2The spontaneous imbibition of water and other liquids into gas-filled 3 fractures in variably-saturated porous media is important in a variety of 4 engineering and geological contexts. However, surprisingly few studies have 5 investigated this phenomenon. We present a theoretical framework for 6 predicting the 1-dimensional movement of water into air-filled fractures 7 within a porous medium based on early-time capillary dynamics and 8 spreading over the rough surfaces of fracture faces. The theory permits 9 estimation of sorptivity values for the matrix and fracture zone, as well as a 10 dispersion parameter which quantifies the extent of spreading of the wetting 11 front. Quantitative data on spontaneous imbibition of water in unsaturated 12 Berea sandstone cores were acquired to evaluate the proposed model. The 13 cores with different permeability classes ranging from 50 to 500 mD and 14 were fractured using the Brazilian method. Spontaneous imbibition in the 15 fractured cores was measured by dynamic neutron radiography at the 16 Neutron Imaging Prototype Facility (beam line CG-1D, HFIR), Oak Ridge 17 National Laboratory. Water uptake into both the matrix and the fracture 18 zone exhibited square-root-of-time behavior. The matrix sorptivities ranged 19 from 2.9 to 4.6 mm s -0.5 , and increased linearly as the permeability class 20 increased. The sorptivities of the fracture zones ranged from 17.9 to 27.1 21 mm s -0.5 , and increased linearly with increasing fracture aperture width. The 22 dispersion coefficients ranged from 23.7 to 66.7 mm 2 s -1 and increased 23 linearly with increasing fracture aperture width and damage zone width. 24 Both theory and observations indicate that fractures can significantly 25 increase spontaneous imbibition in unsaturated sedimentary rock by 26 capillary action and surface spreading on rough fracture faces. Fractures 27 also inrease the dispersion of the wetting front. Further research is needed 28 7

The heterobimetallic actinide compound UO(2)Ce(H(2)O)[C(6)H(4)(PO(3)H)(2)](2)·H(2)O was prepared via the hydrothermal reaction of U(VI) and Ce(IV) in the presence of 1,2-phenylenediphosphonic acid. We demonstrate that this is a kinetic product that is not stable with respect to decomposition to the monometallic compounds. Similar reactions have been explored with U(VI) and Ce(III), resulting in the oxidation of Ce(III) to Ce(IV) and the formation of the Ce(IV) phosphonate, Ce[C(6)H(4)(PO(3)H)(PO(3)H(2))][C(6)H(4)(PO(3)H)(PO(3))]·2H(2)O, UO(2)Ce(H(2)O)[C(6)H(4)(PO(3)H)(2)](2)·H(2)O, and UO(2)[C(6)H(4)(PO(3)H)(2)](H(2)O)·H(2)O. In comparison, the reaction of U(VI) with Np(VI) only yields Np[C(6)H(4)(PO(3)H)(2)](2)·2H(2)O and aqueous U(VI), whereas the reaction of U(VI) with Pu(VI) yields the disordered U(VI)/Pu(VI) compound, (U(0.9)Pu(0.1))O(2)[C(6)H(4)(PO(3)H)(2)](H(2)O)·H(2)O, and the Pu(IV) phosphonate, Pu[C(6)H(4)(PO(3)H)(PO(3)H(2))][C(6)H(4)(PO(3)H)(PO(3))]·2H(2)O. The reactions of Ce(IV) with Np(VI) yield disordered heterobimetallic phosphonates with both M[C(6)H(4)(PO(3)H)(PO(3)H(2))][C(6)H(4)(PO(3)H)(PO(3))]·2H(2)O (M = Ce, Np) and M[C(6)H(4)(PO(3)H)(2)](2)·2H(2)O (M = Ce, Np) structures, as well as the Ce(IV) phosphonate Ce[C(6)H(4)(PO(3)H)(PO(3)H(2))][C(6)H(4)(PO(3)H)(PO(3))]·2H(2)O. Ce(IV) reacts with Pu(IV) to yield the Pu(VI) compound, PuO(2)[C(6)H(4)(PO(3)H)(2)](H(2)O)·3H(2)O, and a disordered heterobimetallic Pu(IV)/Ce(IV) compound with the M[C(6)H(4)(PO(3)H)(PO(3)H(2))][C(6)H(4)(PO(3)H)(PO(3))]·2H(2)O (M = Ce, Pu) structure. Mixtures of Np(VI) and Pu(VI) yield disordered heterobimetallic Np(IV)/Pu(IV) phosphonates with both the An[C(6)H(4)(PO(3)H)(PO(3)H(2))][C(6)H(4)(PO(3)H)(PO(3))]·2H(2)O (M = Np, Pu) and An[C(6)H(4)(PO(3)H)(2)](2)·2H(2)O (M = Np, Pu) formulas.

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