A high performance oxygen storage material for chemical looping processes with CO2 capture

Chemical looping combustion (CLC) is a novel combustion technology that involves cyclic reduction and oxidation of oxygen storage materials to provide oxygen for the combustion of fuels to CO2 and H2O, whilst giving a pure stream of CO2 suitable for sequestration or utilisation. Here, we report a method for preparing of oxygen storage materials from layered double hydroxides (LDHs) precursors and demonstrate their applications in the CLC process. The LDHs precursor enables homogeneous mixing of elements at the molecular level, giving a high degree of dispersion and high-loading of active metal oxide in the support after calcination. Using a Cu-Al LDH precursor as a prototype, we demonstrate that rational design of oxygen storage materials by material chemistry significantly improved the reactivity and stability in the high temperature redox cycles. We discovered that the presence of sodium-containing species were effective in inhibiting the formation of copper aluminates (CuAl2O4 or CuAlO 2) and stabilising the copper phase in an amorphous support over multiple redox cycles. A representative nanostructured Cu-based oxygen storage material derived from the LDH precursor showed stable gaseous O2 release capacity (∼5 wt%), stable oxygen storage capacity (∼12 wt%), and stable reaction rates during reversible phase changes between CuO-Cu 2O-Cu at high temperatures (800-1000 °C). We anticipate that the strategy can be extended to manufacture a variety of metal oxide composites for applications in novel high temperature looping cycles for clean energy production and CO2 capture. © The Royal Society of Chemistry 2013.

Palm frond biochar production and characterisation

Palm oil has been the world's main source of oil and fats since 2004, producing over 45 million tonnes in 2009. Malaysia alone has over 4·5 million hectares planted with oil palm and, based on common practice, ~300 palm fronds are pruned per hectare per year. This agricultural waste is currently either being used as roughage feed or, more frequently, being left between rows of palm trees to prevent soil erosion, or for nutrient recycling purposes. This paper proposes an alternative use for palm frond as a source of biochar. A traditional method commonly use by gardeners in Malaysia to improve soil fertility was used to produce the biochar. A shallow earth pit was dug in the ground for the carbonisation process. The process is described and the impact of carbonisation on the earth wall is analysed and presented. The process was later re-assessed by using TGA-FTIR. Most of the hemicelluloses had fully disintegrated, but the depolymerisation of the cellulose was still incomplete at the carbonisation temperature. Most of the lignin aromatic structure was still present in the biochar. The carbonisation process was repeated in the laboratory and biochar was characterised by using BET, SEM and FTIR. An adsorption isotherm study was conducted and the experimental data were fitted to the Langmuir model. The model predicted Pb2+ adsorption rates of 83·3 mg/g, Cu2+ 41·4 mg/g, Ni2+ 13·0 mg/g and Zn2+ 19·7 mg/g. Copyright © The Royal Society of Edinburgh 2012.

Simultaneous reduction of particulate matter and NOx emissions using 4-way catalyzed filtration systems

The next generation of diesel emission control devices includes 4-way catalyzed filtration systems (4WCFS) consisting of both NOx and diesel particulate matter (DPM) control. A methodology was developed to simultaneously evaluate the NOx and DPM control performance of miniature 4WCFS made from acicular mullite, an advanced ceramic material (ACM), that were challenged with diesel exhaust. The impact of catalyst loading and substrate porosity on catalytic performance of the NOx trap was evaluated. Simultaneously with NOx measurements, the real-time solid particle filtration performance of catalyst-coated standard and high porosity filters was determined for steady-state and regenerative conditions. The use of high porosity ACM 4-way catalyzed filtration systems reduced NOx by 99% and solid and total particulate matter by 95% when averaged over 10 regeneration cycles. A "regeneration cycle" refers to an oxidizing ("lean") exhaust condition followed by a reducing ("rich") exhaust condition resulting in NOx storage and NOx reduction (i.e., trap "regeneration"), respectively. Standard porosity ACM 4-way catalyzed filtration systems reduced NOx by 60-75% and exhibited 99.9% filtration efficiency. The rich/lean cycling used to regenerate the filter had almost no impact on solid particle filtration efficiency but impacted NOx control. Cycling resulted in the formation of very low concentrations of semivolatile nucleation mode particles for some 4WCFS formulations. Overall, 4WCFS show promise for significantly reducing diesel emissions into the atmosphere in a single control device. © 2013 American Chemical Society.

Comparisons of operating envelopes for contaminated soil stabilised/solidified with different cementitious binders

This work initiated the development of operating envelopes for stabilised/solidified contaminated soils. The operating envelopes define the range of operating variables for acceptable performance of the treated soils. The study employed a soil spiked with 3,000 mg/kg each of Cd, Cu, Pb, Ni and Zn, and 10,000 mg/kg of diesel. The binders used for treatment involved Portland cement (CEMI), pulverised fuel ash (PFA), ground granulated blast furnace slag (GGBS) and hydrated lime (hlime). The specific binder formulations were CEMI, CEMI/PFA = 1:4, CEMI/GGBS = 1:9 and hlime/GGBS = 1:4. The water contents employed ranged from 13 % to 21 % (dry weight), while binder dosages ranged from 5 % to 20 % (w/w). We monitored the stabilised/solidified soils for up to 84 days using different performance tests. The tests include unconfined compressive strength (UCS), hydraulic conductivity, acid neutralisation capacity (ANC) and pH-dependent leachability of contaminants. The water content range resulted in adequate workability of the mixes but had no significant effect on leachability of contaminants. We produced design charts, representing operating envelopes, from the results generated. The charts establish relationships between water content, binder dosage and UCS; and binder dosage, leachant pH and leachability of contaminants. The work also highlights the strengths and weaknesses of the different binder formulations. © 2013 Springer-Verlag Berlin Heidelberg.

Sustainability: A new imperative in contaminated land remediation

Land is not only a critical component of the earth's life support system, but also a precious resource and an important factor of production in economic systems. However, historical industrial operations have resulted in large areas of contaminated land that are only slowly being remediated. In recent years, sustainability has drawn increasing attention in the environmental remediation field. In Europe, there has been a movement towards sustainable land management; and in the US, there is an urge for green remediation. Based on a questionnaire survey and a review of existing theories and empirical evidence, this paper suggests the expanding emphasis on sustainable remediation is driven by three general factors: (1) increased recognition of secondary environmental impacts (e.g., life-cycle greenhouse gas emissions, air pollution, energy consumption, and waste production) from remediation operations, (2) stakeholders' demand for economically sustainable brownfield remediation and "green" practices, and (3) institutional pressures (e.g., social norm and public policy) that promote sustainable practices (e.g., renewable energy, green building, and waste recycling). This paper further argues that the rise of the "sustainable remediation" concept represents a critical intervention point from where the remediation field will be reshaped and new norms and standards will be established for practitioners to follow in future years. This paper presents a holistic view of sustainability considerations in remediation, and an integrated framework for sustainability assessment and decision making. The paper concludes that "sustainability" is becoming a new imperative in the environmental remediation field, with important implications for regulators, liability owners, consultants, contractors, and technology vendors. © 2014 Elsevier Ltd.