The earth-abundant and robust aluminum ferrite,AlFeO_(3)(AFO),is mainly studied in the context of ferroelectrics.Herein,we demonstrate that AFO can be used as a stable solar absorber in photoelectrochemical cells for ...The earth-abundant and robust aluminum ferrite,AlFeO_(3)(AFO),is mainly studied in the context of ferroelectrics.Herein,we demonstrate that AFO can be used as a stable solar absorber in photoelectrochemical cells for solar water splitting,exhibiting attractive performance.This is the first report on the photoelectrochemical activity of AFO.AFO thin-film photoelectrodes prepared by solution-processing methods are composed of vertically oriented thin nanosheets,featuring the rhombohedral symmetry(R3c)and n-type conductivity.The as-prepared AFO photoanodes generate a photocurrent density of+0.78 mA·cm^(-2) at 1.23 V vs.reversible hydrogen electrode(RHE)with the photocurrent _(onset) potential(U_(onset))close to the flat band potential of 0.5 V vs.RHE in the presence of hole scavengers.Remarkably,the U_(onset) of AFO for solar water splitting coincides with the flat band potential as well,which is rare in n-type inorganic absorbers.We also report other properties of AFO associated with photoelectrochemical performance.AFO films exhibit a band gap energy of 2.31 eV and positive band edges with low dispersion.Moreover,the carrier lifetimes in AFO films are up to millisecond timescales under the mediation of defect traps.Based on the photoelectrochemical behavior and optoelectronic properties,we believe that AFO has great potential for application in photoelectrochemical cells.展开更多
For Ti-doped hematite photoanodes, high temperature annealing drastically increases the water oxidation plateau photocurrent, but also induces an anodic shift of onset potential by about 100 m V, thus hindering the pe...For Ti-doped hematite photoanodes, high temperature annealing drastically increases the water oxidation plateau photocurrent, but also induces an anodic shift of onset potential by about 100 m V, thus hindering the performance under low applied bias. To the best of our knowledge, the effects of high temperature annealing on the onset potential have been rarely studied. Herein, both X-ray photoelectron spectroscopy（XPS） measurements and theoretical calculations indicated that the increase of surface Ti/Fe atomic ratio after high temperature annealing decreased the adsorption capacity of hydroxide ions on the hematite surface. Subsequently, the flatband potential（i.e., the theoretical onset potential） of Ti doped hematite photoanodes positively shifted, which was supported by the Mott-Schottky measurements.展开更多
Photoelectrochemical(PEC)water splitting for solar energy conversion into chemical fuels has attracted intense research attention.The semiconductor hematite(α-Fe_(2)O_(3)),with its earth abundance,chemical stability,...Photoelectrochemical(PEC)water splitting for solar energy conversion into chemical fuels has attracted intense research attention.The semiconductor hematite(α-Fe_(2)O_(3)),with its earth abundance,chemical stability,and efficient light harvesting,stands out as a promising photoanode material.Unfortunately,its electron affinity is too deep for overall water splitting,requiring additional bias.Interface engineering has been used to reduce the onset potential of hematite photoelectrode.Here we focus instead on energy band engineering hematite by shrinking the crystal lattice,and the water-splitting onset potential can be decreased from 1.14 to 0.61 V vs.the reversible hydrogen electrode.It is the lowest record reported for a pristine hematite photoanode without surface modification.X-ray absorption spectroscopy and magnetic properties suggest the redistribution of 3d electrons in the as-synthesized grey hematite electrode.Density function theory studies herein show that the smaller-lattice-constant hematite benefits from raised energy bands,which accounts for the reduced onset potential.展开更多
Combining a progressive tandem junction design with a unique Si nanowire(SiNW)framework paves the way for the development of high‐onset‐potential photocathodes and enhancement of solar hydrogen production.Herein,a r...Combining a progressive tandem junction design with a unique Si nanowire(SiNW)framework paves the way for the development of high‐onset‐potential photocathodes and enhancement of solar hydrogen production.Herein,a radial tandem junction(RTJ)thin film water‐splitting photo‐cathode has been demonstrated experimentally for the first time.The photocathode is directly fab‐ricated on vapor‐liquid‐solid‐grown SiNWs and consists of two radially stacked p‐i‐n junctions,featuring hydrogenated amorphous silicon(a‐Si:H)as the outer absorber layer,which absorbs short wavelengths,and hydrogenated amorphous silicon germanium(a‐SiGe:H)as the inner layer,which absorbs long wavelengths.The randomly distributed SiNW framework enables highly efficient light‐trapping,which facilitates the use of very thin absorber layers of a‐Si:H(~50 nm)and a‐SiGe:H(~40 nm).In a neutral electrolyte(pH=7),the three‐dimensional(3D)RTJ photocathode delivers a high photocurrent onset of 1.15 V vs.the reversible hydrogen electrode(RHE),accompanied by a photocurrent of 2.98 mA/cm^(2) at 0 V vs.RHE,and an overall applied‐bias photon‐to‐current effi‐ciency of 1.72%.These results emphasize the promising role of 3D radial tandem technology in developing a new generation of durable,low‐cost,high‐onset‐potential photocathodes capable of large‐scale implementation。展开更多
The establishment of multi-component catalytic systems on Fe2O3 photoanodes presents considerable potential for significantly enhancing the performance of photoelectrochemical water splitting systems. In this study, w...The establishment of multi-component catalytic systems on Fe2O3 photoanodes presents considerable potential for significantly enhancing the performance of photoelectrochemical water splitting systems. In this study, we hydrothermally synthesized a Fe2O3 photoanode. In addition, d-Fe OOH synthesized via dip-coating and hydrothermally prepared h-FeOOH were used as cocatalysts and their synergistic combinations with cobalt phosphate(Co-Pi) were investigated. The synergy between h-FeOOH and Co-Pi was remarkable, whereas that between d-Fe OOH and Co-Pi was negligible. For example, the onset potentials of the Co-Pi/h-FeOOH and Co-Pi/d-FeOOH dual catalysts, were cathodically shifted by 270 and 170 m V, respectively. Moreover, the photocurrent density of the Co-Pi/h-FeOOH/Fe2O3 anode was significantly higher than that of the Co-Pi/d-FeOOH/Fe2O3 one. The synergistic effect of Co-Pi and h-FeOOH could be attributed to the significantly inhibited recombination of surface charges owing to the formation of a p-n junction between β-FeOOH and Fe2O3 and the large contact area between the granular h-FeOOH and Co-Pi. However, the thin amorphous FeOOH layer of the Co-Pi/d-FeOOH/Fe2O3 anode acted as a hole-transfer medium, and weakly promoted the kinetics of the charge transfer process.展开更多
Background： This study was to establish a disease differentiation model for ST-segment elevation myocardial infarction （STEMI） youth patients experiencing ischemia and reperfusion via ultra-performance liquid chrom...Background： This study was to establish a disease differentiation model for ST-segment elevation myocardial infarction （STEMI） youth patients experiencing ischemia and reperfusion via ultra-performance liquid chromatography and mass spectrometry （UPLC/MS） platform, which searches for closely related characteristic metabolites and metabolic pathways to evaluate their predictive value in the prognosis after discharge. Methods： Forty-seven consecutive STEMI patients （23 patients under 45 years of age, referred to here as ＂youth,＂ and 24 elderly patients） and 48 healthy control group members （24 youth, 24 elderly） were registered prospectively. The youth patients were required to provide a second blood draw during a follow-up visit one year after morbidity （n - 22, one lost）. Characteristic metabolites and relative metabolic pathways were screened via UPLC/MS platform base on the Kyoto encyclopedia of genes and genomes （KEGG） and Human Metabolome Database. Receiver operating characteristic （ROC） curves were drawn to evaluate the predictive value of characteristic metabolites in the prognosis after discharge. Results： We successfully established an orthogonal partial least squares discriminated analysis model （R2X = 71.2%, R2Y = 79.6%, and Q2 55.9%） and screened out 24 ions; the sphingolipid metabolism pathway showed the most drastic change. The ROC curve analysis showed that ceramide [Cer（dl 8：0/16：0）, Cer（t 18：0/12：0）] and sphinganine in the sphingolipid pathway have high sensitivity and specificity on the prognosis related to major adverse cardiovascular events after youth patients were discharged. The area under curve （AUC） was 0.67 1, 0.750, and 0.711, respectively. A follow-up validation one year after morbidity showed corresponding AUC of 0.778, 0.833, and 0.806. Conclusions： By analyzing the plasma metabolism of myocardial infarction patients, we successfully established a model that can distinguish two different factors simultaneously： patholog展开更多
The occurrence of first hurricane in early summer signifies the onset of an active Atlantic hurricane season.The interannual variation of this hurricane onset date is examined for the period 1979-2013.It is found that...The occurrence of first hurricane in early summer signifies the onset of an active Atlantic hurricane season.The interannual variation of this hurricane onset date is examined for the period 1979-2013.It is found that the onset date has a marked interannual variation.The standard deviation of the interannual variation of the onset day is 17.5 days,with the climatological mean onset happening on July 23.A diagnosis of tropical cyclone（TC） genesis potential index（GPI） indicates that the major difference between an early and a late onset group lies in the maximum potential intensity（MPI）.A further diagnosis of the MPI shows that it is primarily controlled by the local SST anomaly（SSTA）.Besides the SSTA,vertical shear and mid-tropospheric relative humidity anomalies also contribute significantly to the GPI difference between the early and late onset groups.It is found that the anomalous warm（cold） SST over the tropical Atlantic,while uncorrected with the Nino3 index,persists from the preceding winter to concurrent summer in the early（late） onset group.The net surface heat flux anomaly always tends to damp the SSTA,which suggests that ocean dynamics may play a role in maintaining the SSTA in the tropical Atlantic.The SSTA pattern with a maximum center in northeastern tropical Atlantic appears responsible for generating the observed wind and moisture anomalies over the main TC development region.A further study is needed to understand the initiation mechanism of the SSTA in the Atlantic.展开更多
目的:探讨碱性成纤维细胞生长因子(bFGF)对难治性突发性聋的疗效。方法:将208例(266耳)接受正规疗程治疗后,疗效不显著或不满意而有意继续接受治疗,病程在4个月内的突发性聋患者,按照就诊先后顺序分成治疗组104例(135耳)和对照组104例(...目的:探讨碱性成纤维细胞生长因子(bFGF)对难治性突发性聋的疗效。方法:将208例(266耳)接受正规疗程治疗后,疗效不显著或不满意而有意继续接受治疗,病程在4个月内的突发性聋患者,按照就诊先后顺序分成治疗组104例(135耳)和对照组104例(131耳)。治疗组肌注bFGF4000u,qd,连用15～30d;对照组用维生素B_1100mg加维生素B_(12)500μg混合肌注,或B族维生素口服,qd,连用15d。治疗前后均行纯音电测听及脑干听觉诱发电位。结果:治疗前听阈治疗组为(58.36±27.58)dB pe SPL,对照组为(59.82±28.45)dB pe SPL(P>0.05);治疗后治疗组听阈为(41.89±23.45)dB pe SPL,对照组为(56.73±33.15)dB pe SPL(P<0.01)。有效率治疗组为97%,对照组为38.9%,差异有显著性(P<0.01)。结论:bFGF治疗突发性聋有较大的治疗时间窗,疗效可靠、显著。展开更多
基金support from the project of State Key Laboratory of Alternate Electrical Power System with Renewable Energy Sources(Nos.LAPS21004 and LAPS202114)the National Natural Science Foundation of China(Nos.52272200,51972110,52102245,52102203,and 52072121)+6 种基金China Postdoctoral Science Foundation(No.2022M721129)Beijing Science and Technology Project(No.Z211100004621010)Beijing Natural Science Foundation(Nos.2222076 and 2222077)Hebei Natural Science Foundation(No.E2022502022)Huaneng Group Headquarters Science and Technology Project(No.HNKJ20-H88)2022 Strategic Research Key Project of Science and Technology Commission of the Ministry of Education,the Fundamental Research Funds for the Central Universities(Nos.2022MS030,2021MS028,2020MS023,and 2020MS028)the NCEPU“Double First-Class”Program.
文摘The earth-abundant and robust aluminum ferrite,AlFeO_(3)(AFO),is mainly studied in the context of ferroelectrics.Herein,we demonstrate that AFO can be used as a stable solar absorber in photoelectrochemical cells for solar water splitting,exhibiting attractive performance.This is the first report on the photoelectrochemical activity of AFO.AFO thin-film photoelectrodes prepared by solution-processing methods are composed of vertically oriented thin nanosheets,featuring the rhombohedral symmetry(R3c)and n-type conductivity.The as-prepared AFO photoanodes generate a photocurrent density of+0.78 mA·cm^(-2) at 1.23 V vs.reversible hydrogen electrode(RHE)with the photocurrent _(onset) potential(U_(onset))close to the flat band potential of 0.5 V vs.RHE in the presence of hole scavengers.Remarkably,the U_(onset) of AFO for solar water splitting coincides with the flat band potential as well,which is rare in n-type inorganic absorbers.We also report other properties of AFO associated with photoelectrochemical performance.AFO films exhibit a band gap energy of 2.31 eV and positive band edges with low dispersion.Moreover,the carrier lifetimes in AFO films are up to millisecond timescales under the mediation of defect traps.Based on the photoelectrochemical behavior and optoelectronic properties,we believe that AFO has great potential for application in photoelectrochemical cells.
基金supported by the National Natural Science Foundation of China (Nos. 21473090, U1663228)
文摘For Ti-doped hematite photoanodes, high temperature annealing drastically increases the water oxidation plateau photocurrent, but also induces an anodic shift of onset potential by about 100 m V, thus hindering the performance under low applied bias. To the best of our knowledge, the effects of high temperature annealing on the onset potential have been rarely studied. Herein, both X-ray photoelectron spectroscopy（XPS） measurements and theoretical calculations indicated that the increase of surface Ti/Fe atomic ratio after high temperature annealing decreased the adsorption capacity of hydroxide ions on the hematite surface. Subsequently, the flatband potential（i.e., the theoretical onset potential） of Ti doped hematite photoanodes positively shifted, which was supported by the Mott-Schottky measurements.
基金financially supported by the National Natural Science Funds for Distinguished Young Scholars (51725201)the International (Regional) Cooperation and Exchange Projects of the National Natural Science Foundation of China (51920105003)+3 种基金the Innovation Program of Shanghai Municipal Education Commission (E00014)the National Natural Science Foundation of China (51902105)the Shanghai Engineering Research Center of Hierarchical Nanomaterials (18DZ2252400)the Shanghai Sailing Program (19YF1411600)
文摘Photoelectrochemical(PEC)water splitting for solar energy conversion into chemical fuels has attracted intense research attention.The semiconductor hematite(α-Fe_(2)O_(3)),with its earth abundance,chemical stability,and efficient light harvesting,stands out as a promising photoanode material.Unfortunately,its electron affinity is too deep for overall water splitting,requiring additional bias.Interface engineering has been used to reduce the onset potential of hematite photoelectrode.Here we focus instead on energy band engineering hematite by shrinking the crystal lattice,and the water-splitting onset potential can be decreased from 1.14 to 0.61 V vs.the reversible hydrogen electrode.It is the lowest record reported for a pristine hematite photoanode without surface modification.X-ray absorption spectroscopy and magnetic properties suggest the redistribution of 3d electrons in the as-synthesized grey hematite electrode.Density function theory studies herein show that the smaller-lattice-constant hematite benefits from raised energy bands,which accounts for the reduced onset potential.
文摘Combining a progressive tandem junction design with a unique Si nanowire(SiNW)framework paves the way for the development of high‐onset‐potential photocathodes and enhancement of solar hydrogen production.Herein,a radial tandem junction(RTJ)thin film water‐splitting photo‐cathode has been demonstrated experimentally for the first time.The photocathode is directly fab‐ricated on vapor‐liquid‐solid‐grown SiNWs and consists of two radially stacked p‐i‐n junctions,featuring hydrogenated amorphous silicon(a‐Si:H)as the outer absorber layer,which absorbs short wavelengths,and hydrogenated amorphous silicon germanium(a‐SiGe:H)as the inner layer,which absorbs long wavelengths.The randomly distributed SiNW framework enables highly efficient light‐trapping,which facilitates the use of very thin absorber layers of a‐Si:H(~50 nm)and a‐SiGe:H(~40 nm).In a neutral electrolyte(pH=7),the three‐dimensional(3D)RTJ photocathode delivers a high photocurrent onset of 1.15 V vs.the reversible hydrogen electrode(RHE),accompanied by a photocurrent of 2.98 mA/cm^(2) at 0 V vs.RHE,and an overall applied‐bias photon‐to‐current effi‐ciency of 1.72%.These results emphasize the promising role of 3D radial tandem technology in developing a new generation of durable,low‐cost,high‐onset‐potential photocathodes capable of large‐scale implementation。
基金supported by the National Natural Foundation of China (21176111)the National Basic Research Program (973 Program, 2013CB632404)+1 种基金the National High Technology Research and Development Program of China (863 Program, 2011AA11A271)A Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions~~
文摘The establishment of multi-component catalytic systems on Fe2O3 photoanodes presents considerable potential for significantly enhancing the performance of photoelectrochemical water splitting systems. In this study, we hydrothermally synthesized a Fe2O3 photoanode. In addition, d-Fe OOH synthesized via dip-coating and hydrothermally prepared h-FeOOH were used as cocatalysts and their synergistic combinations with cobalt phosphate(Co-Pi) were investigated. The synergy between h-FeOOH and Co-Pi was remarkable, whereas that between d-Fe OOH and Co-Pi was negligible. For example, the onset potentials of the Co-Pi/h-FeOOH and Co-Pi/d-FeOOH dual catalysts, were cathodically shifted by 270 and 170 m V, respectively. Moreover, the photocurrent density of the Co-Pi/h-FeOOH/Fe2O3 anode was significantly higher than that of the Co-Pi/d-FeOOH/Fe2O3 one. The synergistic effect of Co-Pi and h-FeOOH could be attributed to the significantly inhibited recombination of surface charges owing to the formation of a p-n junction between β-FeOOH and Fe2O3 and the large contact area between the granular h-FeOOH and Co-Pi. However, the thin amorphous FeOOH layer of the Co-Pi/d-FeOOH/Fe2O3 anode acted as a hole-transfer medium, and weakly promoted the kinetics of the charge transfer process.
文摘Background： This study was to establish a disease differentiation model for ST-segment elevation myocardial infarction （STEMI） youth patients experiencing ischemia and reperfusion via ultra-performance liquid chromatography and mass spectrometry （UPLC/MS） platform, which searches for closely related characteristic metabolites and metabolic pathways to evaluate their predictive value in the prognosis after discharge. Methods： Forty-seven consecutive STEMI patients （23 patients under 45 years of age, referred to here as ＂youth,＂ and 24 elderly patients） and 48 healthy control group members （24 youth, 24 elderly） were registered prospectively. The youth patients were required to provide a second blood draw during a follow-up visit one year after morbidity （n - 22, one lost）. Characteristic metabolites and relative metabolic pathways were screened via UPLC/MS platform base on the Kyoto encyclopedia of genes and genomes （KEGG） and Human Metabolome Database. Receiver operating characteristic （ROC） curves were drawn to evaluate the predictive value of characteristic metabolites in the prognosis after discharge. Results： We successfully established an orthogonal partial least squares discriminated analysis model （R2X = 71.2%, R2Y = 79.6%, and Q2 55.9%） and screened out 24 ions; the sphingolipid metabolism pathway showed the most drastic change. The ROC curve analysis showed that ceramide [Cer（dl 8：0/16：0）, Cer（t 18：0/12：0）] and sphinganine in the sphingolipid pathway have high sensitivity and specificity on the prognosis related to major adverse cardiovascular events after youth patients were discharged. The area under curve （AUC） was 0.67 1, 0.750, and 0.711, respectively. A follow-up validation one year after morbidity showed corresponding AUC of 0.778, 0.833, and 0.806. Conclusions： By analyzing the plasma metabolism of myocardial infarction patients, we successfully established a model that can distinguish two different factors simultaneously： patholog
基金Supported by the National(Key)Basic Research and Development(973)Program of China(2015CB453200)National Natural Science Foundation of China(41475084)+10 种基金ONR Grant(N00014-16-12260)NRL Grant(N00173-13-1-G902)Jiangsu Natural Science Key Project(BK20150062)Jiangsu Shuang-Chuang Team(R2014SCT001)Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD),Natural Science Foundation of the Higher Education Institutions of Jiangsu Province(14KJB170015)the Startup Foundation for Introducing Talent of NUIST(2013x018)Civil Aviation Center Program(KDQC1302)The International Pacific Research Center is partially sponsored by the Japan Agency for Marine-Earth Science and Technology(JAMSTEC)SOEST contribution number 9619IPRC contribution number 1186ESMC number 103
文摘The occurrence of first hurricane in early summer signifies the onset of an active Atlantic hurricane season.The interannual variation of this hurricane onset date is examined for the period 1979-2013.It is found that the onset date has a marked interannual variation.The standard deviation of the interannual variation of the onset day is 17.5 days,with the climatological mean onset happening on July 23.A diagnosis of tropical cyclone（TC） genesis potential index（GPI） indicates that the major difference between an early and a late onset group lies in the maximum potential intensity（MPI）.A further diagnosis of the MPI shows that it is primarily controlled by the local SST anomaly（SSTA）.Besides the SSTA,vertical shear and mid-tropospheric relative humidity anomalies also contribute significantly to the GPI difference between the early and late onset groups.It is found that the anomalous warm（cold） SST over the tropical Atlantic,while uncorrected with the Nino3 index,persists from the preceding winter to concurrent summer in the early（late） onset group.The net surface heat flux anomaly always tends to damp the SSTA,which suggests that ocean dynamics may play a role in maintaining the SSTA in the tropical Atlantic.The SSTA pattern with a maximum center in northeastern tropical Atlantic appears responsible for generating the observed wind and moisture anomalies over the main TC development region.A further study is needed to understand the initiation mechanism of the SSTA in the Atlantic.
文摘目的:探讨碱性成纤维细胞生长因子(bFGF)对难治性突发性聋的疗效。方法:将208例(266耳)接受正规疗程治疗后,疗效不显著或不满意而有意继续接受治疗,病程在4个月内的突发性聋患者,按照就诊先后顺序分成治疗组104例(135耳)和对照组104例(131耳)。治疗组肌注bFGF4000u,qd,连用15～30d;对照组用维生素B_1100mg加维生素B_(12)500μg混合肌注,或B族维生素口服,qd,连用15d。治疗前后均行纯音电测听及脑干听觉诱发电位。结果:治疗前听阈治疗组为(58.36±27.58)dB pe SPL,对照组为(59.82±28.45)dB pe SPL(P>0.05);治疗后治疗组听阈为(41.89±23.45)dB pe SPL,对照组为(56.73±33.15)dB pe SPL(P<0.01)。有效率治疗组为97%,对照组为38.9%,差异有显著性(P<0.01)。结论:bFGF治疗突发性聋有较大的治疗时间窗,疗效可靠、显著。
