Covalent organic frameworks (COFs) are burgeoning class of crystalline porous material that attracted much attention because of their enormous structural diversity, and tunable pore sizes.1 Especially, applications that aim unravelling environmental issues have surfaced as hottest research areas as a result of their task-specific pore structure modulation.2 In particular, exploring their dynamic behaviour upon exposure to external stimuli is likely to enable unprecedented switchable gas adsorption. From catalytic viewpoint, developing new methodology for constructing carbon–carbon bonds will overwhelmingly dictate the efficacy of organic synthesis, wherein heterogenization of active catalyst over COF backbone could benefit size-selective cross coupling reaction under green reaction conditions. Building on these, we developed an imine-based, diamondoid COF with free N-atom decorated pore-wall that displays selective and multicyclic CO2 adsorption along with solvent-assisted reversible structural dynamism, which triggers unprecedented CO2 adsorption switch.2 Post-synthetic hooking of homogeneous photocatalyst benefits devising first-ever Ru(Bpy)32+ hooked 3D COF (Ru-COF) that performs visible-light mediated, oxidative photocyanation of tertiary amines using molecular oxygen at room temperature in H2O. To the best of Ru-COF, atom-economic photocyanation is realized via in situ generated iminium ion, where larger substrates exhibit insignificant conversion to α-aminonitriles, and validates rarest pore-fitting-induced size selectivity in oxidative Strecker reaction.3
References and Notes:
1. Song, Y.; Sun, Q.; Aguila, B.; Ma, S.; Adv. Sci., 2019, 6, 1970011.
2. (a)Sasmal, H. S.; Halder, A.; Kunjattu, H. S.; Dey, K.; Nadol, A.; Ajithkumar, T. G.; Ravindra Bedadur, P.; Banerjee, R.; J. Am. Chem. Soc., 2019, 141 (51), 20371−20379. (b) Dey, K.; Kunjattu H, S.; Chahande, A. M.; Banerjee, R.; Angew. Chem., Int. Ed., 2020, 59, 1161−1165.
3. Kumar, G.; Singh, M.; Goswami, R.; Neogi, S.; ACS Appl. Mater. Interfaces, 2020, 12, 48642–48653.

Covalent organic frameworks (COFs) are burgeoning class of crystalline porous material that attracted much attention because of their enormous structural diversity, and tunable pore sizes.^1^ Especially, applications that aim unravelling environmental issues have surfaced as hottest research areas as a result of their task-specific pore structure modulation.^2^ In particular, exploring their dynamic behaviour upon exposure to external stimuli is likely to enable unprecedented switchable gas adsorption. From catalytic viewpoint, developing new methodology for constructing carbon–carbon bonds will overwhelmingly dictate the efficacy of organic synthesis, wherein heterogenization of active catalyst over COF backbone could benefit size-selective cross coupling reaction under green reaction conditions. Building on these, we developed an imine-based, diamondoid COF with free N-atom decorated pore-wall that displays selective and multicyclic CO~2~ adsorption along with solvent-assisted reversible structural dynamism, which triggers unprecedented CO~2~ adsorption switch.^2^ Post-synthetic hooking of homogeneous photocatalyst benefits devising first-ever Ru(Bpy)~3~^2+^ hooked 3D COF (Ru-COF) that performs visible-light mediated, oxidative photocyanation of tertiary amines using molecular oxygen at room temperature in H~2~O. To the best of Ru-COF, atom-economic photocyanation is realized via in situ generated iminium ion, where larger substrates exhibit insignificant conversion to α-aminonitriles, and validates rarest pore-fitting-induced size selectivity in oxidative Strecker reaction.^3^
**References and Notes:**
**1.** Song, Y.; Sun, Q.; Aguila, B.; Ma, S.; _Adv. Sci.,_ **2019**, _6_, 1970011.
**2.** (a)Sasmal, H. S.; Halder, A.; Kunjattu, H. S.; Dey, K.; Nadol, A.; Ajithkumar, T. G.; Ravindra Bedadur, P.; Banerjee, R.; _J. Am. Chem. Soc.,_ **2019**, _141 (51)_, 20371−20379. (b) Dey, K.; Kunjattu H, S.; Chahande, A. M.; Banerjee, R.; _Angew. Chem., Int. Ed.,_ **2020**, _59_, 1161−1165.
**3.** Kumar, G.; Singh, M.; Goswami, R.; Neogi, S.; ACS _Appl. Mater. Interfaces,_ **2020**_, 12,_ 48642–48653.

Structural Dynamism Triggered Switchable CO2 Adsorption and Visible-light Mediated Size Selective Cα–H Photocyanation in Pre-functionalized Covalent Organic Framework

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27th CRSI National Symposium in Chemistry

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