Rational interface engineering is essential for minimizing interfacial nonradiative recombination losses and enhancing device performance.Herein,we report the use of bidentate diphenoxybenzene(DPOB)isomers as surface ...Rational interface engineering is essential for minimizing interfacial nonradiative recombination losses and enhancing device performance.Herein,we report the use of bidentate diphenoxybenzene(DPOB)isomers as surface modifiers for perovskite films.The DPOB molecules,which contain two oxygen(O)atoms,chemically bond with undercoordinated Pb^(2+) on the surface of perovskite films,resulting in compression of the perovskite lattice.This chemical interaction,along with physical regulations,leads to the formation of high-quality perovskite films with compressive strain and fewer defects.This compressive strain-induced band bending promotes hole extraction and transport,while inhibiting charge recombination at the interfaces.Furthermore,the addition of DPOB will reduce the zero-dimensional(OD) Cs_4PbBr_6 phase and produce the two-dimensional(2D) CsPb_(2)Br_5 phase,which is also conducive to the improvement of device performance.Ultimately,the resulting perovskite films,which are strain-released and defect-passivated,exhibit exceptional device efficiency,reaching 10.87% for carbon-based CsPbBr_(3) device,14.86% for carbon-based CsPbI_(2)Br device,22,02% for FA_(0.97)Cs_(0.03)PbI_(3) device,respectively.Moreover,the unencapsulated CsPbBr_(3) PSC exhibits excellent stability under persistent exposure to humidity(80%) and heat(80℃) for over 50 days.展开更多
Metallic lithium anode is widely applied to building highenergy-density batteries such as lithium–sulfur and lithium–oxygen batteries because of its high specific capacity(3860 mAh g?1)and lowest negative potential(...Metallic lithium anode is widely applied to building highenergy-density batteries such as lithium–sulfur and lithium–oxygen batteries because of its high specific capacity(3860 mAh g?1)and lowest negative potential(?3.04 V vs.standard hydrogen electrode(SHE))[1,2].However,the practical applications of Li anode remain challenging[3–6].The large volume change during repeated plating/stripping of Li would cause mechanical and interfacial instability[7,8].The solid electrolyte interphase(SEI)layers on lithium surface with poor elasticity are vulnerable to crack under variable stress/strain,leading to continuous side reactions between exposed fresh Li and electrolyte[9–11].In addition,the uncontrollable nucleation and growth of Li incur the formation of dendrites,which could accelerate detrimental parasitic reactions.Because of the uneven stripping,dendritic Li may deteriorate into electrically disconnected or“dead”Li,resulting in poor Coulombic efficiency,rapid capacity decay,and short circuit risk[12–17].展开更多
The ultrafine particles of a new style Fe-Cu-based catalysts for CO hydrogenation were prepared by impregnating the organic sol of Fe（OH）3 and Cu（OH）2 onto the activated Al2O3, in which the organic sol of Fe（OH）...The ultrafine particles of a new style Fe-Cu-based catalysts for CO hydrogenation were prepared by impregnating the organic sol of Fe（OH）3 and Cu（OH）2 onto the activated Al2O3, in which the organic sol of Fe（OH）3 and Cu（OH）2 were prepared in the microemulsion of dodecylbenzenesulfonic acid sodium（S）/n-butanol（A）/toluene（O）/water with V（A）/V（O） = 0.25 and W（A）/W（S） = 1.50. This catalyst was characterized by particle size analysis, XRD and TG. The results of particle size analysis showed that Fe（OH）3 particles with a mean size of 17.1 nm and Cu（OH）2 particles with an average size of 6.65 um were obtained. TG analysis and XRD patterns suggested that 673 K is the optimal calcination temperature. CO hydrogenation produced C＋OH with a high selectivity above 58 wt% by using the ultrafine particles as catalyst, and the total alcohol yield of 0.250 g·ml^-1 ·h^-1 was obtained when the contents of Al2O3 and K were 88.61 wt% and 1.60 wt%, respectively.展开更多
Herein,the catalysts of ultrathin g-C_(3)N_(4)surface-modified hollow spherical Bi2MoO6(g-C_(3)N_(4)/Bi2MoO6,abbreviated as CN/BMO)were fabricated by the co-solvothermal method.The variable valence Mo^(5+)/Mo^(6+)ioni...Herein,the catalysts of ultrathin g-C_(3)N_(4)surface-modified hollow spherical Bi2MoO6(g-C_(3)N_(4)/Bi2MoO6,abbreviated as CN/BMO)were fabricated by the co-solvothermal method.The variable valence Mo^(5+)/Mo^(6+)ionic bridge in CN/BMO catalysts can boost the rapid transfer of photogenerated electrons from Bi2MoO6to g-C_(3)N_(4).And the synergy effect of g-C_(3)N_(4)and Bi2MoO6components remarkably enhance CO_(2)adsorption capability.CN/BMO-2 catalyst has the best performances for visible light-driven CO_(2)reduction compared with single Bi2MoO6and g-C_(3)N_(4),i.e.,its amount and selectivity of CO product are 139.50μmol g-1and 96.88%for 9 h,respectively.Based on the results of characterizations and density functional theory calculation,the photocatalytic mechanism for CO_(2)reduction is proposed.The high-efficient separation efficiency of photogenerated electron-hole pairs,induced by variable valence Mo^(5+)/Mo^(6+)ionic bridge,can boost the rate-limiting steps(COOH*-to-CO*and CO*desorption)of selective visible light-driven CO_(2)conversion into CO.It inspires the establishment of efficient photocatalysts for CO_(2)conversion.展开更多
Pursuit of energy-harvesting or-storage materials to realize outstanding electricity output from nature has been regarded as a promising strategy to resolve the energy-lack issue in the future. Among them,the solar ce...Pursuit of energy-harvesting or-storage materials to realize outstanding electricity output from nature has been regarded as a promising strategy to resolve the energy-lack issue in the future. Among them,the solar cell as a solar-to-electrical conversion device has been attracted enormous interest to improve the efficiency. However, the ability to generate electricity is highly dependent on the weather conditions,in other words, there is nearly zero power output in dark-light conditions, such as rainy, cloudy, and night, lowering the monolithic power generation capacity. Here, we present a bifunctional polyaniline film via chemical bath deposition, which can harvest energy from the rain, yielding an induced current of 2.57 μA and voltage of 65.5 μV under the stimulus of real raindrop. When incorporating the functional PANi film into the traditional dye sensitized solar cell as a counter electrode, the hybridized photovoltaic can experimentally realize the enhanced output power via harvesting energy from rainy and sunny days. The current work may show a new path for development of advanced solar cells in the future.展开更多
基金National Natural Science Foundation of China (62104136, 22179051, 62204098, 52104258)Project of Shandong Province Higher Educational Young Innovative Team (2022KJ218)+3 种基金China Postdoctoral Science Foundation (2023M732104)Qingdao Postdoctoral Funding Program (QDBSH20220201002)Postdoctoral Innovation Project of Shandong Province (SDCX-ZG-202303032)Shandong Provincial Natural Science Foundation (ZR2021ME016)。
文摘Rational interface engineering is essential for minimizing interfacial nonradiative recombination losses and enhancing device performance.Herein,we report the use of bidentate diphenoxybenzene(DPOB)isomers as surface modifiers for perovskite films.The DPOB molecules,which contain two oxygen(O)atoms,chemically bond with undercoordinated Pb^(2+) on the surface of perovskite films,resulting in compression of the perovskite lattice.This chemical interaction,along with physical regulations,leads to the formation of high-quality perovskite films with compressive strain and fewer defects.This compressive strain-induced band bending promotes hole extraction and transport,while inhibiting charge recombination at the interfaces.Furthermore,the addition of DPOB will reduce the zero-dimensional(OD) Cs_4PbBr_6 phase and produce the two-dimensional(2D) CsPb_(2)Br_5 phase,which is also conducive to the improvement of device performance.Ultimately,the resulting perovskite films,which are strain-released and defect-passivated,exhibit exceptional device efficiency,reaching 10.87% for carbon-based CsPbBr_(3) device,14.86% for carbon-based CsPbI_(2)Br device,22,02% for FA_(0.97)Cs_(0.03)PbI_(3) device,respectively.Moreover,the unencapsulated CsPbBr_(3) PSC exhibits excellent stability under persistent exposure to humidity(80%) and heat(80℃) for over 50 days.
基金supported by MOST(2017YFA0206702)NSFC(21871149)+2 种基金MOE(B12015)Tianjin Project(18JCZDJC31100)the Fundamental Research Funds for the Central Universities.
文摘Metallic lithium anode is widely applied to building highenergy-density batteries such as lithium–sulfur and lithium–oxygen batteries because of its high specific capacity(3860 mAh g?1)and lowest negative potential(?3.04 V vs.standard hydrogen electrode(SHE))[1,2].However,the practical applications of Li anode remain challenging[3–6].The large volume change during repeated plating/stripping of Li would cause mechanical and interfacial instability[7,8].The solid electrolyte interphase(SEI)layers on lithium surface with poor elasticity are vulnerable to crack under variable stress/strain,leading to continuous side reactions between exposed fresh Li and electrolyte[9–11].In addition,the uncontrollable nucleation and growth of Li incur the formation of dendrites,which could accelerate detrimental parasitic reactions.Because of the uneven stripping,dendritic Li may deteriorate into electrically disconnected or“dead”Li,resulting in poor Coulombic efficiency,rapid capacity decay,and short circuit risk[12–17].
文摘The ultrafine particles of a new style Fe-Cu-based catalysts for CO hydrogenation were prepared by impregnating the organic sol of Fe（OH）3 and Cu（OH）2 onto the activated Al2O3, in which the organic sol of Fe（OH）3 and Cu（OH）2 were prepared in the microemulsion of dodecylbenzenesulfonic acid sodium（S）/n-butanol（A）/toluene（O）/water with V（A）/V（O） = 0.25 and W（A）/W（S） = 1.50. This catalyst was characterized by particle size analysis, XRD and TG. The results of particle size analysis showed that Fe（OH）3 particles with a mean size of 17.1 nm and Cu（OH）2 particles with an average size of 6.65 um were obtained. TG analysis and XRD patterns suggested that 673 K is the optimal calcination temperature. CO hydrogenation produced C＋OH with a high selectivity above 58 wt% by using the ultrafine particles as catalyst, and the total alcohol yield of 0.250 g·ml^-1 ·h^-1 was obtained when the contents of Al2O3 and K were 88.61 wt% and 1.60 wt%, respectively.
基金supported by the National Natural Science Foundation of China(21972166)the Beijing Natural Science Foundation(2202045)the National Key Research and Development Program of China(2019YFC1907600)。
文摘Herein,the catalysts of ultrathin g-C_(3)N_(4)surface-modified hollow spherical Bi2MoO6(g-C_(3)N_(4)/Bi2MoO6,abbreviated as CN/BMO)were fabricated by the co-solvothermal method.The variable valence Mo^(5+)/Mo^(6+)ionic bridge in CN/BMO catalysts can boost the rapid transfer of photogenerated electrons from Bi2MoO6to g-C_(3)N_(4).And the synergy effect of g-C_(3)N_(4)and Bi2MoO6components remarkably enhance CO_(2)adsorption capability.CN/BMO-2 catalyst has the best performances for visible light-driven CO_(2)reduction compared with single Bi2MoO6and g-C_(3)N_(4),i.e.,its amount and selectivity of CO product are 139.50μmol g-1and 96.88%for 9 h,respectively.Based on the results of characterizations and density functional theory calculation,the photocatalytic mechanism for CO_(2)reduction is proposed.The high-efficient separation efficiency of photogenerated electron-hole pairs,induced by variable valence Mo^(5+)/Mo^(6+)ionic bridge,can boost the rate-limiting steps(COOH*-to-CO*and CO*desorption)of selective visible light-driven CO_(2)conversion into CO.It inspires the establishment of efficient photocatalysts for CO_(2)conversion.
基金financial support from the National Natural Science Foundation of China (61774139, 21503202 and61604143)Shandong Provincial Natural Science Foundation (ZR2015EM024)the Fundamental Research Funds for the Central Universities (201564002, 201762018)
文摘Pursuit of energy-harvesting or-storage materials to realize outstanding electricity output from nature has been regarded as a promising strategy to resolve the energy-lack issue in the future. Among them,the solar cell as a solar-to-electrical conversion device has been attracted enormous interest to improve the efficiency. However, the ability to generate electricity is highly dependent on the weather conditions,in other words, there is nearly zero power output in dark-light conditions, such as rainy, cloudy, and night, lowering the monolithic power generation capacity. Here, we present a bifunctional polyaniline film via chemical bath deposition, which can harvest energy from the rain, yielding an induced current of 2.57 μA and voltage of 65.5 μV under the stimulus of real raindrop. When incorporating the functional PANi film into the traditional dye sensitized solar cell as a counter electrode, the hybridized photovoltaic can experimentally realize the enhanced output power via harvesting energy from rainy and sunny days. The current work may show a new path for development of advanced solar cells in the future.
