Aqueous amine scrubbing was originally developed for natural gas treatment and is currently considered to be the current best available technology for post-combustion capture (PCC) of CO2 from both pulverised fuel (PF) and natural gas combined cycle (NGCC) power plants. A major issue is the severe thermo-oxidative degradation of alkanomaine solvents that occurs in PCC compared to natural gas processing, with the problem being compounded by the presence of acid gases that lead to the formation of heat stable salts (HSS). The accumulation of degradation products is known to reduce CO2 capture efficiency and cause excessive foaming and fouling and unacceptably high corrosion rates. Current measures to compensate for degradation involves purging spent solvent solution for reclaimation, makeup with fresh amine and the addition of anti-foam and oxidation/corrosion inhibitors. Reclaimer technologies based on distillation, ion-exchange and elecrodialysis have been developed to deal primarily with HSS where distillation has the advantage of removing both the HSS and their anions (i.e. formate and acetate). However, these technologies do not deal with the majority of the other degradation products, particularly those arising from thermal and oxidative degradation. Further, it has generally recognised that MEA forms high boiling polymeric material where N-(2-hydroxyethyl)-ethylenediamine (HEEDA), in particular, may continue to degrade in the presence of CO2 to form longer substituted ethlyenediamines. This proposal has been prompted by our extremely promising preliminary results that the thermal and oxidative degradation of an amine polymer (polyethyleneimine) can largely be reversed using both hydrogenation and hydrothermal (hydrous) treatments. We used non-catalytic hydropyrolysis and hydrous pyrolysis treatments at temperatures below 250oC which were clearly effective in reducing oxygen functionalities without causing any degradation of the polymer chain. The challenge is to partially reduce degraded amines to hydroxyamines and also, for polymeric forms, to induce some hydrogenolysis to reduce chain lengths. Hydrous pyrolysis has the potential advantage of not directly requiring hydrogen with water being the hydrogen source. Judicious choice of catalysts provides selectivity for hydrogenation and hydrogenolysis and research on amine degradation in natural gas sweetening has shown degradation products, such as N,N-bis(2-hydroxy-ethyl)piperazine and N,N,N-tris(2-hydroxyethyl)ethylenediamine, can be converted back to hydroxyamines by a hydrotreating reactions . •Directly targeting a high research priority identified by the RAPID Handbook, the proposed research aims to investigate novel reductive approaches for rejuvenating spent amine solutions from PCC plants, namely selective catalytic hydrotreatments at modest temperatures and H2 pressures and hydrous pyrolysis (hydrothermal conversion). The specific objectives are: 1.To apply the hydrogenation/ hydropyrolysis and hydrothermal treatments to individual compounds, including 1-(2-hydroxyethyl)-2-imidazolidone (HEIA), HEEDA, .N-(2-hydroxyethyl)acetamide and N-methylformamide 2.Based on the model compound results, to conduct experiments on actual fractions from degraded amine solvents, notably the residues from distillation containing HSS and the compounds targeted above; and 3.To use the results to define the overall benefits hydrogenation, hydropyrolysis and hydrothermal treatments in solvent rejuvenation and a basis for planning the subsequent research needed to take forward these new treatments, in terms of identifying how these treatments can best be conducted continuously. Grant number: UKCCSRC-C2-189.
This poster on the UKCCSRC (UK Carbon Capture and Storage Research Centre) Call 1 project, Multi-Phase Flow Modelling for Hazardous Assessment, was presented at the Cambridge Biannual, 02.04.14. Grant number: UKCCSRC-C1-07.
This poster on the UKCCSRC Call 2 project Flexible CCS operations combined with online solvent monitoring: A pilot-scale study was presented at the CSLF Call project poster reception, London, 27.06.16. Grant number: UKCCSRC-C2-214. This project focuses on enhancing the flexibility of amine based post-combustion capture systems 1. To evaluate the flexible operation capabilities of current post-combustion CCS plant designs via dynamic scenario testing at pilot scale. 2. To identify hardware bottlenecks to dynamic operation and suggest improvements. 3. To develop new instrumentation, operating strategies and control systems which will enhance operational flexibility. 4. To obtain real plant data to complement dynamic modelling efforts.
This poster on the UKCCSRC Call 2 project, Process-performance indexed design of task-specific ionic liquids for post-combustion CO2 capture, was presented at the Cardiff Biannual, 10.09.14. Grant number: UKCCSRC-C2-199.
UKCCSRC Call 2 Project C2-199. Datasheet providing detailed stream information pertaining to an Ionic Liquids (IL)-based CCS process. This data arises from a process model developed at Imperial College London.
This is a blog (Update, 20.01.15) on the UKCCSRC Call 2 project, Quantifying Residual and Dissolution Trapping in the CO2CRC Otway Injection Site. Grant number: UKCCSRC-C2-204.
This is the dataset to accompany the International Journal of Greenhouse Gas Control manuscript entitled: Using oxygen isotopes to quantitatively assess residual CO2 saturation during the CO2CRC Otway Stage 2B Extension residual saturation test by Serno et al., published in 2016 http://dx.doi.org/10.1016/j.ijggc.2016.06.019. The data was collected at the CO2CRC Otway test site in December 2014, processed in Edinburgh and is now presented as an excel file.
This presentation on the UKCCSRC Call 2 project Performance of Flow Meters with Dense Phase CO2 and CCS Recovery Streams was presented at the UKCCSRC Edinburgh Biannual Meeting, 15.09.2016. Grant number: UKCCSRC-C2-201.
This dataset comprises a series of six .xls workbooks which contain the data auxiliary material for the manuscript "Metrology and Traceability of U-Pb Isotope Dilution Geochronology (EARTHTIME Tracer Calibration Part I)" by Daniel Condon, Blair Schoene, Noah McLean, Samuel Bowring and Randall Parrish, submitted to Geochimica et Cosmochimica Acta (June 2014). These data comprise the input measurement data for the EARTHTIME U-Pb Tracer Calibration experiment, the results of which are documented in the manuscript mentioned above. This data set contains isotope ratio data for the manuscript listed above. ts01.xls Amelin and Davis (2006) Pb reference material isotope ratio data ts02.xls CRM 115 U isotope ratio data ts03.xls Gravimetric-Tracer mixture isotope ratio data ts04.xls GDMS elemental concentration data ts05.xls Tracer-blank Pb isotope ratio data ts06.xls U critical mixture isotope ratio data. Link to Published Paper - Metrology and Traceability of U-Pb Isotope Dilution Geochronology (EARTHTIME Tracer Calibration Part I) http://dx.doi.org/10.1016/j.gca.2015.05.026
The world's population is predicted to grow from the current 7 billions to a plateau of approximately 9.2 billions to be reached within the next 60 years, representing roughly a 30 % increase in a not so distant future. The need for more energy efficient methods of producing synthetic fertilisers to meet the resulting increases in food demand and in crude (and bio) oils refining operations -on crudes of ever poorer quality- motivates the scientific community to reconsider the limitations of the mature technologies of synthetic fertilisers production and hydro-refining processes (HDS, HDN, HDM, HDO, hydrocracking) which both rely on the supply of hydrogen. Synthetic fertilisers necessitate hydrogen and nitrogen as feedstocks to make ammonia, which represents the building block for other fertilisers such as urea or ammonium nitrate. The current cheapest and most common means of producing hydrogen is natural gas steam reforming. With an abundance of natural gas reserves becoming exploitable worldwide in recent years via the hydraulic fracturing of shale gas, and given the ever more severe regulations on atmospheric pollution caused by flaring of associated gas from refineries and oil extraction operations, the production of hydrogen is very likely to remain dominated in the years to come by the process of steam reforming using natural gas as its feedstock (aka 'steam methane reforming' or 'SMR'). Conventional SMR technology usually features many unit operations (desulphurisation, pre-reforming, primary reforming, furnace, high and low temperature water gas shift (HT-WGS, LT-WGS), and final separation, with as many heat integration steps in between the units in order to reach an energy efficiency of roughly 80%. This efficiency is only attainable thanks to economies of scale, and SMR plants are consequently enormous. To avoid storage and transport costs of H2, the ammonia/ammonium nitrate/urea plants, or refinery operations are usually conducted near the site of SMR, therefore the production of the final products of fertilisers or clean fuels is very centralised, and thus vulnerable, as well as incurring large distribution costs. With sources of natural gas becoming more remote, widely distributed, shorter lived and quickly relocated, the process of converting natural gas to the final products fertiliser/clean fuel should become more mobile, down-scaleable, as fracking gas wells see their production decay with time and move to different sites. This proposal seeks to reduce significantly the energy and materials demand for the conversion of natural gas feedstocks into ready separated streams of the H2, N2 and CO2 products of steam reforming (the building blocks of urea production) by coupling the in-situ high temperature CO2 capture during the reforming reactions on a solid sorbent (a process called 'sorption enhancement') with the process of chemical looping steam reforming. A process is proposed with only two reactors, a reformer and a pressure/temperature swing separator, appropriate for the new, mobile, small scale industrial utilisation of natural gas, through realising the multiple synergies that are unique to the coupled process, and through the avoidance of expensive materials and awkward reformer geometries. Grant number: UKCCSRC-C2-181.