School of Chemical Engineering

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The department has a strong research team that is focused on solving problems and providing answers for industry and the wider community. Our work is principally in the areas of:

Biotechnology, food and wine
Energy and the environment
Particle technology, especially particle/fluid interactions
Process control and simulation
Advanced laser diagnostics

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School of Chemical Engineering
Ingkarni Wardli Building
THE UNIVERSITY OF ADELAIDE
SA 5005
AUSTRALIA
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Telephone: +61 8 8313 5446
Facsimile: +61 8 8313 4373

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Now showing 1 - 20 of 3178

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0D (MoS₂)/2D (g-C₃N₄) heterojunctions in Z-scheme for enhancedphotocatalytic and electrochemical hydrogen evolution
(Elsevier, 2018) Liu, Y.; Zhang, H.; Ke, J.; Zhang, J.; Tian, W.; Xu, X.; Duan, X.; Sun, H.; O Tade, M.; Wang, S.
MoS2 quantum dots (MSQDs) with high and stable dispersion in water were prepared via a facile one-pot hydrothermal process. The MSQDs were then applied to decorate graphitic carbon nitride (g-C3N4, CN) nanosheets to obtain modified g-C3N4 photocatalysts (MSQD-CN). Compared to pristine g-C3N4, the hybrid photocatalysts showed a slight red shift and stronger light absorption with remarkably improved photocatalytic activity in water splitting to generate hydrogen. The hydrogen-evolution rate over 0.2 wt% MSQD-CN increased by 1.3 and 8.1 times as high as that of 0.2 wt% Pt-CN and g-C3N4, respectively. With deposition of 2 wt% Pt as a cocatalyst, 5 wt% MSQD-CN exhibited the highest photocatalytic efficiency with an average hydrogen evolution reaction (HER) rate of 577 μmol h−1 g−1. Photoluminescence spectra (PL) and photoelectrochemical measurements inferred that MSQDs introduction drastically promoted the electron transfer for more efficient separation of charge carriers, which could lower HER overpotential barriers and enhance the electrical conductivity. In addition, the well-matched band potentials of the MSQD-CN hybrid with an intimate contact interface of p-n heterojunction also inhibited the recombination of photo-generated carriers, leading to enhanced photocatalytic HER performance. A direct Z-scheme charge transfer mechanism of the MSQD-CN hybrid was proposed to further elaborate the synergistic effect between MSQDs, Pt and g-C3N4. This work underlines the importance of heterojunction interface and presents a feasible protocol for rational construction of g-C3N4 based photocatalysts for various photocatalytic applications.
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0D/2D heterojunctions of Vanadate quantum dots/graphitic carbon nitride nanosheets for enhanced visible-light-driven photocatalysis
(Wiley, 2017) Ye, M.; Zhao, Z.; Hu, Z.; Liu, L.; Ji, H.; Shen, Z.; Ma, T.
0D/2D heterojunctions, especially quantum dots (QDs)/nanosheets (NSs) have attracted significant attention for use of photoexcited electrons/holes due to their high charge mobility. Herein, unprecedent heterojunctions of vanadate (AgVO₃ , BiVO₄ , InVO₄ and CuV₂ O₆ ) QDs/graphitic carbon nitride (g-C₃ N₄ ) NSs exhibiting multiple unique advances beyond traditional 0D/2D composites have been developed. The photoactive contribution, up-conversion absorption, and nitrogen coordinating sites of g-C₃ N₄ NSs, highly dispersed vanadate nanocrystals, as well as the strong coupling and band alignment between them lead to superior visible-light-driven photoelectrochemical (PEC) and photocatalytic performance, competing with the best reported photocatalysts. This work is expected to provide a new concept to construct multifunctional 0D/2D nanocomposites for a large variety of opto-electronic applications, not limited in photocatalysis.
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(0D/3D) MoS₂ on porous graphene as catalysts for enhanced electrochemical hydrogen evolution
(Elsevier, 2017) Liu, Y.; Zhu, Y.; Fan, X.; Wang, S.; Li, Y.; Zhang, F.; Zhang, G.; Peng, W.
A new composite material consisting of 0D MoS2 nanodots and 3D MoS2 nano-flowers grown on porous reduced graphene oxide (P-rGO) was synthesized via a two-step process. The P-rGO with a surface area of 759 m² g⁻¹ was obtained by CO2 activation of reduced graphene oxide (rGO) at 800 °C. MoS2 was then grown on the P-rGO under hydrothermal conditions. Compared to the nonactivated rGO, P-rGO has functional pores for deposition of MoS2 nanodots and less charge transfer resistance, which can provide more active sites for hydrogen generation, thus leading to the improved activity of (0D/3D) MoS2/P-rGO in hydrogen evolution reaction (HER). The overpotential of (0D/3D) MoS2/P-rGO was only ∼150 mV vs. RHE, and the corresponding Tafel slope was ∼56 mV Dec⁻¹, which is comparable to most of the present MoS2/Graphene HER catalysts. The (0D/3D) MoS2/P-rGO exhibits as an efficient noble metal free HER catalyst, and has great potential for the electrochemical hydrogen production.
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~1760 Ma magnetite-bearing protoliths in the Olympic Dam deposit, South Australia: implications for ore genesis and regional metallogeny
(Elsevier, 2020) Courtney-Davies, L.; Ciobanu, C.L.; Verdugo Ihl, M.R.; Cook, N.J.; Ehrig, K.J.; Wade, B.P.; Zhu, Z.Y.; Kamenetsky, V.S.
Spatial associations between banded iron formation and iron-oxide Cu-Au (IOCG) style mineralization are well documented in the Gawler Craton (South Australia), but the possible genetic relationships between these two distinct types of mineralization are hitherto unclear. A texturally conspicuous generation of coarse-grained silician magnetite, intergrown with carbonates and quartz, is observed in drillholes intersecting the ‘outer shell’ of the Olympic Dam IOCG-type deposit. This magnetite is characterised by high U-content (~50 ppm), siliceous chemistry, and unusual zonal textures with respect to Si-Fe-nanoprecipitates. Direct dating of this magnetite by laser ablation inductively coupled plasma mass spectrometry yields reproducible 207Pb/206Pb dates (1761 ± 16 Ma) that are significantly older than the granite hosting the deposit (1593 Ma), or the mineralized breccias constituting the Cu-U-Au-Ag resource (~1592–1589 Ma). The older, Fe-rich crustal material can be correlated with the ~1.76–1.74 Ga (meta)sedimentary Wallaroo Group, host to Fe-rich horizons across the Gawler Craton, including locations ~15 km NW of Olympic Dam. A generation of granitic rocks, which intruded bedrock at ~1.75 Ga are present ~30 km NE of Olympic Dam, and likely exsolved hydrothermal fluids that enriched pre-existing magnetite-bearing protoliths in both U and REE. Such material was physically, and likely chemically, incorporated into the ‘outer shell’ at Olympic Dam some ~150 Ma later, during granite uplift along faults. The coincidence between Fe-rich horizons/BIF and ~1750 Ma granitoids may have provided IOCG systems with an additional source of both Fe and U that predates the ~1.59 Ga craton-scale metallogenic event. The uranium concentrations in some South Australian IOCG systems represent major global anomalies in the element. A combination of the fortuitous geological circumstances outlined here, may help explain the highly anomalous accumulation of uranium found at Olympic Dam.
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1D sub-nanotubes with anatase/bronze TiO₂ nanocrystal wall for high-rate and long-life sodium-ion batteries
(Wiley Online Library, 2018) Chen, B.; Meng, Y.; Xie, F.; He, F.; He, C.; Davey, K.; Zhao, N.; Qiao, S.Z.
The development of 1D nanostructures with enhanced material properties has been an attractive endeavor for applications in energy and environmental fields, but it remains a major research challenge. Herein, this work demonstrates a simple, gel-derived method to synthesize uniform 1D elongated sub-nanotubes with an anatase/bronze TiO2 nanocrystal wall (TiO2 SNTs). The transformation mechanism of TiO2 SNTs is studied by various ex situ characterization techniques. The resulting 1D nanostructures exhibit, synchronously, a high aspect ratio, open tubular interior, and anatase/bronze nanocrystal TiO2 wall. This results in excellent properties of electron/ion transport and reaction kinetics. Consequently, as an anode material for sodium-ion batteries (SIBs), the TiO2 SNTs display an ultrastable long-life cycling stability with a capacity of 107 mAh g-1 at 16 C after 4000 cycles and a high-rate capacity of 94 mAh g-1 at 32 C. This a high-rate and long-life performance is superior to any report on pure TiO2 for SIBs. This work provides new fundamental information for the design and fabrication of inorganic structures for energy and environmental applications.
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1T′-ReS₂ confined in 2D-honeycombed carbon nanosheets as new anode materials for high-performance sodium-ion batteries
(Wiley, 2019) Chen, B.; Li, H.; Liu, H.; Wang, X.; Xie, F.; Deng, Y.; Hu, W.; Davey, K.; Zhao, N.; Qiao, S.Z.
eS₂ (rhenium disulfide) is a new transition‐metal dichalcogenide that exhibits 1T′ phase and extremely weak interlayer van der Waals interactions. This makes it promising as an anode material for sodium‐ion batteries. However, achieving both a high‐rate capability and a long‐life has remained a major research challenge. Here, a new composite is reported, in which both are realized for the first time. 1T′‐ReS₂ is confined through strong interfacial interaction in a 2D‐honeycombed carbon nanosheets that comprise an rGO inter‐layer and a N‐doped carbon coating‐layer (rGO@ReS2@N‐C). The strong interfacial interaction between carbon and ReS2 increases overall conductivity and decreases Na+ diffusion resistance, whilst the intended 2D‐honeycombed carbon protective layer maintains structural morphology and electrochemical activity during long‐term cycling. These findings are confirmed by advanced characterization techniques, electrochemical measurement, and density functional theory calculation. The new rGO@ReS2@N‐C exhibits the greatest rate performance reported so far for ReS₂ of 231 mAh g−1 at 10 A g−1. Significantly, this is together with ultra‐stable long‐term cycling of 192 mAh g−1 at 2 A g−1 after 4000 cycles.
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2- and 3-Stage temperature ramping for the direct synthesis of adipic acid in micro-flow packed-bed reactors
(Elsevier, 2015) Shang, M.; Noël, T.; Wang, Q.; Su, Y.; Miyabayashi, K.; Hessel, V.; Hasebe, S.
The synthesis of adipic acid from cyclohexene and hydrogen peroxide was investigated in micro-flowpacked-bed reactors. The isolated yield of adipic acid increases with increasing residence time inmicro-flow packed-bed reactors. The addition of phosphoric acid cannot effectively improve the isolatedyield of adipic acid though it is generally known to reduce the decomposition of H2O2. Then, differenttemperatures were tested along the reactor length, since the adipic acid synthesis is known to consistof 6 elementary reactions with different temperature needs. For experiments with 2-stage temperatureramping, 70°C and 100°C, respectively, are the optimal temperatures for the first stage and second stagereactor, which lead to 63% isolated yield of adipic acid. Furthermore, 3-stage temperature rampingimproves the yield of adipic acid to 66%. Multi-injection of hydrogen peroxide at different stages doesnot lead to a further increase in adipic acid yield. Although high temperatures are used in this transfor-mation, the in-line recording of temperature profiles along the flow axis shows that safe operation for thisexothermic reaction can be realized in the micro-flow packed-bed reactors. Notably, the space–timeyields in micro-flow packed-bed reactors are more than one order of magnitude higher than thoseobtained in batch reactors.
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2013 Danckwerts special issue on molecular modelling in chemical engineering
(Elsevier, 2015) Biggs, M.; Theodorou, D.
Abstract not available
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2020 roadmap on carbon materials for energy storage and conversion
(Wiley, 2020) Wu, M.; Liao, J.; Yu, L.; Lv, R.; Li, P.; Sun, W.; Tan, R.; Duan, X.; Zhang, L.; Li, F.; Kim, J.; Shin, K.H.; Seok Park, H.; Zhang, W.; Guo, Z.; Wang, H.; Tang, Y.; Gorgolis, G.; Galiotis, C.; Ma, J.
Carbon is a simple, stable and popular element with many allotropes. The carbon family members include carbon dots, carbon nanotubes, carbon fibers, graphene, graphite, graphdiyne and hard carbon, etc. They can be divided into different dimensions, and their structures can be open and porous. Moreover, it is very interesting to dope them with other elements (metal or non-metal) or hybridize them with other materials to form composites. The elemental and structural characteristics offer us to explore their applications in energy, environment, bioscience, medicine, electronics and others. Among them, energy storage and conversion are extremely attractive, as advances in this area may improve our life quality and environment. Some energy devices will be included herein, such as lithium-ion batteries, lithium sulfur batteries, sodium-ion batteries, potassium-ion batteries, dual ion batteries, electrochemical capacitors, and others. Additionally, carbon-based electrocatalysts are also studied in hydrogen evolution reaction and carbon dioxide reduction reaction. However, there are still many challenges in the design and preparation of electrode and electrocatalytic materials. The research related to carbon materials for energy storage and conversion is extremely active, and this has motivated us to contribute with a roadmap on 'Carbon Materials in Energy Storage and Conversion'.
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2D and 3D mapping of microindentations in hydrated and dehydrated cortical bones using confocal laser scanning microscopy
(Springer, 2012) Yin, L.; Venkatesan, S.; Webb, D.; Kalyanasundaram, S.; Qin, Q.
We report on responses of hydrated and dehydrated cortical bone tissues to mechanical loading applied by a Vickers indenter. The Vickers indentations were imaged in two- and three-dimensions (2D and 3D) using confocal laser scanning microscopy (CLSM) to understand mechanical behavior of bone tissues. Serial optical sections of indentation patterns of dry and wet bones were collected using CLSM. The indention surface structures were mapped using topographical CLSM imaging. The observation of CLSM shows the fundamental indentation responses for both the hydrated and dehydrated bone tissues were plastic deformation. No visible fracture was observed in the Vickers indentation patterns in the wet bone tissue, while non-propagating lamellar microcracks occurred in the dry bone tissue. This indicates that drying resulted in increased brittleness of the bone tissue. The Vickers hardness values of dry bone tissue were significantly higher than those of wet bone tissue at any applied loads (analysis of variation, ANOVA, p < 0.05). The resolution limits of confocal microscopy were also discussed for bone tissue scanning.
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2D and 3D simulations of fluid dynamics in the bubble reactor for liquid fuel synthesis: comparisons against experiments
(Taylor & Francis Inc., 2009) Qi, N.; Zhang, K.; Song, Q.; Gao, X.; Zhang, H.; Lu, J.
Flow pattern, bubble size distribution, and gas holdup are investigated in the bubble columns. Simulated results by the standard k-ε turbulence model together with Grace drag model in the commercial computational fluid dynamics software platform (ANSYS CFX 10.0) show good agreement with experimental measurement within the 2D and 3D columns. Three flow regimes (homogeneous bubbly, transitional, and turbulent flows) are identified by the instantaneous velocity profiles of gas and liquid phases, and general flow patterns are summarized under different superficial gas velocities. The findings are useful for designing the slurry bubble columns for synthesizing liquid hydrocarbons and alcohols.
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2D Mesoporous Zincophilic Sieve for High-Rate Sulfur-Based Aqueous Zinc Batteries
(American Chemical Society, 2023) Liu, J.; Ye, C.; Wu, H.; Jaroniec, M.; Qiao, S.-Z.
Sulfur-based aqueous zinc batteries (SZBs) attract increasing interest due to their integrated high capacity, competitive energy density, and low cost. However, the hardly reported anodic polarization seriously deteriorates the lifespan and energy density of SZBs at a high current density. Here, we develop an integrated acid-assisted confined self-assembly method (ACSA) to elaborate a two-dimensional (2D) mesoporous zincophilic sieve (2DZS) as the kinetic interface. The as-prepared 2DZS interface presents a unique 2D nanosheet morphology with abundant zincophilic sites, hydrophobic properties, and small-sized mesopores. Therefore, the 2DZS interface plays a bifunctional role in reducing the nucleation and plateau overpotential: (a) accelerating the Zn2+ diffusion kinetics through the opened zincophilic channels and (b) inhibiting the kinetic competition of hydrogen evolution and dendrite growth via the significant solvation-sheath sieving effect. Therefore, the anodic polarization is reduced to 48 mV at 20 mA cm-2, and the full-battery polarization is reduced to 42% of an unmodified SZB. As a result, an ultrahigh energy density of 866 Wh kgsulfur-1 at 1 A g-1 and a long lifespan of 10,000 cycles at a high rate of 8 A g-1 are achieved.
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2D metal organic framework nanosheet: a universal platform promoting highly efficient visible-light-induced hydrogen production
(Wiley, 2019) Ran, J.; Qu, J.; Zhang, H.; Wen, T.; Wang, H.; Chen, S.; Song, L.; Zhang, X.; Jing, L.; Zheng, R.; Qiao, S.Z.
2D metal organic frameworks (MOF) have received tremendous attention due to their organic–inorganic hybrid nature, large surface area, highly exposed active sites, and ultrathin thickness. However, the application of 2D MOF in light‐to‐hydrogen (H2) conversion is rarely reported. Here, a novel 2D MOF [Ni(phen)(oba)]n·0.5nH2O (phen = 1,10‐phenanthroline, oba = 4,4′‐oxybis(benzoate)) is for the first time employed as a general, high‐performance, and earth‐abundant platform to support CdS or Zn0.8Cd0.2S for achieving tremendously improved visible‐light‐induced H2‐production activity. Particularly, the CdS‐loaded 2D MOF exhibits an excellent H2‐production activity of 45 201 µmol h−1 g−1, even exceeding that of Pt‐loaded CdS by 185%. Advanced characterizations, e.g., synchrotron‐based X‐ray absorption near edge structure, and theoretical calculations disclose that the interactive nature between 2D MOF and CdS, combined with the high surface area, abundant reactive centers, and favorable band structure of 2D MOFs, synergistically contribute to this distinguished photocatalytic performance. The work not only demonstrates that the earth‐abundant 2D MOF can serve as a versatile and effective platform supporting metal sulfides to boost their photocatalytic H2‐production performance without noble‐metal co‐catalysts, but also paves avenues to the design and synthesis of 2D‐MOF‐based heterostructures for catalysis and electronics applications.
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2D MoN-VN heterostructure to regulate polysulfides for highly efficient lithium-sulfur batteries
(Wiley, 2018) Ye, C.; Jiao, Y.; Jin, H.; Slattery, A.; Davey, K.; Wang, H.; Qiao, S.
Lithium-sulfur batteries hold promise for next-generation batteries. A problem however is rapid capacity fading. Moreover, atomic-level understanding of the chemical interaction between sulfur host and polysulfides is poorly elucidated from a theoretical perspective. Here, a two-dimensional (2D) heterostructured MoN-VN is fabricated and investigated as a new model sulfur host. Theoretical calculations indicate that electronic structure of MoN can be tailored by incorporation of V. This leads to enhanced polysulfides adsorption. Additionally, in situ synchrotron X-ray Diffraction and electrochemical measurements reveal effective regulation and utilization of the polysulfides in the MoN-VN. The MoN-VN-based lithium-sulfur batteries have a capacity of 708 mA h g⁻¹ at 2 C and a capacity decay as low as 0.068% per cycle during 500 cycles with sulfur loading of 3.0 mg cm⁻².
Open Access
2D MoN₁.₂rGO Stacked Heterostructures Enabled Water State Modification for Highly Efficient Interfacial Solar Evaporation
(Wiley-VCH, 2023) Yu, H.; Wang, D.; Jin, H.; Wu, P.; Wu, X.; Chu, D.; Lu, Y.; Yang, X.; Xu, H.
Improving interfacial solar evaporation performance is crucial for the practical application of this technology in solar-driven seawater desalination. Lowering evaporation enthalpy is one of the most promising and effective strategies to significantly improve solar evaporation rate. In this study, a new pathway to lower vaporization enthalpy by introducing heterogeneous interactions between hydrophilic hybrid materials and water molecules is developed. 2D MoN₁.₂ nanosheets are synthesized and integrated with rGO nanosheets to form stacked MoN₁.₂-rGO heterostructures with massive junction interfaces for interfacial solar evaporation. Molecular dynamics simulation confirms that atomic thick 2D MoN₁.₂ and rGO in the MoN₁.₂-rGO heterostructures simultaneously interact with water molecules, while the interactions are remarkably different. These heterogeneous interactions cause an imbalanced water state, which easily breaks the hydrogen bonds between water molecules, leading to dramatically lowered vaporization enthalpy and improved solar evaporation rate (2.6 kg m⁻²h⁻¹). This study provides a promising strategy for designing 2D-2D heterostructures to regulate evaporation enthalpy to improve solar evaporate rate for clean water production.
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2D phosphorene as a water splitting photocatalyst: fundamentals to applications
(Royal Society of Chemistry, 2016) Rahman, M.; Kwong, C.; Davey, K.; Qiao, S.
Hydrogen from direct splitting of water molecules using photons is reckoned to be a sustainable and renewable energy solution for the post fossil-fuel era. Efficient photocatalysts, including metal-free photocatalysts, are key determinants of cost-effective hydrogen generation at a large-scale. The search for new materials that are metal-free is therefore ongoing. Recently, 2D phosphorene, a phosphorus analogue of graphene, has been added as a new semiconductor to the family of monolayer-flatland materials. In this review, we focus on analysing the fundamental electronic, optical and chemical properties of 2D phosphorene and assess its suitability as a metal-free water splitting photocatalyst. We also critically analyse its stability against claims from environmental antagonists and attempt to predict its future as a photocatalyst. This review provides timely information for researchers, scientists and professionals devoted to materials research for photocatalysis.
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2D/2D nano-hybrids of γ-MnO₂ on reduced graphene oxide for catalytic ozonation and coupling peroxymonosulfate activation
(Elsevier, 2016) Wang, Y.; Xie, Y.; Sun, H.; Xiao, J.; Cao, H.; Wang, S.
Abstract not available
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2H and 4H silver colloidal suspension synthesis, as a new potential drug carrier
(Elsevier, 2019) Wojnicki, M.; Tokarski, T.; Hessel, V.; Fitzner, K.; Luty-Błocho, M.
In this paper diffusion impact on the silver nanoparticles synthesis and their crystal structure is shown. For this purpose, comparative studies between continuous flow two-phase microdroplets systems vs. two-phase batch reactor were performed. Such two-phase configuration of the investigated system makes it possible to study the impact of mass transfer phenomenon on the nanoparticles formation process. In the case of two-phase microdroplets system, diffusion is replaced by convection, accelerated by interphase friction between water droplets and a continuous organic phase. It was concluded that under diffusion control it was possible to obtain silver nanoparticles with a hexagonal crystal structure. Moreover, for the first time using a chemical method, and diffusion rate-limiting step, the hexagonal structure 4H and 2H of Ag nanoparticles were synthesized. We suggest, that such hexagonal crystals can be applied as a smart drug delivery system, where the drug releases can be controlled by short light impulse. In effects, thermodynamically unstable 4H and 2H crystals transform to more dense-packed FCC structure.
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3-D Finite element modelling of diamond pull-out failure in impregnated diamond bits
(Elsevier, 2017) Xu, J.; Sheikh, A.; Xu, C.
Abstract not available
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3D aluminum hybrid plasmonic nanostructures with large areas of dense hot spots and long-term stability
(Wiley, 2017) Li, X.; Bi, M.; Cui, L.; Zhou, Y.; Du, X.; Qiao, S.; Yang, J.
Plasmonic materials possessing dense hot spots with high field enhancement over a large area are highly desirable for ultrasensitive biochemical sensing and efficient solar energy conversion; particularly those based on low-cost noncoinage metals with high natural abundance are of considerable practical significance. Here, 3D aluminum hybrid nanostructures (3D-Al-HNSs) with high density of plasmonic hot spots across a large scale are fabricated via a highly efficient and scalable nonlithographic method, i.e., millisecond-laser-direct-writing in liquid nitrogen. The nanosized alumina interlayer induces intense and dual plasmonic resonance couplings between adjacent Al nanoparticles with bimodal size distribution within each of the hybrid assemblies, leading to remarkably elevated localized electric fields (or hot spots) accessible to the analytes or reactants. The 3D-stacked nanostructure substantially raises the hot spot density, giving rise to plasmon-enhanced light harvesting from deep UV to the visible, strong enhancement of Raman signals, and a very low limit of detection outperforming reported Al nanostructures, and even comparable to the noble metals. Combined with the long-term stability and good reproducibility, the 3D-Al-HNSs hold promise as a robust low-cost plasmonic material for applications in plasmon-enhanced spectroscopic sensing and light harvesting.

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