In this study,TiO_(2) nanosheets(NSs)grown in situ on extremely conductive Ti_(3)C_(2)T_(x) MXene to form TiO_(2)/Ti_(3)C_(2)T_(x) MXene composites with abundant active sites are proposed to effectively achieve elec‐...In this study,TiO_(2) nanosheets(NSs)grown in situ on extremely conductive Ti_(3)C_(2)T_(x) MXene to form TiO_(2)/Ti_(3)C_(2)T_(x) MXene composites with abundant active sites are proposed to effectively achieve elec‐trocatalytic NH_(3) synthesis.Electron transfer can be promoted by Ti_(3)C_(2)T_(x) MXene with high conduc‐tivity.Meanwhile,the TiO_(2) NSs in‐situ formation can not only avoid Ti_(3)C_(2)T_(x) MXene microstacking but also enhance the surface specific area of Ti_(3)C_(2)T_(x) MXene.The TiO_(2)/Ti_(3)C_(2)T_(x) MXene catalyst reach‐es a high Faradaic efϐiciency(FE)of 44.68%at−0.75 V vs.RHE and a large NH3 yield of 44.17µg h^(-1) mg^(-1)cat.at−0.95 V,with strong electrochemical durability.15N isotopic labeling experiments imply that the N in the produced NH3 originated from the N2 of the electrolyte.DFT calculations were conducted to determine the possible NRR reaction pathways for TiO_(2)/Ti_(3)C_(2)T_(x) MXene composites.MXene catalysts combined with other materials have been rationally designed for efficient ammonia production under ambient conditions。展开更多
Two compounds C_8H_(18)N_2Br_3Mn_(0.5)(1) and C_(12)H_(26)N_2Cl_4Mn(2) based on triethylenediamine derivatives were synthesized by solution method and were characterized by elemental analysis, infrared spectroscopy, s...Two compounds C_8H_(18)N_2Br_3Mn_(0.5)(1) and C_(12)H_(26)N_2Cl_4Mn(2) based on triethylenediamine derivatives were synthesized by solution method and were characterized by elemental analysis, infrared spectroscopy, single-crystal X-ray structure analysis, fluorescence test, circular dichroism(CD) analysis and dielectric measurement, respectively. According to single-crystal X-ray determination, compound 1 crystallizes in the cubic system, space group Pa3 with a = b = c = 13.7246(5) ?, Z = 24, V = 2585.2(3) ?~3; and compound 2 crystallizes in the orthorhombic system, space group P212121 with a = 7.9716(13), b = 15.309(3), c = 15.804(3) ?, Z = 4 and V = 1928.7(6) ?3. Fluorescent analysis of compound 1 showed an intense emission band at 670 nm when the exciting radiation was set at 378 nm and fluorescent analysis of compound 2 showed an intense emission band at 515 nm when the exciting radiation was set at 363 nm. Dielectric constants of compounds 1 and 2 were measured at different frequencies with temperature variation.展开更多
文摘In this study,TiO_(2) nanosheets(NSs)grown in situ on extremely conductive Ti_(3)C_(2)T_(x) MXene to form TiO_(2)/Ti_(3)C_(2)T_(x) MXene composites with abundant active sites are proposed to effectively achieve elec‐trocatalytic NH_(3) synthesis.Electron transfer can be promoted by Ti_(3)C_(2)T_(x) MXene with high conduc‐tivity.Meanwhile,the TiO_(2) NSs in‐situ formation can not only avoid Ti_(3)C_(2)T_(x) MXene microstacking but also enhance the surface specific area of Ti_(3)C_(2)T_(x) MXene.The TiO_(2)/Ti_(3)C_(2)T_(x) MXene catalyst reach‐es a high Faradaic efϐiciency(FE)of 44.68%at−0.75 V vs.RHE and a large NH3 yield of 44.17µg h^(-1) mg^(-1)cat.at−0.95 V,with strong electrochemical durability.15N isotopic labeling experiments imply that the N in the produced NH3 originated from the N2 of the electrolyte.DFT calculations were conducted to determine the possible NRR reaction pathways for TiO_(2)/Ti_(3)C_(2)T_(x) MXene composites.MXene catalysts combined with other materials have been rationally designed for efficient ammonia production under ambient conditions。
基金financially supported by the National Natural Science Foundation of China(21671084)Six Talent Peaks Project in Jiangsu Province(2014-XCL-008)the Qing Lan Project of Jiangsu Province and the Foundation of Jiangsu Educational Committee(16KJB430011)
文摘Two compounds C_8H_(18)N_2Br_3Mn_(0.5)(1) and C_(12)H_(26)N_2Cl_4Mn(2) based on triethylenediamine derivatives were synthesized by solution method and were characterized by elemental analysis, infrared spectroscopy, single-crystal X-ray structure analysis, fluorescence test, circular dichroism(CD) analysis and dielectric measurement, respectively. According to single-crystal X-ray determination, compound 1 crystallizes in the cubic system, space group Pa3 with a = b = c = 13.7246(5) ?, Z = 24, V = 2585.2(3) ?~3; and compound 2 crystallizes in the orthorhombic system, space group P212121 with a = 7.9716(13), b = 15.309(3), c = 15.804(3) ?, Z = 4 and V = 1928.7(6) ?3. Fluorescent analysis of compound 1 showed an intense emission band at 670 nm when the exciting radiation was set at 378 nm and fluorescent analysis of compound 2 showed an intense emission band at 515 nm when the exciting radiation was set at 363 nm. Dielectric constants of compounds 1 and 2 were measured at different frequencies with temperature variation.