1 Control of Carbon Deposition within the AGR Primary Circuit - Chemistry in Energy, Edinburgh, July NOT PROTECTIVELY MARKED
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2 Chemistry in Energy Control of Carbon Deposition within the Primary Circuit of Advanced Gas-Cooled Reactors Clive Mowforth, Carbon Deposition Programme, Lifetime Programmes Kelvin Hinds, Chemistry & CO 2 Oxidation Group, Engineering Division Neal Smith, Chemistry & CO 2 Oxidation Group, Engineering Division EDF Energy Generation 2
3 The Problem 3
4 Advanced Gas-Cooled Reactor (AGR) Fuel channel One of circa 320 Temp up to 750 C Boilers One of 8-12 Temp up to 580 C 4
5 Fuel-Pin Deposit Fine granular morphology Columnar morphology High levels of fuel pin deposition (picture from PIE analysis) Low levels of fuel pin deposition (picture from PIE analysis) 5
6 Boiler Deposit 6 6
7 Mechanism 7
8 Mechanism CO 2 Methane Ethene Nickel particle Carbon deposit and hydrogen 8
9 Deposit Filaments 9
10 Source of Nickel Underlying Alloy Fuel rods (25% Ni) Transverse stripes of deposit aligned with rib-cutting marks (TOR T2020 Element 8) Spirals of deposit associated with electrodeplating (HNB C3636 Element 8) Boiler tubes (up to 70% Ni) Variation across upper transition joint (HNB R3 2006: Boiler D3) 10
11 Source of Nickel Coolant Ni(CO) 4 R3 Gas Bypass Plant HPB IFDF assessments of fuel loaded
12 Control 12
13 Change Surface Chemistry Add protective oxide film to fuel rods - Prevents rapid oxidation and production of Ni by-product - Relatively straight forward - Replaced periodically so feasible - Long lead time Boiler tubes - Cannot be replaced so no change possible Trials with range of moisture concentrations in hydrogen atmosphere of annealing furnace Fuel Element with pre-oxidised fuel rods 13
14 Change Coolant Chemistry Implementation potentially rapid Chemistry more complex Leading candidates - Carbonyl sulphide (COS) - Already exists with minor other S species (equilibrium perturbed by radiation) - Impurity from graphite moderator and oil - Range of vpb - Carbon monoxide (CO) - Essential coolant component - Formed mainly from CH 4 destruction - Allowed to build up to circa 1.0 vol% to reduce moderator graphite oxidation 14
15 Change Coolant Chemistry - COS Long history - High concentrations associated with low deposition Deliberate injection - Successful at controlling boiler deposition in range vpb - Successful on lower fuel elements but not upper - Temperature dependence confirmed with experiments at Birmingham University COS Concentration, vppb depositing non-depositing Temp vs COS predict Temperature, o C Boiler heat-transfer impairment (HTI) results for HRA R1 following start of COS injection in January 1999 T/[COS] matrix on fuel rod alloy 15
16 Change Coolant Chemistry - CO Concentration optimisation - High concentrations associated with high deposition in 1980s at HPB/HNB - Affects mobility of Ni(CO) 4 - Equilibrium p 4 dependence - Formation rate p 2 dependence - Transport to site of deposition Recent results - Negative correlation between fuel rod deposit thickness and [CO] at HRA/HYA - Birmingham University shown that CO affects Ni/Fe catalyst particle composition (only high Ni active) and size - Potential mechanisms - Direct effect of CO on fuel alloy oxidation - Removal as Ni(CO) 4 from site of deposition Number of ppts Fit to HRA R1 fuel rod deposit measurements CO 0.7CO size, nm Effect of [CO] on catalyst particle size 16
17 Summary 17
18 Summary Carbon deposition still occurring in AGRs Greatest problem on fuel rods and boiler tubes - Impairs heat transfer - Catalysed by Ni - Control deposition by controlling Ni Control methods - Change surface chemistry - Add protective oxide to fuel rods during manufacture - Change coolant chemistry - Inject COS - Adjust [CO] 18
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