Synthesis · Coarsening-induced hierarchically interconnected porous carbon polyhedrons for stretchable ionogel-based supercapacitors

15 structured synthesis routes

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

Complete recipeSource: SI

Route 1: Other

text only; SI page not rendered · Method - Synthesis of NIC and HIC

Metal precursorsCu@C_12h containing Cu nanoparticles

Linker precursorscarbon matrix from polymer@MOF

Solvents1 M HCl aqueous solution; DI water or ethanol wash

AdditivesHCl

Atmospherenot specified / ambient workup

Temperatureroom temperature not explicitly stated

Time48

Oxidant / reductantacid etching/removal of Cu nanoparticles

Work-upDispersed in 1 M HCl, shaken vigorously for 2 d with HCl changed daily; washed with DI water or ethanol until pH 7

Activationnone in this route; final CO2 activation is a separate route

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Other	Cu@C_12h	not specified	text only; SI page not rendered · Method - Synthesis of NIC and HIC
Acid	HCl	changed every day for 2 d · 1 M	text only; SI page not rendered · Method - Synthesis of NIC and HIC
Solvent	DI water or ethanol	wash until pH reaches 7	text only; SI page not rendered · Method - Synthesis of NIC and HIC

Complete recipeSource: SI

Route 2: Other

text only; SI page not rendered · Method - Synthesis of NIC and HIC

Metal precursorsCu@C_1h containing Cu nanoparticles

Linker precursorscarbon matrix from polymer@MOF

Solvents1 M HCl aqueous solution; DI water or ethanol wash

AdditivesHCl

Atmospherenot specified / ambient workup

Temperatureroom temperature not explicitly stated

Time48

Oxidant / reductantacid etching/removal of Cu nanoparticles

Work-upDispersed in 1 M HCl, shaken vigorously for 2 d with HCl changed daily; washed with DI water or ethanol until pH 7

Activationnone in this route; final CO2 activation is a separate route

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Other	Cu@C_1h	not specified	text only; SI page not rendered · Method - Synthesis of NIC and HIC
Acid	HCl	changed every day for 2 d · 1 M	text only; SI page not rendered · Method - Synthesis of NIC and HIC
Solvent	DI water or ethanol	wash until pH reaches 7	text only; SI page not rendered · Method - Synthesis of NIC and HIC

Partial recipeSource: SI

Route 3: Other

text only; SI page not rendered · Method - Synthesis of NIC and HIC

Metal precursorspolymer@MOF containing Cu sites

Linker precursorscarbonisable polymer@MOF organic components

Atmospherenot specified in extracted SI text

Temperature800

Time12

Oxidant / reductantthermal carbonisation/coarsening of Cu nanoparticles

Work-upnone reported before HCl etching

ActivationDirect carbonization at 800 degC with ramping rate 12.8 degC min-1

Show 1 structured reagent record

Role	Reagent	Amount / concentration	Source
Other	polymer@MOF	not specified	text only; SI page not rendered · Method - Synthesis of NIC and HIC

Partial recipeSource: SI

Route 4: Other

text only; SI page not rendered · Method - Synthesis of NIC and HIC

Metal precursorspolymer@MOF containing Cu sites

Linker precursorscarbonisable polymer@MOF organic components

Atmospherenot specified in extracted SI text

Temperature800

Time1

Oxidant / reductantthermal carbonisation/coarsening of Cu nanoparticles

Work-upnone reported before HCl etching

ActivationDirect carbonization at 800 degC with ramping rate 12.8 degC min-1

Show 1 structured reagent record

Role	Reagent	Amount / concentration	Source
Other	polymer@MOF	not specified	text only; SI page not rendered · Method - Synthesis of NIC and HIC

Partial recipeSource: Main

Route 5: Other

p002 / journal page 381 · Results and discussion · Figure S4 referenced

Metal precursorspolymer@MOF containing Cu sites

Linker precursorscarbonisable polymer@MOF organic components

Atmospherenot specified in extracted SI text

Temperature800

Time24

Oxidant / reductantthermal carbonisation/coarsening of Cu nanoparticles

Work-upnone reported before HCl etching

ActivationDirect carbonization at 800 degC with ramping rate 12.8 degC min-1

Show 1 structured reagent record

Role	Reagent	Amount / concentration	Source
Other	polymer@MOF	not specified	p002 / journal page 381 · Results and discussion · Figure S4 referenced

Partial recipeSource: SI

Route 6: Other

text only; SI page not rendered · Method - CO2 activation process

Metal precursorsaHIC derived carbon, nominally metal-free after etching

Linker precursorscarbon matrix

AdditivesCO2/N2 gas mixture

AtmosphereN2 heating, then CO2:N2 = 1:1 at 900 degC, then N2 cooling

Temperature900

Timevarious durations until SSA reaches near 3000 m2 g-1

Oxidant / reductantCO2 activation, C(s) + CO2(g) -> 2CO(g)

Work-upGas changed back to N2 after set activation time and cooled to room temperature

ActivationHot CO2 activation in horizontal quartz tube furnace; heating rate 30 degC min-1 under N2

Scalability contextActivation time varied by sample to match SSAs near 3000 m2 g-1.

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Other	aHIC	not specified	text only; SI page not rendered · Method - CO2 activation process
Other	N2	heating/cooling gas	text only; SI page not rendered · Method - CO2 activation process
Other	CO2:N2	activation gas · 1:1	text only; SI page not rendered · Method - CO2 activation process

Partial recipeSource: SI

Route 7: Other

text only; SI page not rendered · Method - CO2 activation process

Metal precursorsaMMC derived carbon, nominally metal-free after etching

Linker precursorscarbon matrix

AdditivesCO2/N2 gas mixture

AtmosphereN2 heating, then CO2:N2 = 1:1 at 900 degC, then N2 cooling

Temperature900

Timevarious durations until SSA reaches near 3000 m2 g-1

Oxidant / reductantCO2 activation, C(s) + CO2(g) -> 2CO(g)

Work-upGas changed back to N2 after set activation time and cooled to room temperature

ActivationHot CO2 activation in horizontal quartz tube furnace; heating rate 30 degC min-1 under N2

Scalability contextActivation time varied by sample to match SSAs near 3000 m2 g-1.

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Other	aMMC	not specified	text only; SI page not rendered · Method - CO2 activation process
Other	N2	heating/cooling gas	text only; SI page not rendered · Method - CO2 activation process
Other	CO2:N2	activation gas · 1:1	text only; SI page not rendered · Method - CO2 activation process

Complete recipeSource: SI

Route 8: Hydrothermal

text only; SI page not rendered · Method - Synthesis of MOF[Cu3(btc2)]

Metal precursorsCu(NO3)2·2.5H2O, 0.5 g

Linker precursors1,3,5-benzenetricarboxylic acid (BTC), 0.3 g

SolventsDMF, 15 mL; MeCN solvent exchange for 7 days

AdditivesNitric acid, 0.06 mL; PVP (M.W. ~55,000), 3.65 g (0.073 mmol) as modulator for 2 um mMOF

AtmosphereSealed vessel during heating; static vacuum during final activation

Temperature90; activation 80

Time16; activation 6

Work-upCentrifuged, washed with DMF 2 times, solvent-exchanged with MeCN for 7 days to remove residual PVP

Activation80 degC under static vacuum for 6 h before VPP

Scalability contextSize variants reported: 1 um MOF used same amounts except no nitric acid; 500 nm MOF used 1.22 g PVP.

Show 6 structured reagent records

Role	Reagent	Amount / concentration	Source
Metal Source	Cu(NO3)2·2.5H2O	0.5 g	text only; SI page not rendered · Method - Synthesis of MOF[Cu3(btc2)]
Linker	1,3,5-Benzenetricarboxylic acid (BTC)	0.3 g	text only; SI page not rendered · Method - Synthesis of MOF[Cu3(btc2)]
Solvent	DMF	15 mL	text only; SI page not rendered · Method - Synthesis of MOF[Cu3(btc2)]
Acid	Nitric acid	0.06 mL	text only; SI page not rendered · Method - Synthesis of MOF[Cu3(btc2)]
Additive	PVP (M.W.~55,000)	3.65 g (0.073 mmol)	text only; SI page not rendered · Method - Synthesis of MOF[Cu3(btc2)]
Solvent	MeCN	solvent exchange for 7 days	text only; SI page not rendered · Method - Synthesis of MOF[Cu3(btc2)]

Partial recipeSource: SI

Route 9: Other

text only; SI page not rendered · Method - Synthesis of MTP and MMC

Metal precursorspolymer@MOF; Cu2+ removed during EDTA etching

Linker precursorspolymer@MOF; btc ligands removed during EDTA etching

Solvents0.025 M EDTA solution, 200 mL; DI water wash

AdditivesEDTA

Atmospherecarbonization atmosphere not specified in extracted SI text

Temperature150 crosslinking; 90 drying; 800 carbonization

Time24 crosslinking; 1 carbonization

Oxidant / reductantselective MOF etching with EDTA; thermal carbonization

Work-upAnnealed 150 degC for 1 day, dispersed in 200 mL 0.025 M EDTA and shaken 2 days with EDTA changed daily; washed with DI water 3 times and dried at 90 degC

ActivationMTP directly carbonized at 800 degC for 1 h at 12.8 degC min-1 to produce aMMC/MMC precursor

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Other	polymer@MOF	not specified	text only; SI page not rendered · Method - Synthesis of MTP and MMC
Additive	EDTA solution	200 mL; changed every day · 0.025 M	text only; SI page not rendered · Method - Synthesis of MTP and MMC
Solvent	DI water	wash 3 times	text only; SI page not rendered · Method - Synthesis of MTP and MMC

Partial recipeSource: SI

Route 10: Other

text only; SI page not rendered · Method - CO2 activation process

Metal precursorsaNIC derived carbon, nominally metal-free after etching

Linker precursorscarbon matrix

AdditivesCO2/N2 gas mixture

AtmosphereN2 heating, then CO2:N2 = 1:1 at 900 degC, then N2 cooling

Temperature900

Timevarious durations until SSA reaches near 3000 m2 g-1

Oxidant / reductantCO2 activation, C(s) + CO2(g) -> 2CO(g)

Work-upGas changed back to N2 after set activation time and cooled to room temperature

ActivationHot CO2 activation in horizontal quartz tube furnace; heating rate 30 degC min-1 under N2

Scalability contextActivation time varied by sample to match SSAs near 3000 m2 g-1.

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Other	aNIC	not specified	text only; SI page not rendered · Method - CO2 activation process
Other	N2	heating/cooling gas	text only; SI page not rendered · Method - CO2 activation process
Other	CO2:N2	activation gas · 1:1	text only; SI page not rendered · Method - CO2 activation process

Complete recipeSource: Both

Route 11: Other

text only; SI page not rendered · Method - Synthesis of polymer@MOF

Metal precursors200 mg thermally activated mMOF/HKUST-1 with Lewis and Bronsted acid sites

Linker precursorsphenol and paraformaldehyde for phenol-formaldehyde polymer

SolventsMeCN wash

Additivesphenol, 340 mg; paraformaldehyde, 260 mg

AtmosphereStatic vacuum treatment for 1 min before heating

Temperature90

Time24

Work-upWashed with MeCN 2 times and dried at 90 degC in a convection oven

ActivationmMOF thermally activated before VPP as in route_mmof_hydrothermal

Show 4 structured reagent records

Role	Reagent	Amount / concentration	Source
Other	thermally activated MOF	200 mg	text only; SI page not rendered · Method - Synthesis of polymer@MOF
Other	phenol	340 mg	text only; SI page not rendered · Method - Synthesis of polymer@MOF
Other	paraformaldehyde	260 mg	text only; SI page not rendered · Method - Synthesis of polymer@MOF
Solvent	MeCN	wash 2 times	text only; SI page not rendered · Method - Synthesis of polymer@MOF

Complete recipeSource: Both

Route 12: Other

text only; SI page not rendered · Method - Fabrication and characterization of stretchable SCs

Metal precursorsHIC active carbon

SolventsDMF for electrode ink

AdditivesSWCNTs; Super-P; P(VDF-HFP); [EMI][TFSI]; Eco-flex rubber substrate/encapsulation

AtmosphereEncapsulated in glove box; electrochemical measurements in air

Temperature130 spray coating; 120 vacuum drying

Time1 bar-sonication; overnight vacuum drying

Substrate orientationpre-strained 100% Eco-flex rubber, released to 0% strain to form wavy electrodes

Work-upInk bar-sonicated, spray-coated, released to 0% strain, vacuum dried overnight, then sandwiched with P(VDF-HFP)/[EMI][TFSI] ionogel and encapsulated

Activationnot applicable

Scalability contextCurrent-collector-free stretchable SC; active-material fraction noted as a future improvement target in main text.

Show 7 structured reagent records

Role	Reagent	Amount / concentration	Source
Other	HIC	1 part by weight in electrode ink	text only; SI page not rendered · Method - Fabrication and characterization of stretchable SCs
Other	SWCNTs	1 part by weight in electrode ink	text only; SI page not rendered · Method - Fabrication and characterization of stretchable SCs
Other	Super-P	1 part by weight in electrode ink	text only; SI page not rendered · Method - Fabrication and characterization of stretchable SCs
Other	P(VDF-HFP)	1 part by weight in electrode ink; also ionogel polymer	text only; SI page not rendered · Method - Fabrication and characterization of stretchable SCs
Solvent	DMF	ink solvent	text only; SI page not rendered · Method - Fabrication and characterization of stretchable SCs
Electrolyte	[EMI][TFSI]	4 parts per 1 part P(VDF-HFP) in ionogel	text only; SI page not rendered · Method - Fabrication and characterization of stretchable SCs
Other	Eco-flex rubber	pre-strained 100% substrate and encapsulation	text only; SI page not rendered · Method - Fabrication and characterization of stretchable SCs

Complete recipeSource: SI

Route 13: Other

SI Method · Symmetric SC assembly

Metal precursorsMDC active carbon: HIC, NIC or MMC

SolventsNMP slurry solvent

AdditivesSuper-P; PVDF; [EMI][BF4] electrolyte; Whatman GF/D separator; Sigracet 29AA carbon paper

AtmosphereAr gas-filled glovebox for CR2032 coin-cell assembly

Temperature90 drying; 120 vacuum solvent-removal

Time24 at 120 degC vacuum

Substrate orientationSigracet 29AA carbon paper current collector

Work-upDip-coated slurry on carbon paper, dried at 90 degC, then heated 120 degC under static vacuum for 24 h

Activationnot applicable

Scalability contextFinal circular-disc electrode mass loading 0.8-1.0 mg through multiple dip coating.

Show 5 structured reagent records

Role	Reagent	Amount / concentration	Source
Other	MDC active carbon (HIC, NIC or MMC)	80 wt% of solids	SI Method · Symmetric SC assembly
Other	Super-P	10 wt% of solids	SI Method · Symmetric SC assembly
Other	PVDF	10 wt% of solids	SI Method · Symmetric SC assembly
Solvent	NMP	slurry solvent	SI Method · Symmetric SC assembly
Electrolyte	[EMI][BF4]	coin-cell electrolyte	SI Method · Symmetric SC assembly

Complete recipeSource: SI

Route 14: Other

SI Method · Symmetric SC assembly

Metal precursorsMDC active carbon: MMC

SolventsNMP slurry solvent

AdditivesSuper-P; PVDF; [EMI][BF4] electrolyte; Whatman GF/D separator; Sigracet 29AA carbon paper

AtmosphereAr gas-filled glovebox for CR2032 coin-cell assembly

Temperature90 drying; 120 vacuum solvent-removal

Time24 at 120 degC vacuum

Substrate orientationSigracet 29AA carbon paper current collector

Work-upDip-coated slurry on carbon paper, dried at 90 degC, then heated 120 degC under static vacuum for 24 h

Activationnot applicable

Scalability contextFinal circular-disc electrode mass loading 0.8-1.0 mg through multiple dip coating.

Show 5 structured reagent records

Role	Reagent	Amount / concentration	Source
Other	MMC	80 wt% of solids	SI Method · Symmetric SC assembly
Other	Super-P	10 wt% of solids	SI Method · Symmetric SC assembly
Other	PVDF	10 wt% of solids	SI Method · Symmetric SC assembly
Solvent	NMP	slurry solvent	SI Method · Symmetric SC assembly
Electrolyte	[EMI][BF4]	coin-cell electrolyte	SI Method · Symmetric SC assembly

Complete recipeSource: SI

Route 15: Other

SI Method · Symmetric SC assembly

Metal precursorsMDC active carbon: NIC

SolventsNMP slurry solvent

AdditivesSuper-P; PVDF; [EMI][BF4] electrolyte; Whatman GF/D separator; Sigracet 29AA carbon paper

AtmosphereAr gas-filled glovebox for CR2032 coin-cell assembly

Temperature90 drying; 120 vacuum solvent-removal

Time24 at 120 degC vacuum

Substrate orientationSigracet 29AA carbon paper current collector

Work-upDip-coated slurry on carbon paper, dried at 90 degC, then heated 120 degC under static vacuum for 24 h

Activationnot applicable

Scalability contextFinal circular-disc electrode mass loading 0.8-1.0 mg through multiple dip coating.

Show 5 structured reagent records

Role	Reagent	Amount / concentration	Source
Other	NIC	80 wt% of solids	SI Method · Symmetric SC assembly
Other	Super-P	10 wt% of solids	SI Method · Symmetric SC assembly
Other	PVDF	10 wt% of solids	SI Method · Symmetric SC assembly
Solvent	NMP	slurry solvent	SI Method · Symmetric SC assembly
Electrolyte	[EMI][BF4]	coin-cell electrolyte	SI Method · Symmetric SC assembly