BACKGROUND Liver transplantation aims to increase the survival of patients with end-stage liver diseases and improve their quality of life.The number of organs available for transplantation is lower than the demand.To...BACKGROUND Liver transplantation aims to increase the survival of patients with end-stage liver diseases and improve their quality of life.The number of organs available for transplantation is lower than the demand.To provide fair organ distribution,predictive mortality scores have been developed.AIM To compare the Acute Physiology and Chronic Health Evaluation IV(APACHE IV),balance of risk(BAR),and model for end-stage liver disease(MELD)scores as predictors of mortality.METHODS Retrospective cohort study,which included 283 adult patients in the postoperative period of deceased donor liver transplantation from 2014 to 2018.RESULTS The transplant recipients were mainly male,with a mean age of 58.1 years.Donors were mostly male,with a mean age of 41.6 years.The median cold ischemia time was 3.1 hours,and the median intensive care unit stay was 5 days.For APACHE IV,a mean of 59.6 was found,BAR 10.7,and MELD 24.2.The 28-day mortality rate was 9.5%,and at 90 days,it was 3.5%.The 28-day mortality prediction for APACHE IV was very good[area under the curve(AUC):0.85,P<0.001,95%CI:0.76-0.94],P<0.001,BAR(AUC:0.70,P<0.001,95%CI:0.58–0.81),and MELD(AUC:0.66,P<0.006,95%CI:0.55-0.78),P<0.008.At 90 days,the data for APACHE IV were very good(AUC:0.80,P<0.001,95%CI:0.71–0.90)and moderate for BAR and MELD,respectively,(AUC:0.66,P<0.004,95%CI:0.55–0.77),(AUC:0.62,P<0.026,95%CI:0.51–0.72).All showed good discrimination between deaths and survivors.As for the best value for liver transplantation,it was significant only for APACHE IV(P<0.001).CONCLUSION The APACHE IV assessment score was more accurate than BAR and MELD in predicting mortality in deceased donor liver transplant recipients.展开更多
目的:鉴于脓毒症的高发病率和高病死率,早期识别高风险患者并及时干预至关重要,而现有死亡风险预测模型在操作、适用性和预测长期预后等方面均存在不足。本研究旨在探讨脓毒症患者死亡的危险因素,构建近期和远期死亡风险预测模型。方法...目的:鉴于脓毒症的高发病率和高病死率,早期识别高风险患者并及时干预至关重要,而现有死亡风险预测模型在操作、适用性和预测长期预后等方面均存在不足。本研究旨在探讨脓毒症患者死亡的危险因素,构建近期和远期死亡风险预测模型。方法:从美国重症监护医学信息数据库IV(Medical Information Mart for Intensive Care-IV,MIMIC-IV)中选取符合脓毒症3.0诊断标准的人群,按7?3的比例随机分为建模组和验证组,分析患者的基线资料。采用单因素Cox回归分析和全子集回归确定脓毒症患者死亡的危险因素并筛选出构建预测模型的变量。分别用时间依赖性曲线下面积(area under the curve,AUC)、校准曲线和决策曲线评估模型的区分度、校准度和临床实用性。结果:共纳入14240例脓毒症患者,28 d和1年病死率分别为21.45%(3054例)和36.50%(5198例)。高龄、女性、高感染相关器官衰竭评分(sepsis-related organ failure assessment,SOFA)、高简明急性生理学评分(simplified acute physiology score II,SAPS II)、心率快、呼吸频率快、脓毒症休克、充血性心力衰竭、慢性阻塞性肺疾病、肝脏疾病、肾脏疾病、糖尿病、恶性肿瘤、高白细胞计数(white blood cell count,WBC)、长凝血酶原时间(prothrombin time,PT)、高血肌酐(serum creatinine,SCr)水平均为脓毒症死亡的危险因素(均P<0.05)。由PT、呼吸频率、体温、合并恶性肿瘤、合并肝脏疾病、脓毒症休克、SAPS II及年龄8个变量构建的模型,其28 d和1年生存的AUC分别为0.717(95%CI 0.710~0.724)和0.716(95%CI 0.707~0.725)。校准曲线和决策曲线表明该模型具有良好的校准度及较好的临床应用价值。结论:基于MIMIC-IV建立的脓毒症患者近期和远期死亡风险预测模型有较好的识别能力,对患者预后风险评估及干预治疗具有一定的临床参考意义。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
At the second order Douglas–Kroll–Hess(DKH2) level, the B3 PW91 functional in conjunction with the relativistic all-electron basis set of valence triple zeta quality plus polarization functions are employed to com...At the second order Douglas–Kroll–Hess(DKH2) level, the B3 PW91 functional in conjunction with the relativistic all-electron basis set of valence triple zeta quality plus polarization functions are employed to compute bond lengths, dissociation energies, vertical ionization potentials, and the highest occupied molecular orbital-lowest unoccupied molecular orbital energy gaps of the small iridium clusters(Irn, n≤8). These results are compared with the experimental and theoretical data available in the literature. Our results confirm the theoretical predictions made by Feng et al. about the catalytic activities of the Ir4 and Ir6 clusters. From the optimized geometries, DKH2 calculations of static electric mean dipole polarizabilities and polarizability anisotropies are also carried out. It is the first time that the polarizabilities of small iridium clusters have been studied. For n≤4, the mean dipole polarizabilities per atom present an odd–even oscillatory behavior,whereas from Ir5 to Ir8, they decrease with the cluster size increasing. The dependence of the polarizability anisotropy on the structure symmetry of the iridium cluster is verified.展开更多
Iridium dioxide with different morphologies(nanorod and nanogranular) is successfully prepared by a modified sol-gel and Adams methods. The catalytic activity of both samples for oxygen reduction reaction is investiga...Iridium dioxide with different morphologies(nanorod and nanogranular) is successfully prepared by a modified sol-gel and Adams methods. The catalytic activity of both samples for oxygen reduction reaction is investigated in an alkaline solution. The electrochemical results show that the catalytic activity of the nanogranular Ir O2 sample is superior to that of the nanorod sample due to its higher onset potential for oxygen reduction reaction and higher electrode current density in low potential region. The results of Koutecky-Levich analysis indicate that the oxygen reduction reaction catalyzed by both samples is a mixture transfer pathway. It is dominated by four electron transfer pathway for both samples in high overpotential area, while it is controlled by two electron transfer process for both samples in low overpotential area.展开更多
A novel iridium-complex,(BPPBI) 2 Ir(2-TFDBC)[BPPBI=2-(biphenyl-4-yl)-1-phenyl-1H-benzo[d]imidazole,2-TFDBC=1-(9-ethyl-9H-carbazol-2-yl)-4,4,4-trifluorobutane-1,3-dione],was synthesized,and its structure and c...A novel iridium-complex,(BPPBI) 2 Ir(2-TFDBC)[BPPBI=2-(biphenyl-4-yl)-1-phenyl-1H-benzo[d]imidazole,2-TFDBC=1-(9-ethyl-9H-carbazol-2-yl)-4,4,4-trifluorobutane-1,3-dione],was synthesized,and its structure and component were confirmed by 1 H NMR and element analysis,respectively.UV-Vis absorption and photoluminescent(PL) spectra of(BPPBI) 2 Ir(2-TFDBC) in dichloromethane were investigated.The Ir-complex exhibited a long wavelength excitation of 470 nm,i.e.,low-energy excitation.So,it is a promising candidate for phosphorescent probe and PL material.(BPPBI) 2 Ir(2-TFDBC)-based electroluminescent devices,ITO/MoO 3(10 nm)/NPB(80 nm)/CBP:x(BPPBI) 2 Ir(2-TFDBC)(20 nm)/TPBi(45 nm)/LiF/Al,were fabricated,where x(%) was of 4% or 8% doping concentration(mass fraction);ITO=indium tin oxides;NBP=N,N'-bis-(1-naphthalenyl)-N,N'-bis-phenyl-(1,1'-biphenyl)4,4'-diamine,CBP=4,4'-bis(N-carbazolyl)-1,1'-biphenyl,TPBi=1,3,5-tris(1-phenyl-1H-benzimidazol-2-yl)benzene.The devices showed a red emission of 620 nm.The maximum current efficiency and brightness were 1.7 cd/A and 4063 cd/m 2 for a device of 8%(mass fraction) doping level,respectively.The moderate luminous efficiency was due to the inadequate energy transfer from the host material to the guest material.展开更多
Iridium oxide (IrOx) has attracted much attention for neural interface applications due to its ability to transfer between ionic and electronic current and to resist corrosion. The physical, mechanical, chemical, elec...Iridium oxide (IrOx) has attracted much attention for neural interface applications due to its ability to transfer between ionic and electronic current and to resist corrosion. The physical, mechanical, chemical, electrical and optical properties of thin films depend on the method and parameters used to deposit the films. In this report, the surface morphology, impedance and charge capacity of activated iridium oxide film (AIROF) and sputtered iridium oxide film (SIROF) were investigated in vitro and compared. The Utah Electrode Array (UEA) having similar electrode area and shape were employed in this study. The electrode coated with AIROF and SIROF were characterized by scanning electron microcopy, cyclic voltammetry, electrochemical impedance spectroscopy and potential transient measurements to measure charge injection capacity (CIC). SIROF and AIROF selectively deposited on electrode tip had dendrite and granular microstructure, respectively. The CIC of unbiased SIROF and AIROF was found to be 2 and 1 mC/cm2, respectively, which is comparable to other published values. The average impedance, at a frequency of 1 kHz was ~65 and ~7 kΩ for the AIROF and SIROF, respectively. Low impedance and high CIC makes SIROF highly recommended stimulation and recording material.展开更多
Electrocatalytic nitrogen reduction reaction(NRR)is considered as a promising candidate to achieve ammonia synthesis because of clean electric energy,moderate reaction condition,safe operating process and harmless by-...Electrocatalytic nitrogen reduction reaction(NRR)is considered as a promising candidate to achieve ammonia synthesis because of clean electric energy,moderate reaction condition,safe operating process and harmless by-products.However,the chemical inertness of nitrogen and poor activated capacity on catalyst surface usually produce low ammonia yield and faradic efficiency.Herein,the microfluidic technology is proposed to efficiently fabricate enriched iridium nanodots/carbon architecture.Owing to in-situ co-precipitation reaction and microfluidic manipulation,the iridium nanodots/carbon nanomaterials possess small average size,uniform dispersion,high conductivity and abundant active sites,producing good proton activation and rapid electrons transmission and moderate adsorption/desorption capacity.As a result,the as-prepared iridium nanodots/carbon nanomaterials realize large ammonia yield of 28.73 μg h^(-1) cm^(-2) and faradic efficiency of 9.14%in KOH solution.Moreover,the high ammonia yield of 11.21 μg h^(-1) cm^(-2) and faradic efficiency of 24.30%are also achieved in H_(2)SO_(4) solution.The microfluidic method provides a reference for large-scale fabrication of nano-sized catalyst materials,which may accelerate the progress of electrocatalytic NRR in industrialization field.展开更多
Developing active and durable electrocatalysts for overall water splitting is desirable but challenging to realize sustainable hydrogen production.Here,we report a facile and general method to prepare ultrafine nickel...Developing active and durable electrocatalysts for overall water splitting is desirable but challenging to realize sustainable hydrogen production.Here,we report a facile and general method to prepare ultrafine nickel(Ni)-iridium(Ir)alloy nanoparticles/graphene hybrids for overall water splitting.The optimized hybrid with 4.9 wt%Ir exhibits much higher catalytic activity and durability than commercial 20 wt%Ir/C for both oxygen evolution reaction(OER)and hydrogen evolution reaction(HER).Theoretical simulations reveal that the incorporation of Ir in metallic Ni lattice regulates hydrogen adsorption free energy to the optimum level,thus improving HER activity,while in situ generated amorphous Ir-Ni hydr(oxy)oxides around metallic Ni-Ir core have been demonstrated to be the active species under OER conditions,which switches OER rate-determining step to energy-favorable pathway.The overall water splitting electrolyzer assembled by the optimized electrocatalyst shows a low cell voltage of only 1.52 V and excellent stability to deliver a current density of 10 m A cm-2.This work provides a powerful strategy toward general synthesis of ultrafine alloy nanoparticles for high-performance overall water splitting.展开更多
Since low overpotential for the anodic ethanol oxidation reaction(EOR)can favor the higher output voltage and power of direct ethanol fuel cells(DEFCs),it is critical to design new EOR catalysts with efficient ethanol...Since low overpotential for the anodic ethanol oxidation reaction(EOR)can favor the higher output voltage and power of direct ethanol fuel cells(DEFCs),it is critical to design new EOR catalysts with efficient ethanol-to-CO_(2)activity at low applied potentials.Thereby,carbon-supported Ir-Bi_(2)O_(3)(Ir-Bi_(2)O_(3)/C)catalysts with highly dispersive bismuth oxide on the iridium surface are designed and prepared,which can merit splitting the ethanol C–C bond and promoting the oxidation of C1 intermediates at the bifunctional interfaces.The as-obtained Ir-Bi2O3/C catalysts show superior EOR mass activity of up to ca.2250 m A mgIr-1.Moreover,they exhibit the record lowest onset oxidation potentials(0.17–0.22 V vs.RHE)and the peak potential(ca.0.58 V vs.RHE),being 130–300 m V lower than the previous landmark noble metallic catalysts.Furthermore,an apparent C1 pathway faraday efficiency(FEC1)of 28%±5.9%at 0.5 V vs.RHE can be obtained at Ir-Bi_(2)O_(3)/C.This work might provide new insights into the new anodic EOR catalysts for increasing the power of DEFCs.展开更多
A systematic study on the structure sensitivity,host effect,and the deactivation mechanism of Ircatalyzed selective hydrogenation of 1,3-butadiene,a key process in the purification of alkadiene for the upgrading of C4...A systematic study on the structure sensitivity,host effect,and the deactivation mechanism of Ircatalyzed selective hydrogenation of 1,3-butadiene,a key process in the purification of alkadiene for the upgrading of C4 cut,is presented by coupling steady-state catalytic testing,in-depth characterization,kinetic evaluation,and density functional theory calculations.We reveal that:(i) 1,3-Butadiene hydrogenation on iridium is structure-sensitive with the optimal particle size of about 2 nm,and the H_(2) dissociation energy is a reliable activity descriptor;(ii) The nature of the NC hosts exerts a critical impact on the catalytic performance,and balanced nitrogen content and speciation seem key for the optimized performance;and (iii) Different deactivation mechanisms occur:fouling by coke deposition on the catalysts with a high N:C ratio (>1),and site blockage due to the competitive adsorption between 1-butene/cis-2-butene and 1,3-butadiene.These molecular insights provide valuable guidelines for the catalyst design in selective hydrogenations.展开更多
To discuss the potential role of iridium(Ir)nanoparticles loaded under atmospheric and high pressures,we prepared a series of cata-lysts with the same active phase but different contents of 10wt%,20wt%,and 30wt%on gam...To discuss the potential role of iridium(Ir)nanoparticles loaded under atmospheric and high pressures,we prepared a series of cata-lysts with the same active phase but different contents of 10wt%,20wt%,and 30wt%on gamma-alumina for decomposition of hydrazine.Un-der atmospheric pressure,the performance of the catalyst was better when 30wt%of the Ir nanoparticles was used with chelating agent that had greater selectivity of approximately 27%.The increase in the reaction rate from 175 to 220 h^(−1)at higher Ir loading(30wt%)was due to a good dispersion of high-number active phases rather than an agglomeration surface.As a satisfactory result of this investigation at high pressure,Ir catalysts with different weight percentages showed the same stability against crushing and activity with a characteristic velocity of approxim-ately 1300 m/s.展开更多
文摘BACKGROUND Liver transplantation aims to increase the survival of patients with end-stage liver diseases and improve their quality of life.The number of organs available for transplantation is lower than the demand.To provide fair organ distribution,predictive mortality scores have been developed.AIM To compare the Acute Physiology and Chronic Health Evaluation IV(APACHE IV),balance of risk(BAR),and model for end-stage liver disease(MELD)scores as predictors of mortality.METHODS Retrospective cohort study,which included 283 adult patients in the postoperative period of deceased donor liver transplantation from 2014 to 2018.RESULTS The transplant recipients were mainly male,with a mean age of 58.1 years.Donors were mostly male,with a mean age of 41.6 years.The median cold ischemia time was 3.1 hours,and the median intensive care unit stay was 5 days.For APACHE IV,a mean of 59.6 was found,BAR 10.7,and MELD 24.2.The 28-day mortality rate was 9.5%,and at 90 days,it was 3.5%.The 28-day mortality prediction for APACHE IV was very good[area under the curve(AUC):0.85,P<0.001,95%CI:0.76-0.94],P<0.001,BAR(AUC:0.70,P<0.001,95%CI:0.58–0.81),and MELD(AUC:0.66,P<0.006,95%CI:0.55-0.78),P<0.008.At 90 days,the data for APACHE IV were very good(AUC:0.80,P<0.001,95%CI:0.71–0.90)and moderate for BAR and MELD,respectively,(AUC:0.66,P<0.004,95%CI:0.55–0.77),(AUC:0.62,P<0.026,95%CI:0.51–0.72).All showed good discrimination between deaths and survivors.As for the best value for liver transplantation,it was significant only for APACHE IV(P<0.001).CONCLUSION The APACHE IV assessment score was more accurate than BAR and MELD in predicting mortality in deceased donor liver transplant recipients.
文摘目的:鉴于脓毒症的高发病率和高病死率,早期识别高风险患者并及时干预至关重要,而现有死亡风险预测模型在操作、适用性和预测长期预后等方面均存在不足。本研究旨在探讨脓毒症患者死亡的危险因素,构建近期和远期死亡风险预测模型。方法:从美国重症监护医学信息数据库IV(Medical Information Mart for Intensive Care-IV,MIMIC-IV)中选取符合脓毒症3.0诊断标准的人群,按7?3的比例随机分为建模组和验证组,分析患者的基线资料。采用单因素Cox回归分析和全子集回归确定脓毒症患者死亡的危险因素并筛选出构建预测模型的变量。分别用时间依赖性曲线下面积(area under the curve,AUC)、校准曲线和决策曲线评估模型的区分度、校准度和临床实用性。结果:共纳入14240例脓毒症患者,28 d和1年病死率分别为21.45%(3054例)和36.50%(5198例)。高龄、女性、高感染相关器官衰竭评分(sepsis-related organ failure assessment,SOFA)、高简明急性生理学评分(simplified acute physiology score II,SAPS II)、心率快、呼吸频率快、脓毒症休克、充血性心力衰竭、慢性阻塞性肺疾病、肝脏疾病、肾脏疾病、糖尿病、恶性肿瘤、高白细胞计数(white blood cell count,WBC)、长凝血酶原时间(prothrombin time,PT)、高血肌酐(serum creatinine,SCr)水平均为脓毒症死亡的危险因素(均P<0.05)。由PT、呼吸频率、体温、合并恶性肿瘤、合并肝脏疾病、脓毒症休克、SAPS II及年龄8个变量构建的模型,其28 d和1年生存的AUC分别为0.717(95%CI 0.710~0.724)和0.716(95%CI 0.707~0.725)。校准曲线和决策曲线表明该模型具有良好的校准度及较好的临床应用价值。结论:基于MIMIC-IV建立的脓毒症患者近期和远期死亡风险预测模型有较好的识别能力,对患者预后风险评估及干预治疗具有一定的临床参考意义。
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supported by the CNPq,CAPES,and FAPES(Brazilian Agencies)
文摘At the second order Douglas–Kroll–Hess(DKH2) level, the B3 PW91 functional in conjunction with the relativistic all-electron basis set of valence triple zeta quality plus polarization functions are employed to compute bond lengths, dissociation energies, vertical ionization potentials, and the highest occupied molecular orbital-lowest unoccupied molecular orbital energy gaps of the small iridium clusters(Irn, n≤8). These results are compared with the experimental and theoretical data available in the literature. Our results confirm the theoretical predictions made by Feng et al. about the catalytic activities of the Ir4 and Ir6 clusters. From the optimized geometries, DKH2 calculations of static electric mean dipole polarizabilities and polarizability anisotropies are also carried out. It is the first time that the polarizabilities of small iridium clusters have been studied. For n≤4, the mean dipole polarizabilities per atom present an odd–even oscillatory behavior,whereas from Ir5 to Ir8, they decrease with the cluster size increasing. The dependence of the polarizability anisotropy on the structure symmetry of the iridium cluster is verified.
基金Funded by the Major State Basic Research Development Program of China(973 Program)(No.2012CB215504)the National Natural Science Foundation of China(No.50632050)+1 种基金the Doctoral Fund of Ministry of Education of China(No.20130143130001)Hubei Provincial Key Laboratory of Fuel Cell(2015FCJ001)
文摘Iridium dioxide with different morphologies(nanorod and nanogranular) is successfully prepared by a modified sol-gel and Adams methods. The catalytic activity of both samples for oxygen reduction reaction is investigated in an alkaline solution. The electrochemical results show that the catalytic activity of the nanogranular Ir O2 sample is superior to that of the nanorod sample due to its higher onset potential for oxygen reduction reaction and higher electrode current density in low potential region. The results of Koutecky-Levich analysis indicate that the oxygen reduction reaction catalyzed by both samples is a mixture transfer pathway. It is dominated by four electron transfer pathway for both samples in high overpotential area, while it is controlled by two electron transfer process for both samples in low overpotential area.
基金Supported by the Natural Science Foundation of Guangdong Province,China(No.10152404801000017)
文摘A novel iridium-complex,(BPPBI) 2 Ir(2-TFDBC)[BPPBI=2-(biphenyl-4-yl)-1-phenyl-1H-benzo[d]imidazole,2-TFDBC=1-(9-ethyl-9H-carbazol-2-yl)-4,4,4-trifluorobutane-1,3-dione],was synthesized,and its structure and component were confirmed by 1 H NMR and element analysis,respectively.UV-Vis absorption and photoluminescent(PL) spectra of(BPPBI) 2 Ir(2-TFDBC) in dichloromethane were investigated.The Ir-complex exhibited a long wavelength excitation of 470 nm,i.e.,low-energy excitation.So,it is a promising candidate for phosphorescent probe and PL material.(BPPBI) 2 Ir(2-TFDBC)-based electroluminescent devices,ITO/MoO 3(10 nm)/NPB(80 nm)/CBP:x(BPPBI) 2 Ir(2-TFDBC)(20 nm)/TPBi(45 nm)/LiF/Al,were fabricated,where x(%) was of 4% or 8% doping concentration(mass fraction);ITO=indium tin oxides;NBP=N,N'-bis-(1-naphthalenyl)-N,N'-bis-phenyl-(1,1'-biphenyl)4,4'-diamine,CBP=4,4'-bis(N-carbazolyl)-1,1'-biphenyl,TPBi=1,3,5-tris(1-phenyl-1H-benzimidazol-2-yl)benzene.The devices showed a red emission of 620 nm.The maximum current efficiency and brightness were 1.7 cd/A and 4063 cd/m 2 for a device of 8%(mass fraction) doping level,respectively.The moderate luminous efficiency was due to the inadequate energy transfer from the host material to the guest material.
文摘Iridium oxide (IrOx) has attracted much attention for neural interface applications due to its ability to transfer between ionic and electronic current and to resist corrosion. The physical, mechanical, chemical, electrical and optical properties of thin films depend on the method and parameters used to deposit the films. In this report, the surface morphology, impedance and charge capacity of activated iridium oxide film (AIROF) and sputtered iridium oxide film (SIROF) were investigated in vitro and compared. The Utah Electrode Array (UEA) having similar electrode area and shape were employed in this study. The electrode coated with AIROF and SIROF were characterized by scanning electron microcopy, cyclic voltammetry, electrochemical impedance spectroscopy and potential transient measurements to measure charge injection capacity (CIC). SIROF and AIROF selectively deposited on electrode tip had dendrite and granular microstructure, respectively. The CIC of unbiased SIROF and AIROF was found to be 2 and 1 mC/cm2, respectively, which is comparable to other published values. The average impedance, at a frequency of 1 kHz was ~65 and ~7 kΩ for the AIROF and SIROF, respectively. Low impedance and high CIC makes SIROF highly recommended stimulation and recording material.
基金supported by the National Natural Science Foundation of China(22025801)and(22208190)National Postdoctoral Program for Innovative Talents(BX2021146)Shuimu Tsinghua Scholar Program(2021SM055).
文摘Electrocatalytic nitrogen reduction reaction(NRR)is considered as a promising candidate to achieve ammonia synthesis because of clean electric energy,moderate reaction condition,safe operating process and harmless by-products.However,the chemical inertness of nitrogen and poor activated capacity on catalyst surface usually produce low ammonia yield and faradic efficiency.Herein,the microfluidic technology is proposed to efficiently fabricate enriched iridium nanodots/carbon architecture.Owing to in-situ co-precipitation reaction and microfluidic manipulation,the iridium nanodots/carbon nanomaterials possess small average size,uniform dispersion,high conductivity and abundant active sites,producing good proton activation and rapid electrons transmission and moderate adsorption/desorption capacity.As a result,the as-prepared iridium nanodots/carbon nanomaterials realize large ammonia yield of 28.73 μg h^(-1) cm^(-2) and faradic efficiency of 9.14%in KOH solution.Moreover,the high ammonia yield of 11.21 μg h^(-1) cm^(-2) and faradic efficiency of 24.30%are also achieved in H_(2)SO_(4) solution.The microfluidic method provides a reference for large-scale fabrication of nano-sized catalyst materials,which may accelerate the progress of electrocatalytic NRR in industrialization field.
基金supported by the National Natural Science Foundation of China(21671039 and 21673241)Natural Science Foundation of Fujian Province(2015J01038)New Century Excellent Talents in Fujian Province University,State Key Laboratory of Structural Chemistry and Program for Innovative Research Team in Science and Technology in Fujian Province University(IRTSTFJ)。
文摘Developing active and durable electrocatalysts for overall water splitting is desirable but challenging to realize sustainable hydrogen production.Here,we report a facile and general method to prepare ultrafine nickel(Ni)-iridium(Ir)alloy nanoparticles/graphene hybrids for overall water splitting.The optimized hybrid with 4.9 wt%Ir exhibits much higher catalytic activity and durability than commercial 20 wt%Ir/C for both oxygen evolution reaction(OER)and hydrogen evolution reaction(HER).Theoretical simulations reveal that the incorporation of Ir in metallic Ni lattice regulates hydrogen adsorption free energy to the optimum level,thus improving HER activity,while in situ generated amorphous Ir-Ni hydr(oxy)oxides around metallic Ni-Ir core have been demonstrated to be the active species under OER conditions,which switches OER rate-determining step to energy-favorable pathway.The overall water splitting electrolyzer assembled by the optimized electrocatalyst shows a low cell voltage of only 1.52 V and excellent stability to deliver a current density of 10 m A cm-2.This work provides a powerful strategy toward general synthesis of ultrafine alloy nanoparticles for high-performance overall water splitting.
基金supported by the National Natural Science Foundation of China(NSFC,22172121)the Natural Science Foundation of Sichuan Province(NSFSC,2023NSFSC1076)+1 种基金the Young Talent Project of State Ethnic Affairs Commissionthe Fundamental Research Funds for the Central Universities(ZYN2023106),Southwest Minzu University。
文摘Since low overpotential for the anodic ethanol oxidation reaction(EOR)can favor the higher output voltage and power of direct ethanol fuel cells(DEFCs),it is critical to design new EOR catalysts with efficient ethanol-to-CO_(2)activity at low applied potentials.Thereby,carbon-supported Ir-Bi_(2)O_(3)(Ir-Bi_(2)O_(3)/C)catalysts with highly dispersive bismuth oxide on the iridium surface are designed and prepared,which can merit splitting the ethanol C–C bond and promoting the oxidation of C1 intermediates at the bifunctional interfaces.The as-obtained Ir-Bi2O3/C catalysts show superior EOR mass activity of up to ca.2250 m A mgIr-1.Moreover,they exhibit the record lowest onset oxidation potentials(0.17–0.22 V vs.RHE)and the peak potential(ca.0.58 V vs.RHE),being 130–300 m V lower than the previous landmark noble metallic catalysts.Furthermore,an apparent C1 pathway faraday efficiency(FEC1)of 28%±5.9%at 0.5 V vs.RHE can be obtained at Ir-Bi_(2)O_(3)/C.This work might provide new insights into the new anodic EOR catalysts for increasing the power of DEFCs.
基金Zhejiang Normal University for providing the financial support (YS304320035, YS304320036, ZZ323205020521005039)Financial support from the National Natural Science Foundation of China (NSFC, 21606199)+1 种基金the Science and Technology Department of Zhejiang Province (LGG20B060004)the National Key Research and Development Program of China (2021YFA1501800, 2021YFA1501801, 2021YFA1501802) are also gratefully acknowledged。
文摘A systematic study on the structure sensitivity,host effect,and the deactivation mechanism of Ircatalyzed selective hydrogenation of 1,3-butadiene,a key process in the purification of alkadiene for the upgrading of C4 cut,is presented by coupling steady-state catalytic testing,in-depth characterization,kinetic evaluation,and density functional theory calculations.We reveal that:(i) 1,3-Butadiene hydrogenation on iridium is structure-sensitive with the optimal particle size of about 2 nm,and the H_(2) dissociation energy is a reliable activity descriptor;(ii) The nature of the NC hosts exerts a critical impact on the catalytic performance,and balanced nitrogen content and speciation seem key for the optimized performance;and (iii) Different deactivation mechanisms occur:fouling by coke deposition on the catalysts with a high N:C ratio (>1),and site blockage due to the competitive adsorption between 1-butene/cis-2-butene and 1,3-butadiene.These molecular insights provide valuable guidelines for the catalyst design in selective hydrogenations.
文摘To discuss the potential role of iridium(Ir)nanoparticles loaded under atmospheric and high pressures,we prepared a series of cata-lysts with the same active phase but different contents of 10wt%,20wt%,and 30wt%on gamma-alumina for decomposition of hydrazine.Un-der atmospheric pressure,the performance of the catalyst was better when 30wt%of the Ir nanoparticles was used with chelating agent that had greater selectivity of approximately 27%.The increase in the reaction rate from 175 to 220 h^(−1)at higher Ir loading(30wt%)was due to a good dispersion of high-number active phases rather than an agglomeration surface.As a satisfactory result of this investigation at high pressure,Ir catalysts with different weight percentages showed the same stability against crushing and activity with a characteristic velocity of approxim-ately 1300 m/s.