Harry Eccles - Academia.edu (original) (raw)
Papers by Harry Eccles
Waste
Nuclear fuel is both the densest form of energy in its virgin state and, once used, one of the mo... more Nuclear fuel is both the densest form of energy in its virgin state and, once used, one of the most hazardous materials known to humankind. Though commonly viewed as a waste—with over 300,000 tons stored worldwide and an additional 7–11,000 tons accumulating annually—spent nuclear fuel (SNF) represents a significant potential source of scarce, valuable strategic materials. Beyond the major (U and Pu) and minor (Np, Am, and Cm) actinides, which can be used to generate further energy, resources including the rare earth elements (Y, La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, and Tb), platinum group metals, (Ru, Rh, Pd, and Ag), noble gases (He, Kr, and Xe), and a range of isotopes useful for medical and energy generation purposes are also produced during fission. One reason for the accumulation of so much SNF is the low uptake of SNF recycle (or reprocessing), primarily due to the high capital and operational costs alongside concerns regarding proliferation and wastes generated. This study will h...
RSC Advances
Amorphous sodium titanates were synthesized using a mid-temperature sol–gel method for evaluation... more Amorphous sodium titanates were synthesized using a mid-temperature sol–gel method for evaluation as selective adsorbents of strontium in the presence of cesium or metal cations (Al3+, Mg2+, Ca2+, and Mn2+) from aqueous solution.
Encyclopedia of Separation Science, 2000
Progress in Ion Exchange, 1997
ABSTRACT The ion exchange industry which has developed significantly over the last five decades, ... more ABSTRACT The ion exchange industry which has developed significantly over the last five decades, is now a worldwide billion pound industry. The application of ion exchange materials varies from the treatment of liquid effluents to the purification of chiral molecules. This paper will address a specific area of application, namely environmental clean-up. As society becomes ever more increasingly aware of environmental issues, pressures on governments to legislate for more stringent environmental controls, will demand that industries employ cleaner technologies and, for the moment, end-of-pipe solutions. An abundance of EU environmental directives has been adopted by the UK and more will have to be adopted before the end of the millennium. Could this mean further growth for the ion exchange industry? This may not be so, because competing separation technologies are now finding favour. These technologies will be described with specific reference to the potential for industrial applications.
With a resurgence of the nuclear industry’s fortunes, waste management will be an even greater co... more With a resurgence of the nuclear industry’s fortunes, waste management will be an even greater consideration; reducing wastes, better segregation and treatment that lowers the impact on waste storage facilities and repositories, in particular geological repositories will help to under pin the sustainability of the industry. UCLan has previously published a new approach to spent fuel reprocessing,1 which is based on the sequential chromatographic separation of fission products and minor actinides from uranium and plutonium, dubbed Highly Active Waste Elimination (HAWE). This publication addresses the removal of one particular fission product, cesium, and its impact on waste management, in particular arising of high level waste (HLW), and the down-stream operations post the PUREX separation circuit. Although HAWE is still in the conceptual stage, it is perceived that it will have a significant impact on the separation circuit, storage of highly active liquid waste and would eventually...
Food and Bioproducts Processing, 1998
The nuclear industry generates large volumes of liquid wastes during decommissioning and decontam... more The nuclear industry generates large volumes of liquid wastes during decommissioning and decontamination activities which require extensive clean-up for recycle and/or disposal. The disposal of spent ion exchange materials used to clean these decontamination liquors is challenging and costly for the nuclear industry due to problematic end-of-life handling and low capacities of these materials for most radionuclides. Certain mixed-metal phosphates could be advantageous in this role due to their inherent vitrification properties and potentially high capacities for cationic and/or anionic radionuclides. Similar ammonium-based ion exchangers like the caesium-selective ammonium phosphomolybdate (AMP) are well known in the nuclear industry, but outside of this, such materials remain largely unexplored for this purpose. In this publication, we assess several metal ammonium phosphates (MAPs) and related compounds prepared using a continuous flow technique for their ability to act as ion exc...
Journal of Chemical Engineering & Process Technology, 2019
In a previous publication, the authors described a chromatographic process for the selective sepa... more In a previous publication, the authors described a chromatographic process for the selective separation of fission products and minor actinides from uranium and plutonium in nitric acid solution. This paper has evaluated commercially available ion exchange materials for capacity, rate of uptake and selectivity for some fission products (inactive) and cerium (iii) and (iv) as surrogate for Pu and U. The fission products studied where Cs, Sr and Zr as these for various reasons present major challenges for the existing PUREX process and waste management. The commercial resins evaluated were various sulfonic acid, chelate ion exchangers and an undisclosed inorganic material all supplied by Purolite Ltd.
Biochemical Society Transactions, 1998
Industrial Biochemistry and Biotechnology Group/Environmental Biotechnology U.K. Group (SCI) Join... more Industrial Biochemistry and Biotechnology Group/Environmental Biotechnology U.K. Group (SCI) Joint Colloquium Organized and Edited by D. Orwin (Faculty of Science & Technology, University of Luton) and Sponsored by Unilever Research. 666th Meeting, held at the University of Sheffield, 29-3 I July 1998. Metal contaminated soilis natural attenuation acceptable?
Journal of Nuclear Materials, 2016
of carbon-13 labelled carbonaceous deposits and their evaluation for potential use as surrogates ... more of carbon-13 labelled carbonaceous deposits and their evaluation for potential use as surrogates to better understand the behaviour of the carbon-14-containing deposit present in irradiated PGA graphite.
This paper explores the array of living microorganisms and dead cell systems which have been eval... more This paper explores the array of living microorganisms and dead cell systems which have been evaluated for waste management in the nuclear industry. The key mechanisms of metal removal for these processes will be indicated and the efficiency of each assessed. Metal mobilising microbial systems have used in the mining industry for about three decades. Bioleaching of metal ores containing uranium, copper, or gold is now a commercial, engineered process. This unique ability to convert sulphur to sulphuric acid is described. A key feature of the paper will be the comparison of biological processes with their chemical counter-parts for nuclear waste management, but importantly to highlight the additional benefits of bioremediation.
Solvent Extraction and Ion Exchange, 2000
ABSTRACT This article discusses the application of separation technologies, in particular solvent... more ABSTRACT This article discusses the application of separation technologies, in particular solvent extraction and ion exchange in the uranium nuclear fuel cycle. The history and decisions in selecting the technology are briefly discussed. The global trends in the energy sector are reviewed and the impact of other energy sources on the nuclear power industry both now and in the future is described. The effect of over capacity in uranium mining and milling, UOC refining and uranium enrichment on the development of new technology is a key feature of this article. Although over capacity is not the case with irradiated fuel reprocessing, other constraints limit the development of new technology and/or process improvements. The environmental considerations of all stages of the uranium nuclear fuel cycle will require better process technology and it is this key balance between the environmental and economic considerations that constitute a key component of this article. Some new solvent extraction processes that may offer a way forward to the segregation of actinides from highly active waste, integrated technologies and non aqueous systems are discussed.
Solvent Extraction and Ion Exchange, 1992
ABSTRACT
Separation Science and Technology, 1993
Abstract Several separative technologies for the removal of thorium isotopes from a waste nitric ... more Abstract Several separative technologies for the removal of thorium isotopes from a waste nitric acid raffinate have been evaluated. The implications of interfering ions and the efficiency of thorium recovery are described. A comparison of the various techniques studied is reported with particular reference to: i. Secondary waste. ii. Scale-up. iii. Overall best practical environmental option.
Journal of Molecular Structure, 2010
The ultrasonic radiation of a mixture of [Mn(CO)5Br], di-2-pyridyl ketone thiophene-2-carboxylic ... more The ultrasonic radiation of a mixture of [Mn(CO)5Br], di-2-pyridyl ketone thiophene-2-carboxylic acid hydrazone (dpktch) and diethyl ether in air gave fac-[Mn(CO)3(η2-N,N-dpktch)Br]. Under refluxing conditions [MnBr2(η3-N,N,O-dpktch)] and [Mn(η3-N,N,O-dpktch-H)2] were isolated from a mixture of Mn(CO)5Br, dpktch, and CH3CN. The infrared spectra of the isolated compounds divulge the facial coordination of the carbonyl (CO) groups in fac-[Mn(CO)3(η2-N,N-dpktch)Br], the absence of the carbonyl (CO) groups in [MnBr2(η3-N,N,O-dpktch)] and [Mn(η3-N,N,O-dpktch-H)2], and the coordination of dpktch/dpktch-H. The electronic absorption spectra of the isolated compounds show two intra-ligand charge transfer (ILCT) transitions that are sensitive to changes in their surroundings. The interconversion between fac-[Mn(CO)3(η2-N,N-dpktch)Br] and its conjugate base fac-[Mn(CO)3(η2-N,N-dpktch-H)Br] in protophilic solvents was demonstrated using stoichiometric amounts of an acid or a base. Acids or bases in concentrations as low as 1.00×10−6M can be detected and determined using protophilic solutions of fac-[Mn(CO)3(η2-N,N-dpktch)Br]. X-ray crystallographic analysis done on crystals of [MnBr2(η3-N,N,O-dpktch)] and [Mn(η3-N,N,O-dpktch-H)2] confirmed their identity and show tetragonal (square pyramidal) coordination about manganese in [MnBr2(η3-N,N,O-dpktch)] and octahedral coordination about manganese in [Mn(η3-N,N,O-dpktch-H)2]. The extended structures of [MnBr2(η3-N,N,O-dpktch)] and [Mn(η3-N,N,O-dpktch-H)2] revealed digitated units of [MnBr2(η3-N,N,O-dpktch)], and anti-parallel stacks of [Mn(η3-N,N,O-dpktch-H)2] locked via a network of hydrogen bonds. Analysis of solvent accessible areas in the solid state of [MnBr2(η3-N,N,O-dpktch)] and [Mn(η3-N,N,O-dpktch-H)2] show the unit cell of the former to be void free while the latter to contain several voids.
International Biodeterioration & Biodegradation, 1996
Waste
Nuclear fuel is both the densest form of energy in its virgin state and, once used, one of the mo... more Nuclear fuel is both the densest form of energy in its virgin state and, once used, one of the most hazardous materials known to humankind. Though commonly viewed as a waste—with over 300,000 tons stored worldwide and an additional 7–11,000 tons accumulating annually—spent nuclear fuel (SNF) represents a significant potential source of scarce, valuable strategic materials. Beyond the major (U and Pu) and minor (Np, Am, and Cm) actinides, which can be used to generate further energy, resources including the rare earth elements (Y, La, Ce, Pr, Nd, Pm, Sm, Eu, Gd, and Tb), platinum group metals, (Ru, Rh, Pd, and Ag), noble gases (He, Kr, and Xe), and a range of isotopes useful for medical and energy generation purposes are also produced during fission. One reason for the accumulation of so much SNF is the low uptake of SNF recycle (or reprocessing), primarily due to the high capital and operational costs alongside concerns regarding proliferation and wastes generated. This study will h...
RSC Advances
Amorphous sodium titanates were synthesized using a mid-temperature sol–gel method for evaluation... more Amorphous sodium titanates were synthesized using a mid-temperature sol–gel method for evaluation as selective adsorbents of strontium in the presence of cesium or metal cations (Al3+, Mg2+, Ca2+, and Mn2+) from aqueous solution.
Encyclopedia of Separation Science, 2000
Progress in Ion Exchange, 1997
ABSTRACT The ion exchange industry which has developed significantly over the last five decades, ... more ABSTRACT The ion exchange industry which has developed significantly over the last five decades, is now a worldwide billion pound industry. The application of ion exchange materials varies from the treatment of liquid effluents to the purification of chiral molecules. This paper will address a specific area of application, namely environmental clean-up. As society becomes ever more increasingly aware of environmental issues, pressures on governments to legislate for more stringent environmental controls, will demand that industries employ cleaner technologies and, for the moment, end-of-pipe solutions. An abundance of EU environmental directives has been adopted by the UK and more will have to be adopted before the end of the millennium. Could this mean further growth for the ion exchange industry? This may not be so, because competing separation technologies are now finding favour. These technologies will be described with specific reference to the potential for industrial applications.
With a resurgence of the nuclear industry’s fortunes, waste management will be an even greater co... more With a resurgence of the nuclear industry’s fortunes, waste management will be an even greater consideration; reducing wastes, better segregation and treatment that lowers the impact on waste storage facilities and repositories, in particular geological repositories will help to under pin the sustainability of the industry. UCLan has previously published a new approach to spent fuel reprocessing,1 which is based on the sequential chromatographic separation of fission products and minor actinides from uranium and plutonium, dubbed Highly Active Waste Elimination (HAWE). This publication addresses the removal of one particular fission product, cesium, and its impact on waste management, in particular arising of high level waste (HLW), and the down-stream operations post the PUREX separation circuit. Although HAWE is still in the conceptual stage, it is perceived that it will have a significant impact on the separation circuit, storage of highly active liquid waste and would eventually...
Food and Bioproducts Processing, 1998
The nuclear industry generates large volumes of liquid wastes during decommissioning and decontam... more The nuclear industry generates large volumes of liquid wastes during decommissioning and decontamination activities which require extensive clean-up for recycle and/or disposal. The disposal of spent ion exchange materials used to clean these decontamination liquors is challenging and costly for the nuclear industry due to problematic end-of-life handling and low capacities of these materials for most radionuclides. Certain mixed-metal phosphates could be advantageous in this role due to their inherent vitrification properties and potentially high capacities for cationic and/or anionic radionuclides. Similar ammonium-based ion exchangers like the caesium-selective ammonium phosphomolybdate (AMP) are well known in the nuclear industry, but outside of this, such materials remain largely unexplored for this purpose. In this publication, we assess several metal ammonium phosphates (MAPs) and related compounds prepared using a continuous flow technique for their ability to act as ion exc...
Journal of Chemical Engineering & Process Technology, 2019
In a previous publication, the authors described a chromatographic process for the selective sepa... more In a previous publication, the authors described a chromatographic process for the selective separation of fission products and minor actinides from uranium and plutonium in nitric acid solution. This paper has evaluated commercially available ion exchange materials for capacity, rate of uptake and selectivity for some fission products (inactive) and cerium (iii) and (iv) as surrogate for Pu and U. The fission products studied where Cs, Sr and Zr as these for various reasons present major challenges for the existing PUREX process and waste management. The commercial resins evaluated were various sulfonic acid, chelate ion exchangers and an undisclosed inorganic material all supplied by Purolite Ltd.
Biochemical Society Transactions, 1998
Industrial Biochemistry and Biotechnology Group/Environmental Biotechnology U.K. Group (SCI) Join... more Industrial Biochemistry and Biotechnology Group/Environmental Biotechnology U.K. Group (SCI) Joint Colloquium Organized and Edited by D. Orwin (Faculty of Science & Technology, University of Luton) and Sponsored by Unilever Research. 666th Meeting, held at the University of Sheffield, 29-3 I July 1998. Metal contaminated soilis natural attenuation acceptable?
Journal of Nuclear Materials, 2016
of carbon-13 labelled carbonaceous deposits and their evaluation for potential use as surrogates ... more of carbon-13 labelled carbonaceous deposits and their evaluation for potential use as surrogates to better understand the behaviour of the carbon-14-containing deposit present in irradiated PGA graphite.
This paper explores the array of living microorganisms and dead cell systems which have been eval... more This paper explores the array of living microorganisms and dead cell systems which have been evaluated for waste management in the nuclear industry. The key mechanisms of metal removal for these processes will be indicated and the efficiency of each assessed. Metal mobilising microbial systems have used in the mining industry for about three decades. Bioleaching of metal ores containing uranium, copper, or gold is now a commercial, engineered process. This unique ability to convert sulphur to sulphuric acid is described. A key feature of the paper will be the comparison of biological processes with their chemical counter-parts for nuclear waste management, but importantly to highlight the additional benefits of bioremediation.
Solvent Extraction and Ion Exchange, 2000
ABSTRACT This article discusses the application of separation technologies, in particular solvent... more ABSTRACT This article discusses the application of separation technologies, in particular solvent extraction and ion exchange in the uranium nuclear fuel cycle. The history and decisions in selecting the technology are briefly discussed. The global trends in the energy sector are reviewed and the impact of other energy sources on the nuclear power industry both now and in the future is described. The effect of over capacity in uranium mining and milling, UOC refining and uranium enrichment on the development of new technology is a key feature of this article. Although over capacity is not the case with irradiated fuel reprocessing, other constraints limit the development of new technology and/or process improvements. The environmental considerations of all stages of the uranium nuclear fuel cycle will require better process technology and it is this key balance between the environmental and economic considerations that constitute a key component of this article. Some new solvent extraction processes that may offer a way forward to the segregation of actinides from highly active waste, integrated technologies and non aqueous systems are discussed.
Solvent Extraction and Ion Exchange, 1992
ABSTRACT
Separation Science and Technology, 1993
Abstract Several separative technologies for the removal of thorium isotopes from a waste nitric ... more Abstract Several separative technologies for the removal of thorium isotopes from a waste nitric acid raffinate have been evaluated. The implications of interfering ions and the efficiency of thorium recovery are described. A comparison of the various techniques studied is reported with particular reference to: i. Secondary waste. ii. Scale-up. iii. Overall best practical environmental option.
Journal of Molecular Structure, 2010
The ultrasonic radiation of a mixture of [Mn(CO)5Br], di-2-pyridyl ketone thiophene-2-carboxylic ... more The ultrasonic radiation of a mixture of [Mn(CO)5Br], di-2-pyridyl ketone thiophene-2-carboxylic acid hydrazone (dpktch) and diethyl ether in air gave fac-[Mn(CO)3(η2-N,N-dpktch)Br]. Under refluxing conditions [MnBr2(η3-N,N,O-dpktch)] and [Mn(η3-N,N,O-dpktch-H)2] were isolated from a mixture of Mn(CO)5Br, dpktch, and CH3CN. The infrared spectra of the isolated compounds divulge the facial coordination of the carbonyl (CO) groups in fac-[Mn(CO)3(η2-N,N-dpktch)Br], the absence of the carbonyl (CO) groups in [MnBr2(η3-N,N,O-dpktch)] and [Mn(η3-N,N,O-dpktch-H)2], and the coordination of dpktch/dpktch-H. The electronic absorption spectra of the isolated compounds show two intra-ligand charge transfer (ILCT) transitions that are sensitive to changes in their surroundings. The interconversion between fac-[Mn(CO)3(η2-N,N-dpktch)Br] and its conjugate base fac-[Mn(CO)3(η2-N,N-dpktch-H)Br] in protophilic solvents was demonstrated using stoichiometric amounts of an acid or a base. Acids or bases in concentrations as low as 1.00×10−6M can be detected and determined using protophilic solutions of fac-[Mn(CO)3(η2-N,N-dpktch)Br]. X-ray crystallographic analysis done on crystals of [MnBr2(η3-N,N,O-dpktch)] and [Mn(η3-N,N,O-dpktch-H)2] confirmed their identity and show tetragonal (square pyramidal) coordination about manganese in [MnBr2(η3-N,N,O-dpktch)] and octahedral coordination about manganese in [Mn(η3-N,N,O-dpktch-H)2]. The extended structures of [MnBr2(η3-N,N,O-dpktch)] and [Mn(η3-N,N,O-dpktch-H)2] revealed digitated units of [MnBr2(η3-N,N,O-dpktch)], and anti-parallel stacks of [Mn(η3-N,N,O-dpktch-H)2] locked via a network of hydrogen bonds. Analysis of solvent accessible areas in the solid state of [MnBr2(η3-N,N,O-dpktch)] and [Mn(η3-N,N,O-dpktch-H)2] show the unit cell of the former to be void free while the latter to contain several voids.
International Biodeterioration & Biodegradation, 1996