Production of H2 by water radiolysis in cement paste under electron irradiation: A joint experimental and theoretical study
Source abstract
Abstract
Long-term confinement of nuclear waste is one of the main challenges faced by the nuclear industry. Fission products such as 90 Sr and 137 Cs, both β − emitters known to induce serious health hazards, represent the largest fraction of nuclear waste. Cement is a good candidate to store them, provided it can resist the effects of irradiation over time. Here, we have investigated the effects of β − decay on cement by performing electron irradiation experiments on different samples. We show that H 2 production in cement, the main effect of water radiolysis, depends strongly on composition and relative humidity. First-principles calculations indicate that the water-rich interlayer regions with Ca 2+ ions act as electron traps that promote the formation of H 2. They also show that holes localize in water-rich regions in low Ca content samples and are then able to participate in H 2 production. This work provides new understanding of radiolysis effects in cements.
Source: openaire · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Radioactive element chemistry and processing · Nuclear materials and radiation effects · Concrete and Cement Materials Research
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (67)
Show source-provided references
1. Call for better oversight of nuclear waste storage10.1038/509267a ↗
2. Nuclear fuel in a reactor accident10.1126/science.1211285 ↗
3. Assessment of individual radionuclide distributions from the Fukushima nuclear accident covering central-east Japan10.1073/pnas.1111724108 ↗
4. The global impact of the Chernobyl reactor accident10.1126/science.3201240 ↗
5. Cesium-137 deposition and contamination of Japanese soils due to the Fukushima nuclear accident10.1073/pnas.1112058108 ↗
6. Composition and density of Nanoscale calcium–silicate–hydrate in cement10.1038/nmat1871 ↗
7. A realistic molecular model of cement hydrates10.1073/pnas.0902180106 ↗
8. Refinements to colloid model of C-S-H in cement: CM-II10.1016/j.cemconres.2007.10.006 ↗
9. Surface relaxation and chemical exchange in hydrating cement pastes: a two-dimensional NMR relaxation study10.1103/PhysRevE.72.011409 ↗
10. Characterisation of intra- and inter-C–S–H gel pore water in white cement based on an analysis of NMR signal amplitudes as a function of water content10.1016/j.cemconres.2010.08.003 ↗
11. Densification of C-S-H measured by H NMR relaxometry10.1021/jp3102964 ↗
12. Spinks · 1990
13. Radiation effects in nuclear waste forms for high-level radioactive waste10.1016/0149-1970(94)00016-Y ↗
14. Gamma irradiation resistance of an early age slag-blended cement matrix for nuclear waste encapsulation10.1557/jmr.2014.404 ↗
15. Review of the current state of knowledge on the effects of radiation on concrete10.3151/jact.14.368 ↗
16. A comprehensive model to describe radiolytic processes in cement medium10.1016/j.jnucmat.2006.10.004 ↗
17. Cement as a waste form for nuclear fission products: the case of 90Sr and its daughters10.1021/acs.est.5b02609 ↗
18. Radiolysis of confined water: hydrogen production at a high dose rate10.1002/cphc.200500185 ↗
19. H2 formation by electron irradiation of SBA-15 materials and the effect of CuII grafting10.1039/c0cp00115e ↗
20. Water radiolysis: influence of oxide surfaces on H2 production under ionizing radiation10.3390/w3010235 ↗
21. Physical aspects of photochemistry and radiation chemistry of molecules adsorbed on SiO2, gamma-Al2O3, zeolites, and clays10.1021/cr00017a014 ↗
22. Water radiolysis in exchanged-montmorillonites: the H2 production mechanisms10.1021/es401490t ↗
23. Reaction mechanisms in talc under ionizing radiation: evidence of a high stability of H atoms10.1021/acs.jpcc.5b11396 ↗
24. Reaction mechanisms in swelling clays under ionizing radiation: influence of the water amount and of the nature of the clay mineral10.1039/C6RA24861F ↗
25. Sassani · 2015
26. Hardin · 2015
27. Mehta · 2006
28. Nelson · 2006
29. Taylor · 1997
30. Nano-chemo-mechanical signature of conventional oil-well cement systems: effects of elevated temperature and curing time10.1016/j.cemconres.2014.08.008 ↗
31. Mercury porosimetry of hardened cement pastes10.1016/S0008-8846(99)00083-6 ↗
32. Alternative binders to ordinary portland cement for radwaste solidification and stabilization
33. Long-term behaviour of cement pastes used for nuclear waste disposal: review of physico-chemical mechanisms of water degradation10.1016/S0008-8846(98)00053-2 ↗
34. Relation between chemical composition and physical properties of C-S-H generated from cementitious materials10.3151/jact.13.275 ↗
35. Bound water in cement pastes and its significance for pore solution compositions10.1557/PROC-85-47 ↗
36. DTA, TG, and XRD studies of sturmanite and ettringite10.2113/gscanmin.40.5.1403 ↗
37. Thermogravimetric analysis
38. Microstructure of cement paste subject to early carbonation curing10.1016/j.cemconres.2011.09.010 ↗
39. The radiolysis project of CEA10.1051/jcp:1999108 ↗
40. Fricke · 1966 · 167
41. The real structure of tobermorite 11 a: normal and anomalous forms, OD character and polytypic modifications10.1127/0935-1221/2001/0013-0577 ↗
42. CP2K: atomistic simulations of condensed matter systems10.1002/wcms.1159 ↗
43. A hybrid Gaussian and plane wave density functional scheme10.1080/00268979709482119 ↗
44. Quickstep: fast and accurate density functional calculations using a mixed Gaussian and plane wave approach10.1016/j.cpc.2004.12.014 ↗
45. Gaussian basis sets for accurate calculations on molecular systems in gas and condensed phases10.1063/1.2770708 ↗
46. Zhao · Theor. Chem. Accounts · 2008 · 120 · 21510.1007/s00214-007-0310-x ↗
47. Generalized gradient approximation made simple10.1103/PhysRevLett.77.3865 ↗
48. Separable dual-space Gaussian pseudopotentials10.1103/PhysRevB.54.1703 ↗
49. Relativistic separable dual-space Gaussian pseudo-potentials from H to Rn10.1103/PhysRevB.58.3641 ↗
50. A consistent and accurate ab initio parametrization of density functional dispersion correction (DFT-D) for the 94 elements H-Pu10.1063/1.3382344 ↗
51. Effect of the damping function in dispersion corrected density functional theory10.1002/jcc.21759 ↗
52. Exchange and correlation in atoms, molecules, and solids by the spin-density-functional formalism10.1103/PhysRevB.13.4274 ↗
53. Ab initio molecular dynamics using hybrid density functionals10.1063/1.2931945 ↗
54. Robust periodic Hartree-Fock exchange for large-scale simulations using Gaussian basis sets10.1021/ct900494g ↗
55. Auxiliary density matrix methods for Hartree-Fock exchange calculations10.1021/ct1002225 ↗
56. QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials10.1088/0953-8984/21/39/395502 ↗
57. Canonical sampling through velocity rescaling10.1063/1.2408420 ↗
58. Time-reversible always stable predictor-corrector method for molecular dynamics of polarizable molecules10.1002/jcc.10385 ↗
59. Effect of relative humidity and air permeability on prediction of the rate of carbonation of concrete10.1680/stbu.2001.146.3.319 ↗
60. Hydration states of AFm cement phases10.1016/j.cemconres.2015.02.011 ↗
61. Investigation of the carbonation mechanism of CH and C-S-H in terms of kinetics, microstructure changes and moisture properties10.1016/j.cemconres.2013.11.015 ↗
62. Electron-hole trapping in X-irradiated calcium carbonate and sodium nitrate10.1021/j100866a001 ↗
63. The solubility product of calcium peroxide octahydrate in relation to temperature; its influence on radiolysis in cement-based materials10.1016/j.jnucmat.2011.09.009 ↗
64. H2 and Cl2 production in the radiolysis of calcium and magnesium chlorides and hydroxides10.1021/jp044166o ↗
65. A review of electron spin spectroscopy and its application to the study of paramagnetic defects in crystalline quartz10.1007/BF00311472 ↗
66. Hydrogen radiolytic release from zeolite 4A/water systems under γ irradiations10.1016/j.radphyschem.2015.01.008 ↗
67. The tobermorite supergroup: a new nomenclature10.1180/minmag.2015.079.2.22 ↗