Photocatalysis is regarded as an ideal technology for solving the urgent environmental and energy issues that we face today.Among the reported photocatalysts,molybdenum disulfide(MoS2) is very promising for applicat...Photocatalysis is regarded as an ideal technology for solving the urgent environmental and energy issues that we face today.Among the reported photocatalysts,molybdenum disulfide(MoS2) is very promising for applications in hydrogen production and pollutant photodegradation.However,its lack of active sites and the difficulty of recovering catalysts in powder form have hindered its wide application.Here,we report the successful preparation of a macroscopic visible-light responsive MoS2/reduced graphene oxide(MoS2/RGO) aerogel.The obtained MoS2/RGO aerogel exhibits enhanced photocatalytic activity towards hydrogen production and photoreduction of Cr(Ⅵ) in comparison with the MoS2 powder.In addition,the low density(56.1 mg/cm^3) of the MoS2/RGO aerogel enables it to be used as an efficient adsorption material for organic pollutants.Our results demonstrate that this very promising multifunctional aerogel has potential applications in environmental remediation and clean energy production.展开更多
An iridium (Ⅲ) bis[(4,6-difluorophenyl)pyridinato-N, C^2][6-(6'-(4"-( 5"-phenyl- 1", 3", 4"-oxadiazole-2"-yl) phenoxy) hexyloxy picolinate) was synthesized and characterized by IH NMR and elementary ...An iridium (Ⅲ) bis[(4,6-difluorophenyl)pyridinato-N, C^2][6-(6'-(4"-( 5"-phenyl- 1", 3", 4"-oxadiazole-2"-yl) phenoxy) hexyloxy picolinate) was synthesized and characterized by IH NMR and elementary analysis in order to study the effect of ancillary ligand of the oxadiazole-based picolinic acid derivative on optophysical properties of its iridium complex, and further to obtain an iridium complex with highly-efficient blue emission. The thermal stability, UV absorption and photoluminescent properties of this iridium complex were investigated. Compared with iridium (Ⅲ) bis[(4,6-difluorophenyl)pyridinato-N, C^2](picolinate) reported as a highly-efficient blue electroluminescent material, this iridium complex bearing an oxadiazole-based picolinic acid derivative presents higher thermal stability, more intense UV absorption at 291 nm and similar photoluminescent spectrum peaked at 469 nm. This indicates that tuning ancillary ligand of picolinic acid with an oxadiazole unit can improve the optophysical properties of its iridium complex.展开更多
Nitric humic acid was prepared by catalytic oxidation between nitric acid and Guizhou coal, with added catalysts. We investigated catalytic oxidation processes and the factors that affect the reactions. The effects of...Nitric humic acid was prepared by catalytic oxidation between nitric acid and Guizhou coal, with added catalysts. We investigated catalytic oxidation processes and the factors that affect the reactions. The effects of different catalysts, including NiSO4 support on active carbon (AC-NiS04), NiS04 support on sil- icon dioxide (SiO2-NiSO4), composites of SO42-1Fe203, Zr-iron and vanadium-iron composite were stud- ied. As well, we investigated nitric humic acid yields and the chemical structure of products by element analysis, FT-IR and E4/E6 (an absorbance ratio at wavelengths of 465 and 665 nm of humic acid alkaline extraction solutions). The results show that the catalytic oxidation reaction with added catalysts can increase humic acid yields by 18.7%, 16.36% 12.94%, 5.61% and 8.59%, respectively. The highest yield of humic acid, i.e., 36.0%, was obtained with AC-NiSO4 as the catalyst. The amounts of C and H decreased with the amount of nitrogen. The increase in the E4/E6 ratio in catalytic oxidation of (Guizhou) coal shows that small molecular weights and high yields of nitric humic acid can be obtained by catalytic oxidation reactions.展开更多
Photocatalytic conversion of“greenhouse gas”CO2is considered to be one of the most effective ways to alleviate current energy and environmental problems without additional energy consumption and pollutant emission.T...Photocatalytic conversion of“greenhouse gas”CO2is considered to be one of the most effective ways to alleviate current energy and environmental problems without additional energy consumption and pollutant emission.The performance of many traditional semiconductor photocatalysts is not efficient enough to satisfy the requirements of practical applications because of their limited specific surface area and low CO2adsorption capacity.Therefore,the exploration of photocatalysts with high CO2uptake is significant in the field of CO2conversion.Recently the porous materials appeared to be a kind of superior candidate for enriching the CO2molecules on the surface of photocatalysts for catalytic conversion.This paper first summarizes the advances in the development of nanoporous adsorbents for CO2capture.Three main classes of porous materials are considered:inorganic porous materials,metal organic frameworks,and microporous organic polymers.Based on systematic research on CO2uptake,we then highlight the recent progress in these porous‐material‐based photocatalysts for CO2conversion.Benefiting from the improved CO2uptake capacity,the porous‐material‐based photocatalysts exhibited remarkably enhanced efficiency in the reduction of CO2to chemical fuels,such as CO,CH4,and CH3OH.Based on reported recent achievements,we predict a trend of development in multifunctional materials with both high adsorption capability and photocatalytic performance for CO2utilization.展开更多
The probe absorption-dispersion spectra of a radio-frequency (RF)-driven five-level atom embedded in a photonic crystal are investigated by considering the isotropic double-band photonic-bandogap (PBG) reservoir. ...The probe absorption-dispersion spectra of a radio-frequency (RF)-driven five-level atom embedded in a photonic crystal are investigated by considering the isotropic double-band photonic-bandogap (PBG) reservoir. In the model used, the two transitions are, respectively, coupled by leading to some curious phenomena. Numerical simulations the upper and lower bands in such a PBG material, thus are performed for the optical spectra. It is found that when one transition frequency is inside the band gap and the other is outside the gap, there emerge three peaks in the absorption spectra. However, for the case that two transition frequencies lie inside or outside the band gap, the spectra display four absorption profiles. Especially, there appear two sharp peaks in the spectra when both transition frequencies exist inside the band gap. The influences of the intensity and frequency of the RF-driven field on the absorptive and dispersive response are analyzed under different band-edge positions. It is found that a transparency window appears in the absorption spectra and is accompanied by a very steep variation of the dispersion profile by adjusting system parameters. These results show that the absorption-dispersion properties of the system depend strongly on the RF-induced quantum interference and the density of states (DOS) of the PBG reservoir.展开更多
This is a mini-review-like article including our recent results and methods for (new) metal oxides and (previously reported) composite materials composed of metal complexes and metal oxides for comparison to enhan...This is a mini-review-like article including our recent results and methods for (new) metal oxides and (previously reported) composite materials composed of metal complexes and metal oxides for comparison to enhance anisotropic structural changes intentionally. Some complex inorganic oxides are known that they may be promising color materials (absorbing visible light of certain wavelengths region) having potential application for environmentally benign catalysts, for example, photocatalysts. Chiral copper(Ⅱ) complexes having bidentate amine ligands ([CuL2]2+) can be acted as cationic building blocks of bimetallic metal complexes. We have prepared some chiral bimetallic complexes with various anionic metal complexes such as [PtCl4]2-, [M02O7]2 and Mn12 clusters (typical single-molecule magnets) which characterized by means of solid-state electronic and CD (circular dichroism) spectra, IR (infrared) spectra, synchrotron XRD (X-ray diffraction) and XAS (soft X-ray absorption spectroscopy). By sintering these precursor chiral bimetallic complexes, we have prepared complex inorganic oxides from them. The IR spectra indicated substituting metal-ligand bonds and losing organic moieties. The XRD pattern indicated complete changes of crystal structures. The XAS revealed replacing coordination atoms as well as oxidation of valences of metal ions. Furthermore, we will also investigate possibility of patterning by homogeneous precipitation method as bimetallic complexes to prepare desirable complex inorganic oxides.展开更多
The application of antimony sulfide(Sb_(2)S_(3))has been limited mainly to the energy storage and photoelectric conversion fields.However,in this work,the application of Sb_(2)S_(3) is extended to the field of electro...The application of antimony sulfide(Sb_(2)S_(3))has been limited mainly to the energy storage and photoelectric conversion fields.However,in this work,the application of Sb_(2)S_(3) is extended to the field of electromagnetic(EM)wave absorption for the first time.High-permittivity Sb_(2)S_(3) singlecrystal nanorods were prepared successfully and exhibited excellent performance,with a low reflection loss of -65.9 dB(13.0 GHz,3.8 mm)and an ultra-wide effective absorption bandwidth of 9.5 GHz(8.5-18.0 GHz,4.1 mm).After excluding the general absorption mechanisms,including conductive losses,interfacial polarization,and dipole polarization,the distinctive single-crystal volume polarization affected by shape anisotropy was proposed.This work not only meets the challenge of a single-component dielectric material design but also introduces a new concept for construction of efficient dielectric EM wave absorption material.展开更多
It is necessary to evaluate the interactions between the different functional layers in optoelectronic devices to optimize device performance.Recently,the I-rich allinorganic perovskite CsPbI2 Br has attracted tremend...It is necessary to evaluate the interactions between the different functional layers in optoelectronic devices to optimize device performance.Recently,the I-rich allinorganic perovskite CsPbI2 Br has attracted tremendous attention for use in solar cell applications because of its suitable band gap and favorable photo and thermal stabilities.It has been reported that the undesirable phase degradation of the photoactiveαphase CsPbI2 Br to the non-perovskiteδphase could be triggered by high humidity.To obtain stable devices,it is thus important to protect CsPbI2 Br from moisture.In this paper,CuI,a non-hygroscopic p-type hole-transporting material,is found to induce the phase degradation ofα-CsPbI2 Br to theδ-CsPbI2 Br.The rate and extent of phase degradation of CsPbI2 Br are closely associated with the heating temperature and coverage of a Cu I granular capping layer.This discovery is different from the widely reported water-induced phase degradation of CsPbI2 Br.Our work highlights the importance of careful selection of hole-transporting materials during the processing of I-rich all-inorganic CsPbX3(X=Br,I)perovskites to realize high-performance optoelectronic devices.展开更多
This article summarized the recent advance on the structural design and synthetic strategies of intramolec- ular charge-transfer compounds as well as their potential ap- plications in two-photon absorption chromophore...This article summarized the recent advance on the structural design and synthetic strategies of intramolec- ular charge-transfer compounds as well as their potential ap- plications in two-photon absorption chromophores, organic photovoltaics and organic light-emitting diodes.展开更多
The rational design and construction of novel two-dimensional(2D)carbon nitrides(CNs)beyond g-C_(3)N_(4) is a hot topic in the fields of chemistry and materials.Inspired by the polymerisation of urea,we have prepared ...The rational design and construction of novel two-dimensional(2D)carbon nitrides(CNs)beyond g-C_(3)N_(4) is a hot topic in the fields of chemistry and materials.Inspired by the polymerisation of urea,we have prepared a series of novel C-C bridged heptazine CNs UO_(x)(where x is the ratio of urea to oxamide,x=1,1.5,2,2.5,and 3),which are similar to(C_(6)N_(7))n,upon the introduction of oxamide.As predicted using density functional theory(DFT)calculations,the conjugated structure of UO_(x) was effectively extended from an individual heptazine to the entire material.Consequently,its bandgap was reduced to 2.05 eV,and its absorption band edge was significantly extended to 600 nm.Furthermore,its carrier transfer and separation were significantly enhanced,establishing its superior photocatalytic activity.The optimised UO_(2) exhibits a superior photocatalytic hydrogen production rate about 108.59 lmol h^(-1)(using 10 mg of catalyst)with an apparent quantum efficiency(AQE)of 36.12%and 0.33%at 420 and 600 nm,respectively,which is one of the most active novel CNs reported to date.Moreover,UO_(2) exhibits excellent photocatalytic activity toward the oxidation of diphenylhydrazine to azobenzene with conversion and selectivity reaching~100%,which represents a promising highly efficient 2D CN material.Regarding phenols degradation,UO_(2) also displayed significantly higher activity and durability during the degradation of phenol when compared to traditional g-C_(3)N_(4),highlighting its significant potential for application in energy,environment and photocatalytic organic reactions.展开更多
基金supported by the National Natural Science Foundation of China (U1232119, 21403172)the Sichuan Youth Science and Technology Foundation (2013JQ0034, 2014JQ0017)the Innovative Research Team of Sichuan Province (2016TD0011)~~
文摘Photocatalysis is regarded as an ideal technology for solving the urgent environmental and energy issues that we face today.Among the reported photocatalysts,molybdenum disulfide(MoS2) is very promising for applications in hydrogen production and pollutant photodegradation.However,its lack of active sites and the difficulty of recovering catalysts in powder form have hindered its wide application.Here,we report the successful preparation of a macroscopic visible-light responsive MoS2/reduced graphene oxide(MoS2/RGO) aerogel.The obtained MoS2/RGO aerogel exhibits enhanced photocatalytic activity towards hydrogen production and photoreduction of Cr(Ⅵ) in comparison with the MoS2 powder.In addition,the low density(56.1 mg/cm^3) of the MoS2/RGO aerogel enables it to be used as an efficient adsorption material for organic pollutants.Our results demonstrate that this very promising multifunctional aerogel has potential applications in environmental remediation and clean energy production.
基金Projects(20772101,50473046) supported by the National Natural Science Foundation of ChinaProject(2007FJ3017) supported by the Hunan Provincial Science Foundation, ChinaProject(07C764) supported by the Science Foundation of the Education Department of Hunan Province,China
文摘An iridium (Ⅲ) bis[(4,6-difluorophenyl)pyridinato-N, C^2][6-(6'-(4"-( 5"-phenyl- 1", 3", 4"-oxadiazole-2"-yl) phenoxy) hexyloxy picolinate) was synthesized and characterized by IH NMR and elementary analysis in order to study the effect of ancillary ligand of the oxadiazole-based picolinic acid derivative on optophysical properties of its iridium complex, and further to obtain an iridium complex with highly-efficient blue emission. The thermal stability, UV absorption and photoluminescent properties of this iridium complex were investigated. Compared with iridium (Ⅲ) bis[(4,6-difluorophenyl)pyridinato-N, C^2](picolinate) reported as a highly-efficient blue electroluminescent material, this iridium complex bearing an oxadiazole-based picolinic acid derivative presents higher thermal stability, more intense UV absorption at 291 nm and similar photoluminescent spectrum peaked at 469 nm. This indicates that tuning ancillary ligand of picolinic acid with an oxadiazole unit can improve the optophysical properties of its iridium complex.
基金sponsored by the Shaanxi Key Scientific and Technological Project, China (No. 2010K07-20)the National Science and Technology Major Project (No. 2011ZX05037-003)
文摘Nitric humic acid was prepared by catalytic oxidation between nitric acid and Guizhou coal, with added catalysts. We investigated catalytic oxidation processes and the factors that affect the reactions. The effects of different catalysts, including NiSO4 support on active carbon (AC-NiS04), NiS04 support on sil- icon dioxide (SiO2-NiSO4), composites of SO42-1Fe203, Zr-iron and vanadium-iron composite were stud- ied. As well, we investigated nitric humic acid yields and the chemical structure of products by element analysis, FT-IR and E4/E6 (an absorbance ratio at wavelengths of 465 and 665 nm of humic acid alkaline extraction solutions). The results show that the catalytic oxidation reaction with added catalysts can increase humic acid yields by 18.7%, 16.36% 12.94%, 5.61% and 8.59%, respectively. The highest yield of humic acid, i.e., 36.0%, was obtained with AC-NiSO4 as the catalyst. The amounts of C and H decreased with the amount of nitrogen. The increase in the E4/E6 ratio in catalytic oxidation of (Guizhou) coal shows that small molecular weights and high yields of nitric humic acid can be obtained by catalytic oxidation reactions.
基金supported by the National Natural Science Foundation of China(21771070,21571071)~~
文摘Photocatalytic conversion of“greenhouse gas”CO2is considered to be one of the most effective ways to alleviate current energy and environmental problems without additional energy consumption and pollutant emission.The performance of many traditional semiconductor photocatalysts is not efficient enough to satisfy the requirements of practical applications because of their limited specific surface area and low CO2adsorption capacity.Therefore,the exploration of photocatalysts with high CO2uptake is significant in the field of CO2conversion.Recently the porous materials appeared to be a kind of superior candidate for enriching the CO2molecules on the surface of photocatalysts for catalytic conversion.This paper first summarizes the advances in the development of nanoporous adsorbents for CO2capture.Three main classes of porous materials are considered:inorganic porous materials,metal organic frameworks,and microporous organic polymers.Based on systematic research on CO2uptake,we then highlight the recent progress in these porous‐material‐based photocatalysts for CO2conversion.Benefiting from the improved CO2uptake capacity,the porous‐material‐based photocatalysts exhibited remarkably enhanced efficiency in the reduction of CO2to chemical fuels,such as CO,CH4,and CH3OH.Based on reported recent achievements,we predict a trend of development in multifunctional materials with both high adsorption capability and photocatalytic performance for CO2utilization.
基金Supported by the National Natural Science Foundation of China under Grant Nos.91021011,10975054,11004069,and 10874050the Doctoral Foundation of the Ministry of Education of China under Grant Nos.200804870051,20100142120081the Innovation Foundation from Huazhong University of Science and Technology under Grant No.2010MS074
文摘The probe absorption-dispersion spectra of a radio-frequency (RF)-driven five-level atom embedded in a photonic crystal are investigated by considering the isotropic double-band photonic-bandogap (PBG) reservoir. In the model used, the two transitions are, respectively, coupled by leading to some curious phenomena. Numerical simulations the upper and lower bands in such a PBG material, thus are performed for the optical spectra. It is found that when one transition frequency is inside the band gap and the other is outside the gap, there emerge three peaks in the absorption spectra. However, for the case that two transition frequencies lie inside or outside the band gap, the spectra display four absorption profiles. Especially, there appear two sharp peaks in the spectra when both transition frequencies exist inside the band gap. The influences of the intensity and frequency of the RF-driven field on the absorptive and dispersive response are analyzed under different band-edge positions. It is found that a transparency window appears in the absorption spectra and is accompanied by a very steep variation of the dispersion profile by adjusting system parameters. These results show that the absorption-dispersion properties of the system depend strongly on the RF-induced quantum interference and the density of states (DOS) of the PBG reservoir.
文摘This is a mini-review-like article including our recent results and methods for (new) metal oxides and (previously reported) composite materials composed of metal complexes and metal oxides for comparison to enhance anisotropic structural changes intentionally. Some complex inorganic oxides are known that they may be promising color materials (absorbing visible light of certain wavelengths region) having potential application for environmentally benign catalysts, for example, photocatalysts. Chiral copper(Ⅱ) complexes having bidentate amine ligands ([CuL2]2+) can be acted as cationic building blocks of bimetallic metal complexes. We have prepared some chiral bimetallic complexes with various anionic metal complexes such as [PtCl4]2-, [M02O7]2 and Mn12 clusters (typical single-molecule magnets) which characterized by means of solid-state electronic and CD (circular dichroism) spectra, IR (infrared) spectra, synchrotron XRD (X-ray diffraction) and XAS (soft X-ray absorption spectroscopy). By sintering these precursor chiral bimetallic complexes, we have prepared complex inorganic oxides from them. The IR spectra indicated substituting metal-ligand bonds and losing organic moieties. The XRD pattern indicated complete changes of crystal structures. The XAS revealed replacing coordination atoms as well as oxidation of valences of metal ions. Furthermore, we will also investigate possibility of patterning by homogeneous precipitation method as bimetallic complexes to prepare desirable complex inorganic oxides.
基金supported by the National Natural Science Foundation of China(51572157,21902085,and 51702188)the Natural Science Foundation of Shandong Province(ZR2019QF012)+1 种基金the Fundamental Research Funds for the Central Universities(2018JC046)Young Scholars Program of Shandong University(2018WLJH25)。
文摘The application of antimony sulfide(Sb_(2)S_(3))has been limited mainly to the energy storage and photoelectric conversion fields.However,in this work,the application of Sb_(2)S_(3) is extended to the field of electromagnetic(EM)wave absorption for the first time.High-permittivity Sb_(2)S_(3) singlecrystal nanorods were prepared successfully and exhibited excellent performance,with a low reflection loss of -65.9 dB(13.0 GHz,3.8 mm)and an ultra-wide effective absorption bandwidth of 9.5 GHz(8.5-18.0 GHz,4.1 mm).After excluding the general absorption mechanisms,including conductive losses,interfacial polarization,and dipole polarization,the distinctive single-crystal volume polarization affected by shape anisotropy was proposed.This work not only meets the challenge of a single-component dielectric material design but also introduces a new concept for construction of efficient dielectric EM wave absorption material.
基金supported primarily by the National Key Research and Development Program of China(2018YFA0209303)the National Natural Science Foundation of China(U1663228,51902153,51972165 and 61377051)the Fundamental Research Funds for the Central Universities of China。
文摘It is necessary to evaluate the interactions between the different functional layers in optoelectronic devices to optimize device performance.Recently,the I-rich allinorganic perovskite CsPbI2 Br has attracted tremendous attention for use in solar cell applications because of its suitable band gap and favorable photo and thermal stabilities.It has been reported that the undesirable phase degradation of the photoactiveαphase CsPbI2 Br to the non-perovskiteδphase could be triggered by high humidity.To obtain stable devices,it is thus important to protect CsPbI2 Br from moisture.In this paper,CuI,a non-hygroscopic p-type hole-transporting material,is found to induce the phase degradation ofα-CsPbI2 Br to theδ-CsPbI2 Br.The rate and extent of phase degradation of CsPbI2 Br are closely associated with the heating temperature and coverage of a Cu I granular capping layer.This discovery is different from the widely reported water-induced phase degradation of CsPbI2 Br.Our work highlights the importance of careful selection of hole-transporting materials during the processing of I-rich all-inorganic CsPbX3(X=Br,I)perovskites to realize high-performance optoelectronic devices.
基金supported by AcRF Tier 1(RG 8/16,RG 133/14 and RG 13/15)from MOE,SingaporeSTU Scientific Research Foundation for Talents(NTF15005)+1 种基金STU Youth Research Fund(YR15001)the Foundation for Young Talents in Higher Education of Guangdong(2015KQNCX042)
文摘This article summarized the recent advance on the structural design and synthetic strategies of intramolec- ular charge-transfer compounds as well as their potential ap- plications in two-photon absorption chromophores, organic photovoltaics and organic light-emitting diodes.
基金supported by the National Key R&D Program of China (2020YFA0406101)the National Natural Science Foundation of China (21771033 and 22071020)+4 种基金the Fundamental Research Funds for the Central Universities (2412018BJ001 and 2412018ZD007)the “Hong Kong Scholar” Programme (XJ2018021)the General Research FundResearch Grants Council of Hong Kong SAR Government (18301117)Dean’s Research Fund [04425], Ed UHK。
文摘The rational design and construction of novel two-dimensional(2D)carbon nitrides(CNs)beyond g-C_(3)N_(4) is a hot topic in the fields of chemistry and materials.Inspired by the polymerisation of urea,we have prepared a series of novel C-C bridged heptazine CNs UO_(x)(where x is the ratio of urea to oxamide,x=1,1.5,2,2.5,and 3),which are similar to(C_(6)N_(7))n,upon the introduction of oxamide.As predicted using density functional theory(DFT)calculations,the conjugated structure of UO_(x) was effectively extended from an individual heptazine to the entire material.Consequently,its bandgap was reduced to 2.05 eV,and its absorption band edge was significantly extended to 600 nm.Furthermore,its carrier transfer and separation were significantly enhanced,establishing its superior photocatalytic activity.The optimised UO_(2) exhibits a superior photocatalytic hydrogen production rate about 108.59 lmol h^(-1)(using 10 mg of catalyst)with an apparent quantum efficiency(AQE)of 36.12%and 0.33%at 420 and 600 nm,respectively,which is one of the most active novel CNs reported to date.Moreover,UO_(2) exhibits excellent photocatalytic activity toward the oxidation of diphenylhydrazine to azobenzene with conversion and selectivity reaching~100%,which represents a promising highly efficient 2D CN material.Regarding phenols degradation,UO_(2) also displayed significantly higher activity and durability during the degradation of phenol when compared to traditional g-C_(3)N_(4),highlighting its significant potential for application in energy,environment and photocatalytic organic reactions.