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Column lengths of 30 to 250 mm are commonly used today, with particles that are 1.5 to 5μm in diameter larger particles are used for preparative separations; see Chapter 15.. 5.2 COLUMN

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196 DETECTION

Figure 4.37 shows an example of the popular post-column derivatization of amino acids with ninhydrin followed by UV detection at 405 nm In this case

45 amino acids and related substances are separated on an ion exchange column followed by reaction with ninhydrin at 130◦C in a 500-μL reactor (residence time

≈45 sec) Sample derivatization and reaction detectors have gradually lost popularity

as other HPLC detectors have been introduced and been made more effective

REFERENCES

1 G Hesse and H Weil, eds., Michael Tswett’s First Paper on Chromatography,

M Woelm, Eschwege, 1954

2 V G Berezkin, ed., Chromatographic Adsorption Analysis: Selected Works of

M S Tswett, Ellis Horwood, New York, 1990.

3 A Tiselius and D Claesson, Arkiv Kemi Mineral Geol., 15B (18) (1942) 1.

4 A J P Martin and S S Randall, Biochem J., 49 (1951) 293.

5 C G Horv ´ath and S R Lipsky, Nature, 211 (1966) 748.

6 J J Kirkland, Anal Chem., 40 (1968) 391.

7 E Haahti and T Nikkari, Acta Chem Scand., 17 (1963) 2565.

8 R P W Scott and J G Lawrence, J Chromatogr Sci., 11 (1970) 65.

9 B G Julin, H W Vandenborn, and J J Kirkland, J Chromatogr., 112 (1975) 443.

10 J W Dolan and J N Seiber, Anal Chem., 49 (1977) 326.

11 L R Snyder and J J Kirkland, Introduction to Modern Liquid Chromatography, 1st

ed., Wiley, New York, 1979, p 136

12 J W Dolan, LCGC, 14 (1996) 378.

13 L R Snyder and J W Dolan, High-Performance Gradient Elution, Wiley, New York,

2007

14 J J Kirkland, W W Yau, H J Stoklosa, and C H Dilks, Jr., J Chromatogr Sci., 15

(1977) 303

15 J C Sternberg, in Advances in Chromatography, Vol 2, J C Giddings and R A Keller,

eds., Dekker, New York, 1966, p 205

16 D Parriott, A Practical Guide to HPLC Detection, Academic Press, San Diego, 1993.

17 R P W Scott, in Handbook of HPLC (Chromatographic Science Series, Vol 78), E.

Katz, R Eksteen, P Schoenmakers, and N Miller, eds., Dekker, New York, 1998, ch 15

18 D T Bach, US Patent 4,867,559 (Sept 19, 1989).

19 M H Garrett, US Patent 6,542,231 (Apr 1, 2003).

20 G Cameron, P E Jackson, and M V Gorenstein, Chem Aust., 60 (1993) 288.

21 A G Frenich, J R Torres-Laasio, K De Braekeleer, D L Massart, J L Martinez-Vidal,

and M M Galera, J Chromatogr A, 855 (1999) 487.

22 Waters 996 Photodiode Detector: Peak Purity III: Interpretation of Peak Purity Plots

Appl Note 970983, Waters, 1996

23 F K Glowka and M Karazniewicz-Lada, J Chromatogr B, 852 (2007) 669.

24 P Vinas, N Balsalobre, C Lopez-Erroz, and M Hernandez-Cordoba, J Agr Food

Chem., 52 (2004) 1789.

25 S R Bakalyar, M P T Bradley, and R Honganen, J Chromatogr., 158 (1978) 277.

26 Y.-T Wu, T.-R Tsai, L.-C Lin, and T.-H Tsai, J Chromatogr B, 853 (2007) 281.

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REFERENCES 197

27 I N Ackworth, Coulometric Electrode Array Detectors for HPLC (Progress in

HPLC-HPCE, Vol 6), Brill Academic, Boston, 1997.

28 R E Parks and R L Marietta, US Patent 4018562 (1975)

29 Model 8060 Nitrogen Specific HPLC Detector, brochure A-8060-99-25M, Antek

Instru-ments, Houston, TX, 1999

30 K Petritis, C Elfakir, and M Dreux, LCGC Europe, 14 (2001) 389.

31 Jasco Incorporated, LCGC Applications Notebook (June 2003) 26.

32 L Kott, W B Holzheuer, M M Wong, and G K Webster, J Pharm Biomed Anal.,

43 (2007) 57

33 F Glowka, M K Lada, G Grund, and J Wachowiak, J Chromatogr B, 850 (2007)

569

34 L B Allen, J A Koropchak, and B Szostek, Anal Chem., 67 (1995) 659.

35 Quant Technologies, QT-500 datasheet (2/ 2007)

36 D Asa, Amer Lab., 38(7) (2006) 16.

37 T Gorecki, F Lynen, R Szucs, and P Sandra, Anal Chem., 78 (2006) 3186.

38 W M A Niessen, Liquid Chromatography-Mass Spectrometry (Chromatographic

Science Series, Vol 97), 3rd ed., Taylor and Francis, London, 2006.

39 M C McMaster, LC-MS: A Practical User’s Guide, Wiley, Hoboken, NJ, 2005.

40 Current Practice in Liquid Chromatography-Mass Spectrometry, W M A Niessen and

R D Voyksner, eds., Elsevier, Amsterdam, 1998

41 I D Wilson and U A Th Brinkman, J Chromatogr A., 1000 (2003) 325.

42 S W Huffman, K Lukasiewicz, S Geldart, S Elliott, J F Sperry, and C W Brown,

Anal Chem., 75 (2003) 4606.

43 G W Somsen, G Gooijer, and U A Th Brinkman, J Chromatogr A., 856 (1999)

213

44 S Down, Spectro Europe, 16 (2004) 8.

45 K Albert, J Chromatogr A, 856 (1999) 199.

46 A J Simpson, L.-H Tseng, M J Simpson, M Spraul, U Braumann, W L Kingery, B

P Kelleher, and M H B Hayes, Analyst, 129 (2004) 1216.

47 K Blau and J M Halket, eds., Handbook of Derivatives for Chromatography, 2nd ed.,

Wiley, New York, 1993

48 Application Manual: Amino Acids, Pickering Laboratories, Mountain View, CA, 2002.

49 Z Xie, W Shi, L Liu, and Q Deng, J Chromatogr B, 857 (2007) 53.

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CHAPTER FIVE THE COLUMN

5.1 INTRODUCTION, 200

5.2 COLUMN SUPPORTS, 200

5.2.1 Particle Characterization, 201

5.2.2 Silica Supports, 203

5.2.3 Porous Polymers, 212

5.2.4 Monoliths, 212

5.2.5 Other Inorganic Particles, 214

5.3 STATIONARY PHASES, 217

5.3.1 ‘‘Bonded’’ Stationary Phases, 218

5.3.2 Other Organic-Based Stationary Phases, 223

5.3.3 Column Functionality (Ligand Type), 225

5.4 COLUMN SELECTIVITY, 227

5.4.1 Basis of RPC Column Selectivity, 227

5.4.2 Column Reproducibility and ‘‘Equivalent’’ Columns, 235

5.4.3 Orthogonal Separation, 236

5.4.4 Other Applications of Column Selectivity, 237

5.5 COLUMN HARDWARE, 238

5.5.1 Column Fittings, 238

5.5.2 Column Configurations, 239

5.6 COLUMN-PACKING METHODS, 240

5.6.1 Dry-Packing, 240

5.6.2 Slurry-Packing of Rigid Particles, 240

5.6.3 Soft Gels, 244

5.7 COLUMN SPECIFICATIONS, 244

5.7.1 Manufacturing Standards, 244

5.7.2 Column Plate Number, 245

5.8 COLUMN HANDLING, 246

Introduction to Modern Liquid Chromatography, Third Edition, by Lloyd R Snyder,

Joseph J Kirkland, and John W Dolan

Copyright © 2010 John Wiley & Sons, Inc.

199

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200 THE COLUMN

The column—the ‘‘heart’’ of the HPLC system—has changed greatly from the beginning of HPLC in the mid-1960s Columns have been improved for greater separation speed and efficiency, as well as increased stability and reproducibility New stationary phases have been introduced for the extension of HPLC to a wider range of sample types, or for better separations of compounds that have in the past proved problematic Today it is rare that a column cannot be found for solving

a particular HPLC separation problem Early columns were made of glass, but the need for higher pressure operation quickly led to the exclusive use of metal columns With the passage of time, columns became shorter and particles smaller

(Fig 1.5g, h) Column lengths of 30 to 250 mm are commonly used today, with

particles that are 1.5 to 5μm in diameter (larger particles are used for preparative separations; see Chapter 15)

In this chapter we will examine the HPLC column, including the bare particle

or support, the added (‘‘bonded’’) stationary phase, and the column hardware.

Porous-silica particles in packed beds (as in Fig 2.2) are most commonly used Particles can also be made from solids other than silica; the main value of non-silica particles is their greater stability for use with extremes of temperature or mobile-phase pH Of special current interest are columns packed with very small particles (<3 μm) for carrying out fast separations (Section 2.5.3.2).

Although very few workers will produce their own bonded-phase particles (‘‘column packings’’), we will describe briefly how these materials are made; this information can prove helpful in choosing a column or for troubleshooting Column characteristics that affect reversed-phase retention and selectivity (Section 5.4) can also influence our selection of a column for a particular application Column-packing methods (Section 5.6) are described as further background for how ‘‘good’’ columns are prepared Column testing is covered in Section 5.7 Finally, column specifications and column handling techniques are covered in Sections 5.7 and 5.8, as an aid for good laboratory practice

Column packings consist of a rigid support plus an attached stationary phase (as

in Fig 2.2b, which shows a silica particle with attached C18 groups) In some cases the support and stationary phase are the same; for example, an unbonded silica particle is often used for normal-phase chromatography (Chapter 8) Silica

monoliths (Section 5.2.4) represent an alternative column support of more recent

vintage Monoliths refer to columns composed of an interconnected, porous bed, as opposed to columns packed with distinct particles (a monolith may be thought of as one big particle that fills the entire column) In this section we will describe column supports, their characterization, and how their properties affect their final use Later,

we will discuss (1) how these supports can be modified to create column packings for different purposes (Section 5.3) and (2) how the final particles are packed into the column (Section 5.6)

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5.2 COLUMN SUPPORTS 201 5.2.1 Particle Characterization

Particles can be characterized by their configuration or type, physical dimensions (particle diameter), the nature and size of pores within the particle, and surface area The importance of particle diameter in influencing separation has been discussed (Fig 1.5 and Section 2.4) Pore size and surface area are usually related reciprocally; as pore diameter increases, the surface area decreases in roughly the same proportion The phase ratio Ψ (Section 2.3.1) is roughly proportional to surface area, and

retention is proportional toΨ (Eq 2.3); therefore retention increases as pore size

decreases and column surface area increases The maximum weight of sample that can be injected is also proportional to surface area (Section 2.6.2), so a greater surface area is usually desirable—which suggests the use of the smallest possible pore diameter (and smallest pores) However, solute molecules must be able to enter the pores without hindrance, and this requires pores that are larger than the solute molecule For compounds with molecular weights <500 Da, the average

pore diameter should preferably be about 9 nm or larger Larger molecules require larger pores; for example, proteins are usually separated with 30-nm-pore particles

(Section 13.3.1.1) The interstitial volume of the column is the space between

particles; it is usually about 40% of the total column volume

The physical characteristics of particles are important, and manufacturers monitor these particle properties in various ways The size of the particles is especially important, as this largely determines the efficiency of the packed column While optical microscopy and air or liquid elutriation (or classification) methods can provide this information, instruments for the measurement of particle size (e.g., the Coulter counter) are more convenient and quantitative; they can also provide

a particle-size distribution A narrow particle-size distribution is preferred, as this

favors larger values of N (Section 5.2.2.1), and provides lower column pressure for

comparable efficiency

Particle surface-area, average pore-diameter, and pore-diameter distribu-tion typically are measured by the adsorpdistribu-tion of nitrogen or argon, using the

Brunauer–Emmett–Teller (BET) procedure Particles with average pore-diameters

>30 nm (which are used less commonly) are preferably characterized by mercury

intrusion, which also can be used to measure pores as small as 3 nm Mercury intrusion does not work well for fragile particles (with a large pore volume) or for soft polymer particles Reference [1] should be consulted for additional information

on the measurement of the physical characteristics of HPLC particles

5.2.1.1 Particle Type

As illustrated in Figure 5.1, several particle configurations are currently available for

HPLC Totally porous silica particles (Fig 5.1a) are the most common because of

their greater column capacity (allowing the injection of a larger sample weight) and availability in a wider variety of options (stationary phase, particle and pore size, column dimensions, etc.) The most popular particles have diameters in the 1.5- to 5-μm range Today these particles are often prepared by the aggregation of much smaller spheres (Section 5.2.2.3)

Pellicular particles (Fig 5.1b) consist of solid, spheres that are covered with a

very thin surface layer of stationary phase These silica- or polymer-based particles (presently 1.5 to 2.5μm in diameter, but much larger in the past) display larger

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202 THE COLUMN

Porous-shell particle

Porous

shell

solid core

throughpores

Perfusion particle

diffusive pore

Micro-pellicular particle

solid core

(b)

(d) (c)

Porous particle

(a)

Figure5.1 Different particle configurations

values of N for macromolecules, because of better stationary-phase mass-transfer

(smaller C-term, Section 2.4.1.1; [2, 3]) Because of their very low surface area, these particles exhibit greatly reduced retention and are limited to much smaller weights

of injected sample (with a proportional decrease in detection sensitivity) Pellicular particles are best suited for the analysis of major components (rather than trace impurities), and have been used mainly for the separation of large biomolecules (Chapter 13)

Superficially porous particles (also called fused-core ™ particles, shell particles,

or controlled-surface-porosity particles) have a solid core with a porous outer shell (Fig 5.1c) These particles typically have diameters of 2 to 5μm, with porous shells

of 0.25 to 0.5 μm in thickness Superficially porous particles have much greater surface areas than pellicular particles (∼3/4 as large as fully porous particles), providing longer retention and allowing a larger weight of injected sample The thin, outer porous shell permits faster separations—especially for macromolecules

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5.2 COLUMN SUPPORTS 203

[4, 5] These particles also provide somewhat higher values of N than totally porous

particles (Section 5.2.2.1)

Perfusion particles (Fig 5.1d) contain very large (e.g., 400- to 800-nm) pores

(through-pores), connected to a network of smaller (e.g., 30- to 100-nm) pores.

By comparison, most other particles have pore diameters of 8 to 30 nm (diffusive

pores) At high flow rates, solutes are carried into and out of perfusion particles by a

combination of diffusion and flow of mobile phase through the particle [6, 7] This

additional contribution to stationary-phase mass transfer is claimed to reduce band broadening, especially for large molecules at higher flow rates Perfusion particles are usually larger (e.g., 10μm), permitting their use at lower pressures These particles are best suited for preparative-scale separations of macromolecules such as proteins; they are little used for the analysis of small molecules

5.2.1.2 Particle Size and Pore Diameter

From 1980 to 2000, particles with diameters of ∼5 μm were generally preferred for routine separation Particles of this size represent a good compromise in terms

of efficiency, pressure drop, convenience, equipment requirements, and column lifetime However, columns with particle diameters of 3 μm and smaller are becoming more popular, mainly as a means for decreasing run time and increasing sample throughput (Sections 2.5.3.2, 9.3.9.2) Because of the very narrow peaks generated by small-particle columns, any extra-column peak broadening must be minimized (Sections 2.4.1.1, 3.9), especially when smaller diameter columns are used Columns with particle diameters<2 μm are used mainly with equipment that

is capable of higher pressure operation (e.g., up to 15,000 psi; Section 3.5.4.3) Table 5.1 summarizes some physical characteristics of HPLC particles and their effect on separation from favorable (‘‘4’’) to unfavorable (‘‘1’’) Totally porous and superficially porous particles with pore diameters of 8 to 12 nm are used most often for the separation of molecules smaller than 10,000 Da These column-packings have surface areas of about 125 to 400 m2/g, which allow injected sample weights

of ≈50 μg (for column inner-diameters of 4–5 mm) Because peaks as small as a few nanograms can be measured, both major and trace components can be assayed

in a single separation (or ‘‘run’’) with these columns

Larger molecules (usually biomolecules such as proteins) require larger pores,

to avoid restricted diffusion within the pore, with a resulting decrease in column efficiency (Section 13.3.1.1) Column packings with ≈30-nm pores typically are used for separating molecules larger than 10,000 Da If the pore diameter is at least four times larger than the hydrodynamic diameter of the solute molecule, hindered

diffusion and lower values of N will be avoided [8] Wider pores also mean smaller

surface areas and decreased sample weights C18 columns are used most often for reversed-phase chromatography (RPC); the physical properties of some popular columns of this type are shown in Table 5.2

5.2.2 Silica Supports

Silica in the form of either particles or monoliths is the most commonly used support for the production of HPLC packings High mechanical strength is a strong advantage for silica particles, allowing the formation of packed beds that are stable for long periods and high operating pressures Silica-based columns also provide

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204 THE COLUMN

Table 5.1

Separation Characteristics of Particles for HPLC Columns

Pore diameter

7- to 12-nm pores Small-molecule separations (<10, 000 Da)

(150–400 m 2 /g)

15- to 100-nm pores Large-molecule separations (>10, 000 Da)

(5–150 m 2 /g)

Note: Ratings in terms of advantage from moderate (1) to high (4).

aAbility to tolerate high pressures or a rapid change in pressure.

Table 5.2

Properties of Some Commercial C 18 Particles

Packing Material Pore Diameter Surface Area Carbon Bonded-Phase

(nm) (m 2 /g) Load (%) Coverage (μmol/m 2 )

aSuperficially porous particles; other particles are totally porous.

bHybrid stationary phase (Section 5.3.2.2).

cData not available.

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5.2 COLUMN SUPPORTS 205

higher values of N, compared to other support materials (Section 5.2.5) Spherical

particles can be synthesized with a wide choice of pore sizes (e.g., 10, 30, 100 nm), particle sizes (e.g., 1.5, 2.7, 3.5, 5μm), and in different particle configurations (as

in Fig 5.1) Silica also can be used for monolithic columns (Section 5.2.4)

Another advantage of silica is that it can be bonded with different ligands (e.g.,

C8, C18, phenyl, and cyano; Section 5.3.1) for use with different samples and to change separation selectivity Silica-based columns are compatible with all organic solvents and water, and do not swell or shrink with a change of solvent (as can be the case for polymeric particles; Section 5.2.3); silica particles are especially suited for gradient elution, where the mobile-phase composition changes during the separation Silica begins to dissolve in the mobile phase at pH> 8 [9], which can result in a short

lifetime for columns packed with silica particles However, special bonded-phases are available that stabilize silica particles at higher pH (Section 5.3.2.1) Alternatively, supports other than silica can be used for increased column stability at high pH (Section 5.2.5) In the case of basic solutes, another limitation of silica has been a tendency for tailing peaks This problem has largely been resolved by the use of higher purity silica (Section 5.2.2.2)

Most silica particles in use today are spherical in shape Spherical particles are more easily and reproducibly packed to yield efficient columns, and spherical particles tend to be stronger Large, irregular particles are used mainly for preparative separations because of the lower cost of these materials and less need for high values

of N (Section 15.3.1.2) Silica-based particles are available that can withstand

pressures of 15,000 psi (especially superficially porous and pellicular particles, because of their solid core) Spherical silica particles can be synthesized by several

different methods (Section 5.2.2.3 [1, 4]) Figure 5.2a shows the visual appearance

(surface topography, shape and size distribution) of some commercially available silica particles, while a closer look at some popular (≈3-μm-diameter) particles is

shown in Figure 5.2b Significant deviations from a true spherical shape can be seen

in some of these examples

5.2.2.1 Column Efficiency

Particle size is a primary factor in determining column efficiency as measured by

the plate number N This is illustrated in Figure 5.3 for several columns of varied particle diameter; the plate height H (inversely proportional to N) is plotted versus mobile-phase velocity u (proportional to flow rate) As the diameter d pof the porous particles decreases from 5 to 1.8μm, the plate height H decreases—corresponding to

an increase in column efficiency per mm of column length For well-packed columns

of totally porous particles, the reduced plate height h = H/d pfor a small molecule is

≈2, which until about 2006 was accepted as a lower limit for well-packed columns filled with totally porous particles (Section 2.4.1)

The type of particle and its particle-size distribution can also affect column efficiency, presumably by influencing the homogeneity of the packed bed An example is shown in Figure 5.3 for the 2.7-μm superficially porous column This

column (with h≈ 1.5) is more efficient than the column packed with 1.8-μm fully porous particles The superior efficiency of the 2.7-μm column may result from two separate factors First, the particle-size distribution of these particles is extremely narrow (±5–6%, 1 SD), as shown in Figure 5.4 This can be compared with a

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