电解水技术是一种生产高纯氢燃料的方法,能够增强可再生能源发电系统的消纳能力.相较于质子交换膜(PEM)电解槽,碱性(ALK)电解槽可以使用非贵金属基催化电极,拥有更高的经济效益和市场占有率.然而,由于ALK电解槽处于质子稀缺环境,阴极氢...电解水技术是一种生产高纯氢燃料的方法,能够增强可再生能源发电系统的消纳能力.相较于质子交换膜(PEM)电解槽,碱性(ALK)电解槽可以使用非贵金属基催化电极,拥有更高的经济效益和市场占有率.然而,由于ALK电解槽处于质子稀缺环境,阴极氢气演化反应(HER)动力学变得更加复杂,需要快速解离水分子提供动态质子微环境.硫化钼(MoS_(2))纳米片边缘具有合适的质子吸附和演化的活性位点,是制备HER催化剂的潜力材料.但其二维基面原子由于配位饱和,显示出较弱的质子吸附能力.如何调控MoS_(2)基面以实现水解动力与质子吸附演化动力的集成,提升MoS_(2)纳米片的碱性HER活性,具有重要的科学和应用意义.本文提出了一种Co/O双原子植入策略,精准调控双活性位点及其电子结构,实现了水解离动力和质子吸附演化动力的高效耦联.首先,利用刻蚀和电沉积的两步实验法,在MoS_(2)基面上成功引入O和Co原子;随后,结合高分辨透射电镜、高角环形暗场-扫描透射电子显微镜、同步辐射X射线吸收精细结构谱等表征分析技术,精准识别了掺杂Co/O原子的位置和配位情况:O原子替换部分S原子,Co原子占据Mo原子的上方,构建出立体凸起的“O-Co-S_(2)”配位构型.催化在线的原位表征分析结果表明:该独特的“O-Co-S_(2)”原子基序发挥着水解离与氢演化反应协同催化效应.密度泛函理论计算结果也证实了该协同机制,其中Co位点促进水的解离反应,而S位点则有助于质子的转化生成氢气.因此,Co/O掺杂MoS_(2)催化剂(Co-O@MoS_(2))表现出较好的碱性HER活性:仅需81 mV的过电位,即可达到100 mA cm^(‒2)的电流密度,Tafel斜率低至42 mV dec^(‒1),在600 mA cm^(‒2)的高电流密度测试中运行300 h活性无衰减.上述碱性HER性能不仅远高于原始的MoS_(2)纳米片,而且也领先于部分已报道结果.综上所述,本文在MoS_(2)基面上构筑了原子级协同催化活性中心,显著促进了碱性HER反应性能,为原子活化工程开发先进催化剂提供参考,在原子级基序构造、表征和功能分析方面提供借鉴.展开更多
Orbital angular momentum(OAM)conversion is critical in understanding interactions between a structural sound field and a planar lattice.Herein,we explore the evolution of a monochromatic acoustic vortex beam(AVB)that ...Orbital angular momentum(OAM)conversion is critical in understanding interactions between a structural sound field and a planar lattice.Herein,we explore the evolution of a monochromatic acoustic vortex beam(AVB)that is scattered by a phononic crystal(PnC)or a correlated random lattice.The phenomenon is ascribed to the enhanced orbit–orbit angular momentum coupling induced by the band structure.By modifying the coupling condition,accurate and continuous micromanipulation of AVBs can be achieved,including the transverse/lateral gravity shift,the dynamics of the phase singularities,and the spatial distribution of acoustic pressure,etc.This research provides insight to the inhomogeneous coupling of AVBs with both propagating Bloch waves and localized Anderson modes,and may facilitate development of novel OAM-based acoustic devices for active sound field manipulation.展开更多
Highly efficient organic solar cells(OSCs)are normally produced using the halogenated solvents chloroform or chlorobenzene,which present challenges for scalable manufacturing due to their toxicity,narrow processing wi...Highly efficient organic solar cells(OSCs)are normally produced using the halogenated solvents chloroform or chlorobenzene,which present challenges for scalable manufacturing due to their toxicity,narrow processing window and low boiling point.Herein,we develop a novel high-speed doctor-blading technique that significantly reduces the required concentration,facilitating the use of eco-friendly,non-halogenated solvents as alternatives to chloroform or chlorobenzene.By utilizing two widely used high-boiling,non-halogenated green solvents-o-xylene(o-XY)and toluene(Tol)-in the fabrication of PM 6:L 8-BO,we achieve power conversion efficiencies(PCEs)of 18.20%and 17.36%,respectively.Additionally,a module fabricated with o-XY demonstrates a notable PCE of 16.07%.In-situ testing and morphological analysis reveal that the o-XY coating process extends the liquid-to-solid transition stage to 6 s,significantly longer than the 1.7 s observed with Tol processing.This prolonged transition phase is crucial for improving the crystallinity of the thin film,reducing defect-mediated recombination,and enhancing carrier mobility,which collectively contribute to superior PCEs.展开更多
金属锂负极由于比容量高(3860 mAh·g^(-1))及氧化还原电位极低(-3.04 V vs.标准氢气电极(SHE)),被认为是实现高能量密度锂电池的理想负极。然而,金属锂电极与电解液反应剧烈,且锂离子在电极表面沉积不均匀容易产生枝晶,导致其循环...金属锂负极由于比容量高(3860 mAh·g^(-1))及氧化还原电位极低(-3.04 V vs.标准氢气电极(SHE)),被认为是实现高能量密度锂电池的理想负极。然而,金属锂电极与电解液反应剧烈,且锂离子在电极表面沉积不均匀容易产生枝晶,导致其循环稳定性和安全性都较差,限制了其应用推广。我们前期通过构建金属锂-碳纳米管(Li-CNT)复合结构,极大的提高了金属锂的比表面积,降低了电极电流密度,从而有效地抑制了锂枝晶的生长,提高了金属锂电极的循环稳定性和安全性能。本工作在前期工作基础上,采用简单的液相反应,利用4-氟苯乙烯(FPS)对Li-CNT进行表面修饰并进行原位聚合,得到了表面富含氟化锂(Li F)保护层的Li-CNT(FPS-Li-CNT)。该表面修饰层能够有效抑制电解液和空气对Li-CNT的侵蚀,显著的提高了LiCNT电极的界面稳定性。FPS-Li-CNT与磷酸铁锂正极(LFP)组成的LFP||FPS-Li-CNT全电池,在正负极容量配比为1:6条件下,能够稳定循环280圈,库伦效率达到97.7%。展开更多
BiFeO_(3)(BFO)是一种新型可回收光响应催化剂,但较高的光生电子/空穴对复合率和较低的量子产率限制了其实际应用。本研究通过水热法制备出还原氧化石墨烯-BFO(RGO-BFO)纳米晶复合材料,表征与测试结果表明,相比于BFO颗粒,复合材料的禁...BiFeO_(3)(BFO)是一种新型可回收光响应催化剂,但较高的光生电子/空穴对复合率和较低的量子产率限制了其实际应用。本研究通过水热法制备出还原氧化石墨烯-BFO(RGO-BFO)纳米晶复合材料,表征与测试结果表明,相比于BFO颗粒,复合材料的禁带宽度E_(g)为2.0 e V,降低约10%;40 min对亚甲基蓝吸附–催化效率接近100%,远高于BFO颗粒(28%),这主要由于复合体系中光生电子/空穴对复合率更低。通过本征磁性回收并重复利用6次后,复合材料仍保持89.1%催化效率,表现出优异催化性能。展开更多
文摘电解水技术是一种生产高纯氢燃料的方法,能够增强可再生能源发电系统的消纳能力.相较于质子交换膜(PEM)电解槽,碱性(ALK)电解槽可以使用非贵金属基催化电极,拥有更高的经济效益和市场占有率.然而,由于ALK电解槽处于质子稀缺环境,阴极氢气演化反应(HER)动力学变得更加复杂,需要快速解离水分子提供动态质子微环境.硫化钼(MoS_(2))纳米片边缘具有合适的质子吸附和演化的活性位点,是制备HER催化剂的潜力材料.但其二维基面原子由于配位饱和,显示出较弱的质子吸附能力.如何调控MoS_(2)基面以实现水解动力与质子吸附演化动力的集成,提升MoS_(2)纳米片的碱性HER活性,具有重要的科学和应用意义.本文提出了一种Co/O双原子植入策略,精准调控双活性位点及其电子结构,实现了水解离动力和质子吸附演化动力的高效耦联.首先,利用刻蚀和电沉积的两步实验法,在MoS_(2)基面上成功引入O和Co原子;随后,结合高分辨透射电镜、高角环形暗场-扫描透射电子显微镜、同步辐射X射线吸收精细结构谱等表征分析技术,精准识别了掺杂Co/O原子的位置和配位情况:O原子替换部分S原子,Co原子占据Mo原子的上方,构建出立体凸起的“O-Co-S_(2)”配位构型.催化在线的原位表征分析结果表明:该独特的“O-Co-S_(2)”原子基序发挥着水解离与氢演化反应协同催化效应.密度泛函理论计算结果也证实了该协同机制,其中Co位点促进水的解离反应,而S位点则有助于质子的转化生成氢气.因此,Co/O掺杂MoS_(2)催化剂(Co-O@MoS_(2))表现出较好的碱性HER活性:仅需81 mV的过电位,即可达到100 mA cm^(‒2)的电流密度,Tafel斜率低至42 mV dec^(‒1),在600 mA cm^(‒2)的高电流密度测试中运行300 h活性无衰减.上述碱性HER性能不仅远高于原始的MoS_(2)纳米片,而且也领先于部分已报道结果.综上所述,本文在MoS_(2)基面上构筑了原子级协同催化活性中心,显著促进了碱性HER反应性能,为原子活化工程开发先进催化剂提供参考,在原子级基序构造、表征和功能分析方面提供借鉴.
基金the National Natural Sciencefoundation of China (Grant No. 12174085)the FundamentalResearch Funds for the Central Universities (GrantNo. B220202018)+1 种基金the Basic Science (Natural Science) ResearchProject for the Universities of Jiangsu Province (GrantNo. 23KJD140002)Natural Science Foundation of Nantong(Grant No. JC2023081).
文摘Orbital angular momentum(OAM)conversion is critical in understanding interactions between a structural sound field and a planar lattice.Herein,we explore the evolution of a monochromatic acoustic vortex beam(AVB)that is scattered by a phononic crystal(PnC)or a correlated random lattice.The phenomenon is ascribed to the enhanced orbit–orbit angular momentum coupling induced by the band structure.By modifying the coupling condition,accurate and continuous micromanipulation of AVBs can be achieved,including the transverse/lateral gravity shift,the dynamics of the phase singularities,and the spatial distribution of acoustic pressure,etc.This research provides insight to the inhomogeneous coupling of AVBs with both propagating Bloch waves and localized Anderson modes,and may facilitate development of novel OAM-based acoustic devices for active sound field manipulation.
基金Project(2022YFB3803300)supported by the National Key Research and Development Program of ChinaProjects(U23A20138,52173192)supported by the National Natural Science Foundation of China+1 种基金Project(GZC20233148)supported by the Postdoctoral Fellowship Program of CPSF,ChinaProject(140050043)supported by the Central South University Postdoctoral Research Funding,China。
文摘Highly efficient organic solar cells(OSCs)are normally produced using the halogenated solvents chloroform or chlorobenzene,which present challenges for scalable manufacturing due to their toxicity,narrow processing window and low boiling point.Herein,we develop a novel high-speed doctor-blading technique that significantly reduces the required concentration,facilitating the use of eco-friendly,non-halogenated solvents as alternatives to chloroform or chlorobenzene.By utilizing two widely used high-boiling,non-halogenated green solvents-o-xylene(o-XY)and toluene(Tol)-in the fabrication of PM 6:L 8-BO,we achieve power conversion efficiencies(PCEs)of 18.20%and 17.36%,respectively.Additionally,a module fabricated with o-XY demonstrates a notable PCE of 16.07%.In-situ testing and morphological analysis reveal that the o-XY coating process extends the liquid-to-solid transition stage to 6 s,significantly longer than the 1.7 s observed with Tol processing.This prolonged transition phase is crucial for improving the crystallinity of the thin film,reducing defect-mediated recombination,and enhancing carrier mobility,which collectively contribute to superior PCEs.
文摘金属锂负极由于比容量高(3860 mAh·g^(-1))及氧化还原电位极低(-3.04 V vs.标准氢气电极(SHE)),被认为是实现高能量密度锂电池的理想负极。然而,金属锂电极与电解液反应剧烈,且锂离子在电极表面沉积不均匀容易产生枝晶,导致其循环稳定性和安全性都较差,限制了其应用推广。我们前期通过构建金属锂-碳纳米管(Li-CNT)复合结构,极大的提高了金属锂的比表面积,降低了电极电流密度,从而有效地抑制了锂枝晶的生长,提高了金属锂电极的循环稳定性和安全性能。本工作在前期工作基础上,采用简单的液相反应,利用4-氟苯乙烯(FPS)对Li-CNT进行表面修饰并进行原位聚合,得到了表面富含氟化锂(Li F)保护层的Li-CNT(FPS-Li-CNT)。该表面修饰层能够有效抑制电解液和空气对Li-CNT的侵蚀,显著的提高了LiCNT电极的界面稳定性。FPS-Li-CNT与磷酸铁锂正极(LFP)组成的LFP||FPS-Li-CNT全电池,在正负极容量配比为1:6条件下,能够稳定循环280圈,库伦效率达到97.7%。
文摘BiFeO_(3)(BFO)是一种新型可回收光响应催化剂,但较高的光生电子/空穴对复合率和较低的量子产率限制了其实际应用。本研究通过水热法制备出还原氧化石墨烯-BFO(RGO-BFO)纳米晶复合材料,表征与测试结果表明,相比于BFO颗粒,复合材料的禁带宽度E_(g)为2.0 e V,降低约10%;40 min对亚甲基蓝吸附–催化效率接近100%,远高于BFO颗粒(28%),这主要由于复合体系中光生电子/空穴对复合率更低。通过本征磁性回收并重复利用6次后,复合材料仍保持89.1%催化效率,表现出优异催化性能。
基金The project was supported by the National Natural Science Foundation of China(21625304,21733012,21773290)the “Strategic Priority Research Program” of CAS(XDA09010600)the Ministry of Science and Technology of China(2016YFA0200703)~~
