Hydrogen peroxide(H_(2)O_(2))production by the electrochemical 2-electron oxygen reduction reaction(2e−ORR)is a promising alternative to the energy-intensive anthraquinone process,and single-atom electrocatalysts show...Hydrogen peroxide(H_(2)O_(2))production by the electrochemical 2-electron oxygen reduction reaction(2e−ORR)is a promising alternative to the energy-intensive anthraquinone process,and single-atom electrocatalysts show the unique capability of high selectivity toward 2e−ORR against the 4e−one.The extremely low surface density of the single-atom sites and the inflexibility in manipulating their geometric/electronic configurations,however,compromise the H_(2)O_(2) yield and impede further performance enhancement.Herein,we construct a family of multiatom catalysts(MACs),on which two or three single atoms are closely coordinated to form high-density active sites that are versatile in their atomic configurations for optimal adsorption of essential*OOH species.Among them,the Cox–Ni MAC presents excellent electrocatalytic performance for 2e−ORR,in terms of its exceptionally high H_(2)O_(2) yield in acidic electrolytes(28.96 mol L^(−1) gcat.^(−1) h^(−1))and high selectivity under acidic to neutral conditions in a wide potential region(>80%,0–0.7 V).Operando X-ray absorption and density functional theory analyses jointly unveil its unique trimetallic Co2NiN8 configuration,which efficiently induces an appropriate Ni–d orbital filling and modulates the*OOH adsorption,together boosting the electrocatalytic 2e−ORR capability.This work thus provides a new MAC strategy for tuning the geometric/electronic structure of active sites for 2e−ORR and other potential electrochemical processes.展开更多
目的采用三维有限元数值模拟方法分析比较骨水泥棒外固定支架与交叉克氏针在力学稳定性方面的差异,为手术治疗第五掌骨颈骨折(特别是第五掌骨颈开放性骨折)提供理论依据。方法选取1名健康志愿者,采集其手腕关节的三维CT图像数据,首先利...目的采用三维有限元数值模拟方法分析比较骨水泥棒外固定支架与交叉克氏针在力学稳定性方面的差异,为手术治疗第五掌骨颈骨折(特别是第五掌骨颈开放性骨折)提供理论依据。方法选取1名健康志愿者,采集其手腕关节的三维CT图像数据,首先利用Mimics Research 21.0、Geomagic Studio 2021软件进行三维图形数据处理,在此基础上应用Solidworks 2020软件构建第五掌骨颈骨折骨水泥棒外固定支架模型(A模型)和第五掌骨颈骨折交叉克氏针固定模型(B模型)。在ANSYS Workbench 17.0中对各模型的材料属性进行赋值、划分网格,建立三维有限元模型。最后通过在第五掌骨头远端关节面进行轴向施加和第五掌骨三点弯曲实验,计算得出两种施压方式的远端骨折块的最大位移,以此评价骨水泥棒外固定支架治疗第五掌骨颈骨折的稳定性。结果(1)轴向施压时,A模型远端骨折块的最大位移、最小位移和平均位移的值大于B模型,A模型近端骨折块的最大位移、最小位移和平均位移的值小于B模型,A模型最大相对位移、最小相对位移和平均相对位移大于B模型。(2)在三点折弯给力时,A模型远端骨折块最大位移小于B模型,远端骨折块最小位移等于B模型,近端骨折块的最大位移和最小位移的均值大于B模型,A模型最大相对位移、最小相对位移和平均相对位移大于B模型。(3)与B模型相比较,A模型的总体应力、固定物应力均明显较小。结论骨水泥棒外固定支架及克氏针交叉固定在治疗第五掌骨颈骨折方面,在轴向和纵向上的位移及总位移均未超过1 mm,差异较小;但骨水泥棒外固定支架在两种施力方式中与交叉克氏针相比应力更小,提示骨水泥棒外固定支架能提供可靠的力学稳定性。展开更多
基金supported by the tight oil development demonstration project of Ordos basin in China(2017 ZX05069)the key scientifi c research program of Shaanxi provincial department of education(20JY056).
基金supported by the Natural Science Foundation of China(Grant Nos.22179093,21905202,and 51972312)the Natural Science Foundation of Liaoning Province,China(Grant No.2020-MS-003)+1 种基金the Australian Research Council through the Discovery Project(No.DP210102215)the Electron Microscopy Center in the University of Wollongong.The theoretical calculations performed in this work were carried out on TianHe-1(A)at the National Supercomputer Center in Tianjin.
文摘Hydrogen peroxide(H_(2)O_(2))production by the electrochemical 2-electron oxygen reduction reaction(2e−ORR)is a promising alternative to the energy-intensive anthraquinone process,and single-atom electrocatalysts show the unique capability of high selectivity toward 2e−ORR against the 4e−one.The extremely low surface density of the single-atom sites and the inflexibility in manipulating their geometric/electronic configurations,however,compromise the H_(2)O_(2) yield and impede further performance enhancement.Herein,we construct a family of multiatom catalysts(MACs),on which two or three single atoms are closely coordinated to form high-density active sites that are versatile in their atomic configurations for optimal adsorption of essential*OOH species.Among them,the Cox–Ni MAC presents excellent electrocatalytic performance for 2e−ORR,in terms of its exceptionally high H_(2)O_(2) yield in acidic electrolytes(28.96 mol L^(−1) gcat.^(−1) h^(−1))and high selectivity under acidic to neutral conditions in a wide potential region(>80%,0–0.7 V).Operando X-ray absorption and density functional theory analyses jointly unveil its unique trimetallic Co2NiN8 configuration,which efficiently induces an appropriate Ni–d orbital filling and modulates the*OOH adsorption,together boosting the electrocatalytic 2e−ORR capability.This work thus provides a new MAC strategy for tuning the geometric/electronic structure of active sites for 2e−ORR and other potential electrochemical processes.
文摘目的采用三维有限元数值模拟方法分析比较骨水泥棒外固定支架与交叉克氏针在力学稳定性方面的差异,为手术治疗第五掌骨颈骨折(特别是第五掌骨颈开放性骨折)提供理论依据。方法选取1名健康志愿者,采集其手腕关节的三维CT图像数据,首先利用Mimics Research 21.0、Geomagic Studio 2021软件进行三维图形数据处理,在此基础上应用Solidworks 2020软件构建第五掌骨颈骨折骨水泥棒外固定支架模型(A模型)和第五掌骨颈骨折交叉克氏针固定模型(B模型)。在ANSYS Workbench 17.0中对各模型的材料属性进行赋值、划分网格,建立三维有限元模型。最后通过在第五掌骨头远端关节面进行轴向施加和第五掌骨三点弯曲实验,计算得出两种施压方式的远端骨折块的最大位移,以此评价骨水泥棒外固定支架治疗第五掌骨颈骨折的稳定性。结果(1)轴向施压时,A模型远端骨折块的最大位移、最小位移和平均位移的值大于B模型,A模型近端骨折块的最大位移、最小位移和平均位移的值小于B模型,A模型最大相对位移、最小相对位移和平均相对位移大于B模型。(2)在三点折弯给力时,A模型远端骨折块最大位移小于B模型,远端骨折块最小位移等于B模型,近端骨折块的最大位移和最小位移的均值大于B模型,A模型最大相对位移、最小相对位移和平均相对位移大于B模型。(3)与B模型相比较,A模型的总体应力、固定物应力均明显较小。结论骨水泥棒外固定支架及克氏针交叉固定在治疗第五掌骨颈骨折方面,在轴向和纵向上的位移及总位移均未超过1 mm,差异较小;但骨水泥棒外固定支架在两种施力方式中与交叉克氏针相比应力更小,提示骨水泥棒外固定支架能提供可靠的力学稳定性。
