Synthesis evidence

2D Conductive Metal-Organic Frameworks Based on Tetraoxa[8]circulenes as Promising Cathode for Aqueous Zinc Ion Batteries

Chang Z., Zhu M., Li Z. et al. · Small · 2024 · 2400923

4 structured synthesis routes

Completeness describes how fully the route could be reconstructed from the main article and supporting information.

Complete recipeSource: Both

Route 1: Other

pp.6-8 · Experimental Section, Synthesis of 8OH-TOC · Scheme S1

Linker precursors2,3,4-trimethoybenzaldehyde; 2,3-dimethoxycyclohexa-2,5-diene-1,4-dione; 2,3,5,6,8,9,11,12-octamethoxyl-tetraoxa[8]circulene
SolventsCH2Cl2, MeOH, H2O, EtOAc/petroleum ether, EtOAc/DCM, DCM/DMSO-d6 for analysis
Additivesm-CPBA, NaHCO3, Na2S2O3, NaOH, HCl, ceric ammonium nitrate, silica gel, BF3·Et2O, BBr3
Atmospherenot specified for most steps; dry DCM used for BBr3 demethylation
Temperature0 °C to room temperature; reflux for circulene formation; -60 °C then room temperature for BBr3 step
Time3 h warming step; 16 h NaOH step; 1.5 h CAN oxidation; 24 h reflux; 2 h at -60 °C plus overnight at room temperature; 2 h quench
Oxidant / reductantm-CPBA and ceric ammonium nitrate oxidation; BBr3 demethylation reagent
Work-upphase separation, aqueous washes, extraction, drying over salts, evaporation, chromatography; final quench with water and filtration
Activationnot specified
Scalability contextReported millimole-scale precursor synthesis and 0.12 mmol final demethylation.
Show 10 structured reagent records
RoleReagentAmount / concentrationSource
Linker2,3,4-trimethoybenzaldehyde 119.62 g, 100.0 mmolpp.6-8 · Experimental Section, Synthesis of 8OH-TOC · Scheme S1
Oxidantm-CPBA85 wt%, 21.93 g, 108.0 mmolpp.6-8 · Experimental Section, Synthesis of 8OH-TOC · Scheme S1
SolventCH2Cl244 mL plus 180 mL plus extraction volumespp.6-8 · Experimental Section, Synthesis of 8OH-TOC · Scheme S1
Baseaqueous NaOH100 mL · 10% (w/v)pp.6-8 · Experimental Section, Synthesis of 8OH-TOC · Scheme S1
Acidaqueous HClused to acidify to pH = 1; 100 mL in circulene workup · 6.0 M and 2.0 Mpp.6-8 · Experimental Section, Synthesis of 8OH-TOC · Scheme S1
Oxidantceric ammonium nitrate138.38 g, 261.0 mmolpp.6-8 · Experimental Section, Synthesis of 8OH-TOC · Scheme S1
AdditiveBF3·Et2O31.0 mLpp.6-8 · Experimental Section, Synthesis of 8OH-TOC · Scheme S1
Linker2,3-dimethoxycyclohexa-2,5-diene-1,4-dione (4)4.20 g, 25.0 mmolpp.6-8 · Experimental Section, Synthesis of 8OH-TOC · Scheme S1
Linker2,3,5,6,8,9,11,12-octamethoxyl-tetraoxa[8]circulene (5)72.06 mg, 0.12 mmolpp.6-8 · Experimental Section, Synthesis of 8OH-TOC · Scheme S1
AdditiveBBr3 in DCM11.52 mL, 11.52 mmol · 1.0 Mpp.6-8 · Experimental Section, Synthesis of 8OH-TOC · Scheme S1
Complete recipeSource: Both

Route 2: Solvothermal

p.8 · Experimental Section, Synthesis of M-TOCs

Metal precursorsCu(NO3)2·2.5H2O
Linker precursors8OH-TOC
Solventsdeionized water (0.8 mL), DMF (0.2 mL)
Atmospheresealed polymerization tube under vacuum
Temperature50
Time48
Work-upwashed with water, DMF and acetone several times in order
Activationdried overnight in vacuum at 60 °C
Scalability contextSmall sealed-tube batch with 9.76 mg ligand.
Show 4 structured reagent records
RoleReagentAmount / concentrationSource
Metal SourceCu(NO3)2·2.5H2O9.30 mg, 0.04 mmolp.8 · Experimental Section, Synthesis of M-TOCs
Linker8OH-TOC9.76 mg, 0.02 mmolp.8 · Experimental Section, Synthesis of M-TOCs
Solventdeionized water0.8 mLp.8 · Experimental Section, Synthesis of M-TOCs
Solventdimethylformamide (DMF)0.2 mLp.8 · Experimental Section, Synthesis of M-TOCs
Complete recipeSource: Both

Route 3: Solvothermal

p.8 · Experimental Section, Synthesis of M-TOCs

Metal precursorsMnCl2·4H2O
Linker precursors8OH-TOC
Solventsdeionized water (0.8 mL), DMF (0.2 mL)
Atmospheresealed polymerization tube under air
Temperature120
Time24
Work-upwashed with water, DMF and acetone several times in order
Activationdried overnight in vacuum at 60 °C
Scalability contextSmall sealed-tube batch with 9.76 mg ligand.
Show 4 structured reagent records
RoleReagentAmount / concentrationSource
Metal SourceMnCl2·4H2O7.92 mg, 0.04 mmolp.8 · Experimental Section, Synthesis of M-TOCs
Linker8OH-TOC9.76 mg, 0.02 mmolp.8 · Experimental Section, Synthesis of M-TOCs
Solventdeionized water0.8 mLp.8 · Experimental Section, Synthesis of M-TOCs
Solventdimethylformamide (DMF)0.2 mLp.8 · Experimental Section, Synthesis of M-TOCs
Complete recipeSource: Both

Route 4: Solvothermal

p.8 · Experimental Section, Synthesis of M-TOCs

Metal precursorsZn(OAc)2
Linker precursors8OH-TOC
Solventsdeionized water (0.8 mL), DMF (0.2 mL)
Atmospheresealed polymerization tube under vacuum
Temperature85
Time48
Work-upwashed with water, DMF and acetone several times in order
Activationdried overnight in vacuum at 60 °C
Scalability contextSmall sealed-tube batch with 9.76 mg ligand.
Show 4 structured reagent records
RoleReagentAmount / concentrationSource
Metal SourceZn(OAc)27.34 mg, 0.04 mmolp.8 · Experimental Section, Synthesis of M-TOCs
Linker8OH-TOC9.76 mg, 0.02 mmolp.8 · Experimental Section, Synthesis of M-TOCs
Solventdeionized water0.8 mLp.8 · Experimental Section, Synthesis of M-TOCs
Solventdimethylformamide (DMF)0.2 mLp.8 · Experimental Section, Synthesis of M-TOCs