This is the accepted version of the paper.This version of the publication may differ from the final published version. 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 2 Rechargeable lithium ion batteries (LIBs) have long been considered as the most effective energy-storage technology and dominated portable electronic market for over two decades.
Permanent repository link1, 2 Based on the intercalation mechanism, state-of-the-art Li-ion technology can exhibit a theoretical specific energy of ~400 Wh/kg, such as LiCoO 2 /graphite system. 3 However, it is urgent to explore new chemistries and materials that can significantly increase the cell energy density, considering the future demand for electronic vehicles and large-scale energy storage plants. 4,5 Graphite, a widely used anode material for the current LIBs, has a theoretical capacity of only 372 mAh/g, given a fully intercalated LiC 6 compound, which is one of the limiting factors for achieving high energy density of the cell 6 . In order to overcome such technical bottleneck, considerable effort has been devoted to design and synthesise new anode materials with higher theoretical specific capacity, such as transition metal oxides (SnO 2 , Co 3 O 4 ,Fe 3 O 4 ), Sn and Si 7 . However, all these materials suffer from severe volume variation during charge-discharge cycling, which results in serious pulverisation of the electrodes, and thus, rapid capacity degradation. For instance, Si has a high specific capacity of 4200 mAh/g if fully lithiated to Li 4.4 Si, however, it also shows a large volume expansion up to 400%. Such volume expansion causes huge mechanical stress of the electrode, and therefore, severely limits the lifetime of Si anode. Although various strategies have been proposed to enhance the structural stability of Si-based materials, including carbon or polymer coating 8,9 , nano-structuring 10-12 and hierarchical hybridization, [13][14][15] it is still very challenge to overcome the issue of the inherent volume change of these materials during cycling.Transition metal dichalcogenides (TMD) MX 2 (M=Mo, Ti, V, and W, X=S or Se) 16,17 with the similar feature of layered structure as graphite could have great potential for alternative anode materials. In general, MX 2 has strong covalent bonds within layers and weak Van der Waals forces between layers, which provide ideal space for intercalation of lithium ions. For instance, MoS 2 has much larger spacing between neighboring layers (0.615 nm) than that of graphite (0.335 nm) and weak van der Waals forces between the layers, which, in principal, may make the Li + diffuse easier. However, certain electrochemical properties of MX 2 can only be achieved in their 1-D or 2-D nanostructured crystals because of the relatively high resistance for Li-ion transport in their bulk form. In addition, the electron conductivity of th...