Designing efficient and long-lasting non-metal electrocatalysts is an urgent task for addressing the issue of kinetic hysteresis in electrochemical oxidation reactions.The bimetallic hydroxides,catalyzing the oxygen e...Designing efficient and long-lasting non-metal electrocatalysts is an urgent task for addressing the issue of kinetic hysteresis in electrochemical oxidation reactions.The bimetallic hydroxides,catalyzing the oxygen evolution reaction(OER),have significant research potential because hydroxide reconstruction to generate an active phase is a remarkable advantage.Herein,the complete reconstruction of ultrathin CoNi(OH)_(2) nanosheets was achieved by embedding Ag nanoparticles into the hydroxide to induce a spontaneous redox reaction(SRR),forming heterojunction Ag@CoNi(OH)_(2) for bifunctional hydrolysis.Theoretical calculations and in situ Raman and ex situ characterizations revealed that the inductive effect of the Ag cation redistributed the charge to promote phase transformation to highly activate Ag-modified hydroxides.The Co-Ni dual sites in Co/NiOOH serve as novel active sites for optimizing the intermediates,thereby weakening the barrier formed by OOH^*.Ag@CoNi(OH)_(2) required a potential of 1.55 V to drive water splitting at a current density of 10 mA cm^(-2),with nearly 98.6% Faraday efficiency.Through ion induction and triggering of electron regulation in the OER via the synergistic action of the heterogeneous interface and surface reconstruction,this strategic design can overcome the limited capacity of bimetallic hydroxides and bridge the gap between the basic theory and industrialization of water decomposition.展开更多
Oxygen evolution from water driven by electrocatalysis or photocatalysis poses a significant challenge as it requires the use of efficient electro-/photo-catalysts to drive the four-electron oxygen evolution reaction(...Oxygen evolution from water driven by electrocatalysis or photocatalysis poses a significant challenge as it requires the use of efficient electro-/photo-catalysts to drive the four-electron oxygen evolution reaction(OER).Herein,we report the development of an effective strategy for the in situ chemical transformation of Fe-based bimetallic MIL-88 metal-organic frameworks(MOFs)into corresponding bimetallic hydroxides,which are composed of amorphous ultrasmall nanoparticles and afford an abundance of catalytically active sites.Optimized MOF-derived NiFe-OH-0.75 catalyst coated on glassy carbon electrodes achieved a current density of 10 mA cm^(-2)in the electrocatalytic OER with a small overpotential of 270 mV,which could be decreased to 235 mV when loading the catalysts on a nickel foam substrate.Moreover,these MOF-derived Fe-based bimetallic hydroxides can be used as efficient cocatalysts when combined with suitable photosensitizers for photocatalytic water oxidation.展开更多
This study aimed to fabricate new and effective material for the efficiency of phosphate adsorption.Two types of adsorbent materials,the zirconium hydroxides embedded in pomegranate peel(Zr/Peel)and zirconium-lanthanu...This study aimed to fabricate new and effective material for the efficiency of phosphate adsorption.Two types of adsorbent materials,the zirconium hydroxides embedded in pomegranate peel(Zr/Peel)and zirconium-lanthanum hydroxides embedded in pomegranate peel(Zr-La/Peel)were developed.Scanning electronic microscopy(SEM),x-ray photoelectron spectroscopy(XPS)and x-ray diffraction(XRD)were evaluated to give insight into the physicochemical properties of these adsorbents.Zr-La/Peel exceeded the adsorption efficiency of Zr/Peel adsorbents in batch adsorption experiments at the same pH level.The peel as a host can strive to have a strong"shielding effect"to increase the steadiness of the entrenched Zr and La elements.La and Zr are hydroxide metals that emit many hydrogen ions during the hydrolysis reaction,which contribute to protonation and electrostatic attraction.The highest adsorption capacity of La-Zr/Peel for phosphate was calculated to be40.21 mg/g,and pseudo second-order equation is very well fitted for kinetic adsorption.Phosphate adsorption efficiency was reduced by an increase of pH.With the background of coexisting Cl-,little effect on adsorption efficiency was observed,while adsorption capacities were reduced by almost 20-30%with the coexistence of SO42-,NO3-and humic acid(HA).展开更多
基金supported by the Inner Mongolia R&D Program Plan(2021ZD0042,2021EEDSCXSFQZD006)the National Natural Science Foundation of China(21902123)the Natural Science Basic Research Program of Shaanxi(2023-JC-ZD-22)。
文摘Designing efficient and long-lasting non-metal electrocatalysts is an urgent task for addressing the issue of kinetic hysteresis in electrochemical oxidation reactions.The bimetallic hydroxides,catalyzing the oxygen evolution reaction(OER),have significant research potential because hydroxide reconstruction to generate an active phase is a remarkable advantage.Herein,the complete reconstruction of ultrathin CoNi(OH)_(2) nanosheets was achieved by embedding Ag nanoparticles into the hydroxide to induce a spontaneous redox reaction(SRR),forming heterojunction Ag@CoNi(OH)_(2) for bifunctional hydrolysis.Theoretical calculations and in situ Raman and ex situ characterizations revealed that the inductive effect of the Ag cation redistributed the charge to promote phase transformation to highly activate Ag-modified hydroxides.The Co-Ni dual sites in Co/NiOOH serve as novel active sites for optimizing the intermediates,thereby weakening the barrier formed by OOH^*.Ag@CoNi(OH)_(2) required a potential of 1.55 V to drive water splitting at a current density of 10 mA cm^(-2),with nearly 98.6% Faraday efficiency.Through ion induction and triggering of electron regulation in the OER via the synergistic action of the heterogeneous interface and surface reconstruction,this strategic design can overcome the limited capacity of bimetallic hydroxides and bridge the gap between the basic theory and industrialization of water decomposition.
文摘Oxygen evolution from water driven by electrocatalysis or photocatalysis poses a significant challenge as it requires the use of efficient electro-/photo-catalysts to drive the four-electron oxygen evolution reaction(OER).Herein,we report the development of an effective strategy for the in situ chemical transformation of Fe-based bimetallic MIL-88 metal-organic frameworks(MOFs)into corresponding bimetallic hydroxides,which are composed of amorphous ultrasmall nanoparticles and afford an abundance of catalytically active sites.Optimized MOF-derived NiFe-OH-0.75 catalyst coated on glassy carbon electrodes achieved a current density of 10 mA cm^(-2)in the electrocatalytic OER with a small overpotential of 270 mV,which could be decreased to 235 mV when loading the catalysts on a nickel foam substrate.Moreover,these MOF-derived Fe-based bimetallic hydroxides can be used as efficient cocatalysts when combined with suitable photosensitizers for photocatalytic water oxidation.
基金supported by the National Natural Science Foundation of China(No.51978384)Tai Shan Scholar Foundation(No.ts20151003)
文摘This study aimed to fabricate new and effective material for the efficiency of phosphate adsorption.Two types of adsorbent materials,the zirconium hydroxides embedded in pomegranate peel(Zr/Peel)and zirconium-lanthanum hydroxides embedded in pomegranate peel(Zr-La/Peel)were developed.Scanning electronic microscopy(SEM),x-ray photoelectron spectroscopy(XPS)and x-ray diffraction(XRD)were evaluated to give insight into the physicochemical properties of these adsorbents.Zr-La/Peel exceeded the adsorption efficiency of Zr/Peel adsorbents in batch adsorption experiments at the same pH level.The peel as a host can strive to have a strong"shielding effect"to increase the steadiness of the entrenched Zr and La elements.La and Zr are hydroxide metals that emit many hydrogen ions during the hydrolysis reaction,which contribute to protonation and electrostatic attraction.The highest adsorption capacity of La-Zr/Peel for phosphate was calculated to be40.21 mg/g,and pseudo second-order equation is very well fitted for kinetic adsorption.Phosphate adsorption efficiency was reduced by an increase of pH.With the background of coexisting Cl-,little effect on adsorption efficiency was observed,while adsorption capacities were reduced by almost 20-30%with the coexistence of SO42-,NO3-and humic acid(HA).