C H A P T E R

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c0001 IntroductionRuren Xu

Jilin University, China

p0010 Synthetic chemistry is at the core of modern chem-istry; it provides the most powerful means for chemiststo create the material foundation for our envisionedworld. Its main objective is to create a large variety ofcompounds, phases, materials, and ordered chemicalsystems needed by our rapidly advancing society, goingconsiderably beyond just finding and synthesizing natu-rally existing compounds. According to recently pub-lished studies, over 50 million compounds, naturallyexisting or not, have been discovered or synthesized,some of which have become indispensable to our dailylife. These compounds have provided the basis formany scientific and technological advances in the recenthistory. In turn, these advances have created rapidlyincreasing needs for new materials with specific struc-tures and functions, posing challenges to, as well ascreating opportunities for synthetic chemists. Specifi-cally, we see increasing needs in this new century, fornovel synthesis strategies and techniques, as well asfor the related scientific understanding, gearing towardgreen synthesis, bionic synthesis, inorganic synthesisunder extreme conditions, and molecular and tectonicengineering of inorganic materials, in efficient, ratio-nally designed and economic manners. We believe thatthese are among the most essential key elements forthe continuing and rapid advancement of Science andtechnology in this new century [1,2].

p0015 In the past century, advances in synthetic chemistryhave often been the key driving force for the industrialrevolutions and birth of new science and technolo-gies; examples of this sort have been numerous [2].For instance, F. Haber, in the early twentieth century,invented a high-pressure technique to synthesizeammonia, the key ingredient of chemical fertilizers,from the abundantly available H2 and N2 using osmiumas the catalyst. Twenty years later, C. Bosch improved thetechnique by using inexpensive iron instead of expensive

osmium as the catalyst, which laid a solid foundation forthe human society to maintain a continued increase infood production to keep up with the human populationincrease; amajor challenge thatwehave been facing sincethe past century. Because of their profound contributionsto science as well as to the human society, Haber andBosch received Nobel prizes in chemistry in 1918 and1931, respectively. Health industry is another area wheresynthetic chemistry has been playing pivotal roles.Outstanding examples since the mid-twentieth centuryinclude the successful syntheses of SAS drug, penicillin,a variety of antibiotics and other medicines, which havesubstantially improved and continue to improve ouroverall abilities in treating human diseases and fightingagainst them. Our ability in producing the three majorclasses of synthetic materials, namely synthetic fiber,synthetic plastic, and synthetic rubber, has paved theway for many of the recent industrial and agriculturaladvances. There is no doubt that chemistry, especiallysynthetic chemistry, has been making considerablecontributions to improve the living conditions of thehuman society.

p0020From a scientific perspective, a pool of very largenumber of new materials created by synthetic chemistryhas provided plenty of samples for studying thestructureefunction (property) relationships of materialsas well as their syntheses, facilitating scientists to studythe fundamental chemistry of these materials, which hasbecome a driving force in the recent developments ofchemistry and related sciences. For example, thesuccessful preparation of single crystalline silicon andnumerous semiconductive materials has fueled theemergence of information technology; the productionand posttreatment of nuclear fuel of uranium and pluto-nium, the key to the nuclear technology and safe appli-cation, have all been built on chemical technologies withroots in synthetic chemistry. Similar can be said about

1Modern Inorganic Synthetic Chemistry, DOI: 10.1016/B978-0-444-53599-3.10001-0 Copyright � 2011 Elsevier B.V. All rights reserved.

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other high technologies such as laser, nanotech, aviation,and space technology. Without a doubt, the so-called sixgreat technology inventions in the twentieth centurywould have never materialized without the founda-tional work by generations of synthetic chemists inthe past. The same is true about other technologicalbreakthroughs and growth points in related sciencessuch as semiconductor, super conduction, cluster, andnanotechnology.

p0025 Modern inorganic synthetic chemistry, an importantbranch of synthetic chemistry, has evolved considerablyfrom the traditional synthesis and preparation of inor-ganic compounds, which now includes the synthesis,assembly, and preparation of supramolecular and high-level ordered structures in its studies. In recent years,we have been witnessing that an increasingly largenumber of new inorganic compounds, phases, andcomplexmaterials are being synthesized and assembled,having made inorganic synthetic chemistry a key driverfor many new scientific and technological developmentsand advancements. We anticipate that inorganicsynthetic chemistry will continue to play equally ormore important roles in science as well as in ourupcoming life.

s0010 1.1. FRONTIERS IN MODERNINORGANIC SYNTHETIC CHEMISTRY

p0030 Development of new synthetic reactions, syntheticroutes, technologies and associated basic scientificstudies. The following summarizes the five main classesof inorganic compounds and materials of particularinterest to modern inorganic synthesis and preparation.

s0015 1.1.1. The Basic Inorganic Compoundsp0035 This basic class includes covalently bonded molec-

ular compounds, coordination compounds, clustercompounds, metal organic compounds, nonstoichio-metric compounds and inorganic polymer, amongothers.

s0020 1.1.2. Inorganics and Materials with SpecificStructures

p0040 Study of inorganic compounds and phases withspecific structures is becoming increasingly importantas the need for materials with specific properties andfunctions continues to rise. It is well understood thatthe properties and functions of materials are determinedby their structures and compositions. More specifically,such properties and functions are often determined bythe characteristics of high-level molecular structuressuch as those ofmolecular aggregates, orderedmolecular

assemblies, and structures in condensed states instead ofsinglemolecular structures. Take defects for example, theproperties and functions of materials often result fromvarious forms of structural defects in their componentcompounds or phases in condensed state. For example,a key reason that many complex oxides are being usedas popular substrates for functional materials is thatthey can form many types of structural defects in addi-tion to their many adjustable component elements.Hence, it has become amajor topic at the forefront of inor-ganic chemistry research to study the preparation ofsolid-state matters with specific structural defects andthe associated principles aswell as relateddetection tech-niques. In addition, the key research topics in today’sinorganic chemistry also include preparation of surfacesand interfaces with specific structures and properties,stacking of layered compounds, preparation of specificpolytypes and their intergrowths as well as intercalationstructures and low-dimensional structures of inorganiccompounds, synthesis and preparation of inorganiccompounds with mixed valence complexes and clus-tered compounds with specific structures, as well as therapidly emerging and increasingly useful porouscompounds with specific channel structures such asmicroporous crystals, meso- and hierarchical porousmaterials. Also particularly interesting is the preparationof phases that tend to form distinct structures and areable to form large varieties of distinct structures underextreme synthetic conditions like high or ultrahigh pres-sures. While a few synthesis examples with the afore-mentioned characteristics have been reported in theliterature, such studies have generally been done inrather ad hoc manners, often accomplished throughutilizing the particularity of specific reactions or specificsynthesis techniques rather than based on new under-standing of a general class of synthesis problems andnew synthesis technologies. The latter is clearly moreimportant for the future development of syntheticchemistry.

s00251.1.3. Inorganics and Materials in SpecialAggregate States

p0045Another important class of materials are thecompounds in special aggregate state, such as in nanostate, ultrafine particles, clusters, noncrystalline state,glass state, ceramic, single crystal, and other matterswith varying crystalline morphologies such as whiskerand fiber. The rapid emergence of nanoscience and tech-nology strongly suggests that different aggregate statesof the same matter could exhibit different propertiesand have different functions. The understanding ofthis could have substantial implications to the futuredevelopment of science as well as new functionalmaterials.

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s0030 1.1.4. Assembly of High-level OrderedStructures

p0050 There is an emerging class of functional inorganicmaterials, commonly characterized as being highlyordered supramolecular systems, formed via self-assembly among molecules or molecular aggregatesthrough molecular recognition. The key interactionforces in the formation of such large molecular assem-blies are intermolecular non- or weak-bond interactions(van der Waals and hydrogen bond). Examples of suchmaterials include coordination polymers, inorganicpolymers, and molecular systems with specific struc-tural features such as nanosystems, capsula, ultrathinmembrane (monolayer membrane, multilayer compos-ited membrane), interfaces, two-dimensional layeredstructures, and three-dimensional biological systems;many of which have been widely used for fabricatinghigh-tech microdevices. Self-assembly is increasinglybecoming a key and practical technique in thesynthesis and preparation of complex functionalsystems. It has even been suggested that the introduc-tion of self-assembly-based synthesis techniques couldfundamentally advance the chemical productionprocesses that are being widely used in the currentindustries [2].

s0035 1.1.5. Composition, Assembly, andHybridization of Inorganic Functional Materials

p0055 The following areas have received considerable atten-tion in recent years: (1) multi-phase composition ofmaterials including enhanced or reinforced fiber- (orwhisker-)based materials, the second-phase particledispersion materials, two- or multi-phase compositematerials, inorganic and organic materials, inorganicsand metals, and functional gradient materials as wellas nanomaterials; and (2) composite material-relatedhosteguest chemistry, which represents a highly inter-esting and a very challenging research area. Theresearch focuses include, for example, the assembly ofdifferent types of chemical entities in hosts with micro-porous or mesoporous frameworks such as quantumdot or super lattice-forming semiconductive clusters,nonlinear optical molecules, molecular conductorsmade of linear conductive polymers and electron trans-fer chains as well as DeA transfer pairs. All thesecomplex composites could be assembled throughsynthetic routes consisting of ion exchanges, CVDs,“ships in bottle” and microwave dispersion; (3) nano-hybridization of inorganics and organics, which repre-sents a rapidly emerging interdisciplinary field. Itstudies the formation of new hybrid materials throughcombining polymerization and solegel processes. Thesehybrid materials possess those properties which are

generally absent in pure inorganics or pure organics,and are increasingly being used in fiber optics, wavepropagation, and nonlinear materials. It is worth notingthat the first survey about this emerging field was pub-lished in 1996 by P. Judeinstein [3].

p0060As outlined above, a key task in today’s inorganicsynthetic chemistry is to develop novel synthetic reac-tions, synthetic routes, and associated techniques aim-ing to create new functional materials with specificallydesired multilevel structures in condensed states. Asper the past experience, the discovery of a novel andeffective synthetic route or technique has typically ledto the creation of a large class of new matters and mate-rials. For example, the advent of solegel synthetic routehas been a key reason for the development and emer-gence of nano-states and nanocomposite materials, glassstates and glass composites, ceramic and ceramic-basedcomposites, fibers and related composites, inorganicmembranes and composite membranes, and hybridmaterials. The core chemistry of this synthetic route ishydrolysis and polymerization of starting reactantmolecules (or ions) in aqueous solution, i.e., frommolecular/ polymeric state/ sol/ gel/ crystallinestate (or noncrystalline state). This synthetic processcould possibly be regulateddifferently at each individualreaction step so as to create solid-state compounds ormaterials with different structures or in different aggre-gate states. While highly promising, we are clearlynot there yet due to the complexity as well as our limitedunderstanding of polymerization processes of inorganicmolecules in both theoretical and experimentalexecutions. Thus, fundamental studies of these issuesrepresent key areas of focus in today’s inorganicsynthetic chemistry.

p0065In summary, the near and intermediate-term objec-tives for today’s inorganic synthetic chemists are todevelop novel and more effective synthetic technologiesand to carry out related theoretical studies aiming to gainbetter understanding of the desired new synthesis capa-bilities which are both economical and environment-friendly.

s00401.2. BASIC RESEARCH IN SUPPORTOF GREEN SYNTHESIS

p0070The vast majority of known synthetic reactions, espe-cially those used in the preparation of a large variety ofrare elements from their ores or raw materials in theproduction of fine chemicals as well as in medical andpharmaceutical industries, produce large amounts ofby-products, which, along with the used chemicals,solvents, additives, and catalysts, often add majorpollutants to our environment and have created consid-erable environmental issues in the past. Thus, it has

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become absolutely essential to study ways to consider-ably lower or completely remove environmental pollu-tion produced by the current chemical industry. Whilethis has posed substantial challenges for synthetic chem-ists, it has also created new opportunities to furtherdevelop synthetic chemistry toward new and healthierdirections. Green chemistry, clean technologies, andenvironment-friendly chemical processes have nowbecome a common conviction of many chemists. Idealsynthesis, a concept proposed by Wender [4] in 1996,aims to “make complex molecules from simple startingmaterials in a manner that is operationally simple, fast,safe, environmentally acceptable and resource effica-cious.” This definition has essentially defined thegeneral direction for realizing green syntheses. In 2009,Noyori [5] proposed that we should aim at synthesizingtarget compounds with a 100% yield and 100% selec-tivity and avoid the production of waste. This processmust be economical, safe, resource-efficient, energy effi-cient, and environmentally benign. In this regard, theatom economy and the E-factor should be taken intoaccount. The 3Rs (reduction, recycling, and reuse) ofresources are particularly important. Such “GreenChemistry” is creative and brings about prosperity.The following research directions have received consid-erable attention in the recent years, frommany syntheticchemists [6]: development and applications of greensynthetic reactions with efficient atomic economy, envi-ronmental friendliness, and energy efficiency; develop-ment and application of environment-friendly sourcematerials, reaction media and solvents, additives andcatalysts and highly efficient and selective syntheticreactions as well as associated theoretical studies. Thesehave become the major focuses at the forefront ofsynthetic chemistry research.

s0045 1.3. BASIC RESEARCH ON SYNTHETICAND PREPARATIVE ROUTES UNDER

EXTREME CONDITIONS

p0075 There have been many cases of successfully synthe-sizing materials under extreme conditions such asultrahigh pressure, temperature, vacuum, ultralowtemperature, strong magnetic and electric fields, laserand plasma which are not possible to synthesize undernormal experimental conditions. A large variety of newcompounds, phases and materials as well as newsynthetic routes and techniques have been developedspecifically for chemical syntheses under extremeconditions. For example, ultrapure crystals with nodislocation defects can be synthesized in ultrahighvacuum with zero-gravity. It has even been suggestedthat the Periodic Table of Elements may need to besignificantly modified under ultrahigh pressure since

the width of the forbidden band and the distancebetween the internal and the external electronic orbitsfor many matters may be changed under such condi-tions which can lead to significant differences in thestable valances of an element under the normal versusultrahigh pressures. It has also been observed thatchanges in reactivity and reaction rules of reactantsunder ultrahigh pressure have led to the formation ofa variety of new species and more interestingly, ofnew phases. It is also worth noticing that compoundswith specific valence, configuration, and crystalmorphology can be formed under hydrothermal condi-tions with medium temperature and pressure, whichhelps to overcome the issue caused by the lack ofsuccessful synthesis routes in solid states for many inor-ganic functional materials under high temperature.Hence, further studies of the general rules and princi-ples of chemical synthesis under extreme conditionshave become one of the major research frontiers insynthetic chemistry.

s00501.4. BIOMIMETIC SYNTHESIS ANDAPPLICATIONS OF BIOTECHNOLOGY

IN INORGANIC SYNTHESIS

p0080Biomimetic synthesis typically refers to synthesesthat mimic biological synthesis processes in livingorganisms. An ultimate goal is to develop synthesistechniques and processes that can lead to the creationof new materials with similar or better/improvedproperties of naturally existing biological materials orto synthesize new materials with specifically desiredproperties using naturally existing materials. As arapidly emerging research field, biomimetic synthesishas attracted great interest of researchers from a numberof fields and is being considered a new frontier insynthetic chemistry in the twenty-first century. Aninteresting observation has been that some of the highlycomplex synthesis processes using traditional app-roaches become easy and efficient through biomimeticsynthesis. Here we use “biominerals” and “biomineral-ization” as examples to illustrate some basic ideas ofbiomimetic synthesis. Various biomineralized materialshave been formed as parts of living organisms asa result of genetic mutations and selection by evolutionsuch as bones, teeth, pearls, shells, diatoms, andspider silk. The formation of such special tissues,though by accidents, has given special advantages tothe relevant organisms and hence has been kept(selected) during evolution. The inorganic componentsin these special tissues such as calcium carbonate,calcium phosphates, calcium oxalate, metal sulfates,amorphous silica, iron oxide, and iron sulfide are gener-ally called biominerals.

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p0085 Biomineralization refers to the formation process ofbiominerals inside living organisms. The process typi-cally involves a sequence of chemical reactions leadingto the formation of new tissuesmostlymade of inorganicphases. The fundamental difference between biomineral-ization and mineralization in general is that in biominer-alization the precipitation of inorganic mineral phases isaccomplished through interactions between bio-macro-molecules and inorganic ions at the interface betweencells and body fluids which are controlled at the molec-ular level. Because of the unique formation process, bio-minerals often have special multilevel structures distinctfrom inorganic structures existing outside living organ-isms. They tend to have specific characteristics of crystalswith highly uniform sizes, clear structure and composi-tion boundaries, highly ordered spatial arrangements,complexmorphologies, andwell-defined crystal orienta-tions and tend to have clearly defined multilevel struc-tures. In a nutshell, biomineralization is a controlledprecipitation and deposition process of biomineralswith highly ordered, regular and multilevel structuresas the final products. The biomineralization processinside a living organism generally consists of four inter-twined and interactive steps: supramolecular preorgani-zation, interfacial molecular recognition, vectorialregulation, and cellular regulation and processing.

p0090 A key characteristic of biomineralization is the nucle-ation and growth of inorganic minerals around supra-molecular templates in a highly regulated manner.During the biomineralization process, the morphology,size, orientation, and structure of the biominerals arecontrolled in a sophisticated manner by organic compo-nents such as bio-macromolecules involved in theprocess. Understanding the mechanisms of biominerali-zation can be useful to guide biomimetic syntheses ofnew functional materials at multi-scales ranging fromthe meso- to macro-scale. This is rapidly becoming oneof the important research directions in material chem-istry as well as in inorganic synthetic chemistry. Thehighly interesting and unique properties of biomineral-ized materials, such as (a) lotus leaves and insect wingswith self-cleaning properties, (b) cameo shells withspecially high strength, toughness, and abrasion resis-tance, (c) rat’s tooth enamel, (d) spider silk with superbstrength and elasticity, and (e) iron oxides located insidefish heads serving as natural compasses, are all results ofdifferent structural characteristics of the self-assembledbiominerals at multiple scales. Fueled by these observa-tions, a new branch of chemistry, biomimetic materialchemistry, is being formed and is rapidly growing withthe key aims of elucidating relationships between func-tions and coordination effects among the multilevelstructures of biomineralized materials, to design desiredmultilevel structures, to apply learned mechanisms ofbiomineralization to the synthesis of inorganic

materials, and to synthesize materials with specificmultilevel structures and desired properties. In addi-tion, more and more attention is being paid to the devel-opment of new techniques that directly mimicbiochemical processes in inorganic syntheses, prepara-tion, and assemblies. For example, a number of synthesismethods such as widely used enzymatic catalysis,microorganism-mediated (such as virus and bacteria)synthetic reactions, and template effect used in synthesisand assembly of inorganic functional materials are allinspired by biological synthesis processes.

p0095Another example is the emergence of combinatorialsynthesis technique, which is regarded as a major break-through in the recent history of synthesis techniques.By organizing a large number of polypeptides in anarray as catalysts, combinatorial synthesis allows rapidsyntheses of astonishingly many new compoundswithin a short period of time. Such techniques havesignificantly shortened the screening time, for example,for potentially new drugs and new pesticides. Asa result, combinatorial syntheses are being extensivelyused in the preparation and hydrothermal synthesis ofinorganic materials.

s00551.5. RATIONAL SYNTHESIS ANDMOLECULAR ENGINEERING OFINORGANIC COMPOUNDS WITH

SPECIFIC STRUCTURES ANDFUNCTIONS

p0100There have been some cases of newmaterial synthesisthrough molecular design and engineering in recentyears. Traditionally, creation of new compounds withdesired properties typically involves syntheses of a largenumber of compounds and a selection process for thedesired compounds from these synthesized compounds.Since 1950s, the number of synthesized compoundshas increased from 2 million to more than 50 million,which has formed a large and highly useful compoundlibrary.

p0105The emerging field of molecular engineering takesa rather different approach to chemical synthesis. Thebasic idea is that it starts with desired functionalitiesof a to-be-synthesized material, designs the possiblestructures of the material based on the specified func-tionalities, and then creates the material throughrational synthesis. The biggest impact of the emergenceof molecular engineering on chemistry is that it hasgreatly broadened our view about the relationshipsamong the functionalities, structures, and synthesisprocesses, allowing us to better appreciate and under-stand the relationships between functions and high-level structures beyond single molecular structures.While this field is still in its nascent stage, it is already

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believed that this is the future direction of syntheticchemistry. Researchers have already started synthe-sizing new materials based on the general principles ofmolecular engineering in a number of selected fields.Among these studies, molecular design and rationalsynthesis of microporous crystal systems represent oneof the relatively mature research areas.

p0110 Microporous crystals generally have specific andregular channel structures [7]. The chemical interactionsbetween the guest molecules inside the channels andthe composition of the framework tend to be consider-ably stronger than those of other porous materials,and hence the structural features and properties of thechannels of such materials, such as the pore size, shape,dimension, orientation, composition of the channelwalls, cavities, cages, and structural defects, generallyhave significantly stronger effects on the diffusion,adsorption, and desorption, the formation of intermedi-ates and the selectivity of molecular reactions inside thechannels than those for other porous materials. Thus,microporous crystals represent the most unique system,and could potentially become one of the largest classesof catalysts and adsorptioneseparation materials.Microporous crystals as well as other porous materialssuch as mesoporous, macroporous, and porous MOFmaterials are being increasingly used in emerginghigh technologies, showing great potentials in thedevelopment of new materials in the future. As ofnow, 191 framework types of microporous zeolitesand 1000 types of zeolite-related inorganic open-framework materials, such as aluminosilicates andaluminophosphates, have been synthesized in laborato-ries. Over the years, extensive studies about these struc-tures have been done on the structural features, theframework structures, and their effects on the move-ment and reactivity of the molecules inside their chan-nels, the rules and principles of the pore-creatingreactions, crystallization, and modifications of the chan-nels, windows, and internal surfaces. Therefore, it isreasonable to select the microporous crystals as a casestudy in molecular engineering. While substantialwork has been done in this area, it should be notedthat only a small number of true success stories havebeen reported as of now.

p0115 The design and rational synthesis of microporouszeolites need to be done based on thorough study ofthe relationships between the specified functions ofthe to-be-synthesized material and channel structures.Initial channel models of the desired crystal could bedone with the help of computer programs. Subse-quently ideal structural models will be selected accord-ing to the established relationship between propertiesand structures of the microporous crystals derivedfrom known structures and functions of such crystalsin relevant databases. Finally, a rational synthesis plan

of these ideal structures will be made based on the rela-tionship between the structures and the synthesisconditions. But it is generally not possible to achievetrue rational syntheses like those done in organicsynthesis via analyzing reaction paths and steps,because their formation mechanism remains elusiveand relationship between the synthetic parametersand structural characters remains unclear. Despite thedifficulties associated with the rational synthesis,considerable efforts have been made to establish waystoward the rational design and synthesis of targetzeolitic materials. Our group has built up a ZEOBANKthat includes a database of zeolite synthesis and a data-base of zeolite structures with the aim to explore a novelway to guide the synthesis of zeolitic materials throughdata mining.

p0120Engineering the synthesis of new matters withdesired structures and functions has attracted consider-able attention in the areas of chemistry and materialscience. In Chapter 24 of this book, we will describeour efforts toward the rational design and synthesis ofzeolitic inorganic open-framework materials.

p0125Currently, our group as well as several other researchgroups has been actively carrying out studies in thefollowing areas: (1) method development for rationaldesign of structures, (2) development and update ofthe ZEOBANK synthesis and structure database andsynthetic approach guided by data mining for micropo-rous compounds, (3) in-depth study of the formationmechanisms of microporous compounds and thestructure-directing effect via experiments and computa-tional simulation, (4) derivation of potential synthesismechanisms as well as empirical relationship betweensynthesis conditions and resulting structures derivedbased on known synthesis data and computer simula-tion results, which could be used to guide rational struc-ture design and directed synthesis of desired materials,(5) performing combinatorial synthesis for microporouscompounds with specific structures and properties, and(6) structural modification, fine-tuning of the chemicalproperties of channels, windows and internal surfaces,and rational addition of specific active sites such asions, metal particles, oxides or salts, complex ions, andclusters into specific channels or onto the internalsurfaces based on the desired functions and propertiesof the microporous material.

p0130I would like to end this chapter with the words ofRyoji Noyori, the winner of Nobel Prize in 2001, in hisfeature article “Synthesizing our future” [5] that“Synthesis has a central role in chemistry; chemicalsynthesis has now reached an extraordinary level ofsophistication, but there is vast room for improvement;and chemical synthesis must pursue ‘practical elegance’that is, it must be logically elegant but must at the sametime lead to practical application.”

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References

[1] M.B. Rudy, Chemistry’s golden age, C&EN News (1998). Jan 12.[2] Committee on Challenges for the Chemical Sciences in the 21st

Century, Beyond the Molecular Frontier: Challenges for Chem-istry and Chemical Engineering, National Academy of Sciences,2003.

[3] P. Judeinstein, C. Sanchez, J. Mater. Chem. 6 (1996) 511e525.[4] P.A. Wender, Chem. Rev. 96 (1996) 1e2.[5] R. Noyori, Nat. Chem. 1 (2009) 5e6.[6] J.H. Clark, Nat. Chem. 1 (2009) 12e13.[7] R.R. Xu, W.Q. Pang, J.H. Yu, Q.S. Huo, J.S. Chen, Chemistry of

Zeolites and Related Porous Materials: Synthesis and Structure,John Wiley & Sons, Singapore, 2007.

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