The high-efficiency conversion of biomass resources to biofuels has attracted widespread attention, and the active sites and synergistic effect of catalysts significantly impact their surface arrangement and electroni...The high-efficiency conversion of biomass resources to biofuels has attracted widespread attention, and the active sites and synergistic effect of catalysts significantly impact their surface arrangement and electronic structure. Here, a nickel-based transition metal carbide catalyst(Ni/TMC) with high Lewis acidity was prepared by self-assembly of transition metal carbide(TMC) and nickel, which exhibited excellent performance on synergistic hydrogenation and hydrogenolysis of 5-hydroxymethylfurfural(HMF) into liquid biofuel 2,5-dimethylfuran(DMF).Notably, Ni/WC with the highest Lewis acidity(4728.3 μmol g^(-1)) can achieve 100% conversion of HMF to 97.6% yield of DMF, with a turnover frequency of up to 46.5 h^(-1). The characterization results demonstrate that the rich Lewis acid sites yielded by the synergistic effect between Ni species and TMC are beneficial for the C=O hydrogenation and C–O cleavage, thereby accelerating the process of hydrodeoxygenation(HDO). Besides, a kinetic model for the HDO of HMF to DMF process has been established based on the experimental results, which elucidated a significant correlation between the measured and the predicted data(R~2> 0.97). Corresponding to the adsorption configuration of Ni/WC and substrate determined by in-situ FTIR characterization, this study provides a novel insight into the selective conversion of HMF process for functional biofuel and bio-chemicals.展开更多
Converting carbohydrates into 5-hydroxymethylfurfural(5-HMF) is an attractive and promising route for value-added utilization of agricultural and forestry biomass resource. As an important platform compound, 5-HMF pos...Converting carbohydrates into 5-hydroxymethylfurfural(5-HMF) is an attractive and promising route for value-added utilization of agricultural and forestry biomass resource. As an important platform compound, 5-HMF possesses high active furan structure with hydroxymethyl and aldehyde group for production of various bio-chemicals and materials, meanwhile, which suffer from low stability and poor yield during the industrial biorefinery process. Hence, selective production of 5-HMF with high-yield and low-cost has attracted extensive attention from scientific and industrial researchers. This review sorted and described the latest advanced research on solvent and catalyst system, as well as energy field effect for production of 5-HMF with different feedstock in detail, emphatically discussing the solvent effect and its synergistic effect with other aspects. Besides, the future prospects and challenges for production of 5-HMF from carbohydrates were also presented, which provide a profound insight into industrial 5-HMF process with economic and environmental feature.展开更多
Flourishing rare earth superhydrides are a class of recently discovered materials that exhibit near-room-temperature superconductivity at high pressures,ushering in a new era of superconductivity research at high pres...Flourishing rare earth superhydrides are a class of recently discovered materials that exhibit near-room-temperature superconductivity at high pressures,ushering in a new era of superconductivity research at high pressures.Yttrium superhydrides drew the most attention among these superhydrides due to their abundance of stoichiometries and excellent superconductivities.Here,we carried out a comprehensive study of yttrium superhydrides in a wide pressure range of 140 GPa-300 GPa.We successfully synthesized a series of superhydrides with the compositions of YH_(4),YH_(6),YH_(7),and YH_(9),and reported superconducting transition temperatures of 82 K at 167 GPa,218 K at 165 GPa,29 K at 162 GPa,and230 K at 300 GPa,respectively,as evidenced by sharp drops in resistance.The structure and superconductivity of YH_(4) were taken as a representative example and were also examined using x-ray diffraction measurements and the superconductivity suppression under external magnetic fields,respectively.Clathrate YH_(10),a candidate for room-temperature superconductor,was not synthesized within the study pressure and temperature ranges of up to 300 GPa and 2000 K.The current study established a detailed foundation for future research into room-temperature superconductors in polynary yttrium-based superhydrides.展开更多
基金Fundamental Research Foundation of CAF (CAFYBB2022QB001)National Nature Science Foundation of China for Excellent Young Scientists Fund (32222058)。
文摘The high-efficiency conversion of biomass resources to biofuels has attracted widespread attention, and the active sites and synergistic effect of catalysts significantly impact their surface arrangement and electronic structure. Here, a nickel-based transition metal carbide catalyst(Ni/TMC) with high Lewis acidity was prepared by self-assembly of transition metal carbide(TMC) and nickel, which exhibited excellent performance on synergistic hydrogenation and hydrogenolysis of 5-hydroxymethylfurfural(HMF) into liquid biofuel 2,5-dimethylfuran(DMF).Notably, Ni/WC with the highest Lewis acidity(4728.3 μmol g^(-1)) can achieve 100% conversion of HMF to 97.6% yield of DMF, with a turnover frequency of up to 46.5 h^(-1). The characterization results demonstrate that the rich Lewis acid sites yielded by the synergistic effect between Ni species and TMC are beneficial for the C=O hydrogenation and C–O cleavage, thereby accelerating the process of hydrodeoxygenation(HDO). Besides, a kinetic model for the HDO of HMF to DMF process has been established based on the experimental results, which elucidated a significant correlation between the measured and the predicted data(R~2> 0.97). Corresponding to the adsorption configuration of Ni/WC and substrate determined by in-situ FTIR characterization, this study provides a novel insight into the selective conversion of HMF process for functional biofuel and bio-chemicals.
基金supported by the National Nature Science Foundation of China (32222058, 32001274)the Youth Talent Support Program for Science & Technology Innovation of National Forestry and Grassland (2019132603) for financial support。
文摘Converting carbohydrates into 5-hydroxymethylfurfural(5-HMF) is an attractive and promising route for value-added utilization of agricultural and forestry biomass resource. As an important platform compound, 5-HMF possesses high active furan structure with hydroxymethyl and aldehyde group for production of various bio-chemicals and materials, meanwhile, which suffer from low stability and poor yield during the industrial biorefinery process. Hence, selective production of 5-HMF with high-yield and low-cost has attracted extensive attention from scientific and industrial researchers. This review sorted and described the latest advanced research on solvent and catalyst system, as well as energy field effect for production of 5-HMF with different feedstock in detail, emphatically discussing the solvent effect and its synergistic effect with other aspects. Besides, the future prospects and challenges for production of 5-HMF from carbohydrates were also presented, which provide a profound insight into industrial 5-HMF process with economic and environmental feature.
基金Project supported by the National Key Research and Development Program of China(Grant Nos.2021YFA1400203 and 2018YFA0305900)the National Natural Science Foundation of China(Grant Nos.52090024,11874175,12074139,12074138,11874176,and 12034009)+1 种基金the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB33000000)Program for JLU Science and Technology Innovative Research Team(JLUSTIRT)。
文摘Flourishing rare earth superhydrides are a class of recently discovered materials that exhibit near-room-temperature superconductivity at high pressures,ushering in a new era of superconductivity research at high pressures.Yttrium superhydrides drew the most attention among these superhydrides due to their abundance of stoichiometries and excellent superconductivities.Here,we carried out a comprehensive study of yttrium superhydrides in a wide pressure range of 140 GPa-300 GPa.We successfully synthesized a series of superhydrides with the compositions of YH_(4),YH_(6),YH_(7),and YH_(9),and reported superconducting transition temperatures of 82 K at 167 GPa,218 K at 165 GPa,29 K at 162 GPa,and230 K at 300 GPa,respectively,as evidenced by sharp drops in resistance.The structure and superconductivity of YH_(4) were taken as a representative example and were also examined using x-ray diffraction measurements and the superconductivity suppression under external magnetic fields,respectively.Clathrate YH_(10),a candidate for room-temperature superconductor,was not synthesized within the study pressure and temperature ranges of up to 300 GPa and 2000 K.The current study established a detailed foundation for future research into room-temperature superconductors in polynary yttrium-based superhydrides.
