208603)Users with Excellence Program of Hefei Science Center CAS(No.2020HSC-UE003)Postdoc Matching Fund Scheme of the Hong Kong Polytechnic University(No.1-W144)。
文摘Anodic oxygen evolution reaction(OER)is the key bottleneck for water electrolysis technique owing to its sluggish reaction kinetics.Interfacial engineering on the rationally designed heterostructure can regulate the electronic states efficiently for intrinsic activity improvement.Here,we report a co-phosphorization approach to construct a VPO_(4)-Ni_(2)P heterostructure on nickel foam with strongly chemical binding,wherein phosphate acts as electronic modifier for Ni_(2)P electrocatalyst.Profiting from the interfacial interaction,it is uncovered that electron shifts from Ni_(2)P to VPO_(4)to render valence increment in Ni species.Such an electronic manipulation rationalizes the chemical affinities of various oxygen intermediates in OER pathway,giving a substantially reduced energy barrier.As a result,the advanced VPO_(4)-Ni_(2)P heterostructure only requires an overpotential of 289 mV to deliver a high current density of 350 mA/cm^(2)for OER in alkaline electrolyte,together with a Tafel slope as low as 28 mV/dec.This work brings fresh insights into interfacial engineering for advanced electrocatalyst design.
基金supported by the National Natural Science Foundation of China(Nos.52303380,52025132,52273305,22205185,21621091,22021001,and 22121001)Fundamental Research Funds for the Central Universities(No.20720240041)+3 种基金the 111 Project(Nos.B17027 and B16029)the National Science Foundation of Fujian Province of China(No.2022J02059)the Science and Technology Projects of Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province(No.RD2022070601)the New Cornerstone Science Foundation through the XPLORER PRIZE。
文摘Excessive Fe^(3+) ion concentrations in wastewater pose a long-standing threat to human health.Achieving low-cost,high-efficiency quantification of Fe^(3+) ion concentration in unknown solutions can guide environmental management decisions and optimize water treatment processes.In this study,by leveraging the rapid,real-time detection capabilities of nanopores and the specific chemical binding affinity of tannic acid to Fe^(3+),a linear relationship between the ion current and Fe^(3+) ion concentration was established.Utilizing this linear relationship,quantification of Fe^(3+) ion concentration in unknown solutions was achieved.Furthermore,ethylenediaminetetraacetic acid disodium salt was employed to displace Fe^(3+) from the nanopores,allowing them to be restored to their initial conditions and reused for Fe^(3+) ion quantification.The reusable bioinspired nanopores remain functional over 330 days of storage.This recycling capability and the long-term stability of the nanopores contribute to a significant reduction in costs.This study provides a strategy for the quantification of unknown Fe^(3+) concentration using nanopores,with potential applications in environmental assessment,health monitoring,and so forth.
基金the financial assistance provided by University Grants Commission, New Delhi, India, under Special Assistance Program (SAP) to the Department of Petroleum Engineering, Indian School of Mines, Dhanbad, India
文摘A low-viscosity emulsion of crude oil in water can be believed to be the bulk of a flow regime in a pipeline.To differentiate which crude oil would and which would not counter the blockage of flow due to gas hydrate formation in flow channels,varying amount of crude oil in water emulsion without any other extraneous additives has undergone methane gas hydrate formation in an autoclave cell.Crude oil was able to thermodynamically inhibit the gas hydrate formation as observed from its hydrate stability zone.The normalized rate of hydrate formation in the emulsion has been calculated from an illustrative chemical affinity model,which showed a decrease in the methane consumption（decreased normalized rate constant） with an increase in the oil content in the emulsion.Fourier transform infrared spectroscopy（FTIR） of the emulsion and characteristic properties of the crude oil have been used to find the chemical component that could be pivotal in selfinhibitory characteristic of the crude oil collected from Ankleshwar,India,against a situation of clogged flow due to formation of gas hydrate and establish flow assurance.
基金financially supported by the Strategic Priority Research Program of Chinese Academy of Sciences(No.XDB20000000)the Key Research Program of Frontier Sciences,Chinese Academy of Sciences(No.QYZDB-SSW-SLH019)the National Natural Science Foundation of China(Nos.21771177,51603206 and 21203117).
文摘Hydrogen isotope separation is a challenging task due to their similar properties.Herein,based on the chemical affinity quantum sieve(CAQS)effect,the D_(2)/H_(2)separation performance of M_(2)(m-dobdc)(M=Co,Ni,Mg,Mn;m-dobdc^(4-)=4,6-dioxido-1,3-benzenedicarboxylate),a series of honeycomb-shaped MOFs with high stability and abundant open metal sites,are studied by gases sorption and breakthrough experiments,in which two critical factors,gas uptake and adsorption enthalpy,are taken into consideration.Among these MOFs,Co_(2)(m-dobdc)exhibits the longest D_(2)retention time of 180 min/g(H_(2)/D_(2)/Ne:1/1/98)at 77 K because of its second-highest adsorption enthalpy(10.7 kJ/mol for H_(2)and 11.8 kJ/mol for D_(2))and the best sorption capacity(5.22 mmol/g for H_(2)and 5.49 mmol/g for D_(2))under low pressure of 1 kPa and 77 K,which make it a promising material for industrial hydrogen isotope separation.Moreover,the results indicate that H_(2)and D_(2)capacities under low pressure(about 1 kPa)dominate the final D_(2)/H_(2)separation property of MOFs.
文摘Spectroscopic measurements of pharmaceutical compound 5-fluorouracil(5-FU)drug was achieved in solvents with different polarity.The drug gave clear absorption peak at 259,269,270 and 266 nm in hexane,dimethyl sulfoxide(DMSO),N,N-dimethylformamide(DMF)and ethanol,as well as phosphate buffer respectively,which was consistent with the standard values in literatures.The results of extension coefficient(ε)and wave length(λmax)showed reduction in polar medium as compared to non-polar medium.The calibration curve of 5-FU drug was achieved by using serials solutions dis–6–4 solved in phosphate buffer(pH=7.4 and T=37℃)within the range of 1×10^(-6)~1×10^(-4) M.The sta–5 bility of 5-FU drug was studied in phosphate buffer at pH=5,6,7,7.4 and 8 with 1×10^(-5) M and T=37℃,according to the equation of first-order reaction.The hydrolysis of 5-FU disappeared at alkaline solution,but had noticeable hydrolysis in acidic solutions with the rate constant 25,14 and 20 at pH of 5,6 and 7 respectively.The calculation of molar extension coefficient and half-life(t_(1/2))showed same sequence of 5-FU hydrolysis.Then,rearrangement of obtained results offered complicated reversible equilibrium state by the combination between thermodynamic and kinetic behaviors of 5-FU hydrolysis;with Keq=8.46,6.11 and 142.8 at pH of 5,6 and 7 respectively.The acidic hydrolysis of 5-FU occurred spontaneously within free energy(ΔG)did not exceed 10 kJ/mol,which meant the electro motive forces of interactions were weak,notable to release energy such as Van der Waals forces or hydrogen bonding.
