Synthesis · Dimensional Control of Highly Anisotropic and Transparent Conductive Coordination Polymers for Solution-Processable Large-Scale 2D Sheets

20 structured synthesis routes

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

Complete recipeSource: SI

Route 1: Solution Shearing

3 · Experimental Method

Metal precursors59.87 mg CuCl2 in 10 mL ethanol

Linker precursors40.13 mg (3,5-dimethylphenyl)thiourea in 10 mL ethanol

SolventsEthanol; additional 30 mL

Atmosphereambient/air

Temperatureroom temperature

Time1

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Metal Source	CuCl2	59.87 mg CuCl2 · in 10 mL ethanol	3 · Experimental Method
Linker	40.13 mg (3	40.13 mg (3,5-dimethylphenyl)thiourea · in 10 mL ethanol	3 · Experimental Method
Solvent	Ethanol; additional 30 mL	see solvents field	3 · Experimental Method

Complete recipeSource: SI

Route 2: Solution Shearing

3 · Experimental Method

Metal precursors27.16 mg CuCl2 in 10 mL ethanol

Linker precursors72.84 mg (3,5-dimethylphenyl)thiourea in 20 mL ethanol

SolventsEthanol plus additional 20 mL ethylene glycol

Atmosphereambient/air

Temperatureroom temperature

Time1.5

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Metal Source	CuCl2	27.16 mg CuCl2 · in 10 mL ethanol	3 · Experimental Method
Linker	72.84 mg (3	72.84 mg (3,5-dimethylphenyl)thiourea · in 20 mL ethanol	3 · Experimental Method
Solvent	Ethanol plus additional 20 mL ethylene glycol	see solvents field	3 · Experimental Method

Complete recipeSource: Both

Route 3: Solution Shearing

7 · Experimental Section

Metal precursorsCuCl2, 63.86 mg in 10 mL ethanol

Linker precursorsThiourea, 36.14 mg in 10 mL ethanol

SolventsEthanol; additional 30 mL ethanol

Atmosphereambient/air

Temperatureroom temperature

Time0.5

Oxidant / reductantCu(II) reduced to Cu(I) during CuCl-TU formation

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Metal Source	CuCl2	63.86 mg · in 10 mL ethanol	7 · Experimental Section
Linker	thiourea	36.14 mg · in 10 mL ethanol	7 · Experimental Section
Solvent	ethanol	10 mL + 10 mL + 30 mL · 99.9% for initial solutions	7 · Experimental Section

Complete recipeSource: Both

Route 4: Liquid Liquid Interface

7 · Experimental Section

Metal precursorsCuCl2, 31.93 mg in 5 mL ethanol

Linker precursorsThiourea, 18.07 mg in 45 mL diethylene glycol; 5 mL aliquot layered

SolventsEthanol and diethylene glycol (DEG)

Atmosphereambient/air

Temperatureroom temperature

Work-upNanosheets quickly extracted from intermediate liquid layer/interface before rolling-up.

Show 4 structured reagent records

Role	Reagent	Amount / concentration	Source
Metal Source	CuCl2	31.93 mg · in 5 mL ethanol	7 · Experimental Section
Linker	thiourea	18.07 mg · in 45 mL DEG; 5 mL used	7 · Experimental Section
Solvent	diethylene glycol	45 mL	7 · Experimental Section
Solvent	ethanol	5 mL	7 · Experimental Section

Complete recipeSource: Both

Route 5: Solution Shearing

7 · Experimental Section

Metal precursorsCuCl2, 44.0 mg in 20 mL ethanol

Linker precursorsThiourea, 25.0 mg in 20 mL ethanol

SolventsEthanol; additional 60 mL ethanol

Atmosphereambient/air

Temperatureroom temperature

Time0.167

Oxidant / reductantCu(II) reduced to Cu(I) during exchange of chlorine with thiourea ligand

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Metal Source	CuCl2	44.0 mg · in 20 mL ethanol	7 · Experimental Section
Linker	thiourea	25.0 mg · in 20 mL ethanol	7 · Experimental Section
Solvent	ethanol	20 mL + 20 mL + 60 mL	7 · Experimental Section

Complete recipeSource: SI

Route 6: Drop Cast

3 · Experimental Method

Metal precursorsCuCl2 as in route_cucl_tu_2d

Linker precursorsThiourea as in route_cucl_tu_2d

SolventsEthanol/DEG interfacial CuCl-TU solution

AdditivesPt coating on silicon wafer by ion sputter

Atmosphereair; dried in vacuum after washing

Temperatureroom temperature

Time0.5 drying

Substrate orientationPt-coated silicon wafer, 20 x 20 mm; also Si/SiO2/Au pads for electrical measurement

Work-upDrop 0.2 mL interfacial solution on wafer, dry 30 min in air, gently wash with hexane, dry in vacuum.

Show 2 structured reagent records

Role	Reagent	Amount / concentration	Source
Other	Pt-coated silicon wafer	20x20 mm; sputtered at 15 mA for 20 s	3 · Experimental Method
Solvent	hexane	wash	3 · Experimental Method

Complete recipeSource: SI

Route 7: Drop Cast

4 · Experimental Method

Metal precursorsCuCl2 as in route_cucl_tu_2d

Linker precursorsThiourea as in route_cucl_tu_2d

SolventsEthanol/DEG interfacial CuCl-TU solution

AdditivesSurface-treated superhydrophilic PC film with SiOx coating

Atmosphereair drying followed by vacuum drying

Temperatureroom temperature

Time0.5 air drying plus 5 h vacuum drying

Substrate orientationO2-plasma and HMDSO/O2-treated PC film, 30 x 30 mm

Work-upDrop 0.2 mL on treated PC, dry 30 min in air, dip into hexane for washing, dry in vacuum for 5 h.

Show 2 structured reagent records

Role	Reagent	Amount / concentration	Source
Other	surface treated polycarbonate film	30x30 mm · SiOx layer 20 nm	4 · Experimental Method
Solvent	hexane	wash	4 · Experimental Method

Complete recipeSource: SI

Route 8: Solution Shearing

2 · Experimental Method

Metal precursors56.34 mg CuCl2 in 10 mL ethanol

Linker precursors43.66 mg N-(ethyl)thiourea in 10 mL ethanol

SolventsEthanol; additional 30 mL

Atmosphereambient/air

Temperatureroom temperature

Time2

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Metal Source	CuCl2	56.34 mg CuCl2 · in 10 mL ethanol	2 · Experimental Method
Linker	43.66 mg N-(ethyl)thiourea	43.66 mg N-(ethyl)thiourea · in 10 mL ethanol	2 · Experimental Method
Solvent	Ethanol; additional 30 mL	see solvents field	2 · Experimental Method

Complete recipeSource: SI

Route 9: Liquid Liquid Interface

2 · Experimental Method

Metal precursors28.16 mg CuCl2 in 1 mL ethanol

Linker precursors21.84 mg N-(ethyl)thiourea in 49 mL DEG; 3 mL aliquot layered

SolventsEthanol/diethylene glycol

Atmosphereambient/air

Temperatureroom temperature

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Metal Source	CuCl2	28.16 mg CuCl2 · in 1 mL ethanol	2 · Experimental Method
Linker	21.84 mg N-(ethyl)thiourea	21.84 mg N-(ethyl)thiourea · in 49 mL DEG; 3 mL aliquot layered	2 · Experimental Method
Solvent	Ethanol/diethylene glycol	see solvents field	2 · Experimental Method

Complete recipeSource: SI

Route 10: Solution Shearing

2 · Experimental Method

Metal precursors56.34 mg CuCl2 in 20 mL ethanol

Linker precursors43.66 mg N-(ethyl)thiourea in 20 mL ethanol

SolventsEthanol; additional 60 mL

Atmosphereambient/air

Temperatureroom temperature

Time2

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Metal Source	CuCl2	56.34 mg CuCl2 · in 20 mL ethanol	2 · Experimental Method
Linker	43.66 mg N-(ethyl)thiourea	43.66 mg N-(ethyl)thiourea · in 20 mL ethanol	2 · Experimental Method
Solvent	Ethanol; additional 60 mL	see solvents field	2 · Experimental Method

Complete recipeSource: SI

Route 11: Solution Shearing

3 · Experimental Method

Metal precursors44.71 mg CuCl2 in 10 mL ethanol

Linker precursors55.29 mg N-(m-tolyl)thiourea in 10 mL ethanol

SolventsEthanol; additional 30 mL

Atmosphereambient/air

Temperatureroom temperature

Time1

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Metal Source	CuCl2	44.71 mg CuCl2 · in 10 mL ethanol	3 · Experimental Method
Linker	55.29 mg N-(m-tolyl)thiourea	55.29 mg N-(m-tolyl)thiourea · in 10 mL ethanol	3 · Experimental Method
Solvent	Ethanol; additional 30 mL	see solvents field	3 · Experimental Method

Complete recipeSource: SI

Route 12: Other

4 · Experimental Method · Figure S32

Metal precursors3D CuCl-(m-tolyl)TU powder, 25 mg

Linker precursorsN-(m-tolyl)thiourea already incorporated

Solvents50 mL ethanol

AdditivesZirconia balls, 1 mm, 3 mm and 10 mm diameter

Atmosphereambient/air

Temperatureroom temperature

Time2 h milling plus 0.5 h ultrasonication

Work-upBall-milled at 60 rpm for 2 h, then ultrasonicated for 30 min.

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Other	3D CuCl-(m-tolyl)TU powder	25 mg · in 50 mL ethanol	4 · Experimental Method · Figure S32
Solvent	ethanol	50 mL	4 · Experimental Method · Figure S32
Other	zirconia balls	1, 3, and 10 mm diameter	4 · Experimental Method · Figure S32

Complete recipeSource: SI

Route 13: Solution Shearing

3 · Experimental Method

Metal precursors24.44 mg CuCl2 in 10 mL ethanol

Linker precursors75.56 mg N-(m-tolyl)thiourea in 10 mL ethanol

SolventsEthanol; additional 30 mL

Atmosphereambient/air

Temperatureroom temperature

Time1

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Metal Source	CuCl2	24.44 mg CuCl2 · in 10 mL ethanol	3 · Experimental Method
Linker	75.56 mg N-(m-tolyl)thiourea	75.56 mg N-(m-tolyl)thiourea · in 10 mL ethanol	3 · Experimental Method
Solvent	Ethanol; additional 30 mL	see solvents field	3 · Experimental Method

Complete recipeSource: SI

Route 14: Solution Shearing

2 · Experimental Method

Metal precursors59.86 mg CuCl2 in 10 mL ethanol

Linker precursors40.14 mg N-(methyl)thiourea in 10 mL ethanol

SolventsEthanol; additional 30 mL

Atmosphereambient/air

Temperatureroom temperature

Time0.5

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Metal Source	CuCl2	59.86 mg CuCl2 · in 10 mL ethanol	2 · Experimental Method
Linker	40.14 mg N-(methyl)thiourea	40.14 mg N-(methyl)thiourea · in 10 mL ethanol	2 · Experimental Method
Solvent	Ethanol; additional 30 mL	see solvents field	2 · Experimental Method

Complete recipeSource: SI

Route 15: Liquid Liquid Interface

2 · Experimental Method

Metal precursors29.93 mg CuCl2 in 3 mL ethanol

Linker precursors20.07 mg N-(methyl)thiourea in 47 mL DEG; 5 mL aliquot layered

SolventsEthanol/diethylene glycol

Atmosphereambient/air

Temperatureroom temperature

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Metal Source	CuCl2	29.93 mg CuCl2 · in 3 mL ethanol	2 · Experimental Method
Linker	20.07 mg N-(methyl)thiourea	20.07 mg N-(methyl)thiourea · in 47 mL DEG; 5 mL aliquot layered	2 · Experimental Method
Solvent	Ethanol/diethylene glycol	see solvents field	2 · Experimental Method

Complete recipeSource: SI

Route 16: Solution Shearing

2 · Experimental Method

Metal precursors59.86 mg CuCl2 in 20 mL ethanol

Linker precursors40.14 mg N-(methyl)thiourea in 20 mL ethanol

SolventsEthanol; additional 60 mL

Atmosphereambient/air

Temperatureroom temperature

Time0.5

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Metal Source	CuCl2	59.86 mg CuCl2 · in 20 mL ethanol	2 · Experimental Method
Linker	40.14 mg N-(methyl)thiourea	40.14 mg N-(methyl)thiourea · in 20 mL ethanol	2 · Experimental Method
Solvent	Ethanol; additional 60 mL	see solvents field	2 · Experimental Method

Complete recipeSource: SI

Route 17: Solution Shearing

3 · Experimental Method

Metal precursors69.47 mg CuCl2 in 10 mL ethanol

Linker precursors20.53 mg N-(propyl)thiourea in 10 mL ethanol

SolventsEthanol; additional 30 mL

Atmosphereambient/air

Temperatureroom temperature

Time1

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Metal Source	CuCl2	69.47 mg CuCl2 · in 10 mL ethanol	3 · Experimental Method
Linker	20.53 mg N-(propyl)thiourea	20.53 mg N-(propyl)thiourea · in 10 mL ethanol	3 · Experimental Method
Solvent	Ethanol; additional 30 mL	see solvents field	3 · Experimental Method

Complete recipeSource: SI

Route 18: Solution Shearing

3 · Experimental Method

Metal precursors36.25 mg CuCl2 in 10 mL ethanol

Linker precursors63.75 mg N-(propyl)thiourea in 10 mL ethanol

SolventsEthanol; additional 30 mL

Atmosphereambient/air

Temperatureroom temperature

Time1

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Metal Source	CuCl2	36.25 mg CuCl2 · in 10 mL ethanol	3 · Experimental Method
Linker	63.75 mg N-(propyl)thiourea	63.75 mg N-(propyl)thiourea · in 10 mL ethanol	3 · Experimental Method
Solvent	Ethanol; additional 30 mL	see solvents field	3 · Experimental Method

Complete recipeSource: SI

Route 19: Solution Shearing

2 · Experimental Method

Metal precursors50.42 mg CuCl2 in 10 mL ethanol

Linker precursors49.58 mg N-(tert-butyl)thiourea in 10 mL ethanol

SolventsEthanol; additional 30 mL

Atmosphereambient/air

Temperatureroom temperature

Time0.5

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Metal Source	CuCl2	50.42 mg CuCl2 · in 10 mL ethanol	2 · Experimental Method
Linker	49.58 mg N-(tert-butyl)thiourea	49.58 mg N-(tert-butyl)thiourea · in 10 mL ethanol	2 · Experimental Method
Solvent	Ethanol; additional 30 mL	see solvents field	2 · Experimental Method

Complete recipeSource: SI

Route 20: Solution Shearing

2 · Experimental Method

Metal precursors50.42 mg CuCl2 in 10 mL ethanol

Linker precursors49.58 mg N-(tert-butyl)thiourea in 10 mL ethanol

SolventsEthanol; additional 30 mL

Atmosphereambient/air

Temperatureroom temperature

Time12

Show 3 structured reagent records

Role	Reagent	Amount / concentration	Source
Metal Source	CuCl2	50.42 mg CuCl2 · in 10 mL ethanol	2 · Experimental Method
Linker	49.58 mg N-(tert-butyl)thiourea	49.58 mg N-(tert-butyl)thiourea · in 10 mL ethanol	2 · Experimental Method
Solvent	Ethanol; additional 30 mL	see solvents field	2 · Experimental Method