Atomically thin MoSe_(2) layers,as a core member of the transition metal dichalcogenides(TMDs)family,benefit from their appealing properties,including tunable band gaps,high exciton binding energies,and giant oscillat...Atomically thin MoSe_(2) layers,as a core member of the transition metal dichalcogenides(TMDs)family,benefit from their appealing properties,including tunable band gaps,high exciton binding energies,and giant oscillator strengths,thus pro-viding an intriguing platform for optoelectronic applications of light-emitting diodes(LEDs),field-effect transistors(FETs),sin-gle-photon emitters(SPEs),and coherent light sources(CLSs).Moreover,these MoSe_(2) layers can realize strong excitonic emis-sion in the near-infrared wavelengths,which can be combined with the silicon-based integration technologies and further encourage the development of the new generation technologies of on-chip optical interconnection,quantum computing,and quantum information processing.Herein,we overview the state-of-the-art applications of light-emitting devices based on two-dimensional MoSe_(2) layers.Firstly,we introduce recent developments in excitonic emission features from atomically thin MoSe_(2) and their dependences on typical physical fields.Next,we focus on the exciton-polaritons and plasmon-exciton polaritons in MoSe_(2) coupled to the diverse forms of optical microcavities.Then,we highlight the promising applications of LEDs,SPEs,and CLSs based on MoSe_(2) and their heterostructures.Finally,we summarize the challenges and opportunities for high-quality emis-sion of MoSe_(2) and high-performance light-emitting devices.展开更多
The strong metal-support interaction inducing combined effect plays a crucial role in the catalysis reaction. Herein, we revealed that the combined advantages of MoSe_(2), Ru, and hollow carbon spheres in the form of ...The strong metal-support interaction inducing combined effect plays a crucial role in the catalysis reaction. Herein, we revealed that the combined advantages of MoSe_(2), Ru, and hollow carbon spheres in the form of Ru nanoparticles(NPs) anchored on a two-dimensionally ordered MoSe_(2) nanosheet-embedded mesoporous hollow carbon spheres surface(Ru/MoSe_(2)@MHCS) for the largely boosted hydrogen evolution reaction(HER) performance. The combined advantages from the conductive support, oxyphilic MoSe_(2), and Ru active sites imparted a strong synergistic effect and charge redistribution in the Ru periphery which induced high catalytic activity, stability, and kinetics for HER. Specifically, the obtained Ru/MoSe_(2)@MHCS required a small overpotential of 25.5 and 38.4 mV to drive the kinetic current density of 10 mA cm^(-2)both in acid and alkaline media, respectively, which was comparable to that of the Pt/C catalyst. Experimental and theoretical results demonstrated that the charge transfer from MoSe_(2) to Ru NPs enriched the electronic density of Ru sites and thus facilitated hydrogen adsorption and water dissociation. The current work showed the significant interfacial engineering in Ru-based catalysts development and catalysis promotion effect understanding via the metal-support interaction.展开更多
电催化水分解是实现绿色制氢的理想方法之一.然而,阳极析氧反应(OER)固有的缓慢动力学和高理论电压(1.23V),使得电解水制氢的能效受到严重限制.采用理论电位更低和热力学更有利的小分子氧化反应替代OER过程,可以在降低电能耗的同时降解...电催化水分解是实现绿色制氢的理想方法之一.然而,阳极析氧反应(OER)固有的缓慢动力学和高理论电压(1.23V),使得电解水制氢的能效受到严重限制.采用理论电位更低和热力学更有利的小分子氧化反应替代OER过程,可以在降低电能耗的同时降解污染物或生成有附加值的产物,能够带来多重效益.尿素氧化反应(UOR)具有较低的理论电压(0.37V),是替代OER的潜在反应之一.然而,UOR中复杂的六电子转移严重阻碍了尿素电解的整体效率.因此,设计经济且高效的电催化剂来促进UOR固有的缓慢动力学过程非常必要.硒化镍具有电子构型多样和结构调控灵活等优点,被认为是有效的UOR催化剂.然而,UOR过程涉及催化剂表面多种反应中间体的吸附/解吸,单相催化剂要同时满足多种反应中间的吸附/解吸是一项艰巨的挑战.众所周知,非均相电催化涉及电子转移以及电催化剂表面反应物和产物的吸附和解吸.因此,催化剂的电催化性能在很大程度上取决于材料表面的电子特性.通过构建异质结构是一种有效策略,可以调节电催化剂的电子结构,优化反应中间体的化学吸附行为,实现不同组份高效协同电催化.研究表明,通过界面工程优化结构和电子特性可进一步促进UOR的动力学.MoSe_(2)具有良好的稳定性和导电性,与镍基催化剂组合构建异质结构能够改善电催化反应中的催化动力学.本文通过简单的水热和低温硒化方法构建了异质NiSe_(2)/MoSe_(2)微球作为UOR的电催化剂.差分电荷密度和Mulliken电荷分析结果表明,MoSe_(2)与NiSe_(2)的耦合引起界面处的电荷重新分布,促使电子从NiSe_(2)向MoSe_(2)转移,更容易形成高价态Ni(NiOOH)活性物种.另外,异质界面的构建优化了催化剂表面的电子结构并调节d带中心,改变反应途径,降低反应能垒,从而提高UOR的反应活性.异质结NiSe_(2)/MoSe_(2)微球由于其独特的结构特征、强的协同耦合作用、增加的活性中心和高含量的高价Ni3+物种的综合优势而具有高效的催化性能.当负载在玻碳电极上时,仅需1.33 V的电压就能驱动10 m Acm^(-2)的电流密度,该活性优于大多数已报道的非贵金属UOR催化剂.将NiSe_(2)/MoSe_(2)催化剂组装到UOR//HER电解槽中时,NiSe_(2)/MoSe_(2)|Pt/C具有较低的操作电压和长期稳定性,在1.47 V的电池电压下电流密度达到10 m Acm^(-2),比单纯的水电解降低了约220 m V.与OER相比,热力学上有利的UOR可以作为阳极OER替代反应.综上,本文为能源/环境相关的催化反应提供了一个有效的催化剂体系,对构建高效异质结催化系统具有借鉴意义.展开更多
基金This work is supported by the National Natural Science Foundation of China(No.61904151)the National Key Research and Development Program of China(No.2021YFA1200803)the Joint Research Funds of the Department of Science&Technology of Shaanxi Province and Northwestern Polytechnical University(No.2020GXLH-Z-020).
文摘Atomically thin MoSe_(2) layers,as a core member of the transition metal dichalcogenides(TMDs)family,benefit from their appealing properties,including tunable band gaps,high exciton binding energies,and giant oscillator strengths,thus pro-viding an intriguing platform for optoelectronic applications of light-emitting diodes(LEDs),field-effect transistors(FETs),sin-gle-photon emitters(SPEs),and coherent light sources(CLSs).Moreover,these MoSe_(2) layers can realize strong excitonic emis-sion in the near-infrared wavelengths,which can be combined with the silicon-based integration technologies and further encourage the development of the new generation technologies of on-chip optical interconnection,quantum computing,and quantum information processing.Herein,we overview the state-of-the-art applications of light-emitting devices based on two-dimensional MoSe_(2) layers.Firstly,we introduce recent developments in excitonic emission features from atomically thin MoSe_(2) and their dependences on typical physical fields.Next,we focus on the exciton-polaritons and plasmon-exciton polaritons in MoSe_(2) coupled to the diverse forms of optical microcavities.Then,we highlight the promising applications of LEDs,SPEs,and CLSs based on MoSe_(2) and their heterostructures.Finally,we summarize the challenges and opportunities for high-quality emis-sion of MoSe_(2) and high-performance light-emitting devices.
基金supported by the National Natural Science Foundation of China (21972124, 22272148)the Priority Academic Program Development of Jiangsu Higher Education Institution。
文摘The strong metal-support interaction inducing combined effect plays a crucial role in the catalysis reaction. Herein, we revealed that the combined advantages of MoSe_(2), Ru, and hollow carbon spheres in the form of Ru nanoparticles(NPs) anchored on a two-dimensionally ordered MoSe_(2) nanosheet-embedded mesoporous hollow carbon spheres surface(Ru/MoSe_(2)@MHCS) for the largely boosted hydrogen evolution reaction(HER) performance. The combined advantages from the conductive support, oxyphilic MoSe_(2), and Ru active sites imparted a strong synergistic effect and charge redistribution in the Ru periphery which induced high catalytic activity, stability, and kinetics for HER. Specifically, the obtained Ru/MoSe_(2)@MHCS required a small overpotential of 25.5 and 38.4 mV to drive the kinetic current density of 10 mA cm^(-2)both in acid and alkaline media, respectively, which was comparable to that of the Pt/C catalyst. Experimental and theoretical results demonstrated that the charge transfer from MoSe_(2) to Ru NPs enriched the electronic density of Ru sites and thus facilitated hydrogen adsorption and water dissociation. The current work showed the significant interfacial engineering in Ru-based catalysts development and catalysis promotion effect understanding via the metal-support interaction.
文摘电催化水分解是实现绿色制氢的理想方法之一.然而,阳极析氧反应(OER)固有的缓慢动力学和高理论电压(1.23V),使得电解水制氢的能效受到严重限制.采用理论电位更低和热力学更有利的小分子氧化反应替代OER过程,可以在降低电能耗的同时降解污染物或生成有附加值的产物,能够带来多重效益.尿素氧化反应(UOR)具有较低的理论电压(0.37V),是替代OER的潜在反应之一.然而,UOR中复杂的六电子转移严重阻碍了尿素电解的整体效率.因此,设计经济且高效的电催化剂来促进UOR固有的缓慢动力学过程非常必要.硒化镍具有电子构型多样和结构调控灵活等优点,被认为是有效的UOR催化剂.然而,UOR过程涉及催化剂表面多种反应中间体的吸附/解吸,单相催化剂要同时满足多种反应中间的吸附/解吸是一项艰巨的挑战.众所周知,非均相电催化涉及电子转移以及电催化剂表面反应物和产物的吸附和解吸.因此,催化剂的电催化性能在很大程度上取决于材料表面的电子特性.通过构建异质结构是一种有效策略,可以调节电催化剂的电子结构,优化反应中间体的化学吸附行为,实现不同组份高效协同电催化.研究表明,通过界面工程优化结构和电子特性可进一步促进UOR的动力学.MoSe_(2)具有良好的稳定性和导电性,与镍基催化剂组合构建异质结构能够改善电催化反应中的催化动力学.本文通过简单的水热和低温硒化方法构建了异质NiSe_(2)/MoSe_(2)微球作为UOR的电催化剂.差分电荷密度和Mulliken电荷分析结果表明,MoSe_(2)与NiSe_(2)的耦合引起界面处的电荷重新分布,促使电子从NiSe_(2)向MoSe_(2)转移,更容易形成高价态Ni(NiOOH)活性物种.另外,异质界面的构建优化了催化剂表面的电子结构并调节d带中心,改变反应途径,降低反应能垒,从而提高UOR的反应活性.异质结NiSe_(2)/MoSe_(2)微球由于其独特的结构特征、强的协同耦合作用、增加的活性中心和高含量的高价Ni3+物种的综合优势而具有高效的催化性能.当负载在玻碳电极上时,仅需1.33 V的电压就能驱动10 m Acm^(-2)的电流密度,该活性优于大多数已报道的非贵金属UOR催化剂.将NiSe_(2)/MoSe_(2)催化剂组装到UOR//HER电解槽中时,NiSe_(2)/MoSe_(2)|Pt/C具有较低的操作电压和长期稳定性,在1.47 V的电池电压下电流密度达到10 m Acm^(-2),比单纯的水电解降低了约220 m V.与OER相比,热力学上有利的UOR可以作为阳极OER替代反应.综上,本文为能源/环境相关的催化反应提供了一个有效的催化剂体系,对构建高效异质结催化系统具有借鉴意义.
