THE CRYSTAL, MOLECULAR, AND ELECTRONIC STRUCTURE OF

µ-NITROGEN-DECAAMMINEDIRUTHENIUM(II) Introduction

Ten years ago, molecular nitrogen was described as an inert gas. In 1960, only the reaction of N2 (g) with metallic lithium giving the nitride, Li₃N, was known to proceed under mild conditions.

There were, however, intimations of a dormant reactivity in N₂^• The well publicized, but hardly understood, fixation of atmospheric nitrogen by plants served as a constant source of speculation for chemists. Even then, it was thought that this facile conversion of N₂ into NH₃ was being effected by enzymes containing transition metal centers. (68)

In the subsequent ten years molybdenum and iron have definitely been identified as metals present at the active sites of plant enzymes used in the fixation process. (53

) Equally important, the synthesis of transition metal compounds which bind molecular nitrogen has been

achieved in the last five years. Currently, there are about 20 well characterized transition metal compounds which contain molecular N₂ as a ligand. These compounds contain a variety of transition metals, Ir, Co, Rh, Ru, Fe, Os, Ni, almost all in lower oxidation states. (59 , 7o) As of yet, most of these synthetic compounds do not permit reduction of their molecular N2 to NH₃ by common reducing agents. So far, only the titanium alkoxide/ sodium napthalide/ alcohol systems of

van Tamelen, (7l) and the titanocenyl dichloride/ethylmagnesim:n br.omide

system of Vol' pin (72) have been found to abstract atmospheric

nitrogen, which is reducible to ammonia. Nevertheless, the transition metal compounds having N₂ as ligands are still of major import.

Even if reduction to NH₃ is unattainable at present, these compounds serve as models for the first step of the proposed fixation-reduction- protonation cycle for N₂ (g) - NH₃(g) conversion. (5B)

Of these compounds, Ru(NH_{3) 5}N₂ 2+ is perhaps the most important, not only because it was the first one prepared, but also because it alone is made up of extremely simple auxiliary ligands, i.e., NH₃ rather than more complex ligands like phosphines. This compound was first prepared in 1965 by refluxing an aqueous solution of RuC1₃ and N₂H₄ ^• HCl, and has subsequently been prepared in a number of different ways. It has been found to possess a v(N-N)

of - 2100-21 70 cm-¹ with variations ascribable to the anion present. (73) In 1967, Harrison and Taube(74

) found that equimolar amounts

2+ 2+

of Ru(NH₃)i;N₂ and Ru(NH_{3) 5}liz0 condense quantitatively to give the dimer (NH₃⁾₅RuN₂Ru(NH₃⁾₅ 4+ ^• This was the first nitrogen dimer

made. These two cations are easily distinguishable by their electronic absorptions; the monomer has a Amax = 221 nm and the dimer a Amax = 263 nm.

Itzkovich and Page (75 ) studied the monomeric and dimeric ..

compounds , and found that both were very much more resistant to oxidation than normal Ru(II) pentaammine-X salts. Also perplexing

2+ . .

was the fact that Ru(NH₃⁾₅N₂ had such an unusually strong affm1ty for Ru(II)-HzO, almost completely replacing the aquo group via

nucleophilic attack, despite a 500 fold excess of water over Ru(II)-N_{2 •}

This compound was not only perplexing, but important when viewed with the biological nitrogen fixation process in mind. It is thought that in plants, initial nitrogen binding is a result of entrapment

between two metal centers (perhaps

~ven

atoms of different metals). (69) This fact makes the ruthenium dimer extremely important, and an

understanding of its bonding necessary.

Because nitrogen has two rr bonds, a number of alternate modes of bonding in the dimer are possible(69):

M-N N N

~

/

"

M-N=N-M N-M ^M M

(A)

(B)

^(C)

N N N

M---111---M

/.,111- -

-M

i&

/ "

N M" N ^M M

(D) (E) (F)

The dimer N-N stretch was known to be inactive in the infrared(74); a structure without a center of symmetry such as (C), (E) ₁ and (F) could therefore be eliminated. Determination of the structure of the ruthenium monomer had already been attempted, (?6) but because of disorder in the crystal, exact bond lengths could not be gotten. However, from the limited data obtained, the M-N₂ unit appeared to be linear. This information could not be used to

extrapolate to the dimer. In the dimer, it could be argued, additional electronic density would be transferred from the second metal to the

bridging N₂ to produce a trans-azo structure (B). Such a structure, with rutheniums in a formal oxidation state of three, conceivably could explain the difficulty in oxidizing a supposedly Ru(II) dimer.

In addition to the question of the RuNNRu angle, the question of the N-N length in the dimer was important. It was reasoned that the back bonding from Ru d orbitals to the empty rr* orbital of N₂ was not very extensive, at least in the monomer, because the v(N-N) in the monomer was reduced only about 150-200 cm-¹ from the free N₂(g) value of 2331 cm ^{- i .} The bond order here has to be almost three as in free N_{2 •} Azo compounds with a formal bond order of two have N-N stretches in the 1500-1600 cm-¹ region. Again, it could be argued that with an· additional Ru atom, enough electronic density could be placed in the rr* orbital to reduce the bond order significantly and produce a structure like (B).

To answer the questions of bond angle and bond order, an

X-ray structural determination of the ruthenium dimer was undertaken.

In addition to its importance as a model for the intermediates in plant fixation of atmospheric N_{2 ,} the structure would aid in understanding the electronic absorptions of the dimer and monomer. These spectra are in themselves of interest because they would help in understanding the interactions of metals and rr-acceptor ligands. The dimer is an important link in the class of binuclear compounds containing simple diatomic bridging ligands such as 0₂ ^- and CN-.

Experimental Section

The crystals used in our study were prepared by the procedure described in the literature. (74) A 0. 05 M solution of Ru(NH_{3) 5}Cl ·

C~

(0. 1 Min HzS0_{4 )} was reduced with Zn(Hg) under argon. After 50 min. , the solution was separated from excess Zn. Nitrogen was bubbled in for 10 hrs. , and the solution was then allowed to sit in a nitrogen-filled glove bag for another four days. The color changed from an initial dark blue to green and then finally to golden yellow.

Following this, the solution was filtered in the absence of air into an excess of KBF_{4 •} A few days later, small golden yellow octahedral crystals were found buried under an excess of fluoroborate. A number of these crystals were separated, washed with ethanol,

mounted on glass fibers, and used for X-ray studies. These crystals exhibited an absorption at 262 nm, with an extinction coefficient of .... 4. 8

x

10^4, a value which agrees with that found in the literature. <⁷⁴)

Weissenberg photographs (CuKa radiation) of the hkO, hkl, and hk2 layers showed the systematic absences of the Old reflections with k

=

2n + 1, hOQ reflections with £.

=

2n + 1, and hkO reflections with h

=

2n + 1, confirming the space group as orthorhombic

15 •

D2h - Pbca' Umt cell constants were gotten by a least-squares fit of seven reflections, measured on an automated diffractometer. The

dimensions obtained were a ⁼ 12. 777(5), b ⁼ 15. 531 (6), c ⁼ 13. 342(4).A.

The observed density obtained by flotation in a carbontetrachloride- 1, 2-dibromoethane mixture was 1. 96 g/cm . This is in excellent 3

agreement with the value of 1. 97 g/ cm calculated for four dimeric 3

cations, sixteen BF_{4 -} anions, and eight water molecules per unit cell.

In the Pbca space group, each dimeric cation must lie on a center of symmetry.

Intensity data were collected, using zirconium-filtered

MoKa radiation. The crystal 1:1sed was mounted with its body diagonal approximately parallel to the <I> axis of a Datex-automated General Electric XRD-6 diffractometer. Measurements were made using a fJ-2() scanning rate of 4 ° per minute. Background was counted for 30 seconds at the end of the scan. The scan range was 2 ° at low angles, and 4 ° at higher angles. An intense reflection, 408, was chosen as a check reflection, and measured every 20 reflections.

During the period of data collection, about 8 days, this reflection remained constant to within 2 percent, indicating the lack of serious decomposition.

Of 3040 independent reflections, 2645 were calculated as greater than zero, and were used in the refinement of the structure.

The 1490 reflection was deleted in the refinement because of an obviously false scintillation count.

Treatment of the Data

The value of the observed intensities, Iobsvd'were derived from B1 + Bz t

the formula Iobsvd = S - 2 (

30),

where Sis the scan count, B₁ and B₂ the two background counts, and t the scan time in seconds.

Negative values of Iobsvd' calculated from the formula, were set equal to zero.

The standard deviation for each reflection was calculated using

B1 + B2 t z

a₂ (Iobsvd) = S + 2 (30

f

⁺ (O. 02S) . The intensities and their standard deviations were corrected for Lorentz and polarization factors, but not for absorption. The standard deviations calculated in this way were the basis for the weights used in the least squa,.res refinement.

Determination and Refinement of the Structure

The approximate coordinates of the ruthenium atoms were easily found from a three-dimensional sharpened Patterson map.

A structure-factor calculation using these coordinates gave an

~IF

I-IF I

R index of u. 42 (R = ⁰

I I

c ) . An electron density map quickly

~ Fo

revealed all the other non-hydrogenic atoms. After four cycles of full matrix least-squares, varying in a single matrix the scale factor, the positional parameters for all non-hydrogen atoms, anisotropic

temperature factors for the ruthenium atoms, and isotropic temperature factors for all the other atoms, the R index was reduced to 0.17.

Introducing anisotropic temperature factors for all non-hydrogenic atoms into a subsequent least-squares calculation (163 parameters) brought R down to 0. 099.

At this point in the refinement, difference maps were

calculated in the planes where the ammine hydrogens were expected. No distinct peaks appeared; rather smeared out rings of electron

density were present. A number of different choices for each hydrogen were tried. The one giving the most satisfactory distances and angles was used. Computations showed that a preferential orientation, due

to hydrogen bonding between the ammino hydrogens and the BF _{4 -} fluorines, was not present, and therefore the smeared out rings on the difference maps were reasonable. The water hydrogens were placed on lines connecting the oxygen with their nearest fluorine

neighbors, at what is the usual OH distance. The hydrogen coordinates, together with their isotropic temperature factors, were varied in a least-squares cycle. Together with the previously refined coordinates and anisotropic factors of the non-hydrogen atoms, they produced a final R of 0. 090. In this least-squares cycle, 154 parameters were refined. The final weighted R index was 0. 013. The goodness of fit,

1

[ z;w(F

0 2

- F c² /k²⁾² /(m - s)] ~, where m is the number of reflections, s the number of refineable parameters, and k the scale factor, was 1. 63.

Calculations were carried out on IBM 360-75 and IBM 7094 computers at the California Institute of Technology, using subprograms operating under the CRYM and CRYRM crystallographic computing system. The quantity minimized in the least-squares calculations

2 2 2 2

was l;w(F

0 · - F c ) where w = 1/ a (F

0) • Ato1;llic form factors for

ruthenium, nitrogen, oxygen, fluorine, and boron were taken from the "International Tables. "(77 ) The form factor for hydrogen was that calculated by Stewart, Davidson, and Simpson. (?S) Correction for the real part of anamolous dispersion was applied to the ruthenium atom.

Table ill-1 contains the observed and calculated structure factors. The final parameters and their standard deviations for the

non-hydrogen atoms are listed in Table III-2. Positional parameters for the hydrogen atoms are contained in Table III-3. Interatomic distances and bond angles can be found in Tables III-4 and III-5, respectively.

The estimated standard deviations (e. s. d.) for the positional

0 0

parameters are about 0. 0005A for the ruthenium atoms, 0. 005A for

0 0

the ammino nitrogens, 0. 005A for the nitrogeno nitrogens, 0. 007A for

0 0

oxygen, 0. OlA for the boron, and 0. 006A for fluorine. These latter two numbers apply only to the well-behaved BF ₄^- group. These

0 0

e. s. d. 's lead to an e. s. d. of 0. 006A for the Ru-NH₃ bond, 0. 006A

0 0

for the Ru-N₂ bond, 0. 015Afor the N-N bond, O. 002A for the Ru-Ru distance, and 0. 5° for the Ru-N-N angle.

Description and Discussion of the Structure The Cation

~

Of primary interest in this investigation was the configuration of the Ru-N₂-Ru unit. The bridging group was found to be very nearly linear with a Ru-N--N angle of 178. 3(5) ^{0 •} The N-N distance was found to be 1.124(15)A, only slightly larger than free N₂

(1.0976A)(79 ) or N₂+ (1.118A). (30) It is well below the N-N distance in hydrazine (1. 46A)

~

⁸¹

)

Our N-N length is almost equal to that found in N₂0 (1.126.A), (3l) and the unprotonated N-N distance in HN₃ (1.128A). (Bl) Five ammonia groups complete the octahedral coordination about each ruthenium with the two equatorial sets of ammonias in an eclipsed conformation, as required by symmetry.

Table III-1

Observed and Calculated Structure Factors for ((NH_{3) 5}RuN₂Ru(NH_{3) 5 ]} (BF_{4 ) 4 •} 2~0

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