Synthesis evidence

Modulating the electrical conductivity of metal-organic framework films with intercalated guest π-systems

Guo Z., Panda D.K., Maity K. et al. · Journal of Materials Chemistry C · 2016 · 894-899

10 structured synthesis routes

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

Complete recipeSource: Both

Route 1: Solvothermal

S2 · BMOF Synthesis

Metal precursorsZn(NO3)2·6H2O (60 mg, 0.2 mmol)
Linker precursorsTCPB strut (56 mg, 0.1 mmol); BPDPNDI pillar (56 mg, 0.1 mmol)
SolventsDMF (10 mL)
Atmosphere20 mL screw-capped vial; gas atmosphere not otherwise specified
Temperature80
Time24
Work-upCooled slowly to room temperature over 6 h; rod-shaped navy-blue crystals obtained (60 mg, yield ≈ 35%).
ActivationFor gas sorption, a separate sample was DMF-washed, THF-exchanged and vacuum activated.
Show 4 structured reagent records
RoleReagentAmount / concentrationSource
Metal SourceZn(NO3)2·6H2O60 mg, 0.2 mmolS2 · BMOF Synthesis
LinkerTCPB strut56 mg, 0.1 mmolS2 · BMOF Synthesis
LinkerBPDPNDI pillar56 mg, 0.1 mmolS2 · BMOF Synthesis
SolventDMF10 mLS2 · BMOF Synthesis
Complete recipeSource: Both

Route 2: Solvothermal

S4 · Preparation of BMOF Films and Devices

Metal precursorsZn(NO3)2.6H2O (15 mg, 0.5 mmol; unit as printed in SI despite stoichiometric inconsistency)
Linker precursorsTCPB (14 mg, 0.25 mmol); BPDPNDI (14 mg, 0.25 mmol)
SolventsDMF (10 mL); fresh DMF wash; MeNO2 solvent exchange
AdditivesZnO-coated substrate; optional Au/Ti electrodes pre-deposited for devices
Atmosphere20 mL screw-capped vials; oven atmosphere not otherwise specified
Temperature80
Time2 h pre-nucleation plus typically ca. 1 h film growth; 0.5-1 h gives coverage
Substrate orientationZnO films immersed upright or slightly slanted with ZnO-coated side facing down
Work-upSlides withdrawn, soaked in fresh DMF to remove trapped/unreacted precursors, immersed in MeNO2 to remove DMF, then dried and/or guest-loaded.
ActivationMeNO2 exchange before drying/guest immersion.
Scalability contextAuthors state the bottom-up film growth method could simplify device integration and testing of MOFs.
Show 5 structured reagent records
RoleReagentAmount / concentrationSource
Metal SourceZn(NO3)2.6H2O15 mg, 0.5 mmolS4 · Preparation of BMOF Films and Devices
LinkerTCPB14 mg, 0.25 mmolS4 · Preparation of BMOF Films and Devices
LinkerBPDPNDI14 mg, 0.25 mmolS4 · Preparation of BMOF Films and Devices
SolventDMF10 mLS4 · Preparation of BMOF Films and Devices
OtherZnO-coated glass/FTO slideca. 4 cm x 1.1 cm; ZnO area 2 cm x 1.1 cmS4 · Preparation of BMOF Films and Devices
Complete recipeSource: SI

Route 3: Other

S3 · Gas Adsorption Analysis · Fig. S3

Metal precursorsAs-synthesised BMOF crystals
SolventsFresh DMF; THF
AtmosphereHigh vacuum activation
Temperatureroom temperature activation; 273 K sorption
TimeDMF wash over 3 d; THF exchange over 3 d; high-vacuum activation 24 h
Work-upWashed with fresh DMF six times over 3 d, soaked in THF with solvent refreshed over 3 d, activated under high vacuum until outgas rate <5 micrometre Hg/min.
ActivationHigh vacuum at room temperature for 24 h.
Scalability contextActivation protocol for porosity measurement; batch size not specified.
Show 3 structured reagent records
RoleReagentAmount / concentrationSource
Otheras-synthesised BMOF crystalsnot specifiedS3 · Gas Adsorption Analysis · Fig. S3
Solventfresh DMFsix washes over 3 daysS3 · Gas Adsorption Analysis · Fig. S3
SolventTHFrefreshed several times over 3 daysS3 · Gas Adsorption Analysis · Fig. S3
Complete recipeSource: SI

Route 4: Other

S1-S2 · II. Synthesis of and Characterization of BPDPNDI Pillar · Scheme S1

Linker precursorsNDA via DBrNDA, DBrNDI and 2,6-dipyrrolo-NDI intermediates
Solventsconcentrated H2SO4; AcOH; pyrrolidine; anhydrous DMAc; CHCl3/MeOH chromatography solvent
Additivesdibromoisocyanuric acid; NH4OAc; 4-pyridinylboronic acid; Cu(OAc)2; Et3N; molecular sieves (4 A)
AtmosphereO2 purge 30 min and O2 environment for final Cu(II)-mediated coupling; earlier steps not specified
Temperature100 for DBrNDA; reflux for DBrNDI and dipyrrolo-NDI; 55 for final coupling
Time15; 3; 16; final 5 d total
Oxidant / reductantdibromoisocyanuric acid bromination reagent; Cu(OAc)2/O2-mediated coupling
Work-upDBrNDA filtered and washed with H2O/hot MeOH; DBrNDI filtered and washed with AcOH/diethyl ether; dipyrrolo-NDI washed with hexanes/MeOH; final product filtered, DMF-washed, hot CHCl3-extracted, and purified by SiO2 chromatography.
ActivationNot applicable for molecular ligand; isolated as navy-blue solid.
Scalability contextGram-scale intermediates; final BPDPNDI 0.72 g, yield ≈ 40%.
Show 10 structured reagent records
RoleReagentAmount / concentrationSource
LinkerNDA2.68 g, 10 mmolS1-S2 · II. Synthesis of and Characterization of BPDPNDI Pillar · Scheme S1
Oxidantdibromoisocyanuric acid11.48 g, 20 mmolS1-S2 · II. Synthesis of and Characterization of BPDPNDI Pillar · Scheme S1
Acidconcentrated H2SO410 mL + 10 mL · concentratedS1-S2 · II. Synthesis of and Characterization of BPDPNDI Pillar · Scheme S1
AdditiveNH4OAc15.5 g, 188 mmolS1-S2 · II. Synthesis of and Characterization of BPDPNDI Pillar · Scheme S1
SolventAcOH40 mLS1-S2 · II. Synthesis of and Characterization of BPDPNDI Pillar · Scheme S1
Additivepyrrolidine20 mLS1-S2 · II. Synthesis of and Characterization of BPDPNDI Pillar · Scheme S1
Linker4-pyridinylboronic acid3.96 g, 32.3 mmol plus 1.98 g, 16.2 mmolS1-S2 · II. Synthesis of and Characterization of BPDPNDI Pillar · Scheme S1
OxidantCu(OAc)25.83 g, 32.3 mmol plus 2.92 g, 16.2 mmolS1-S2 · II. Synthesis of and Characterization of BPDPNDI Pillar · Scheme S1
BaseEt3N4.5 mL, 32.3 mmol plus 2.3 mL, 16.2 mmolS1-S2 · II. Synthesis of and Characterization of BPDPNDI Pillar · Scheme S1
Solventanhydrous DMAc100 mL plus 25 mLS1-S2 · II. Synthesis of and Characterization of BPDPNDI Pillar · Scheme S1
Complete recipeSource: SI

Route 5: Other

S4 · Doping BMOF Films with Guest pi-Systems

Metal precursorsPristine BMOF/ZnO film/device
SolventsMeNO2 for MV2+, DFDNB and DNT; toluene for C60
AdditivesC60
Atmosphereambient soaking; atmosphere not otherwise specified
Temperatureroom temperature / ambient conditions
Timesaturated in toluene; 7 d
Substrate orientationBMOF/ZnO film/device immersed in guest solution
Oxidant / reductantpi-acidic guest system; not a redox synthesis step
Work-upQuick washing with fresh solvents tested for doped films; prolonged fresh-solvent soaking led to dopant loss.
ActivationFilms were MeNO2-exchanged before guest immersion.
Show 2 structured reagent records
RoleReagentAmount / concentrationSource
OtherBMOF/ZnO filmnot specifiedS4 · Doping BMOF Films with Guest pi-Systems
AdditiveC60not specified · saturated in toluene; 7 dS4 · Doping BMOF Films with Guest pi-Systems
Complete recipeSource: SI

Route 6: Other

S4 · Doping BMOF Films with Guest pi-Systems

Metal precursorsPristine BMOF/ZnO film/device
SolventsMeNO2 for MV2+, DFDNB and DNT; toluene for C60
Additives1,5-difluoro-2,4-dinitrobenzene (DFDNB)
Atmosphereambient soaking; atmosphere not otherwise specified
Temperatureroom temperature / ambient conditions
Time30 mM / MeNO2; Table S1 lists 44 h, prose says 24 h to maximum
Substrate orientationBMOF/ZnO film/device immersed in guest solution
Oxidant / reductantpi-acidic guest system; not a redox synthesis step
Work-upQuick washing with fresh solvents tested for doped films; prolonged fresh-solvent soaking led to dopant loss.
ActivationFilms were MeNO2-exchanged before guest immersion.
Show 2 structured reagent records
RoleReagentAmount / concentrationSource
OtherBMOF/ZnO filmnot specifiedS4 · Doping BMOF Films with Guest pi-Systems
Additive1,5-difluoro-2,4-dinitrobenzene (DFDNB)not specified · 30 mM / MeNO2; Table S1 lists 44 h, prose says 24 h to maximumS4 · Doping BMOF Films with Guest pi-Systems
Complete recipeSource: SI

Route 7: Other

S4 · Doping BMOF Films with Guest pi-Systems

Metal precursorsPristine BMOF/ZnO film/device
SolventsMeNO2 for MV2+, DFDNB and DNT; toluene for C60
Additivesdinitrotoluene (DNT)
Atmosphereambient soaking; atmosphere not otherwise specified
Temperatureroom temperature / ambient conditions
Time30 mM / MeNO2; Table S1 lists 48 h, prose says 24 h to maximum
Substrate orientationBMOF/ZnO film/device immersed in guest solution
Oxidant / reductantpi-acidic guest system; not a redox synthesis step
Work-upQuick washing with fresh solvents tested for doped films; prolonged fresh-solvent soaking led to dopant loss.
ActivationFilms were MeNO2-exchanged before guest immersion.
Show 2 structured reagent records
RoleReagentAmount / concentrationSource
OtherBMOF/ZnO filmnot specifiedS4 · Doping BMOF Films with Guest pi-Systems
Additivedinitrotoluene (DNT)not specified · 30 mM / MeNO2; Table S1 lists 48 h, prose says 24 h to maximumS4 · Doping BMOF Films with Guest pi-Systems
Complete recipeSource: Both

Route 8: Other

S4 · Depositing Au Electrodes on ZnO-Glass Films

Metal precursorsAu electrodes on Ti adhesion pads
AdditivesPatterned stainless-steel shadow masks
AtmosphereThermal evaporation under vacuum
Substrate orientationFour electrodes deposited 1 mm apart on ZnO-coated nonconducting glass slides
Work-upAfter electrode deposition, exposed ZnO-covered areas remained available for BMOF film growth.
Scalability contextDevice pattern uses 1 cm x 1 cm shadow mask; effective electrode length 4 mm for conductivity calculation.
Show 3 structured reagent records
RoleReagentAmount / concentrationSource
OtherAu~100 nm thick padsS4 · Depositing Au Electrodes on ZnO-Glass Films
OtherTi~10 nm thick padsS4 · Depositing Au Electrodes on ZnO-Glass Films
OtherZnO-coated nonconducting glass slidesnot specifiedS4 · Depositing Au Electrodes on ZnO-Glass Films
Complete recipeSource: SI

Route 9: Other

S4 · Doping BMOF Films with Guest pi-Systems

Metal precursorsPristine BMOF/ZnO film/device
SolventsMeNO2 for MV2+, DFDNB and DNT; toluene for C60
AdditivesMV2+
Atmosphereambient soaking; atmosphere not otherwise specified
Temperatureroom temperature / ambient conditions
Time30 mM / MeNO2; 70 h for Table S1 maximum
Substrate orientationBMOF/ZnO film/device immersed in guest solution
Oxidant / reductantpi-acidic guest system; not a redox synthesis step
Work-upQuick washing with fresh solvents tested for doped films; prolonged fresh-solvent soaking led to dopant loss.
ActivationFilms were MeNO2-exchanged before guest immersion.
Show 2 structured reagent records
RoleReagentAmount / concentrationSource
OtherBMOF/ZnO filmnot specifiedS4 · Doping BMOF Films with Guest pi-Systems
AdditiveMV2+not specified · 30 mM / MeNO2; 70 h for Table S1 maximumS4 · Doping BMOF Films with Guest pi-Systems
Complete recipeSource: SI

Route 10: Other

S4 · Preparation of ZnO Films

Metal precursorsZnO/EtOH suspension, 40 wt%, ZnO particle size ~130 nm
SolventsEtOH in commercial ZnO suspension
AdditivesScotch tape mask to define ZnO-free margins
AtmosphereAir/in oven; not otherwise specified
Temperature350
Time0.5
Substrate orientationFTO-coated or nonconducting glass slides masked along opposite lengths; exposed midsection spin-coated
Work-upTape removed; slides annealed, cooled slowly, and cut to ca. 4 cm x 1.1 cm with 2 cm x 1.1 cm ZnO-coated area.
ActivationAnnealing at 350 C for 30 min.
Show 2 structured reagent records
RoleReagentAmount / concentrationSource
OtherZnO/EtOH suspension40 wt%; spin-coated 1000 rpm, 50 s · ZnO particle size ~130 nmS4 · Preparation of ZnO Films
OtherFTO-coated and nonconducting glass slidesca. 6 cm x 4 cmS4 · Preparation of ZnO Films