The electrocatalytic oxidation of biomass-derived furfural(FF)feedstocks into 2-furoic acid(FA)holds immense industrial potential in optics,cosmetics,polymers,and food.Herein,we fabricated Co O/Ni O/nickel foam(NF)and...The electrocatalytic oxidation of biomass-derived furfural(FF)feedstocks into 2-furoic acid(FA)holds immense industrial potential in optics,cosmetics,polymers,and food.Herein,we fabricated Co O/Ni O/nickel foam(NF)and Cu_(2)O/Ni O/NF electrodes via in situ pulsed laser irradiation in liquids(PLIL)for the bifunctional electrocatalysis of oxygen evolution reaction(OER)and furfural oxidation reaction(FOR),respectively.Simultaneous oxidation of NF surface to NiO and deposition of CoO and/or Cu_(2)O on NF during PLIL offer distinct advantages for enhancing both the OER and FOR.CoO/NiO/NF electrocatalyst provides a consistently low overpotential of~359 m V(OER)at 10 m A/cm^(2),achieving the maximum FA yield(~16.37 m M)with 61.5%selectivity,79.5%carbon balance,and a remarkable Faradaic efficiency of~90.1%during 2 h of FOR at 1.43 V(vs.reversible hydrogen electrode).Mechanistic pathway via in situ electrochemical-Raman spectroscopy on CoO/NiO/NF reveals the involvement of phase transition intermediates(NiOOH and CoOOH)as surface-active centers during electrochemical oxidation.The carbonyl carbon in FF is attacked by hydroxyl groups to form unstable hydrates that subsequently undergo further oxidation to yield FA products.This method holds promise for large-scale applications,enabling simultaneous production of renewable building materials and fuel.展开更多
A novel coordination polymer [Nd2(PDB)2(CH3COO)2(H2O)3] (H2PDB = pyridine- 3,4-dicarboxylic acid) has been synthesized by the reaction of Nd(CH3COO)3 with pyridine- 3,4-dicarboxylic acid under hydrothermal conditions....A novel coordination polymer [Nd2(PDB)2(CH3COO)2(H2O)3] (H2PDB = pyridine- 3,4-dicarboxylic acid) has been synthesized by the reaction of Nd(CH3COO)3 with pyridine- 3,4-dicarboxylic acid under hydrothermal conditions. Elemental analysis, IR spectra and X-ray crystal structure analysis were carried out to determine the composition and crystal structure of the title complex which belongs to the triclinic system, space group P1 with a = 6.9409(14), b = 7.5497(15), c = 22.530(5) , α = 84.79(3), β = 88.15(3), γ = 75.55(3)°, C18H18N2O15Nd2, Mr = 790.82, Z = 2, V = 1138.5(4) 3, Dc = 2.307 g/cm3, μ = 4.593 mm-1, –6≤h≤8, –5≤k≤8, –26≤l≤ 26, F(000) = 760, Rint = 0.0298, R = 0.0314 and wR = 0.0695 (I > 2σ(I)). Nd(1) and Nd(2) are linked into zigzag chains by carboxylate groups of acetate with interesting μ3-η2:η2 fashion. The zigzag chains are bridged by PDB to form a 2D framework, and a 3D supramolecular network is further constructed via π-π stacking.展开更多
Combustion catalyst La0.8Sr0.2CoO3 （LSC） is expected to possess relatively high activity for the oxidation of carbon monoxide and many hydrocarbons. If γ-Al2O3 is used as its support, cobalt ions can easily react w...Combustion catalyst La0.8Sr0.2CoO3 （LSC） is expected to possess relatively high activity for the oxidation of carbon monoxide and many hydrocarbons. If γ-Al2O3 is used as its support, cobalt ions can easily react with γ-Al2O3 at not very high temperature to form spinel CoAl2O4 or spinel-like, which decreases the activity of the combustion catalyst. In this paper, MgAl2O4 and CaAl2O4 were pre-coated on γ-Al2O3 by impregnation respectively, which formed compound support for LSC. It is shown that, when MgAl2O4 layer is covered on the surface of MgAl2O4 by impregnation, the entering of cobalt ions into γ-Al2O3 lattice is restrained, then LSC formed on the surface of MgAl2O4, which leads to a good catalytic activity of xylene complete oxidation. But the layer of MgAl2O4 should be thick enough to reach 30% （mass fraction） MgO in the support due to large size particle of MgAl2O4 crystalline. If polyvinyl alcohol （PVA） is added into the impregnation solution adequately, MgAl2O4 particles formed on the surface of γ-Al2O3 are getting smaller, and less amount of MgAl2O4 is needed to cover up the surface of γ-Al2O3. If CaAl2O4 layer substituted for MgAl2O4, more closed cover is obtained in virtue of fine particles of CaAl2O4. The activity examination shows that smaller particles of MgAl2O4 or CaAl2O4 can be more effective to hinder cobalt ions entering the lattice of γ-Al2O3, and better activities will be obtained.展开更多
基金supported by the Korea Basic Science Institute(National research Facilities and Equipment Center)grant funded by the Ministry of Education(2019R1A6C1010042,2021R1A6C103A427)the financial support from the National Research Foundation of Korea(NRF)(2022R1A2C2010686,2022R1A4A3033528,2021R1I1A1A01060380,2021R1C1C2010726,2019H1D3A1A01071209)。
文摘The electrocatalytic oxidation of biomass-derived furfural(FF)feedstocks into 2-furoic acid(FA)holds immense industrial potential in optics,cosmetics,polymers,and food.Herein,we fabricated Co O/Ni O/nickel foam(NF)and Cu_(2)O/Ni O/NF electrodes via in situ pulsed laser irradiation in liquids(PLIL)for the bifunctional electrocatalysis of oxygen evolution reaction(OER)and furfural oxidation reaction(FOR),respectively.Simultaneous oxidation of NF surface to NiO and deposition of CoO and/or Cu_(2)O on NF during PLIL offer distinct advantages for enhancing both the OER and FOR.CoO/NiO/NF electrocatalyst provides a consistently low overpotential of~359 m V(OER)at 10 m A/cm^(2),achieving the maximum FA yield(~16.37 m M)with 61.5%selectivity,79.5%carbon balance,and a remarkable Faradaic efficiency of~90.1%during 2 h of FOR at 1.43 V(vs.reversible hydrogen electrode).Mechanistic pathway via in situ electrochemical-Raman spectroscopy on CoO/NiO/NF reveals the involvement of phase transition intermediates(NiOOH and CoOOH)as surface-active centers during electrochemical oxidation.The carbonyl carbon in FF is attacked by hydroxyl groups to form unstable hydrates that subsequently undergo further oxidation to yield FA products.This method holds promise for large-scale applications,enabling simultaneous production of renewable building materials and fuel.
基金Project supported by the National Natural Science Foundation of China (No. 20671064)Foundation of Education Committee of Liaoning Province (No. 2005336)
文摘A novel coordination polymer [Nd2(PDB)2(CH3COO)2(H2O)3] (H2PDB = pyridine- 3,4-dicarboxylic acid) has been synthesized by the reaction of Nd(CH3COO)3 with pyridine- 3,4-dicarboxylic acid under hydrothermal conditions. Elemental analysis, IR spectra and X-ray crystal structure analysis were carried out to determine the composition and crystal structure of the title complex which belongs to the triclinic system, space group P1 with a = 6.9409(14), b = 7.5497(15), c = 22.530(5) , α = 84.79(3), β = 88.15(3), γ = 75.55(3)°, C18H18N2O15Nd2, Mr = 790.82, Z = 2, V = 1138.5(4) 3, Dc = 2.307 g/cm3, μ = 4.593 mm-1, –6≤h≤8, –5≤k≤8, –26≤l≤ 26, F(000) = 760, Rint = 0.0298, R = 0.0314 and wR = 0.0695 (I > 2σ(I)). Nd(1) and Nd(2) are linked into zigzag chains by carboxylate groups of acetate with interesting μ3-η2:η2 fashion. The zigzag chains are bridged by PDB to form a 2D framework, and a 3D supramolecular network is further constructed via π-π stacking.
文摘Combustion catalyst La0.8Sr0.2CoO3 （LSC） is expected to possess relatively high activity for the oxidation of carbon monoxide and many hydrocarbons. If γ-Al2O3 is used as its support, cobalt ions can easily react with γ-Al2O3 at not very high temperature to form spinel CoAl2O4 or spinel-like, which decreases the activity of the combustion catalyst. In this paper, MgAl2O4 and CaAl2O4 were pre-coated on γ-Al2O3 by impregnation respectively, which formed compound support for LSC. It is shown that, when MgAl2O4 layer is covered on the surface of MgAl2O4 by impregnation, the entering of cobalt ions into γ-Al2O3 lattice is restrained, then LSC formed on the surface of MgAl2O4, which leads to a good catalytic activity of xylene complete oxidation. But the layer of MgAl2O4 should be thick enough to reach 30% （mass fraction） MgO in the support due to large size particle of MgAl2O4 crystalline. If polyvinyl alcohol （PVA） is added into the impregnation solution adequately, MgAl2O4 particles formed on the surface of γ-Al2O3 are getting smaller, and less amount of MgAl2O4 is needed to cover up the surface of γ-Al2O3. If CaAl2O4 layer substituted for MgAl2O4, more closed cover is obtained in virtue of fine particles of CaAl2O4. The activity examination shows that smaller particles of MgAl2O4 or CaAl2O4 can be more effective to hinder cobalt ions entering the lattice of γ-Al2O3, and better activities will be obtained.
