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ABSTRACT CT: exchangers problem dairy industry ever year It ery ear. ABSTRACT: Fouling of heat exchangers is a problem in the dairy industry and costs billions of dollars ever y year. It has been studied extensively by researchers around the world, and a large number of studies are reported in the literature. This review focuses on the mechanisms of milk fouling, investigating the role of protein denaturation and aggregation endeavor review have well transfer ansfer. as well as mass transfer. We also endeavor to review the effect of a number of factors which have been classified into 5 categories: quality, operating conditions, character acteristics exchangers changers, presence categories: (1) milk quality, (2) operating conditions, (3) type and characteristics of heat exchangers, (4) presence of microorganisms, and (5) transfer of location where fouling takes place. Different aspects have been discussed with the view of possible industrial applications and future direction for research. It may not be possible to alter the properties of milk since they are dependent on the source, collection schedule, season, and many other factors. Lowering the surface temperature and increasing the flow velocity tend to reduce fouling. Reducing the heat transfer surface roughness and wettability is likely to lower the tendency of the proteins to adsorb onto the surface. The use of newer technologies like microwave heating and ohmic heating is gaining momentum because these result in lower fouling; presence microor oorganisms creates problem. however further resear er, esearch requir equired realiz ealize however, further research is required to realize their full potential. The presence of microorganisms creates problem. The situation gets worse when the microorganisms get released into the process stream. The location where fouling takes place is of paramount importance because controlling fouling within the heat exchanger may yield little benefit in case fouling starts taking place elsewhere in the plant.
Introduction
Thermal processing is an energy-intensive process in the dairy industry because every product is heated at least once (de Jong 1997). Processing of billions of liters of milk every year in countries such as India, the United States, and New Zealand means the efficiency of the heating process is of paramount importance (FCG 2004). Fouling of heat exchangers is an issue because it reduces heat transfer efficiency and increases pressure drop and hence affects the economy of a processing plant (Toyoda and others 1994; Mller-Steinhagen 1993). As a result of fouling, there is a possibility of deterioration in product quality because the process fluid cannot be heated up to the required temperature (for pasteurization or sterilization). Also the deposits dislodged by the flowing fluid can cause contamination. Fouling-related costs are additional energy, lost productivity, additional equipment, manpower, chemicals, and environmental impact (Gillham and others 2000). Generally, milk fouling is so rapid that heat exchangers need to be cleaned every day to maintain production capability and efficiency and meet strict hygiene standards. In comparison, the heat exchangers in other major
MS 20050437 Submitted 7/20/05, Revised 9/15/05, Accepted 1/3/06. The authors are with Dept. of Chemical and Materials Engineering, Univ. of Auckland, Auckland, New Zealand. Fonterra Cooperative Group Limited, Palmerston North, New Zealand. Direct inquiries to author Bansal (E-mail: b.bansal@fonterra.com) or Chen (E-mail: d.chen@auckland.ac.nz)
processing plants such as petroleum, petrochemical, and so forth need to be cleaned only once or twice a year. According to Georgiadis and others (1998), in the dairy industry the cost due to the interruption in production can be dominant compared with the cost due to reduction in performance efficiency. Along with the cost, quality issues are equally important, and in fact many times a shutdown is required due to concerns of product quality/contamination instead of the performance of a heat exchanger. According to van Asselt and others (2005), about 80% of the total production costs in the dairy industry can be attributed to fouling and cleaning of the process equipment. In this study, we endeavored to review a wide range of articles reported in literature and interpret the given information on fouling in heat exchangers. The aim was to generate some new interest in this field and to elaborate on some possible new direction for research. It is not intended at all to suggest that this article proposes the only way to understand the problem.
place at temperatures between 75 C and 110 C. The deposits are white, soft, and spongy (milk film), and their composition is 50% to 70% proteins, 30% to 40% minerals, and 4% to 8% fat. Type B (mineral) fouling takes place at temperatures above 110 C. The deposits are hard, compact, granular in structure, and gray in color (milk stone), and their composition is 70% to 80% minerals (mainly calcium phosphate), 15% to 20% proteins, and 4% to 8% fat. Whey proteins constitute only about 5% of the milk solids, but they account for more than 50% of the fouling deposits in type A fouling. -Lactoglobulin ( -Lg) and -lactalbumin ( -La) are the 2 major whey proteins, but the dominant protein in heat-induced fouling is only -Lg. It has high heat sensitivity and hence figures prominently in the fouling process (Lyster 1970; Lalande and others 1985; Gotham and others 1992; Delplace and others 1994; Bylund 1995). Caseins are resistant to thermal processing but do precipitate upon acidification (Fox 1989; Visser and Jeurnink 1997). Although the exact mechanisms and reactions between different milk components are not yet fully understood, a relationship between the denaturation of native -Lg and fouling of heat exchangers has been established (Dalgleish 1990). Upon heating of milk, the native proteins ( -Lg) 1st denature (unfold) and expose the core containing reactive sulphydryl groups. The denatured or unfolded protein molecules then react with the similar or other types of protein molecules such as casein and -La and form aggregates (Jeurnink and de Kruif 1993). The rate of fouling may be different for the denatured and aggregated proteins. Also, being larger in size, the transport of the aggregated proteins from the bulk to the heat transfer surfaces may be more difficult compared with the denatured proteins (Treybal 1981; Chen 2000). Delplace and others (1994) experimentally observed that only 3.6% of the denatured -Lg was involved in deposit formation. Lalande and others (1985) found this figure to be about 5%. However, it is not clear whether fouling is primarily caused by the aggregated proteins or the denatured proteins deposit 1st on the heat-transfer surfaces and the aggregation takes place subsequently. According to Changani and others (1997), fouling occurs when the aggregation takes place next to the heated surfaces. Toyoda and others (1994) modeled the milk fouling process based on the assumption that only aggregated proteins resulted in fouling. According to Delplace and others (1997), fouling is controlled by the aggregation reaction of proteins. de Jong and others (1992) found that the formation of protein aggregates reduces fouling. van Asselt and others (2005) believe that -Lg aggregates are not involved in fouling reactions. Chen and others (1998a, 2000, 2001), Bansal and Chen (2005), and Bansal and others (2005) in their mathematical modeling considered that along with aggregated proteins, denatured proteins also took part in deposit formation. Usually an induction period is required for the formation of the protein aggregates or insoluble mineral complexes before noticeable amount of deposits are formed (Elofsson and others 1996; Visser and Jeurnink 1997; de Jong and others 1998). This time pe28
riod varies between 1 and 60 min for tubular heat exchangers (de Jong 1997) but is much shorter or even instantaneous in plate heat exchangers where intense mixing of fluid takes place due to higher turbulence (Belmar-Beiny and others 1993). Activation energies of deposition reactions for both types of heat exchangers are reported to be similar, which suggests that the underlying processes are same in both cases (Fryer and Belmar-Beiny 1991). The native proteins may attach on the heat transfer surface at low temperatures (even at room temperature) with coverage of about 2 mg/m2 but this does not result in any further deposition (Arnebrant and others 1987; Wahlgren and Arnebrant 1990, 1991; Jeurnink and others 1996b). Denaturation of native proteins in heat exchangers starts only at temperatures above 70 C to 74 C (Fryer and Belmar-Beiny 1991). According to Delsing and Hiddink (1983) and Visser and Jeurnink (1997), mainly proteins form the 1st deposit layer. Belmar-Beiny and Fryer (1993) analyzed the deposits with contact heating times down to 4 s and observed that the 1st layer was made of proteinaceous material. Analysis of deposits after fouling for an extended period usually shows that the deposits near the surface contain a higher proportion of minerals. This is caused by the diffusion of minerals through the deposits to the surface rather than minerals forming 1st on the surface (Belmar-Beiny and others 1993). In contrast, according to Tissier and Lalande (1986), Foster and others (1989), and Fryer and Belmar-Beiny (1991), a dense, high-mineral-containing sublayer forms 1st and is followed by a more spongy, proteinaceous layer. Fouling in a heat exchanger depends on bulk and surface processes. The deposition is a result of a number of stages (Belmar-Beiny and Fryer 1993). The 1st stage involves denaturation and aggregation of proteins in the bulk followed by the transport of the aggregated proteins to the heat-transfer surface. Then surface reactions take place, resulting in incorporation of the proteins into the deposit layer. The deposit layer is subjected to fluid hydrodynamic forces and as a result there is possible re-entrainment or removal of the deposits. The step controlling the overall fouling may either be related to physical/chemical changes in the proteins or the mass transfer of the proteins between the fluid and the heat-transfer surface. In some cases, it may be a combination of both. Belmar-Beiny and others (1993) and Schreier and Fryer (1995) proposed that fouling was dependent on the bulk and surface reactions and not on the mass transfer. It was also proposed that the fouling rate was independent of the concentration of foulant in the liquid (Schreier and Fryer 1995). de Jong and van der Linden (1992), de Jong and others (1992), and Grijspeerdt and others (2004) observed that the fouling process was reactioncontrolled and was not limited by mass transfer. Sahoo and others (2005) and Nema and Datta (2005) used a similar concept in their fouling model. Toyoda and others (1994), Georgiadis and others (1998), Georgiadis and Macchietto (2000), Chen and others (1998a, 2000, 2001), Chen (2000), Bansal and Chen (2005), and Bansal and others (2005) considered that fouling is dependent on mass transfer as well as bulk and surface reactions. According to Lalande and others (1985), Hege and Kessler (1986), Arnebrant and others (1987), and Kessler and Beyer (1991), protein denaturation is the governing reaction. On the other hand, Lalande and Ren (1988) and Gotham and others (1992) observed that protein aggregation is the governing reaction. de Jong and others (1992) found that the deposition of milk constituents in heat exchangers is reaction-controlled adsorption of denatured proteins. According to Toyoda and others (1994), only aggregated proteins present in thermal boundary layer are able to cause deposition. Delplace and others (1997) believed that the formation of aggregates reduces fouling and that mixing can be used to promote aggregation and hence control fouling. de Wit and Swinkles (1980), Anema and McKenna (1996), Changani and others (1997), and Chen and others (1998a) suggested that the protein unfolding or denaturation step is reversible
whereas Ruegg and others (1977), Lalande and others (1985), Arnebrant and others (1987), Gotham and others (1992), and Roefs and de Kruif (1994), and Karlsson and others (1996) have found evidence that the denaturation step is irreversible. In comparison, the protein aggregation step has been reported to be always irreversible (Mulvihill and Donovan 1987, Anema and McKenna 1996, Changani and others 1997, and Chen and others 1998a). Chen (2000), Chen and others (2000, 2001), Bansal and Chen (2005), and Bansal and others (2005) suggested that fouling is caused by both denatured and aggregated proteins and perhaps primarily influenced by the presence of the denatured proteins in the bulk. The simulated results of Chen (2000) and Chen and others (2000, 2001) show that for hot surfacecold fluid scenario, different combinations of unfolded and aggregated proteins lead to similar accuracy of the fouling predictions. However, for cold surfacehot fluid scenario, different mechanisms lead to different predictions. Hence, there is a need for further study of the cold surface effect. In general, a cold surface is not expected to promote aggregation to the extent that a hot surface would do. Also, aggregated proteins would have a lesser tendency to deposit on a surface compared with denatured proteins due to their relatively compact structure and perhaps a cold surface would not provide any further assistance. Table 2 summarizes important aspects of the fouling mechanisms mentioned above.
The composition of milk depends on its source and hence may not be possible to change. A seasonal variation in milk fouling is attributed to differences in its composition (Burton 1967; BelmarBeiny and others 1993; de Jong 1997). Increasing the protein concentration results in higher fouling (Toyoda and others 1994; Changani and others 1997; Kessler 2002). The effect of pH on fouling is not straightforward. In general, the
heat stability of milk proteins decreases with a reduction in pH (Foster and others 1989; Xiong 1992; Corredig and Dalgleish 1996; de Jong and others 1998). A decrease in pH will also result in an increase in concentration of ionic calcium, possibly due to the dissolution of calcium phosphate from casein micelle and its increased solubility (Lewis and Heppell 2000). A slight increase in pH has been observed to increase processing time (Skudder and others 1986). The calcium ions present in milk influence the denaturation temperature of -Lg, promote aggregation by attaching to -Lg, and enhance the deposition by forming bridges between the proteins adsorbed on the heat transfer surface and aggregates formed in the bulk (Xiong 1992; Changani and others 1997; Christian and others 2002). In addition, the solubility of calcium phosphate decreases with heating. The addition of calcium ions enhances deposition and there is a greater amount of caseins present in the deposits, suggesting an increased instability of casein micelles (Delsing and Hiddink 1983; Daufin and others 1987; Grandison 1988; de Jong 1997; de Jong and others 1998). The enrichment of milk with calcium salts is gaining interest to achieve higher calcium intake per serving; however, its impact on the heat stability of milk depends on the source and level of calcium fortification (Vyas and Tong 2004). According to Jeurnink and de Kruif (1995), both increasing as well as decreasing the calcium content of milk compared with normal milk results in lower heat stability and hence more fouling. The fat present in milk has little effect on fouling (Foster and others 1989; Visser and Jeurnink 1997). However, decreasing the pH is found to increase the amount of fat within the deposits (Lewis and Heppell 2000). Lactose is not involved in the fouling process as such until it is involved in the Maillard reaction at a high temperature (Visser and others 1997). Additives may reduce fouling by enhancing the heat stability of milk but may not be permitted in many countries (Lyster 1970; Skudder and others 1981; Changani and others 1997). Holding milk for up to 24 h at 4 C before processing results in less fouling, although further aging increases fouling (Burton 1968; Changani and others 1997; Lewis and Heppell 2000). Prolonged storage of milk for a few days may enhance fouling due to the action of proteolytic enzymes (Burton 1968; de Jong 1997). However, storage at a lower temperature of 2 C for more than 14 d has been found to have no significant impact on fouling (Lewis and Heppell 2000). Reconstituted milk gives much less fouling because about 25% of -Lg is denatured during the production of milk powders
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perature was the most important factor in initiating fouling. When the surface temperature was less than 68 C, no fouling was observed, even though the bulk temperature was up to 84 C. Preheating of milk (often termed forewarming) causes denaturation and aggregation of proteins before the heating section, which then leads to lower fouling in heat exchangers (Bell and Sanders 1944; Burton 1968; Mottar and Moermans 1988; Foster and others 1989). The main effect of forewarming is the denaturation of -Lg and its association with casein micelle and hence a reduction in the amount of type A deposits. Also, there is a reduction in the availability of ionic calcium with preheating as calcium phosphate gets attached to casein micelle (Lewis and Heppell 2000).
Type and characteristics of heat exchangers
Important operating parameters that can be varied in a heat exchanger are air content, velocity/turbulence, and temperature. The presence of air in milk enhances fouling (Burton 1968; de Jong 1997; de Jong and others 1998). However, fouling is enhanced only when the air bubbles are formed on the heat-transfer surface, which then act as nuclei for deposit formation (Burton 1968; de Jong 1997). The solubility of air in milk decreases with heating as well as a reduction in the pressure (de Jong 1997; de Jong and others 1998). Also, the formation of air bubbles is enhanced by mechanical forces induced by valves, expansion vessels, and free-falling streams (de Jong 1997). Although it is usually reported that the presence of a deaerator will reduce fouling, there is no reported evidence (Lewis and Heppell 2000). Fouling decreases with increasing turbulence (Belmar-Beiny and others 1993; Santos and others 2003). According to Paterson and Fryer (1988) and Changani and others (1997), the thickness and subsequently the volume of laminar sublayer decrease with increasing velocity and as a result, the amount of foulant depositing on the heat-transfer surface decreases. Delplace and others (1997) observed that significant variations in Reynolds number and average boundary layer thickness had no effect on the fouling rate. Higher flow velocities also promote deposit re-entrainment through increased fluid shear stresses (Rakes and others 1986). Higher turbulence and different flow characteristics are in fact found to result in a smaller induction period in plate heat exchangers compared with tubular heat exchangers (Belmar-Beiny and others 1993). The reason for this may be the presence of low-velocity zones near the contact points between the adjacent plates. The use of pulsatile flow was found to mitigate fouling when only the wall region near the heat-transfer surface was hot enough to cause the protein denaturation and aggregation reactions (Bradley and Fryer 1992). The reason was that the fluid spent less time near the wall due to higher mixing. The pulsations, however, enhanced fouling when the bulk fluid was also hot enough for the protein reactions to take place. Chen and others (2001) predicted that mixing caused by in-line mixers can reduce fouling substantially. Temperature of milk in a heat exchanger is probably the single most important factor controlling fouling (Burton 1968; Kessler and Beyer 1991; Belmar-Beiny and others 1993; Toyoda and others 1994; Corredig and Dalgleish 1996; Elofsson and others 1996; Jeurnink and others 1996b; Santos and others 2003). Increasing the temperature results in higher fouling. Beyond 110 C, the nature of fouling changes from type A to type B (Burton 1968). It is worth mentioning that both the absolute temperature and temperature difference are important for fouling. This means that it is feasible to have fouling in coolers where the wall temperature is lower than the bulk temperature. Chen and Bala (1998) investigated the effect of surface and bulk temperatures on fouling of whole milk, skim milk, and whey protein and found that the surface tem30
Plate heat exchangers are used commonly in the dairy industry because they offer advantages of superior heat-transfer performance, lower temperature gradient, higher turbulence, ease of maintenance, and compactness over tubular heat exchangers. However, plate heat exchangers are prone to fouling because of their narrow flow channels (Delplace and others 1994) and contact points between adjacent plates (Belmar-Beiny and others 1993). Also, milk fouling in a heat exchanger is difficult to completely eliminate, simply due to the fact that the temperature of the heat-transfer surface needs to be considerably higher than the bulk temperature to have efficient heat transfer. Complex hydraulic and thermal characteristics in plate heat exchangers make it very difficult to analyze milk fouling. The use of co-current and counter-current flow passages within the same heat exchanger further complicates the problem. The heat-transfer surface to which the deposits stick affects fouling (Wahlgren and Arnebrant 1990, 1991). It influences the adhesion of microorganisms as well (Flint and others 2000). The surface characteristics are generally important only until the surface gets covered with the deposits. The surface treatment can be of great benefit in case fouling occurs after a time delay and the strength of the adhesion of the deposits onto the metal surfaces is weaker, giving way to an easier cleaning process. Stainless steel is the standard material used for surfaces that are in contact with milk. Factors that may affect fouling of a stainless-steel surface are presence of a chromium oxide or passive layer, surface charge, surface energy, surface microstructure (roughness and other irregularities), presence of active sites, residual materials from previous processing conditions, and type of stainless steel used (Jeurnink and others 1996a; Visser and Jeurnink 1997). Modifications of the heat-transfer surface characteristics through electro-polishing and surface coatings can reduce fouling by altering the surface roughness, charge, and wettability (Yoon and Lund 1994; Pie linger-Schweiger 2001; Santos and others 2001, 2004; Beuf and others 2003; Rosmaninho and others 2003, 2005; Ramachandra and others 2005, Rosmaninho and Melo 2006). It is generally reported that hydrophobic surfaces adsorb more protein than hydrophilic surfaces (Wahlgren and Arnebrant 1991). Increasing the surface roughness provides a larger effective surface area and results in a higher effective surface energy than a smooth surface (Yoon and Lund 1994). As a result, the adhesion of deposits with a rough surface would be comparatively stronger. The effect of different surface coatings tends to be less on the deposit formation but more on their adhesion strength (Britten and others 1988). Magnetic field treatment has been observed to have no effect on the milk fouling rate (Yoon and Lund 1994). There has been an increasing use of heat exchangers that foul comparatively less, for example, fluidized bed heat exchangers (Klaren 2003), Helixchanger heat exchangers (Master and others 2003), and heat exchangers equipped with turbulence promoters (Gough and Rogers 1987). However, the information available about their use in thermal processing of dairy fluids is limited. The use of pulsatile flow exchanger results in higher mass transfer that may enhance fouling in case the deposition process is mass trans-
The formation of deposits promotes the adhesion of microorganisms to heat-transfer surface, resulting in bio-fouling. Furthermore, the deposits provide nutrients to microorganisms, ensuring their growth. It is worth mentioning here that a lot of processes in the dairy industry are carried out at temperatures below 100 C. For example, pasteurization is generally achieved by heating milk at 72 C for 15 s in a continuous flow system. At this temperature, only the pathogenic bacteria along with some vegetative cells are killed. A higher temperature of 85 C is required to kill the remaining vegetative cells. Spores are much more heat-resistant and remain active well beyond this temperature. Their inactivation is important for the products with longer shelf life. Bio-fouling, either microorganism deposition or biofilm formation, in a heat exchanger raises serious quality concerns. Flint and coworkers have investigated the effect of bio-fouling in dairy manufacturing plants (Flint and Hartley 1996; Flint and others 1997, 1999, 2000). According to Bott (1993), bio-fouling takes place through 2 different mechanisms: deposition of microorganisms directly on the heat-transfer surfaces of the heat exchanger, and deposition/attachment/entrapment of microorganisms on/in the deposit layer forming on the heat-transfer surfaces. With the supply of nutrients by the deposits, microorganisms multiply. The presence of microorganisms in the process stream and/or deposit layer not only affects the product quality, it influences the fouling process as well (Flint and others 1997, 1999; Yoo and others 2005). When microorganisms get released into the process fluid due to hydrodynamic forces, they contaminate downstream sections. This may also result in microbial growth in areas that otherwise are not conducive to bio-fouling. The release pattern of thermophilic bacteria Bacillus stearothermophilus into the process stream has been studied in detail by Chen and others (1998b) and Yoo and Chen (2002).
Location of fouling
Protein denaturation and aggregation reactions take place as soon as milk is heated. The relative amounts of denatured and aggregated proteins depend on a number of factors such as operating conditions, type and design of heat exchanger, and properties of heat transfer surface. The use of an efficient technology may help to mitigate fouling within a heat exchanger; however, the processed milk at the exit of the heat exchanger would still have a lot of denatured and aggregated proteins. This would result in severe fouling at various locations further downstream. Hence, controlling fouling only within the heat exchanger may not yield effective results and an overall strategy is required to mitigate fouling over the entire setup (Petermeier and others 2002; Grijspeerdt and others 2004). An example of such a strategy is the preheating of milk before the heating section as mentioned previously (Bell and Sanders 1944; Burton 1968; Mottar and Moermans 1988; Foster and others 1989). The installation of an additional section at a constant temperature (holding section) within the cascade of heat exchangers is also known to reduce fouling (de Jong and others 1992, 1994; de Jong and van der Linden 1992; de Jong 1997). This outcome is attributed to the fact that denatured -Lg is transformed into aggregated -Lg in the holding section. This aggregated form is inactive and is unable to form aggregates with other components of milk and hence does not play an active role in the fouling process in the downstream sections (de Jong and van der Linden 1992). Hence, successful mitigation of fouling depends on controlling local thermal and hydraulic conditions as
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Conclusions
Fouling of heat exchangers in the dairy industry is a complex phenomenon and the mechanisms are not completely understood. Although there is an established link between protein denaturation and fouling, the relative impact of the denatured and aggregated proteins on the deposit formation is not clear. In general, it is believed that fouling is controlled by the aggregation reaction of proteins and the formation of protein aggregates reduces fouling. The mass transfer of proteins between the fluid and heat transfer surface also plays an important role. It may not be possible to completely eliminate fouling in heat exchangers simply due to the fact that denaturation and aggregation reactions initiate as soon as milk is subjected to heating. Fouling, however, can be controlled and mitigated by selecting appropriate thermal and hydraulic conditions. Both increasing the flow rate and decreasing the temperature reduce fouling. Plate heat exchangers tend to have lower fouling compared with tubular heat exchangers because they have higher turbulence and the surface temperature is also comparatively lower. Microwave heating and ohmic heating also result in less fouling; however, the information available about these technologies is limited. Bio-fouling aggravates the problem and raises concerns about the product quality as well. The release of microorganisms from the fouling deposits into the process stream can contaminate the plant well beyond the heat exchangers. Finally, it is important that a holistic approach is taken to mitigate fouling because controlling fouling within the heat exchangers may be of little use in case it shifts to other parts of the plant. The impact of fouling needs to be assessed for the entire plant before a mitigation strategy is devised. To date, a significant amount of research has been done, but still there is a lack of generalized methodologies and techniques to control fouling. Further concentrated and joint efforts among industry, research institutes, and academia are required to combat this serious problem.
References
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