Enhancing the separation efficiency of photogenerated carriers is propitious for the promotion of photocatalytic hydrogen production from formic acid decomposition.Herein,MoS2/Zn3In2S6(MoS2/ZIS6)composite photocatalys...Enhancing the separation efficiency of photogenerated carriers is propitious for the promotion of photocatalytic hydrogen production from formic acid decomposition.Herein,MoS2/Zn3In2S6(MoS2/ZIS6)composite photocatalysts containing varying mass percentages of MoS2 were obtained by a straightforward synthetic method.The results confirmed that MoS2,as a cocatalyst,markedly promoted the photogenerated charge separation efficiency and visible light-driven hydrogen production activity of ZIS6(λ>400 nm).Specifically,the as-prepared 0.5%MoS2/ZIS6 photocatalyst exhibited the highest photocatalytic hydrogen production rate(74.25μmol·h^-1),which was approximately 4.3 times higher than that of ZIS6(17.47μmol·h^-1).The excellent performance of the 0.5%MoS2/ZIS6 photocatalyst may be due to the fact that MoS2 has a low Fermi energy level and can thus enrich photogenerated electrons from ZIS6,and furthermore reduce H+derived from formic acid,to form hydrogen.The structure and morphology of the MoS2/ZIS6 photocatalysts and the reactive species were determined by X-ray diffraction,transmission electron microscopy,and field emission scanning electron microscopy,among others;a plausible mechanistic rationale is discussed based on the results.展开更多
The Bunsen reaction is the center reaction for both the sulfur–iodine water splitting cycle for hydrogen production and the novel hydrogen sulfide splitting cycle for hydrogen and sulfuric acid production from the su...The Bunsen reaction is the center reaction for both the sulfur–iodine water splitting cycle for hydrogen production and the novel hydrogen sulfide splitting cycle for hydrogen and sulfuric acid production from the sulfur-containing gases.This paper reviews the research progress of the Bunsen reaction in recent 10–15 years.Researches were initially focused on the optimization of the operating conditions of the conventional Bunsen reaction requiring excessive water and iodine to improve the products separation efficiency and to avoid the side reactions and iodine vapor deposition.Alternative methods including electrochemical methods,precipitation methods,and non-aqueous solvent methods had their respective advantages,but still faced challenges.In development of the technology of H2S splitting cycle,dissolving iodine in toluene solvent could render the Bunsen reaction to occur with the flowable I2 stream at ambient temperature such that the side reactions and iodine vaporization can be avoided and the corrosion hazard lessened.It also prevented the Bunsen reaction from using excessive iodine and water.The products from the Bunsen reaction including HI,H2SO4,H2O,and toluene could be directly electrolyzed.展开更多
A novel Sr2CulnO3S oxysulfide p-type semiconductor photocatalyst has been prepared by solid state reaction method and it exhibits intriguing visible light absorption properties with a bandgap of 2.3 eV. The p-type sem...A novel Sr2CulnO3S oxysulfide p-type semiconductor photocatalyst has been prepared by solid state reaction method and it exhibits intriguing visible light absorption properties with a bandgap of 2.3 eV. The p-type semiconductor character of the synthesized Sr2CuInO3 S was confirmed by Hall efficient measurement and Mott-Schottky plot analysis. First-principles density functional theory calculations （DFT） and electrochem ical measurements were performed to elucidate the electronic structure and the energy band locations. It was found that the as-synthesized Sr2CuInO3S photocatalyst has appreciate conduction and valence band positions for hydrogen and oxygen evolution, respectively. Photocat alytic hydrogen production experiments under a visible light irradiation （A〉420 nm） were carried out by loading different metal and metal-like cocatalysts on Sr2CuInO3S and Rh was found to be the best one among the tested ones.展开更多
Ultrathin small MoS2nanosheets exhibit a higher electrocatalytic activity for the hydrogen evolution reaction.However,strong interactions between MoS2layers may result in aggregation;together with the low conductivity...Ultrathin small MoS2nanosheets exhibit a higher electrocatalytic activity for the hydrogen evolution reaction.However,strong interactions between MoS2layers may result in aggregation;together with the low conductivity of MoS2,this may lower its electrocatalytic activity.In this paper we present a method that we developed to directly produce solid S,N co‐doped carbon(SNC)with a graphite structure and multiple surface groups through a hydrothermal route.When Na2MoO4was added to the reaction,polymolybdate could be anchored into the carbon materials via a chemical interaction that helps polymolybdate disperse uniformly into the SNC.After a high temperature treatment,polymolybdate transformed into MoS2at800°C for6h in a N2atmosphere at a heating rate of5°C/min,owing to S2?being released from the SNC during the treatment(denoted as MoS2/SNC‐800‐6h).The SNC effectively prevents MoS2from aggregating into large particles,and we successfully prepared highly dispersed MoS2in the SNC matrix.Electrochemical characterizations indicate that MoS2/SNC‐900‐12h exhibits a low onset potential of115mV and a low overpotential of237mV at a current density of10mA/cm2.Furthermore,MoS2/SNC‐900‐12h also had an excellent stability with only^2.6%decay at a current density of10mA/cm2after5000test cycles.展开更多
文摘Enhancing the separation efficiency of photogenerated carriers is propitious for the promotion of photocatalytic hydrogen production from formic acid decomposition.Herein,MoS2/Zn3In2S6(MoS2/ZIS6)composite photocatalysts containing varying mass percentages of MoS2 were obtained by a straightforward synthetic method.The results confirmed that MoS2,as a cocatalyst,markedly promoted the photogenerated charge separation efficiency and visible light-driven hydrogen production activity of ZIS6(λ>400 nm).Specifically,the as-prepared 0.5%MoS2/ZIS6 photocatalyst exhibited the highest photocatalytic hydrogen production rate(74.25μmol·h^-1),which was approximately 4.3 times higher than that of ZIS6(17.47μmol·h^-1).The excellent performance of the 0.5%MoS2/ZIS6 photocatalyst may be due to the fact that MoS2 has a low Fermi energy level and can thus enrich photogenerated electrons from ZIS6,and furthermore reduce H+derived from formic acid,to form hydrogen.The structure and morphology of the MoS2/ZIS6 photocatalysts and the reactive species were determined by X-ray diffraction,transmission electron microscopy,and field emission scanning electron microscopy,among others;a plausible mechanistic rationale is discussed based on the results.
基金financial supports from the National Natural Science Foundation of China(21576183)Natural Science and Technology Research Council of Canada(STPGP-350428-07)
文摘The Bunsen reaction is the center reaction for both the sulfur–iodine water splitting cycle for hydrogen production and the novel hydrogen sulfide splitting cycle for hydrogen and sulfuric acid production from the sulfur-containing gases.This paper reviews the research progress of the Bunsen reaction in recent 10–15 years.Researches were initially focused on the optimization of the operating conditions of the conventional Bunsen reaction requiring excessive water and iodine to improve the products separation efficiency and to avoid the side reactions and iodine vapor deposition.Alternative methods including electrochemical methods,precipitation methods,and non-aqueous solvent methods had their respective advantages,but still faced challenges.In development of the technology of H2S splitting cycle,dissolving iodine in toluene solvent could render the Bunsen reaction to occur with the flowable I2 stream at ambient temperature such that the side reactions and iodine vaporization can be avoided and the corrosion hazard lessened.It also prevented the Bunsen reaction from using excessive iodine and water.The products from the Bunsen reaction including HI,H2SO4,H2O,and toluene could be directly electrolyzed.
基金financially supported by the National Natural Science Foundation of China(Grant No.21090341 and 21361140346)the National Basic Research Program(973 Program)of the Ministry of Science and Technology of China(Grant No.2014CB239401)
文摘A novel Sr2CulnO3S oxysulfide p-type semiconductor photocatalyst has been prepared by solid state reaction method and it exhibits intriguing visible light absorption properties with a bandgap of 2.3 eV. The p-type semiconductor character of the synthesized Sr2CuInO3 S was confirmed by Hall efficient measurement and Mott-Schottky plot analysis. First-principles density functional theory calculations （DFT） and electrochem ical measurements were performed to elucidate the electronic structure and the energy band locations. It was found that the as-synthesized Sr2CuInO3S photocatalyst has appreciate conduction and valence band positions for hydrogen and oxygen evolution, respectively. Photocat alytic hydrogen production experiments under a visible light irradiation （A〉420 nm） were carried out by loading different metal and metal-like cocatalysts on Sr2CuInO3S and Rh was found to be the best one among the tested ones.
基金supported by the National Natural Science Foundation of China(21671011)Beijing High-Level Talent program~~
文摘Ultrathin small MoS2nanosheets exhibit a higher electrocatalytic activity for the hydrogen evolution reaction.However,strong interactions between MoS2layers may result in aggregation;together with the low conductivity of MoS2,this may lower its electrocatalytic activity.In this paper we present a method that we developed to directly produce solid S,N co‐doped carbon(SNC)with a graphite structure and multiple surface groups through a hydrothermal route.When Na2MoO4was added to the reaction,polymolybdate could be anchored into the carbon materials via a chemical interaction that helps polymolybdate disperse uniformly into the SNC.After a high temperature treatment,polymolybdate transformed into MoS2at800°C for6h in a N2atmosphere at a heating rate of5°C/min,owing to S2?being released from the SNC during the treatment(denoted as MoS2/SNC‐800‐6h).The SNC effectively prevents MoS2from aggregating into large particles,and we successfully prepared highly dispersed MoS2in the SNC matrix.Electrochemical characterizations indicate that MoS2/SNC‐900‐12h exhibits a low onset potential of115mV and a low overpotential of237mV at a current density of10mA/cm2.Furthermore,MoS2/SNC‐900‐12h also had an excellent stability with only^2.6%decay at a current density of10mA/cm2after5000test cycles.
