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 effect of CaF2-doped ZrO2 catalyst for the synthesis of dimethyl carbonate （DMC） was studied by X-ray diffraction （XRD）, CO2-temperature programmed desorption （TPD）, Raman spectra, and X-ray photoelectron sp...The effect of CaF2-doped ZrO2 catalyst for the synthesis of dimethyl carbonate （DMC） was studied by X-ray diffraction （XRD）, CO2-temperature programmed desorption （TPD）, Raman spectra, and X-ray photoelectron spectroscopy （XPS）. Catalytic performance was evaluated in the bath and distillation reactors. Results showed that the CaF2/ZrO2 catalysts had activity and stability for DMC synthesis.展开更多
Copper （Cu）-doped ZrO2 （CZO） films with different Cu content （0 at.%- 8.07 at.%） are successfully deposited on Si （100） substrates by direct current （DC） and radio frequency （RF） magnetron co-sputtering. T...Copper （Cu）-doped ZrO2 （CZO） films with different Cu content （0 at.%- 8.07 at.%） are successfully deposited on Si （100） substrates by direct current （DC） and radio frequency （RF） magnetron co-sputtering. The influences of Cu content on structural, morphological, optical and electrical properties of CZO films are discussed in detail. The CZO films exhibit ZrO2 monocline （1^-11） preferred orientation, which indicates that Cu atoms are doped in ZrO2 host lattice. The crystallite size estimated form x-ray diffraction （XRD） increases by Cu doping, which accords with the result observed from the scanning electron microscope （SEM）. The electrical resistivity decreases from 2.63 Ω·cm to 1.48 Ω·cm with Cu doping content increasing, which indicates that the conductivity of CZO film is improved. However, the visible light transmittances decrease slightly by Cu doping and the optical band gap values decrease from 4.64 eV to 4.48 eV for CZO fihns.展开更多
A S 2O 2- 8/ZrO 2 Al 2O 3 type solid superacid catalyst was prepared from ZrOCl 2·8H 2O, AlCl 3· 6H 2O and (NH 4) 2S 2O 8 by coprecipitation, maceration and calcination processes. Their crystal structures an...A S 2O 2- 8/ZrO 2 Al 2O 3 type solid superacid catalyst was prepared from ZrOCl 2·8H 2O, AlCl 3· 6H 2O and (NH 4) 2S 2O 8 by coprecipitation, maceration and calcination processes. Their crystal structures and acidities were determined by XRD and Hammett method, respectively. The activity of the catalyst was studied as function of Al 2O 3 content, calcination temperature and time in the esterification of acetic acid with butanol, and a conversion of 96 5% was obtained. The catalyst gave also higher yields in syntheses of ketals and acetals: cyclohexanone ethylene ketal(86 2%), acetophenone ethylene ketal(78 5%), acetylacetic ester ketal(88 5%), benzaldehyde glycol acetal(76 3%). The chemical structures of the products were confirmed by IR spectra.展开更多
以纳米ZrO 、微米Al O 为原料,采用无压烧结方式制备了ZTA 复相陶瓷。结果表明:nano-ZrO 的 2 2 3 2加入有利于制备细晶ZTA 复相陶瓷。此外,nano-ZrO 的加入对 Al O 陶瓷的显微结构也产生影响,ZrO ...以纳米ZrO 、微米Al O 为原料,采用无压烧结方式制备了ZTA 复相陶瓷。结果表明:nano-ZrO 的 2 2 3 2加入有利于制备细晶ZTA 复相陶瓷。此外,nano-ZrO 的加入对 Al O 陶瓷的显微结构也产生影响,ZrO 颗粒以 2 2 3 2“晶内型”和晶界型两种形式存在。合理的配方组成及制备工艺有利于 Z r O 以四方亚稳相存在。Z r O 含量为 2 23 0 w t % 时,其四方相含量可达 6 9 %,有利于应力诱导相变增韧,该 Z T A 复相陶瓷的抗弯强度、断裂韧性分别达到 604MPa、6.87MPa·m1/2。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Project supported by the National Natural Science Foundation of China(Grant No.10271074)
文摘The effect of CaF2-doped ZrO2 catalyst for the synthesis of dimethyl carbonate （DMC） was studied by X-ray diffraction （XRD）, CO2-temperature programmed desorption （TPD）, Raman spectra, and X-ray photoelectron spectroscopy （XPS）. Catalytic performance was evaluated in the bath and distillation reactors. Results showed that the CaF2/ZrO2 catalysts had activity and stability for DMC synthesis.
基金supported by the National Natural Science Foundation of China(Grant Nos.51272224 and 11164031)
文摘Copper （Cu）-doped ZrO2 （CZO） films with different Cu content （0 at.%- 8.07 at.%） are successfully deposited on Si （100） substrates by direct current （DC） and radio frequency （RF） magnetron co-sputtering. The influences of Cu content on structural, morphological, optical and electrical properties of CZO films are discussed in detail. The CZO films exhibit ZrO2 monocline （1^-11） preferred orientation, which indicates that Cu atoms are doped in ZrO2 host lattice. The crystallite size estimated form x-ray diffraction （XRD） increases by Cu doping, which accords with the result observed from the scanning electron microscope （SEM）. The electrical resistivity decreases from 2.63 Ω·cm to 1.48 Ω·cm with Cu doping content increasing, which indicates that the conductivity of CZO film is improved. However, the visible light transmittances decrease slightly by Cu doping and the optical band gap values decrease from 4.64 eV to 4.48 eV for CZO fihns.
文摘A S 2O 2- 8/ZrO 2 Al 2O 3 type solid superacid catalyst was prepared from ZrOCl 2·8H 2O, AlCl 3· 6H 2O and (NH 4) 2S 2O 8 by coprecipitation, maceration and calcination processes. Their crystal structures and acidities were determined by XRD and Hammett method, respectively. The activity of the catalyst was studied as function of Al 2O 3 content, calcination temperature and time in the esterification of acetic acid with butanol, and a conversion of 96 5% was obtained. The catalyst gave also higher yields in syntheses of ketals and acetals: cyclohexanone ethylene ketal(86 2%), acetophenone ethylene ketal(78 5%), acetylacetic ester ketal(88 5%), benzaldehyde glycol acetal(76 3%). The chemical structures of the products were confirmed by IR spectra.
文摘以纳米ZrO 、微米Al O 为原料,采用无压烧结方式制备了ZTA 复相陶瓷。结果表明:nano-ZrO 的 2 2 3 2加入有利于制备细晶ZTA 复相陶瓷。此外,nano-ZrO 的加入对 Al O 陶瓷的显微结构也产生影响,ZrO 颗粒以 2 2 3 2“晶内型”和晶界型两种形式存在。合理的配方组成及制备工艺有利于 Z r O 以四方亚稳相存在。Z r O 含量为 2 23 0 w t % 时,其四方相含量可达 6 9 %,有利于应力诱导相变增韧,该 Z T A 复相陶瓷的抗弯强度、断裂韧性分别达到 604MPa、6.87MPa·m1/2。
