Structural Characterization and Chemistry of the Industrially Important Zinc Borate, Zn[B 3 O 4 (OH) 3 ] David M. Schubert,* Fazlul Alam, Mandana Z. Visi, and Carolyn B. Knobler U.S. Borax Inc., 26877 Tourney Road, Valencia, California 91355 Received August 13, 2002. Revised Manuscript Received November 28, 2002 Several unique crystalline zinc borates are known, a few of which find industrial use in significant tonnages. Although the most important of these has been a commercial product for more than 3 decades, it was never before structurally characterized. The structure of Zn[B 3 O 4 (OH) 3 ](1) was determined for the first time by single-crystal X-ray diffraction, revealing it to be a complex network consisting of infinite polytriborate chains cross-linked by coordination with zinc and further integrated by hydrogen bonding. The structure of 1 bears similarities to certain borate minerals, most notably, studenitsite (Ca[B 3 O 4 (OH) 3 ]) and colemanite (Ca[B 3 O 4 (OH) 3 ]H 2 O); however, significant differences are described. Hydrolytic and thermochemical properties of 1 are discussed. This compound illustrates the important role played by metal cations in directing the spatial arrangement of anionic polyborate structural units in metal borates. This new structural information leads to a revision in the chemical formula, 2ZnO3B 2 O 3 3.5H 2 O, typically used to describe this material as an article of commerce, to 2ZnO3B 2 O 3 3H 2 O. Compound 1 crystallizes in the monoclinic space group P2 1 /n with a ) 6.845(2) Å, b ) 9.798(2) Å, c ) 7.697(2) Å, ) 106.966(4)°, V ) 493.8 (2) Å 3 , and Z ) 4. Introduction Occurring in both mineral and synthetic forms, metal borates in which boron is bound only to oxygen are numerous and find extensive industrial use. Many synthetic metal borates resemble minerals in structure, containing isolated polyborate anions or complex po- lyborate rings, chains, sheets, or networks. However, structure-stability theories recently developed for bo- rate minerals do not consistently apply to synthetic borates. Understanding how cations direct borate struc- tural units in borate compounds is fundamental to the development of synthetic strategies for metal borates having useful properties. Metal borates can be divided into two categories, hydrated and anhydrous. So-called hydrated borates, which account for the majority of known boron-contain- ing minerals and synthetic borates consumed by indus- try, have structures containing B-OH groups (hydroxyl- hydrated borates) and may also contain interstitial water. Although structural details for most commer- cially relevant crystalline hydrated borates are known, the structures of several important zinc borates, includ- ing the title compound 1, have not been described. There is good evidence for the existence of at least eight unique crystalline hydrated zinc borates. These have compositions 4ZnOB 2 O 3 H 2 O (2), 1 ZnOB 2 O 3 1.12H 2 O(3), 2 ZnOB 2 O 3 2H 2 O(4), 2 6ZnO5B 2 O 3 3H 2 O(5), 3 2ZnO3B 2 O 3 7H 2 O(6), 4 2ZnO3B 2 O 3 3H 2 O (1), 3ZnO5B 2 O 3 14H 2 O, 5 and ZnO5B 2 O 3 4.5H 2 O, 3 spanning a range of B 2 O 3 /ZnO mole ratios from 0.25 to 5.0. Each of these compounds can be prepared selec- tively by reactions of zinc oxide with boric acid in water, the specific product obtained determined by reactant concentrations and temperature. Aside from the title compound, to date only the structures of 3 and 6 have been reported; the latter has the structural formula Zn- [B 3 O 3 (OH) 5 ]H 2 O and contains a monomeric triborate dianion. 4 Zinc borates have found industrial use since the 1940s, 6 with 2ZnO3B 2 O 3 7H 2 O and 3ZnO5B 2 O 3 14H 2 O primarily utilized in the earlier period. However, these compounds had a limited range of applications owing to their low dehydration temperatures. The most im- portant commercial zinc borate today, 1, was introduced more than 30 years ago and now has a worldwide annual production exceeding 10 000 metric tons. It is primarily used as a polymer additive and as a preserva- tive in wood composites. As a polymer additive, it serves as a fire retardant synergist, char promoter, antidrip agent, smoke and afterglow suppressant, and modifier of electrical and optical properties. Addition of 1 to ceramic bodies can improve green strength and reduce firing times, temperatures, and pyroplastic deformation. * To whom correspondence should be addressed. McCullough Crystallographic Laboratory, Department of Chem- istry and Biochemistry, University of California, Los Angeles. (1) Schubert, D. M. U.S. Patent 5,342,533, 1994. (2) Choudhury, A.; Neeraj, S.; Natarajan, S.; Rao, C. N. J. Chem. Soc., Dalton Trans. 2002, 7, 1535-1538. The recently characterized 3 is apparently a different compound from 4, also known in trade literature as 2ZnO2B2O33H2O, which has been an article of commerce for many years. (3) Lehmann, H.-A.; Sperscheider, K.; Kessler, G. Z. Anorg. Allg. Chem. 1967, 354, 37-43. (4) Ozols, J.; Tetere, I.; Ievins, A. Izv. Akad. Latv. Nauk. SSR, Ser. Kim. 1973, 1,3-7. (5) Putnins, J.; Ievins, A. Latv. Valsts Univ. Kim. Fak. Zinat. Raksti 1958, 22, 69. This compound has been referred to as 2ZnO3B 2O39H2O in trade literature. (6) The Crown 1944, 9, 31. 866 Chem. Mater. 2003, 15, 866-871 10.1021/cm020791z CCC: $25.00 © 2003 American Chemical Society Published on Web 01/25/2003