The oxygen reduction reaction （ORR） is traditionally performed using noble‐metals catalysts, e.g. Pt. However, these metal‐based catalysts have the drawbacks of high costs, low selectivity, poor stabili‐ties, and...The oxygen reduction reaction （ORR） is traditionally performed using noble‐metals catalysts, e.g. Pt. However, these metal‐based catalysts have the drawbacks of high costs, low selectivity, poor stabili‐ties, and detrimental environmental effects. Here, we describe metal‐free nitrogen‐doped carbon nanoblocks （NCNBs） with high nitrogen contents （4.11%）, which have good electrocatalytic proper‐ties for ORRs. This material was fabricated using a scalable, one‐step process involving the pyrolysis of tris（hydroxymethyl）aminomethane （Tris） at 800℃. Rotating ring disk electrode measurements show that the NCNBs give a high electrocatalytic performance and have good stability in ORRs. The onset potential of the catalyst for the ORR is-0.05 V （vs Ag/AgCl）, the ORR reduction peak potential is-0.20 V （vs Ag/AgCl）, and the electron transfer number is 3.4. The NCNBs showed pronounced electrocatalytic activity, improved long‐term stability, and better tolerance of the methanol crosso‐ver effect compared with a commercial 20 wt%Pt/C catalyst. The composition and structure of, and nitrogen species in, the NCNBs were investigated using Fourier‐transform infrared spectroscopy, scanning electron microscopy, X‐ray photoelectron spectroscopy, and X‐ray diffraction. The pyroly‐sis of Tris at high temperature increases the number of active nitrogen sites, especially pyridinic nitrogen, which creates a net positive charge on adjacent carbon atoms, and the high positive charge promotes oxygen adsorption and reduction. The results show that NCNBs prepared by pyrolysis of Tris as nitrogen and carbon sources are a promising ORR catalyst for fuel cells.展开更多
Three polymeric adsorbents with hydrogen bonding acceptors, methylamine, N-methyl-acetamide and aminotri(hydroxymethyl)methane modified resins are synthesized from chloromethylated X-5 resin. Adsorption isotherms of p...Three polymeric adsorbents with hydrogen bonding acceptors, methylamine, N-methyl-acetamide and aminotri(hydroxymethyl)methane modified resins are synthesized from chloromethylated X-5 resin. Adsorption isotherms of phenol and theophylline onto the three modified resins and the original X-5 resin from aqueous solution are measured. The results show that adsorption of compounds with hydrogen bonding donor onto methylamine and N-methylacetamide modified resins is enhanced as compared with that onto X-5 resin, and adsorption mechanism between the adsorbents and the adsorbates is mainly based on hydrogen bonding and hydrophobic interaction. While adsorption of compounds with hydrogen bonding donor onto aminotri(hydroxymethyl)methane modified resin is lowered as compared with that onto X-5 resin, and adsorption mechanism between the adsorbent and the adsorbates is mainly based on hydrophobic interaction.展开更多
A novel mixed-valent heterometallic pentanuclear CoⅢ3 CoⅡ Dy Ⅲ cluster has been rationally assembled taking advantage of a bifunctional ligand with o-vanillin and tripodal tris(hydroxymethyl)aminomethane units. Thi...A novel mixed-valent heterometallic pentanuclear CoⅢ3 CoⅡ Dy Ⅲ cluster has been rationally assembled taking advantage of a bifunctional ligand with o-vanillin and tripodal tris(hydroxymethyl)aminomethane units. This unique heterometallic cluster represents a rare example of T-shaped molecules exhibiting slow magnetic relaxation.展开更多
基金supported by the National Natural Science Foundation of China (21375088,21575090)Scientific Research Project of Beijing Educational Committee (KM201410028006)+1 种基金Scientific Research Base Development Program of the Beijing Municipal Commission of EducationYouth Talent Project of the Beijing Municipal Commission of Education (CIT & TCD201504072)~~
文摘The oxygen reduction reaction （ORR） is traditionally performed using noble‐metals catalysts, e.g. Pt. However, these metal‐based catalysts have the drawbacks of high costs, low selectivity, poor stabili‐ties, and detrimental environmental effects. Here, we describe metal‐free nitrogen‐doped carbon nanoblocks （NCNBs） with high nitrogen contents （4.11%）, which have good electrocatalytic proper‐ties for ORRs. This material was fabricated using a scalable, one‐step process involving the pyrolysis of tris（hydroxymethyl）aminomethane （Tris） at 800℃. Rotating ring disk electrode measurements show that the NCNBs give a high electrocatalytic performance and have good stability in ORRs. The onset potential of the catalyst for the ORR is-0.05 V （vs Ag/AgCl）, the ORR reduction peak potential is-0.20 V （vs Ag/AgCl）, and the electron transfer number is 3.4. The NCNBs showed pronounced electrocatalytic activity, improved long‐term stability, and better tolerance of the methanol crosso‐ver effect compared with a commercial 20 wt%Pt/C catalyst. The composition and structure of, and nitrogen species in, the NCNBs were investigated using Fourier‐transform infrared spectroscopy, scanning electron microscopy, X‐ray photoelectron spectroscopy, and X‐ray diffraction. The pyroly‐sis of Tris at high temperature increases the number of active nitrogen sites, especially pyridinic nitrogen, which creates a net positive charge on adjacent carbon atoms, and the high positive charge promotes oxygen adsorption and reduction. The results show that NCNBs prepared by pyrolysis of Tris as nitrogen and carbon sources are a promising ORR catalyst for fuel cells.
基金The National Natural Science Foundation of China (No.: 29974015 and 20174017)
文摘Three polymeric adsorbents with hydrogen bonding acceptors, methylamine, N-methyl-acetamide and aminotri(hydroxymethyl)methane modified resins are synthesized from chloromethylated X-5 resin. Adsorption isotherms of phenol and theophylline onto the three modified resins and the original X-5 resin from aqueous solution are measured. The results show that adsorption of compounds with hydrogen bonding donor onto methylamine and N-methylacetamide modified resins is enhanced as compared with that onto X-5 resin, and adsorption mechanism between the adsorbents and the adsorbates is mainly based on hydrogen bonding and hydrophobic interaction. While adsorption of compounds with hydrogen bonding donor onto aminotri(hydroxymethyl)methane modified resin is lowered as compared with that onto X-5 resin, and adsorption mechanism between the adsorbent and the adsorbates is mainly based on hydrophobic interaction.
基金supported by the National Natural Science Foundation of China (91022009, 20921002)
文摘A novel mixed-valent heterometallic pentanuclear CoⅢ3 CoⅡ Dy Ⅲ cluster has been rationally assembled taking advantage of a bifunctional ligand with o-vanillin and tripodal tris(hydroxymethyl)aminomethane units. This unique heterometallic cluster represents a rare example of T-shaped molecules exhibiting slow magnetic relaxation.
