FTO(Fischer-Tropsch to olefins)作为合成气制备低碳烯烃(C_(2)^(=)~C_(4)^(=))的代替路径在工业上具有重要意义。CoMnNa作为FTO反应催化剂而备受关注,但由于反应过程中CO_(2)C活性相的形成,导致CO_(2)选择性较高。引入AlO(OH)载体,制...FTO(Fischer-Tropsch to olefins)作为合成气制备低碳烯烃(C_(2)^(=)~C_(4)^(=))的代替路径在工业上具有重要意义。CoMnNa作为FTO反应催化剂而备受关注,但由于反应过程中CO_(2)C活性相的形成,导致CO_(2)选择性较高。引入AlO(OH)载体,制备了Co_(1)Mn_(1)Na/AlO(OH)催化剂,通过XRD、STEM、EDX-mapping、N_(2)吸附-脱附等温线、孔径分布曲线对催化剂进行了表征,通过H_(2)-TPR对催化剂的还原性进行了分析,并对催化剂的FTO反应性能进行了评价。结果表明,利用载体与CoMn的相互作用,降低了CoMn氧化物的还原性,有效抑制了CoMn中Co的析出及CO_(2)C的形成,减少了CoMn体系中Co和CO_(2)C活性相;在低碳烯烃选择性高达32.4%的情况下,成功将CO_(2)选择性降至10%以下。展开更多
Urea and oxalic acid are critical component in various chemical manufacturing industries.However,achieving simultaneous generation of urea and oxalic acid in a continuous-flow electrolyzer is a challenge.Herein,we rep...Urea and oxalic acid are critical component in various chemical manufacturing industries.However,achieving simultaneous generation of urea and oxalic acid in a continuous-flow electrolyzer is a challenge.Herein,we report a continuous-flow electrolyzer equipped with 9-square centime-ter-effective area gas diffusion electrodes(GDE)which can simultaneously catalyze the glycerol oxidation reaction in the anode region and the reduction reaction of CO_(2) and nitrate in the cathode region,producing oxalic acid and urea at both the anode and cathode,respectively.The current density at low cell voltage(0.9 V)remained above 18.7 mA cm^(-2) for 10 consecutive electrolysis cycles(120 h in total),and the Faraday efficiency of oxalic acid(67.1%) and urea(70.9%)did not decay.Experimental and theoretical studies show that in terms of the formation of C-N bond at the cathode,Pd-sites can provide protons for the hydrogenation process of CO_(2) and NO_(3)^(-),Cu-sites can promote the generation of *COOH and Bi-sites can stabilize *COOH.In addition,in terms of glycerol oxidation,the introduction of Cu and Bi into Pd metallene promotes the oxidation of hydroxyl groups and the cleavage of C-C bond in glycerol molecules,respectively.展开更多
文摘FTO(Fischer-Tropsch to olefins)作为合成气制备低碳烯烃(C_(2)^(=)~C_(4)^(=))的代替路径在工业上具有重要意义。CoMnNa作为FTO反应催化剂而备受关注,但由于反应过程中CO_(2)C活性相的形成,导致CO_(2)选择性较高。引入AlO(OH)载体,制备了Co_(1)Mn_(1)Na/AlO(OH)催化剂,通过XRD、STEM、EDX-mapping、N_(2)吸附-脱附等温线、孔径分布曲线对催化剂进行了表征,通过H_(2)-TPR对催化剂的还原性进行了分析,并对催化剂的FTO反应性能进行了评价。结果表明,利用载体与CoMn的相互作用,降低了CoMn氧化物的还原性,有效抑制了CoMn中Co的析出及CO_(2)C的形成,减少了CoMn体系中Co和CO_(2)C活性相;在低碳烯烃选择性高达32.4%的情况下,成功将CO_(2)选择性降至10%以下。
文摘Urea and oxalic acid are critical component in various chemical manufacturing industries.However,achieving simultaneous generation of urea and oxalic acid in a continuous-flow electrolyzer is a challenge.Herein,we report a continuous-flow electrolyzer equipped with 9-square centime-ter-effective area gas diffusion electrodes(GDE)which can simultaneously catalyze the glycerol oxidation reaction in the anode region and the reduction reaction of CO_(2) and nitrate in the cathode region,producing oxalic acid and urea at both the anode and cathode,respectively.The current density at low cell voltage(0.9 V)remained above 18.7 mA cm^(-2) for 10 consecutive electrolysis cycles(120 h in total),and the Faraday efficiency of oxalic acid(67.1%) and urea(70.9%)did not decay.Experimental and theoretical studies show that in terms of the formation of C-N bond at the cathode,Pd-sites can provide protons for the hydrogenation process of CO_(2) and NO_(3)^(-),Cu-sites can promote the generation of *COOH and Bi-sites can stabilize *COOH.In addition,in terms of glycerol oxidation,the introduction of Cu and Bi into Pd metallene promotes the oxidation of hydroxyl groups and the cleavage of C-C bond in glycerol molecules,respectively.
基金supported by the National Key Research and Development Program of China(2020YFB0606404)National Natural Science Foundation of China(21991092,22272195,U2003123,U1910203).
