Nitration of Halobenzenes and Thin Layer Chromatography

Purpose
: Nitrate a halobenzene and analyze the products by Thin Layer Chromatography (TLC) and PMR Spectroscopy.

Reading Preparation for the following week's lab:
Read Mayo, et al. pp. 122-124 and 148-150, and McMurry Ch.16.1-16.7.

Procedure
:  Add a spin vane and 2 ml of a prepared 1:1 mixture of concentrated nitric acid (16 molar) and concentrated sulfuric acid in a 5 mL conical vial.
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Safety note: Both nitric and sulfuric acids are very corrosive and cause serious burns. Treat these acids with caution!
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Attach the air condenser to the vial with a screw cap and an O-ring. Add 0.5 mL of halobenzene (obtain unknown from stockroom) with a pipet extending through the condenser; stir the reaction well. Add another 0.5 mL of the halobenzene five minutes later. Stir the reaction in a basin of hot water, maintained at 80oC, for 15 minutes. What evidence of a reaction have you observed?

Cool the vial to room temperature, remove the condenser and pour/scrape the reaction mixture into a 20 mL beaker containing 5 mL of water with 5 g ice.  Break up any lumps with a small spatula. (The experiment can be interrupted at this point.)

The product mixture can now be separated into a solid fraction and an oil fraction. Isolate the crude solid product by suction filtration with a Hirsch funnel attached to a clean test tube with sidearm. Wash the filter cake with 3-5 mL of ice water with aspiration.  Allow the ice water to drain through the crystals under suction and continue the aspiration until the solid is nearly dry. Weigh this crude solid product before purifying it by recrystallization in the next step.  Transfer the oil from the sidearm test tube to a smaller test tube for subsequent TLC analysis. What product(s) have possibly formed.

Transfer the crude solid from the filtration to a 25 mL Erlenmeyer flask and add 1 mL of 95% ethyl alcohol. Heat this mixture to boiling on the steam bath in order to dissolve the crude product. Set the flask aside and allow the contents to cool slowly to room temperature. Isolate the nearly pure crystals of nitrated product by suction filtration (clean Hirsch funnel.) Wash the crystals with ice cold alcohol, allowing the washes to drain into the filter flask.  Dry the crystals completely.  When the crystals have dried obtain their weight and melting point.   (Be sure to include all your solid product in a sealed plastic bag with your notebook upon submission of your report.)  About 0.6 g of crystals may be expected.   From the melting point, which isomer is it?  Obtain a PMR spectrum (see "additional common practices...") of the crystalline product in deuterated chlorofrom.   Make spectroscopic assignments of the important peaks and comment on the purity of your sample.  What is your pure product? 

The filtrate contains water and oil.  Be certain the oil has come through the Hirsch funnel or your yield of oil will be low.  The oil will be analyzed by TLC (thin layer chromatography, Mayo pp. 148-150) to identify the possible number of products formed. Using a Pasteur pipet transfer only the oil from the two-phase mixture into a 3 ml conical vial; add a small spatula-full of anhydrous Na2SO4 (What does anhydrous mean?) to remove traces of water from the oil (termed the mother liquor). Let the mother liquor dry for a few minutes and then transfer it with a Pasteur filter pipet (Mayo, et al. p 41) to a pre-weighed, clean, dry vial; reweigh, and save for TLC analysis.

Thin Layer Chromatography (TLC):
  Each student will carry out a TLC and report an Rf value for each spot obtained and estimate the ratio of the nitrohalobenzenes obtained.  As always, consult your lab text (Mayo pp. 148-150) for background information on TLC.

Prepare several micropipet spotters: snap off and discard the closed ends of several melting point capillary tubes. With both hands, rotate the tube in a flame until the glass softens. Remove the glass from the flame and immediately pull the tube into a fine capillary, approximately 30 cm long. Finally, snap off most of the fine part, approximately 6 cm from each open end. Two spotters can be made from each melting point tube. By dipping the narrow end of the spotter into a solution, approximately 2 µL of liquid will rise into the capillary.  This may take some practice and will vary depending on the nature of the solution you are spotting.

Obtain a 3½ x 10 cm TLC sheet which consists of a layer of silica gel spread over a plastic sheet (Mayo, et al. p. 148). Pencil in a faint starting line 1 cm from the edge of the plate (Fig. 5.53). Place a tiny spot (the smaller and more concentrated, the better) of your oil product mixture by tapping the tip of the spotter on the line. Allow the solvent to evaporate and re-tap the same point. Similarly place another spot from a solution of a small amount of the crystalline product dissolved in 1 drop of chloroform on another point on the line. Place the plate in a jar or beaker containing 0.25 cm of a 9:1 (v:v) hexane:chloroform solution (Fig. 5.54 - the TLC plate should be more upright), cover the jar or beaker and observe this solution rise on the plate. (Now might be a good time to get the melting point of the crystalline product while the TLC is developing.) When the solvent front has crept to within 1-2 cm from the top, remove the plate and immediately mark the point where the solvent front reached its highest point. Use the short wave ultraviolet lamp in the hood (always point this lamp away from you) to outline the developed spots with pencil. Use the centers of these spots to calculate the Rf values (Fig. 5.55) for each component of the mixture. Since a compound will have about the same Rf value whether it is run by itself or in a mixture, one of the spots from the mother liquor should coincide with the spot for the pure solid product. While it is under the lamp, make a visual estimate of the relative amounts of the two spots from the mother liquor (e.g. 1 part a : 3 parts b).

Spotting and developing the plates takes time and practice; be prepared to repeat this process many times until you get satisfactory results. Save the best plate in a sealed plastic bag and make a careful, scaled drawing of the spots on your plate in your notebook.  Place the "best" chromatogram in a sealed plastic bag in your notebook.

Discussion:
Usually the compound in a product mixture with the higher melting point will form crystals first. Was this the case in your product mixture?  Identify the compounds you formed and provide a rationale for your answer.

With TLC, the stationary phase, silica, is more polar than the solvent, hexane-chloroform; therefore, the less polar compounds will associate more with the mobile phase and thus travel farther. Based on drawings of the nitrated products, decide which isomer will have a larger Rf value. Is this the case?  Explain completely.

Look up in the Handbook the melting points, molar masses and densities of the mono-nitro derivatives you produced. Create a Reaction Table based on a balanced equation for the nitration (combine all products as if they were one product for this calculation) and tabulate under each compound the molar mass, density, and mass used as necessary to calculate the number of moles used of each reactant. Based on the amount of crude yield (crystals plus mother liquor) collected, calculate the percent yield overall for the nitration reaction.

Now setting the total crude yield as 100%, calculate the amounts of the individual products; one of the isomers will be all the crystals plus a fraction of the mother liquor based on the visual inspection of your TLC.  Show your calculations and reasoning. Compare this percent you obtained with the data in McMurry Table 16.1.

Conclusions
:  Identify the principal products of the reaction, their percent yields and melting points. Comment on the relationship between each compound's structure and its mobility in TLC. What information did the PMR spectrum provide?   Should you be able to distinguish between the isomers using PMR?   Why or why not?  What other technique could you use to differentiate between the isomers and specifically what results would you anticipate for each?

References:

"Mayo et al.": Mayo, D.W., Pike, R.M., Butcher, S.S. and Trumper, P.K. Microscale Techniques for the Organic Laboratory; Wiley: New York, 1991

"McMurry": McMurry, John, Organic Chemistry, 4th ed., Brooks/Cole Publishing Co.: Pacific Grove, CA, 1995.

The "Handbook": any of the recent editions of Weast, R.D. Handbook of Chemistry and Physics; The Chemical Rubber Co.: Cleveland, 1960-present.

Revised by SLP on 3/22/99.