It is widely recognized that the development of ZABs is impeded by the kinetic bottleneck of oxygen evolution reaction(OER)and oxygen reduction reaction(ORR).The application of conformational entropy strategy to oxide...It is widely recognized that the development of ZABs is impeded by the kinetic bottleneck of oxygen evolution reaction(OER)and oxygen reduction reaction(ORR).The application of conformational entropy strategy to oxides often involves introducing multiple elements with different properties,thereby providing outstanding bifunctional catalytic activity for OER/ORR.Nevertheless,the possible underlying catalytic pathways and potential interactions between various components are still poorly understood.This paper presents an excellent medium-entropy perovskite oxide,Sr(FeCoNiMo)_(1/4)O_(3−δ)(lower overpotential of 301 mV at 10 mA cm^(−2)).Zinc-air batteries employing it as a cathode catalyst demonstrate excellent round-trip efficiency(62%).By combining theoretical calculation with experiments,we aim to establish the link between the electronic structure of perovskite oxides with different elemental compositions and their OER mechanism.Research reveals that the conformational entropy strategy can simultaneously shift the O 2p-band center and metal d-band center of perovskite oxide towards the vicinity of the Fermi energy level,thereby triggering a more favorable lattice oxygen-participated mechanism(LOM)during the OER process.The outcomes of this work provide crucial insights into the role of conformational entropy strategies in oxygen catalysis and offer potential avenues for constructing efficient and stable electrocatalysts.展开更多
1.27μm波段的氧分子近红外气辉是火星大气最重要的气辉辐射之一,该气辉高光谱分辨辐射传输模型的建立对于研制火星探测载荷,反演火星大气的风场温度场与臭氧浓度,以及研究火星空间物理,有重要的科学价值与工程意义.在研究火星大气O_(2)...1.27μm波段的氧分子近红外气辉是火星大气最重要的气辉辐射之一,该气辉高光谱分辨辐射传输模型的建立对于研制火星探测载荷,反演火星大气的风场温度场与臭氧浓度,以及研究火星空间物理,有重要的科学价值与工程意义.在研究火星大气O_(2)(a^(1)Δ_(g))气辉光化学反应模型的基础上,提出了O_(2)(a^(1)Δ_(g))气辉体辐射率的计算方法,并建立了火星大气气辉辐射传输理论;通过与用于研究火星大气特征的光谱学探测仪(Spectroscopy Spectrograph for the Investigation of Characteristics of the Atmosphere of Mars,SPICAM)的实测数据进行对比,验证了所建立的火星O_(2)(a^(1)Δ_(g))气辉高光谱分辨辐射传输模型的准确性;针对火星与地球大气的O_(2)(a^(1)Δ_(g))气辉,在体辐射率、自吸收效应,以及临边辐射光谱特性三个方面进行了系统深入的比较,对比结果表明,火星大气由于密度低、氧气丰度小,其自吸收效应可以忽略不计,但其O_(2)(a^(1)Δ_(g))气辉辐射强度与地球大气相当,可以用于火星大气的风场温度场与臭氧浓度的探测与反演.展开更多
基金the financial support from the National Natural Science Foundation of China (51872067 and 21773048)
文摘It is widely recognized that the development of ZABs is impeded by the kinetic bottleneck of oxygen evolution reaction(OER)and oxygen reduction reaction(ORR).The application of conformational entropy strategy to oxides often involves introducing multiple elements with different properties,thereby providing outstanding bifunctional catalytic activity for OER/ORR.Nevertheless,the possible underlying catalytic pathways and potential interactions between various components are still poorly understood.This paper presents an excellent medium-entropy perovskite oxide,Sr(FeCoNiMo)_(1/4)O_(3−δ)(lower overpotential of 301 mV at 10 mA cm^(−2)).Zinc-air batteries employing it as a cathode catalyst demonstrate excellent round-trip efficiency(62%).By combining theoretical calculation with experiments,we aim to establish the link between the electronic structure of perovskite oxides with different elemental compositions and their OER mechanism.Research reveals that the conformational entropy strategy can simultaneously shift the O 2p-band center and metal d-band center of perovskite oxide towards the vicinity of the Fermi energy level,thereby triggering a more favorable lattice oxygen-participated mechanism(LOM)during the OER process.The outcomes of this work provide crucial insights into the role of conformational entropy strategies in oxygen catalysis and offer potential avenues for constructing efficient and stable electrocatalysts.
文摘1.27μm波段的氧分子近红外气辉是火星大气最重要的气辉辐射之一,该气辉高光谱分辨辐射传输模型的建立对于研制火星探测载荷,反演火星大气的风场温度场与臭氧浓度,以及研究火星空间物理,有重要的科学价值与工程意义.在研究火星大气O_(2)(a^(1)Δ_(g))气辉光化学反应模型的基础上,提出了O_(2)(a^(1)Δ_(g))气辉体辐射率的计算方法,并建立了火星大气气辉辐射传输理论;通过与用于研究火星大气特征的光谱学探测仪(Spectroscopy Spectrograph for the Investigation of Characteristics of the Atmosphere of Mars,SPICAM)的实测数据进行对比,验证了所建立的火星O_(2)(a^(1)Δ_(g))气辉高光谱分辨辐射传输模型的准确性;针对火星与地球大气的O_(2)(a^(1)Δ_(g))气辉,在体辐射率、自吸收效应,以及临边辐射光谱特性三个方面进行了系统深入的比较,对比结果表明,火星大气由于密度低、氧气丰度小,其自吸收效应可以忽略不计,但其O_(2)(a^(1)Δ_(g))气辉辐射强度与地球大气相当,可以用于火星大气的风场温度场与臭氧浓度的探测与反演.
