The development of an efficient artificial H_(2)O_(2) photosynthesis system is a challenging work using H_(2)O and O_(2) as starting materials.Herein,3D In_(2.77)S_(4) nanoflower precursor was in-situ deposited on K^(...The development of an efficient artificial H_(2)O_(2) photosynthesis system is a challenging work using H_(2)O and O_(2) as starting materials.Herein,3D In_(2.77)S_(4) nanoflower precursor was in-situ deposited on K^(+)-doped g-C_(3)N_(4)(KCN)nanosheets using a solvothermal method,then In_(2.77)S_(4)/KCN(IS/KCN)het-erojunction with an intimate interface was obtained after a calcination process.The investigation shows that the photocatalytic H_(2)O_(2) production rate of 50IS/KCN can reach up to 1.36 mmol g^(-1)h^(-1)without any sacrificial reagents under visible light irradiation,which is 9.2 times and 4.1 times higher than that of KCN and In_(2.77)S_(4)/respectively.The enhanced activity of the above composite can be mainly attributed to the S-scheme charge transfer route between KCN and In_(2.77)S_(4) according to density functional theory calculations,electron paramagnetic resonance and free radical capture tests,leading to an expanded light response range and rapid charge separation at their interface,as well as preserving the active electrons and holes for H_(2)O_(2) production.Besides,the unique 3D nanostructure and surface hydrophobicity of IS/KCN facilitate the diffusion and transportation of O_(2) around the active centers,the energy barriers of O_(2) protonation and H_(2)O_(2) desorption steps are ef-fectively reduced over the composite.In addition,this system also exhibits excellent light harvesting ability and stability.This work provides a potential strategy to explore a sustainable H_(2)O_(2) photo-synthesis pathway through the design of heterojunctions with intimate interfaces and desired reac-tion thermodynamics and kinetics.展开更多
The synthesis of atomic-scale metal catalysts is a promising but very challenging project. In this work, we successfully fabricated a hybrid catalyst of PL/Ni（OH）2 with atomic-scale Pt clusters uniformly decorated o...The synthesis of atomic-scale metal catalysts is a promising but very challenging project. In this work, we successfully fabricated a hybrid catalyst of PL/Ni（OH）2 with atomic-scale Pt clusters uniformly decorated on porous Ni（OH）2 nanowires （NWs） via a facile room-temperature synthesis strategy. The as-obtained Ptc/Ni（OH）2 catalyst exhibits highly efficient hydrogen evolution reaction （HER） performance under basic conditions. In 0.1moll-1 KOH, the Ptc/Ni（OH）2 has an onset overpotential of -0 mV vs. RHE, and a significantly low overpotential of 32 mV at a current density of 10mAcm-2, lower than that of the com- mercial 20% Pt/C （58 mV）. The mass current density data illustrated that the PL/Ni（OH）2 reached a high current den- sity of 6.34Amg^-1i at an overpotential of 50 mV, which was approximately 28 times higher than that of the commercial Pt/C （0.223Amg^-1i） at the same overpotential, proving the high-efficiency electrocatalytic activity of the as-obtained Ptc/Ni（OH）2 for HER under alkaline conditions.展开更多
文摘The development of an efficient artificial H_(2)O_(2) photosynthesis system is a challenging work using H_(2)O and O_(2) as starting materials.Herein,3D In_(2.77)S_(4) nanoflower precursor was in-situ deposited on K^(+)-doped g-C_(3)N_(4)(KCN)nanosheets using a solvothermal method,then In_(2.77)S_(4)/KCN(IS/KCN)het-erojunction with an intimate interface was obtained after a calcination process.The investigation shows that the photocatalytic H_(2)O_(2) production rate of 50IS/KCN can reach up to 1.36 mmol g^(-1)h^(-1)without any sacrificial reagents under visible light irradiation,which is 9.2 times and 4.1 times higher than that of KCN and In_(2.77)S_(4)/respectively.The enhanced activity of the above composite can be mainly attributed to the S-scheme charge transfer route between KCN and In_(2.77)S_(4) according to density functional theory calculations,electron paramagnetic resonance and free radical capture tests,leading to an expanded light response range and rapid charge separation at their interface,as well as preserving the active electrons and holes for H_(2)O_(2) production.Besides,the unique 3D nanostructure and surface hydrophobicity of IS/KCN facilitate the diffusion and transportation of O_(2) around the active centers,the energy barriers of O_(2) protonation and H_(2)O_(2) desorption steps are ef-fectively reduced over the composite.In addition,this system also exhibits excellent light harvesting ability and stability.This work provides a potential strategy to explore a sustainable H_(2)O_(2) photo-synthesis pathway through the design of heterojunctions with intimate interfaces and desired reac-tion thermodynamics and kinetics.
基金financial support from the National Natural Science Foundation of China(21425103,21673280 and 11374039)
文摘The synthesis of atomic-scale metal catalysts is a promising but very challenging project. In this work, we successfully fabricated a hybrid catalyst of PL/Ni（OH）2 with atomic-scale Pt clusters uniformly decorated on porous Ni（OH）2 nanowires （NWs） via a facile room-temperature synthesis strategy. The as-obtained Ptc/Ni（OH）2 catalyst exhibits highly efficient hydrogen evolution reaction （HER） performance under basic conditions. In 0.1moll-1 KOH, the Ptc/Ni（OH）2 has an onset overpotential of -0 mV vs. RHE, and a significantly low overpotential of 32 mV at a current density of 10mAcm-2, lower than that of the com- mercial 20% Pt/C （58 mV）. The mass current density data illustrated that the PL/Ni（OH）2 reached a high current den- sity of 6.34Amg^-1i at an overpotential of 50 mV, which was approximately 28 times higher than that of the commercial Pt/C （0.223Amg^-1i） at the same overpotential, proving the high-efficiency electrocatalytic activity of the as-obtained Ptc/Ni（OH）2 for HER under alkaline conditions.
