Further examination of the substrate scope of all sorts of α,β-unsaturated 2-acyl imidazoles, which were employed to test the generality of this asymmetric Michael addition/Cyclization process (Scheme 3). Initially, α,βunsaturated 2-acyl imidazoles with electron-donating substituted phenyl ring were evaluated, and in all case (4a-4c, 4g-4h), high yields (89-93%) with excellent enantioselectivities (93-98%) were achieved. The absolute stereochemistry of 4c was assigned unambiguously by singlecrystal X-ray diffraction analysis and that of the other derivatives were assigned by analogy (for details see the supporting information). The introduction of electronwithdrawing groups such as Cl and Br substituents on the phenyl rings also afforded the cooresponding products (4d-4e) in 90-91% yields with 97-98% ee values. The introduction of ethynyl group on the phenyl rings also afforded the corresponding product (4f) in 94% yield with 98% ee values. The substrates with 2-naphthyl or hetero-aromatic substituents worked well, affording 4i-4j in 92-94% yields with up to 96% ee. In addition to aromatic substituents, alkyl substituents such as styryl-substituted α,β-unsaturated 2-acyl imidazoles were also tolerated, delivering the desired product (4k) in 89% yield with 92% enantiomeric excess. In addition, the replacement of N-Me with i Pr of α,β-unsaturated 2-acyl imidazoles has no influence on the outcome of the reaction, affording the corresponding product in good yield with excellent enantioselectivity (Scheme 3, 4l). Scheme 3. Substrate Scope: α,β-Unsaturated 2-Acyl Imidazoles. a a Reaction conditions: Ni(OTf)2 (5 mol %), L1(5.5 mol %), 1a (0.12 mmol), and 2 (0.10 mmol) in 1.0 mL of CH2Cl2 at 25 ℃.