© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim 3687 wileyonlinelibrary.com COMMUNICATION 2D Monolayer MoS 2 –Carbon Interoverlapped Superstructure: Engineering Ideal Atomic Interface for Lithium Ion Storage Hao Jiang, Dayong Ren, Haifeng Wang,* Yanjie Hu, Shaojun Guo,* Haiyang Yuan, Peijun Hu, Ling Zhang, and Chunzhong Li* Prof. H. Jiang, D. Ren, Dr. Y. Hu, Dr. L. Zhang, Prof. C. Li Key Laboratory for Ultrafine Materials of Ministry of Education School of Materials Science and Engineering East China University of Science & Technology Shanghai 200237, China E-mail: czli@ecust.edu.cn Dr. H. Wang, H. Yuan, Prof. P. Hu State Key Laboratory of Chemical Engineering Centre for Computational Chemistry and Research Institute of Industrial Catalysis East China University of Science and Technology Shanghai 200237, China E-mail: hfwang@ecust.edu.cn Dr. S. Guo Physical Chemistry and Applied Spectroscopy Los Alamos National Laboratory Los Alamos, NM 87545, USA E-mail: sguo@lanl.gov; Shaojun.guo.nano@gmail.com Prof. P. Hu School of Chemistry and Chemical Engineering The Queen's University of Belfast Belfast BT9 5AG, UK DOI: 10.1002/adma.201501059 rials, resulting in continuous capacity fading during cycling (less than 200 cycles). [15,16] To circumvent these obstacles, recent significant advances have focused on engineering new MoS 2 /C- based nanocomposites with special design for partly enhancing the capacity, rate capability, and stability of LIBs by the cre- ating/or introducing MoS 2 /carbon interface. This has experi- mentally been demonstrated on the synthesis of MoS 2 -coated 3D graphene networks, [17–19] few-layer MoS 2 grown on the sur- face of carbon nanotubes (CNTs) nanocomposites, [20] graphene- like MoS 2 dispersed in amorphous carbon, [21,22] and few-layer MoS 2 anchored on carbon nanosheet, [23] etc., for improving the performance of LIBs. Despite these strategies can facilitate the electron/ion transport with the suppressed mechanical fracture by conductive carbon protection for a partly improved capacity and stability for LIBs, these specially designed MoS 2 -based nanocomposites have to suffer from the very limited interface efficiency between MoS 2 and carbon ( Scheme 1a,b). In this regard, maximizing the atomic (or nano) interface contact/ or interaction between MoS 2 and carbon by rational design of MoS 2 /carbon hybrids with special architecture becomes very important for maximizing the performance of MoS 2 -based LIBs with long cycle life and extremely high energy and power densities. 2D monolayer MoS 2 nanosheet, as a new inorganic graphene analogue, has been recently extensively studied for the renew- able energy related applications due to the emergence of many unique and fascinating properties in single-layer structure, including electrochemical and photoelectrochemical hydrogen fuel production, [24] LIBs, [5] hydrodesulphurization of crude oil, [25] and so forth. As LIBs-based anode materials, 2D single- layer MoS 2 nanosheet can provide the best opportunity for the lithium storage due to their largest surface area in all the MoS 2 - based nanomaterials, but still not effective to date because they suffer from the very limited conductivity. In this regard, clearly, the combination of 2D MoS 2 with carbon nanosheet (e.g., gra- phene) may generate new class of 2D composite materials with the maximized atomic interface for very high LIB capacity, rate ability, and stability that outperform all the existing MoS 2 -based materials, but still a great challenge to date. Herein, to well address the key challenging issues on MoS 2 materials for LIBs, we demonstrate a novel materials design on the synthesis of 2D MoS 2 /mesoporous carbon (MoS 2 /m-C) hybrid nanoarchitecture with ideal MoS 2 /m-C atomic inter- face, in which single-layer MoS 2 and m-C are sandwiched in alternating sequence, by first the amidation of oleic acid (OA)- protected single-layer MoS 2 nanosheet with dopamine, then Advanced energy storage technology is the key to manage the energy supply and demand for future sustainable and renew- able resources. Lithium-ion batteries (LIBs) are becoming one of the major power sources for future portable electronic devices and hybrid electric vehicles due to their high energy density, long lifespan, and environment benignity compared to other alternatives. [1–4] To date, the popular LIBs using graphite as anode material cannot meet the stringent demands for its low theoretical specific capacity (372 mAh g -1 ). Molybdenum disulfide (MoS 2 ) shows a much higher theoretical lithium storage capacity of 670 mAh g -1 . [5–10] It also exhibits the theo- retically good rate capability and cycling stability because the weak van der Waals interaction between MoS 2 layers can facili- tate the reversible Li + intercalation and extraction without a remarkable volume change and also prevents the pulverization problem of active materials caused by the repeated lithiation and delithiation process. [11] Nevertheless, practically, it usually has very limited conductivity between two adjacent S–Mo–S sheets ( c-direction) for impacting the electron/ion transfer, thus leading to significant capacity loss. [12–14] Furthermore, just like lithium sulfide batteries, a polysulfide shuttling effect may cause the electrochemical degradation of the active MoS 2 mate- Adv. Mater. 2015, 27, 3687–3695 www.advmat.de www.MaterialsViews.com