Review of Catalytic Hydrogen Generation in the Defense Waste Processing Facility (DWPF) Chemical Processing Cell

Abstract

EXECUTIVE SUMMARYThis report was prepared to fulfill the Phase I deliverable for HLW/DWPF/TTR-98-0018, Rev. 2, "Hydrogen Generation in the DWPF Chemical Processing Cell", 6/4/2001. The primary objective for the preliminary phase of the hydrogen generation study was to complete a review of past data on hydrogen generation and to prepare a summary of the findings. The understanding was that the focus should be on catalytic hydrogen generation, not on hydrogen generation by radiolysis. The secondary objective was to develop scope for follow-up experimental and analytical work.The majority of this report provides a summary of past hydrogen generation work with radioactive and simulated Savannah River Site (SRS) waste sludges. The report also includes some work done with Hanford waste sludges and simulants. The review extends to idealized systems containing no sludge, such as solutions of sodium formate and formic acid doped with a noble metal catalyst. This includes general information from the literature, as well as the focused study done by the University of Georgia for the SRS.

Review of Catalytic Hydrogen Generation in the DWPF Chemical Processing Cell, Part II

“…The data in Figure 3 and Figure 4 may be evidence to support the hydrogen work done for SRS at the University of Georgia that suggested that a nitro rhodium complex, Rh(NO 2 ) 6 3-, was the most active form of rhodium for hydrogen generation, Koopman (2004). The rate of hydrogen generation could increase as more of this complex is formed.…”

“…Results from these three runs are given in Figure 5. Run 5-Ru more Ru than Rh because of the U-235 fission yields as discussed in the earlier review report, Koopman (2004). It is possible that Rh is important in complexing the residual nitrite in the slurry before Ru can become active.…”

“…D. P. Lambert was the lead researcher. The data were located during the collection of raw hydrogen generation data prior to preparation of the initial hydrogen generation review report, Koopman (2004). It was noted in the review report that the analysis and conclusions from that set of tests had not been documented.…”

“…through Sludge Batch 2. Now issued, see Koopman (2004). Analyze some 1998 data found during the review.…”

“…This phase was also used to evaluate and report on data taken in 1998 under the direction of D. P. Lambert, referred to as the "Boley-Lambert data" in Koopman (2004). This was a preliminary study into the impact of nitrite on rhodium catalyzed hydrogen generation.…”