Volume 3, Issue 1

February 2016

Process Intensification: Research and Industrial Applications in China

Jun Li, Guifeng Ma

Department of Chemical and Biochemical Engineering, College of Chemistry and Chemical Engineering, Xiamen University, National Engineering Laboratory for Green Chemical Productions of Alcohols, Ethers and Esters, Xiamen 361005, P. R. China.

Corresponding author. Tel./fax: +86 592 2183055. E-mail address: junnyxm@xmu.edu.cn (J. Li).

Abstract

Process intensification (PI) involves at least one of the intensification elements of mass transfer, momentum transfer, heat transfer, and reaction rate/selectivity/productivity. As the main direction of chemical industry, it has been attracting more and more academic and industrial interest. PI in China has met great opportunity due to the important issues on energy saving and waste reducing appeared in the national plan. In this review, PI researches and industrial applications in China are summarized; PI is classified as four general types (miniaturization, external field intensification, special medium/solvent intensification, and coupling intensification) with corresponding applications in three major areas (separation, reaction, and heat transfer). The review points out that PI needs more engineering and engineering-trained researchers for industrial implementations.

Keywords: process intensification; microtechnology; external field; high pressure; ionic liquid; coupling; separation; reaction; heat transfer.

1. Introduction

Process intensification (PI) now is familiar to researches in chemical engineering and chemistry disciplines. It has a broad concept although its primary goal is to reduce the capital cost of production systems from its beginning pioneered by Colin Ramshaw of Imperical Chemical Industries Ltd in the late 1970s[1]. In this point of view, PI can be looked as a component of the much wider concept, green chemistry, which includes reducing production cost, energy, waste, hazard, risk, environmental impact, and so on. Nevertheless, at least one of the intensification/enhancement elements of mass transfer, momentum transfer, heat transfer, and reaction rate/selectivity/productivity should be included when referring to the PI concept. Therefore, PI is typically symbolized by microtechnology/miniaturization, external field intensification, coupling processes, membrane technology, and supercritical fluid-assisted processes.

It is no doubt that PI is the main direction of technologies in chemical industry; it has been attracting more and more academic and industrial interests after intensive researches more than 40 years. From Web of Science and CNKI (a China knowledge resource), search shows that PI with the title in publications started from 1970s (Chinese papers from 1990s) and it is still rapidly increasing. Among them, there are more than 50 papers reviewing the PI topics from Web of Science and more than 20 review papers in Chinese journals from CNKI. Most of them are about specific PI directions such as microtechnology/miniaturization [2, 3], ultrasonic external field intensification [4], reactive distillation coupling process [5], membrane technology [6, 7], and catalytic reaction [8]. Some of them are general bout PI [9-12] [1], PI in reaction/synthesis [13], PI in separation [14], and about intensified unit operation level[15] and PI fundamental level[16]. On the other hand, there are many meetings about PI, e.g., International Conference on Process intensification for Chemical Industry (started from 1995), Process Innovation and process Intensification (2002), European Process Intensification Conference, and Asia-Pacific Symposium on Process Intensification & Sustainability (annually, started from 2014). In China, there are, for examples, National Chemical Process Intensification Conference, Fine Chemicals and Process Intensification Conference, Green Chemical Technology and Process Intensification Symposium. Furthermore, the traditional journal, Chemical Engineering Process, has been a special journal in PI since 2007 (now it is Chemical Engineering Process: Process Intensification) although large amount of PI works appear in other journals. Also there are several typical books in PI, for examples,Re-Engineering the Chemical Processing Plant: Process Intensification by A. Stankiewicz and J.A. Moulijn (Marcel Dekker, 2004), Process Intensification by Reay David; Ramshaw Colin; Harvey Adam (2013), Modern Drying Process: Process Intensification by Tsotsas Evangelos, MuJumdar Arun S (Wiley-VCH, 2014).

From the Twelfth National Plan (2011-2015) proposed by Chinese government, energy saving and waste reducing have been among the key issues in China’s industry; therefore, PI in China has met great opportunity. In this review, for clearer indication, PI methods corresponding to PI application areas in China are summarized (see Table 1). In method, PI is classified as four general types: miniaturization /microtechnology, external field intensification, special medium/solvent intensification, and coupling intensification. In application, three major areas are mentioned: separation, reaction, and heat transfer.

Table 1

2. PI due to external fields

Field externally imposed to traditional systems for intensification is the most important PI approach due to the obvious improvement/enhancement of mass transfer, energy transfer, momentum transfer and sometimes chemical reaction rate/selectivity/productivity from the views of both chemical engineering and chemistry disciplines. External fields mainly include electric field, flow field (such as impinging stream, pins/barriers in tube), gravity/high gravity field, magnetic field, plasma field, ultrasonic field, and microwave field. All these fields have been applied to the PI processes in reaction, separation and heat transfer areas as shown in Table 1. Among them, magnetic field, ultrasonic field and microwave are the most studied in recent years because of their convenient implementation and effective intensification although other fields such as electric field and flow field were popular in mass/heat transfer and reaction enhancement and had important industrial applications, for examples, electric field for desalting from raw oils, pins in tube for enhancement of heat exchangers, in last several decades.

By using magnetic field, it has a long history for enhancing separation of ore minerals [90] or metals or other solid mixtures [91]. It can obviously enhance the flux of membranes through ameliorating membrane fouling [20, 92]; it can enhance the distillation of azetropic ethanol-water mixture [93] and other separations such as extraction, adsorption, absorption, flocculation, and precipitation [94]. Magnetic field for the enhancement of reaction had been in doubt due to the ignorable energy imposed; however, enhancement was shown in enzymatic reactions [95, 96], photochemical reactions [97], polymerization [98], esterification[99], electrolysis[100] and others. In addition, magnetic field is known to be effective to enhance heat transfer [101, 102] for magnetic fluids including the condensation heat transfer [33]; it was reported to be effective to heat transfer in diesel engine under magnetic field [103]. It is not surprising that separation of ore minerals or metals or other solid mixtures has been widely implemented within industrial plants in China.

By using ultrasonic field, it is well known to enhance the mass transfer in various chemical engineering studies[104] and then various separations, for examples, the enhancement of gas-liquid mass transfer coefficient in bubble column[105], membrane flux through alleviating the fouling problem[106, 107], crystallization performance[108, 109], dewatering/leaching/extraction processes[110-112], adsorption/ desorption performance[113, 114]. External ultrasonic field is also used to enhance reactions, for examples, synthesis of nanoparticles by precipitation/sol-gel/other methods [115-117], epoxidation[118], electrolysis[119], photocatalytic synthesis[120], aerobic digestion[121], and so on. It is known that ultrasonic field can enhance heat transfer, such as, that in heat exchanger [34] and in evaporation process [122]. Setups with externally imposed ultrasonic field have huge market in China, normally, for dewatering/leaching/ extraction processes; many companies can manufacture complete setups installed with ultrasonic field with capacity of several cubic meters or several cubic meters/h.

Microwave is very effective for heating because of its short wavelength (~1mm-1m) and high frequency (~300 MHz-300GHz); the heating is selective to matters with large dielectric constant such as water. The enhancement is through the friction between molecules under the field. Microwave heating is particularly interesting in food processing [123], and has been applied to separations and reactions [124] (although non-heating factors may also take effect) widely. In separation, it has been applied to fast drying/dewatering [125, 126], extraction/leaching processes (particularly from natural products)[127], demulsification[128]. In reactions, it was reported to enhance the photo/catalytic oxidation [129, 130], syntheses of nanoparticles[131], and other reactions such as alkylation, esterification, sulfonation, Diels-Alder reaction, condensation, cyclization/ decyclization, and rearrangement[132]. Microwave has large market in China, particularly, for drying, concentrating and extraction processes; companies in China can manufacture complete setups installed with microwave with capacity as large as several cubic meters.

3. PI from miniaturization  

The initial definition of PI was connected to miniaturization of chemical engineering processes for reducing the danger and cost of productions. Miniaturization is also known as microtechnology. Charpentier [2] and Pohar and Plazl [3] in their reviews provided detailed description; Sun and Chen [133] had a subtopic for reviewing microtechnonlogy in chemical engineering.

Miniaturization/microtechnology includes reaction and heat exchange in microchannel for reducing cost, improving safety, integration and efficiency because of enhanced fluid flowing and excellent mass/heat transfers [134, 135]between different phases in limited space. In this sense, micorchannels with considering different shapes provide excellent mixing technology; some fundamental studies were implemented for, such as, liquid-liquid mixing/dispersion [36, 136], gas-liquid mixing[38, 137], gas-liquid-lqiuid mixing[138]. Although few publications were reported about microtechnology in separation, in fact, hollow membrane could be typical separation in microchannels; blood plasma was reported to separate in microchannel[139], magetophoresis was implemeted in microchannel[74].

Micochannel reactor has been widely studied for synthesis of miro-/nanoparticles [140, 141], and enhancing multiphase (e.g., gas-liquid, liquid-liquid) reactions[142] such as oxidation[143], cyclization[144], bromination[145], and nitrification[146]). Lots of studies proved that microchannel/microfluid could improve heat transfer[134, 147]; the microchannel heat exhanger may have potential applications in microelectronic chip systems [148]. Intensification in microchannel by using additonal variables (such as varied sections, offset of pins) is another attractive research topic[41, 42, 149].

In applications, implementation of CaCO3 in microreactor was commerciallized by Qinghua University; an integration of mixing, reaction and heat exchanger were implemented for production of NH4H2PO4 with 8t/a by Dalian Institute of Technology[133]. It is worth mentioning that other intensification methods, such as continous processes, can also miniaturize reactor or separator. For examples, the special meidium (see Section 4) involved high pressure continous carbonation process made the large volume (90m3) stirred tank reactor be about 2 m3 reactor with the same productivty[150]. A continous eseterification process largely reduced the size of tradtional stirred tank reactor (from 5m3 to about 0.05m3), which was implemeneted in a factory[151].

4. PI from special medium

Supercritical fluids/high pressure fluid, ILs and plasma as the intensification media are very attractive. Although supercritical fluids and ILs are the most common solvents in green chemistry, people also look them as the intensification solvents because of their enhancement of mass/heat transfer or reaction rate.

Supercritical fluid is known as its comparable diffusion coefficient to that of gases, but its density to that of liquids. Supercritical fluid extraction as the typical PI process can remarkably shorten extraction time; its industrial implementation in China is still blooming after more than 30-year intensive academic researches due to the abundant traditional Chinese herbs and the increasing demand in “organic products”. Supercritical fluid as an intensification medium in particle formation has been intensively developing more than 20 years in China; however, to my best knowledge, still no successful industrial plant has been reported up to now. Supercritical fluid as a dyeing medium can enhance the dyeing rate besides its green chemistry property; Dalian Polytechic University has developed several pilot plants towards industry scale. Supercritical fluid as a drying medium can rapidly remove solvent in porous materials and preserve the pores; large drying vessels as large as 2 m3 in China are valid, however, with batch or semi-continuous processes. Supercritical fluid in reactions can be used as both reactant and reaction medium for its enhanced mixing with other substances (for example, supercritical water becomes miscible with benzene) and high permeability to carry reactant to contact with catalysts. Research in reactions has been long time with typical industrial plants including polymerization of ethylene, supercritical water oxidation in China. A continuous supercritical fluid drying for porous materials by Xiamen University is now in an industrial plant design procedure [152]. Supercritical fluid is also well known to intensify heat transfer around critical point; for example, water at 377oC and 22.8 MPa (pseudo critical point) reaches highest heat transfer coefficient in tube [153]. This phenomenon has attracted many investigations for various fluids [154, 155], particularly for supercritical water due to much interest from the nuclear reactor [156] and ultra-supercritical coal-fired power plant.

Because of the designable properties from both cation and anion, IL as the medium of PI has attracted much attention in recent 20 years. Many researches from both theoretical (for molecular design with quantum chemistry and molecular simulation) and experimental investigations in China have greatly contributed to understanding the properties of ILs and guidance of syntheses of ILs. In separation, besides replacing traditional solvents with considering green chemistry, ILs were also investigated as the effective liquid membranes[157], sorbents particularly in gas/CO2 separation/capture[158-160] and chromatography[161, 162], extraction solvents[163-165], solvent to dissolve and separate cellulose[166], and in extractive distillation[167]. In reaction, ILs were widely used as catalysts to enhance reaction rate or reaction selectivity, such as alkylation[152], epoxidation[168], oxidation[169], Knoevenagel reaction[170], condensation[171], hydration [172], esterification[173], and other intensification of organic reactions[174]. ILs are also known as the effective sorbent for absorption heat pump [52] due to the intensification of heat transfer and heat capacity for storage. Although few report about industrial applications of ILs in separation in China, many industrial plants were implemented with ILs as the reaction solvent and/or catalyst, for examples, production of cinnamaldyhyde (1000t/a) with IL as the solvent and catalyst in Zhejiang, alkane isomerization and alkylation of olefins with IL replacing sulfuric acid or hydrofluoric acid by PetroChina, s-trioxane production with IL as the catalyst by CNOOC, and glycol production with IL as the catalyst by SinoPec [133].

Plasma is a kind of sate of matter; it can be looked as a special medium in PI since large amount of active species in plasma provide special environments to enhance chemical reactions from atoms and molecules. On the other side, the special properties of plasma change the phase contact from mesoscale and form specific hydrodynamics, mass transfer and reactions for multiphase fluids [49]. Besides many other reactions, it is particularly useful to be applied to reactions which are normally difficult with high activation energy, for examples, CO2 conversion and hydrogen production [175, 176]. It is also helpful to prepare highly dispersed catalysts [177]. Although it is not normal to use plasma in separation intensification, it was used to modify different separation membranes or directly prepare membranes to enhance the membranes performance [46, 178]. There are many studies about hydrodynamics and heat transfer in plasma [53, 179, 180]. It is sure that plasma can enhance the heat transfer due to the active species; however, to my best knowledge, there is still no quantitative report on this heat transfer enhancement.

5. PI from coupling

Coupling processes, including coupling different intensification approaches and different applications, are always the most attractive processes in PI. Sometimes, several approaches are coupled together, for examples, ILs in reaction coupling with separation process[83], esterification process coupling with pervaporation and distillation [84], for product preparation by more efficient intensification.

In separation, as shown in Table 1, distillation [54-59], membrane [60-67], ultrasonic field [68-72] to be enhanced by coupling with various separation technologies are the active areas; coupling of different fields [68-71] or coupling these fields with various separation methods [63,72-74] are also very effective. In reaction, as shown in Table 1, reactions coupling with various separation methods [75-79] are the most attractive and many plants (e.g., reactive distillation) have been implemented in industry. Coupling supercritical fluids and IL separately with external fields can be interesting [68],[181], and coupling the two green chemistry solvents themselves can also be enhanced gas-liquid reaction systems [81, 82].

In heat transfer, as shown in Table 1, coupling of different heat transfer modes (conduction, convection and radiation) is the most concerned[85, 86]; external fields coupled with microchannel are helpful for heat transfer intensification[87]; coupling heat transfer with reaction and mass transfer is finally desirable for process optimization by PI in chemical industry [88, 89].

6. Conclusions

PI methods corresponding to PI applications in China are summarized in this review. For clearer indication, PI method is classified as four general types and three main applications. From the review, we can see that PI researches in China have already covered almost all sections and have achieved great progress. Some typical technologies have been successfully implemented in industry, including high gravity technologies, miniaturization of reactors for inorganic nano/microparticles, membrane technologies, supercritical fluid extraction technology, IL technologies, and reactions in plasma. However, compared to the abundant publications, the application-directing researches still need to be strengthened to meet the national plan’s energy saving and waste reducing. As mentioned, PI at least involves one of the intensification/enhancement elements (mass, momentum, heat transfer, and reaction rate/selectivity/productivity); therefore, PI needs more engineering (such as process optimization and design, setup design and manufacture) and engineering-trained researchers/developers.

Acknowledgement

We gratefully acknowledge financial support from National Natural Science Foundation of China (NSFC) (No. 21276212 and No. 21476186).

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