Copper-based nanomaterials have been widely used in catalysis,electrodes,and other applications due to their unique electron-transfer properties.In this work,an efficient electrochemical sensor based on an electrode m...Copper-based nanomaterials have been widely used in catalysis,electrodes,and other applications due to their unique electron-transfer properties.In this work,an efficient electrochemical sensor based on an electrode modified with one-dimensional Cu(OH)_(2)/carboxymethyl cellulose(CMC)composite nanofibers was fabricated and investigated for the detection of aspirin.Scanning electron microscopy was employed to examine the morphological characteristics of these composite nanofibers.Cyclic voltammetry and electrochemical impedance spectroscopy were used to assess the electrochemical performance of a Cu(OH)_(2)/CMC composite nanofiber-modified electrode.The findings indicate that the modified electrode has a very high sensitivity to aspirin.The observed enhanced performance could be a result of the high surface-to-volume ratio of the composite nanofibers and their superior electron-transport characteristics,which may hasten electron transfer between aspirin and the surfaces of the modified electrode.This detection technique also demonstrated strong selectivity for aspirin.These findings imply that the technique can be applied as a highly effective and selective approach to aspirin measurement in biological science.展开更多
Rational design of oxygen evolution reaction(OER)catalysts at low cost would greatly benefit the economy.Taking advantage of earth-abundant elements Si,Co and Ni,we produce a unique-structure where cobalt-nickel silic...Rational design of oxygen evolution reaction(OER)catalysts at low cost would greatly benefit the economy.Taking advantage of earth-abundant elements Si,Co and Ni,we produce a unique-structure where cobalt-nickel silicate hydroxide[Co_(2.5)Ni_(0.5)Si_(2)O_(5)(OH)_(4)]is vertically grown on a reduced graphene oxide(rGO)support(CNS@rGO).This is developed as a low-cost and prospective OER catalyst.Compared to cobalt or nickel silicate hydroxide@rGO(CS@rGO and NS@rGO,respectively)nanoarrays,the bimetal CNS@rGO nanoarray exhibits impressive OER performance with an overpotential of 307 mV@10 mA cm^(-2).This value is higher than that of CS@rGO and NS@rGO.The CNS@rGO nanoarray has an overpotential of 446 mV@100 mA cm^(-2),about 1.4 times that of the commercial RuO_(2)electrocatalyst.The achieved OER activity is superior to the state-of-the-art metal oxides/hydroxides and their derivatives.The vertically grown nanostructure and optimized metal-support electronic interactions play an indispensable role for OER performance improvement,including a fast electron transfer pathway,short proton/electron diffusion distance,more active metal centers,as well as optimized dualatomic electron density.Taking advantage of interlay chemical regulation and the in-situ growth method,the advanced-structural CNS@rGO nanoarrays provide a new horizon to the rational and flexible design of efficient and promising OER electrocatalysts.展开更多
A simple method was proposed to activate alkaline Cu(OH)_(2)with an acidic ionomer,Nafion,to regulate its surface microenvironment,including hydrophobicity and local basicity.In particular,the direct complete neutrali...A simple method was proposed to activate alkaline Cu(OH)_(2)with an acidic ionomer,Nafion,to regulate its surface microenvironment,including hydrophobicity and local basicity.In particular,the direct complete neutralization reaction between Cu(OH)_(2)and Nafion in aqueous solution induces the exposing of vast anions which can exclude the in-situ-formed hydroxides and raise the local basicity.Remarkably,the optimal Nafionactivated Cu(OH)_(2)-derived Cu can efficiently suppress the hydrogen evolution reaction(HER)and improve the selectivity for multi-carbon products in the CO_(2)electroreduction reaction(eCO_(2)RR).The H2 Faradaic efficiency(FE)decreased to 11%at a current density of 300 mA/cm2(−0.76 V vs.RHE)in a flow cell,while the bare one with H2 had an FE of 40%.The total eCO_(2)RR FE reaches as high as 83%,along with an evidently increased C2H4 FE of 44%as compared with the bare one(24%),and good stability(8000 s),surpassing that of most of the reported Cu(OH)_(2)-derived Cu.The experimental and theoretical results both show that the strong hydrophobicity and high local basicity jointly boosted the eCO_(2)RR as acquired by felicitously introducing ionomer on the Cu(OH)_(2)-derived Cu surface.展开更多
Design of the catalyst for efficient water dissociation and hydrogen recombination is paramount in enhancement of the alkaline water electrolysis kinetics.Herein,we reported a delicate hierarchical(VO)_(2) P_(2)O_(7)-...Design of the catalyst for efficient water dissociation and hydrogen recombination is paramount in enhancement of the alkaline water electrolysis kinetics.Herein,we reported a delicate hierarchical(VO)_(2) P_(2)O_(7)-Ni_(2) P@NF(VPO-Ni_(2) P@NF)hybrid catalyst that operated efficiently in alkaline media.The VPO and Ni_(2) P respectively act as the water dissociation promoter and the hydrogen recombination center,which synergistically propel water adsorption/dissociation and H intermediates recombination.The resulting synergistic interfaces between VPO and Ni_(2) P are verified to afford the catalyst an outstanding performance for hydrogen evolution reaction in alkaline media with an overpotential of 154 mV at 10 mA cm^(-2),Tafel slope of 65 mV dec^(-1),and remarkable durability.Furthermore,the catalyst presents the potential for overall water splitting.This work may shed fresh light on the high-performance electrocatalyst design and the application of VPO on water electrolysis.展开更多
Electrocatalytic nitrate(NO_(3)^(−))reduction to ammonia(NH_(3))offers a viable approach for sustainable NH_(3)production and environmental denitrification.Copper(Cu)possesses a distinctive electronic structure,which ...Electrocatalytic nitrate(NO_(3)^(−))reduction to ammonia(NH_(3))offers a viable approach for sustainable NH_(3)production and environmental denitrification.Copper(Cu)possesses a distinctive electronic structure,which can augment the reaction kinetics of NO_(3)^(−)and impede hydrogen evolution reaction(HER),rendering it a promising contender for the electrosynthesis of NH_(3)from NO_(3)^(−).Nevertheless,the role of Cu_(2)O in copper-based catalysts still requires further investigation for a more comprehensive understanding.Herein,the Cu_(2)O/Cu(OH)_(2)heterostructures are successfully fabricated through liquid laser irradiation using CuO nanoparticles as a precursor.Experimental and theoretical researches reveal that Cu_(2)O/Cu(OH)_(2)heterostructure exhibits enhanced electrocatalytic performance for NO_(3)^(−)to NH_(3)because Cu(OH)_(2)promotes electron transfer and reduces the valence state of Cu active site in Cu_(2)O.At−0.6 V(vs.reversible hydrogen electrode(RHE)),the NH_(3)yield reaches its maximum at 1630.66±29.72μg·h^(−1)·mgcat^(−1),while the maximum of Faraday efficiency(FE)is 76.95%±5.51%.This study expands the technical scope of copper-based catalyst preparation and enhances the understanding of the electrocatalytic mechanism of NO_(3)^(−)to NH_(3).展开更多
Cu doped Mg(OH)_(2) nanoparticles were synthesized with varying concentrations from 0 to 10%by a chemical synthesis technique of coprecipitation.X-rays diffraction (XRD) of the samples confirms that all the samples ac...Cu doped Mg(OH)_(2) nanoparticles were synthesized with varying concentrations from 0 to 10%by a chemical synthesis technique of coprecipitation.X-rays diffraction (XRD) of the samples confirms that all the samples acquire the hexagonal crystal structure.XRD results indicated the solubility limit of dopant in the host material and the secondary phase of CuO was observed beyond 3%Cu doping in Mg(OH)_(2).The reduction in the size of nanoparticles was observed from 166 to 103 nm for Mg(OH)_(2) and 10% Cu doped Mg(OH)_(2)samples,respectively.The shift in absorption spectra exhibited the systematical enhancement in optical bandgap from 5.25 to 6.085 eV.A good correlation was observed between the bandgap energy and crystallite size of the nanocrystals which confirmed the size induced effect in the nanoparticles.The transformation in the sample morphology was observed from irregular spherical particles to sepals like shapes with increasing the Cu concentration in the host material.The energy dispersive X-Ray (EDX) analysis confirmed the purity of mass percentage composition of the elements present in the samples.展开更多
基金The authors wish to acknowledge financial support from the Science and Technology Projects in Jilin Province Department of Education(Grant No.JJKH20220239KJ).
文摘Copper-based nanomaterials have been widely used in catalysis,electrodes,and other applications due to their unique electron-transfer properties.In this work,an efficient electrochemical sensor based on an electrode modified with one-dimensional Cu(OH)_(2)/carboxymethyl cellulose(CMC)composite nanofibers was fabricated and investigated for the detection of aspirin.Scanning electron microscopy was employed to examine the morphological characteristics of these composite nanofibers.Cyclic voltammetry and electrochemical impedance spectroscopy were used to assess the electrochemical performance of a Cu(OH)_(2)/CMC composite nanofiber-modified electrode.The findings indicate that the modified electrode has a very high sensitivity to aspirin.The observed enhanced performance could be a result of the high surface-to-volume ratio of the composite nanofibers and their superior electron-transport characteristics,which may hasten electron transfer between aspirin and the surfaces of the modified electrode.This detection technique also demonstrated strong selectivity for aspirin.These findings imply that the technique can be applied as a highly effective and selective approach to aspirin measurement in biological science.
基金supported by the Fundamental Research Funds for the Central Universities(DUT21LK34)Natural Science Foundation of Liaoning Province(2020-MS-113).
文摘Rational design of oxygen evolution reaction(OER)catalysts at low cost would greatly benefit the economy.Taking advantage of earth-abundant elements Si,Co and Ni,we produce a unique-structure where cobalt-nickel silicate hydroxide[Co_(2.5)Ni_(0.5)Si_(2)O_(5)(OH)_(4)]is vertically grown on a reduced graphene oxide(rGO)support(CNS@rGO).This is developed as a low-cost and prospective OER catalyst.Compared to cobalt or nickel silicate hydroxide@rGO(CS@rGO and NS@rGO,respectively)nanoarrays,the bimetal CNS@rGO nanoarray exhibits impressive OER performance with an overpotential of 307 mV@10 mA cm^(-2).This value is higher than that of CS@rGO and NS@rGO.The CNS@rGO nanoarray has an overpotential of 446 mV@100 mA cm^(-2),about 1.4 times that of the commercial RuO_(2)electrocatalyst.The achieved OER activity is superior to the state-of-the-art metal oxides/hydroxides and their derivatives.The vertically grown nanostructure and optimized metal-support electronic interactions play an indispensable role for OER performance improvement,including a fast electron transfer pathway,short proton/electron diffusion distance,more active metal centers,as well as optimized dualatomic electron density.Taking advantage of interlay chemical regulation and the in-situ growth method,the advanced-structural CNS@rGO nanoarrays provide a new horizon to the rational and flexible design of efficient and promising OER electrocatalysts.
基金National Natural Science Foundation of China,Grant/Award Numbers:52201227,21972126,51872209,52072273Zhejiang Provincial Special Support Program for High-level Talents,Grant/Award Number:2019R52042Key Project of Zhejiang Provincial Natural Science Foundation,Grant/Award Number:LZ20B030001。
文摘A simple method was proposed to activate alkaline Cu(OH)_(2)with an acidic ionomer,Nafion,to regulate its surface microenvironment,including hydrophobicity and local basicity.In particular,the direct complete neutralization reaction between Cu(OH)_(2)and Nafion in aqueous solution induces the exposing of vast anions which can exclude the in-situ-formed hydroxides and raise the local basicity.Remarkably,the optimal Nafionactivated Cu(OH)_(2)-derived Cu can efficiently suppress the hydrogen evolution reaction(HER)and improve the selectivity for multi-carbon products in the CO_(2)electroreduction reaction(eCO_(2)RR).The H2 Faradaic efficiency(FE)decreased to 11%at a current density of 300 mA/cm2(−0.76 V vs.RHE)in a flow cell,while the bare one with H2 had an FE of 40%.The total eCO_(2)RR FE reaches as high as 83%,along with an evidently increased C2H4 FE of 44%as compared with the bare one(24%),and good stability(8000 s),surpassing that of most of the reported Cu(OH)_(2)-derived Cu.The experimental and theoretical results both show that the strong hydrophobicity and high local basicity jointly boosted the eCO_(2)RR as acquired by felicitously introducing ionomer on the Cu(OH)_(2)-derived Cu surface.
基金supported by the National Natural Science Foundation of China(No.51902232)。
文摘Design of the catalyst for efficient water dissociation and hydrogen recombination is paramount in enhancement of the alkaline water electrolysis kinetics.Herein,we reported a delicate hierarchical(VO)_(2) P_(2)O_(7)-Ni_(2) P@NF(VPO-Ni_(2) P@NF)hybrid catalyst that operated efficiently in alkaline media.The VPO and Ni_(2) P respectively act as the water dissociation promoter and the hydrogen recombination center,which synergistically propel water adsorption/dissociation and H intermediates recombination.The resulting synergistic interfaces between VPO and Ni_(2) P are verified to afford the catalyst an outstanding performance for hydrogen evolution reaction in alkaline media with an overpotential of 154 mV at 10 mA cm^(-2),Tafel slope of 65 mV dec^(-1),and remarkable durability.Furthermore,the catalyst presents the potential for overall water splitting.This work may shed fresh light on the high-performance electrocatalyst design and the application of VPO on water electrolysis.
基金Scientific Research Project in Anhui Jianzhu University(No.2023QDZ04).
文摘Electrocatalytic nitrate(NO_(3)^(−))reduction to ammonia(NH_(3))offers a viable approach for sustainable NH_(3)production and environmental denitrification.Copper(Cu)possesses a distinctive electronic structure,which can augment the reaction kinetics of NO_(3)^(−)and impede hydrogen evolution reaction(HER),rendering it a promising contender for the electrosynthesis of NH_(3)from NO_(3)^(−).Nevertheless,the role of Cu_(2)O in copper-based catalysts still requires further investigation for a more comprehensive understanding.Herein,the Cu_(2)O/Cu(OH)_(2)heterostructures are successfully fabricated through liquid laser irradiation using CuO nanoparticles as a precursor.Experimental and theoretical researches reveal that Cu_(2)O/Cu(OH)_(2)heterostructure exhibits enhanced electrocatalytic performance for NO_(3)^(−)to NH_(3)because Cu(OH)_(2)promotes electron transfer and reduces the valence state of Cu active site in Cu_(2)O.At−0.6 V(vs.reversible hydrogen electrode(RHE)),the NH_(3)yield reaches its maximum at 1630.66±29.72μg·h^(−1)·mgcat^(−1),while the maximum of Faraday efficiency(FE)is 76.95%±5.51%.This study expands the technical scope of copper-based catalyst preparation and enhances the understanding of the electrocatalytic mechanism of NO_(3)^(−)to NH_(3).
文摘Cu doped Mg(OH)_(2) nanoparticles were synthesized with varying concentrations from 0 to 10%by a chemical synthesis technique of coprecipitation.X-rays diffraction (XRD) of the samples confirms that all the samples acquire the hexagonal crystal structure.XRD results indicated the solubility limit of dopant in the host material and the secondary phase of CuO was observed beyond 3%Cu doping in Mg(OH)_(2).The reduction in the size of nanoparticles was observed from 166 to 103 nm for Mg(OH)_(2) and 10% Cu doped Mg(OH)_(2)samples,respectively.The shift in absorption spectra exhibited the systematical enhancement in optical bandgap from 5.25 to 6.085 eV.A good correlation was observed between the bandgap energy and crystallite size of the nanocrystals which confirmed the size induced effect in the nanoparticles.The transformation in the sample morphology was observed from irregular spherical particles to sepals like shapes with increasing the Cu concentration in the host material.The energy dispersive X-Ray (EDX) analysis confirmed the purity of mass percentage composition of the elements present in the samples.
