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过渡金属硫属化合物层间异质结构的可控制备和能源应用

ISSN号：0023-074X
期刊名称：《科学通报》
时间：0
分类：O641.4[理学—物理化学;理学—化学]
作者机构：[1]北京大学工学院材料科学与工程系,北京100871, [2]北京大学化学与分子工程学院纳米化学研究中心,北京100871
相关基金：科技部重点研发计划（2016YFA0200103）; 国家自然科学基金（51472008,51290272,21201012,51121091,51072004,51201069）; 北京市科学技术委员会（Z151100003315013）; 清华大学低维量子物理国家重点实验室开放基金（KF201601）资助

关键词：石墨烯, 过渡金属硫属化合物, 层间异质结构, 电催化析氢反应, 光催化析氢反应, graphene, transition metal dichalcogenides, vertical heterostructures, electrocatalytic hydrogen evolution reaction, photocatalytic hydrogen evolution reaction

中文摘要：

随着石墨烯及其优异性质被发现以来,二维层状材料成为了材料科学领域研究的热点.二维层状材料每个片层内的原子通过化学键连接,片层间以弱范德华力相互堆垛.这种几何结构使得二维层状材料在晶格不匹配和生长方法不兼容的情况下,彼此之间仍然能够相互混合和匹配,从而衍生出很多范德华层间异质结构.这种异质结构利用了不同堆垛材料迥异的物理和化学性质,在电子、光电子器件、可再生能源储存和转化等领域得到了广泛的应用.需要指出的是,大面积、大畴区、可控制备本征层间异质结构是实现其实际应用的首要条件.本文总结了基于过渡金属硫属化合物（MX2）和石墨烯（graphene）层间异质结构的最新研究成果,重点描述了MX2/graphene和MX2/MX2层间异质结构的化学气相沉积（CVD）可控制备、新奇物理性质探索以及这两类异质结构在能源领域（电/光催化析氢反应）中的应用,并讨论了所存在的问题和未来发展方向.

英文摘要：

Two-dimensional（2D） layered materials have been a central focus of materials research since the discovery of graphene. Each layer in 2D layered materials consists of a covalently bonded and is weakly bound to neighboring layers by van der Waals interactions. This makes it feasible to mix and match highly disparate atomic layers to create a wide range of vertical heterostructures without the constraints of lattice matching and processing compatibility. In these heteros-tructures, different physical and chemical properties accompany with the stacked materials are combined, furthermore, many applications in electronic/optoelectronic devices and renewable energy storage/conversions are demonstrated. Notably, the controllable syntheses of large area, large domain size and intrinsic vertical heterostructures are the first step. In this review, recent research achievements towards the controllable syntheses and novel physical properties of MX2/graphene and MX2/MX2 vertical heterostructures, as well as their applications in electrocatalytic/photocatalytic hydrogen evolution reaction are highlighted. Firstly, by using a facile chemical vapor deposition（CVD） approach, high quality and coverage-tunable monolayer MoS2/graphene vertical heterostructures on conventional Au foil substrates are demonstrated. The unique system is selected in view of the tunability of the coverage of MoS2, or the densities of active sites in hydrogen evolution reaction（HER）, as well as its compatibility with scanning tunneling microscopy/spectroscopy（STM/STS） observations. Spectroscopic characterizations reveal a quasi-freestanding monolayer MoS2 feature, which is evidenced by a very weak n-doping effect and an intrinsic bandgap of MoS2 in the MoS2/graphene/Au sandwich, as obtained from STM/STS characterizations. Moreover, the exciton binding energy is also deduced by combining photoluminescence measurements. For monolayer MoS2 synthesized on graphene/Au foils, a dramatic decrease of the bandgap from 2.20 to 0.30 eV occurs at the d