https://nova.newcastle.edu.au/vital/access/ /manager/Index ${session.getAttribute("locale")} 5 Nitrogen-doped phosphorene for electrocatalytic ammonia synthesis https://nova.newcastle.edu.au/vital/access/ /manager/Repository/uon:41019 Thu 21 Jul 2022 12:08:17 AEST ]]> Ruthenium(iii) polyethyleneimine complexes for bifunctional ammonia production and biomass upgrading https://nova.newcastle.edu.au/vital/access/ /manager/Repository/uon:46657 3), electrocatalytic nitrogen reduction reactions (NRRs) under ambient conditions using renewable energy sources (e.g. solar) have attracted significant attention; however, the design of an efficient electrocatalyst for the NRR is a challenging task and has been of central research interest. Herein, we report the synthesis of ruthenium(iii) polyethyleneimine (Ru(iii)-PEI) catalysts supported on carboxyl-modified carbon nanotubes (Ru(iii)-PEI@MWCNTs) by a self-assembly process driven by electrostatic forces at room temperature. Our newly designed Ru(iii)-PEI@MWCNTs were employed as bifunctional catalysts for the NRR and 5-hydroxymethylfurfural (HMF) oxidation. At -0.10 V vs. the reversible hydrogen electrode (RHE), our Ru(iii)-PEI@MWCNTs exhibited the high NH3 yield rate of 188.90 μgNH3 mgcat.-1 h-1 and the faradaic efficiency (FE) of 30.93% at room temperature. Furthermore, owing to its favorable thermodynamics for HMF oxidation, the Ru(iii)-PEI@MWCNT electrode demonstrated an impressive electrocatalytic HMF oxidation at 1.24 V, 220 mV lower than that for oxygen evolution. The two-electrode electrolyzer employing Ru(iii)-PEI@MWCNTs as a bifunctional catalyst for both the cathode and the anode showed the current density of 0.50 mA cm-2 with the cell voltage of only 1.34 V over 27 hours of stable electrolysis with a 94% FE for 2,5-furandicarboxylic acid (FDCA) production; this suggested an outstanding performance of this electrolyzer for the coupling of NRR with HMF oxidation. This study represents the first attempt at the ground demonstration of combining NH3 production with biomass upgrading.]]> Thu 07 Dec 2023 11:10:30 AEDT ]]> Surface oxidized two-dimensional antimonene nanosheets for electrochemical ammonia synthesis under ambient conditions https://nova.newcastle.edu.au/vital/access/ /manager/Repository/uon:46344 −1 mgCAT−1 and faradaic efficiency (FE) of 11.6% are achieved using our antimonene nanosheets. Theoretical calculations suggest that the oxidized species of antimonene act as the active catalytic sites for the NRR process. This work opens up a new avenue towards the development of 2D electrocatalysts for clean energy.]]> Mon 29 Jan 2024 17:48:27 AEDT ]]> Structural engineering to maintain the superior capacitance of molybdenum oxides at ultrahigh mass loadings https://nova.newcastle.edu.au/vital/access/ /manager/Repository/uon:46663 3−x) electrode with an ultrahigh mass loading of 15.4 mg cm−2 on a functionalized partially exfoliated graphite substrate using a facile electrochemical method. In addition to the highly open graphene nanosheets atop, the unique layered structures of intercalated graphite sheets ensure efficient ionic transport in the entire MoO3−x electrode. The oxygen-containing functional groups on the exfoliated graphene can bind strongly with the MoO3−x via formation of C–O–Mo bonding, which provides a fast electron transport path from graphene to MoO3−x and thus allows high reversible capacity and excellent rate performance. The optimized MoO3−x electrode delivers an outstanding areal capacitance of 4.03 F cm−2 at 3 mA cm−2 with an excellent rate capability which is significantly higher than the values of other molybdenum oxide based electrodes reported to date. More importantly, the areal capacitance increases proportionally with the MoO3−x mass loading, indicating that the capacitive performance is not limited by ion diffusion even at such a high mass loading. An asymmetric supercapacitor (ASC) assembled with an MoO3−x anode delivers a maximum volumetric energy density of 2.20 mW h cm−3 at a volumetric power density of 3.60 mW cm−3, which is superior to those of the majority of the state-of-the-art supercapacitors.]]> Mon 28 Nov 2022 18:32:21 AEDT ]]> Zinc-nickel-cobalt ternary hydroxide nanoarrays for high-performance supercapacitors https://nova.newcastle.edu.au/vital/access/ /manager/Repository/uon:48488 −2 on a carbon cloth substrate is achieved, accompanied by substantially improved facile ionic and electronic transport due to the highly open well-defined nanoarray architecture. The growth mechanism of Zn–Ni–Co TOH was studied in depth by scanning electron microscopy analysis. The optimized Zn–Ni–Co TOH-130 nanowire array electrode delivered an outstanding areal capacitance of 2.14 F cm−2 (or a specific capacitance of 305 F g−1) at 3 mA cm−2 and an excellent rate capability. Moreover, the asymmetric supercapacitor assembled with our Zn–Ni–Co TOH-130 cathode exhibited a maximum volumetric energy density of 2.43 mW h cm−3 at a volumetric power density of 6 mW cm−3 and a long-term cycling stability (153% retention after 10 000 cycles), which is superior to the majority of the state-of-the-art supercapacitors. This work paves the way for the construction of high-capacity cathode materials for widespread applications including next-generation wearable energy-storage devices.]]> Mon 20 Mar 2023 11:30:42 AEDT ]]> Surface engineering to reduce the interfacial resistance for enhanced photocatalytic water oxidation https://nova.newcastle.edu.au/vital/access/ /manager/Repository/uon:40875 µmol/g·h, which is approximately 14 times higher than that of the bare am@TiO₂. Moreover, an apparent quantum yield (AQY) of 18.99% is obtained under LED-405 illumination. This work provides a direction for improving the photocatalytic performance and helps to gain a fundamental understanding of the water oxidation steps.]]> Mon 08 Aug 2022 15:49:38 AEST ]]> Surface-halogenation-induced atomic-site activation and local charge separation for superb CO₂ photoreduction https://nova.newcastle.edu.au/vital/access/ /manager/Repository/uon:36540 Mon 01 Jun 2020 12:07:38 AEST ]]> Unsaturated p-Metal-Based Metal-Organic Frameworks for Selective Nitrogen Reduction under Ambient Conditions https://nova.newcastle.edu.au/vital/access/ /manager/Repository/uon:41229 3 yield: 10.6 μg h–1 cm–2 mgcat.–1 and Faradaic efficiency: 22.6%) at a low overpotential (177 mV). Investigation indicates that the catalyst shows excellent N2-selective captures due to the unsaturated metal sites binding with N2. More specifically, as the Al 3p band can strongly interact with N 2p orbitals, Al as a main group metal presents a high and selective affinity to N2. The utilization of multifunctional MOF catalysts delivers both high N2 selectivity and abundant catalytic sites, resulting in remarkable efficiency for NH3 production.]]> Fri 29 Jul 2022 11:49:26 AEST ]]> A luminescent terbium coordination complex as multifunctional sensing platform https://nova.newcastle.edu.au/vital/access/ /manager/Repository/uon:38173 2(NO3)2 (HPU-10) (H2L = 2,6-bis-(5-pyridin-4-yl-1H-[1,2,4]triazol-3-yl)- pyridine), and demonstrate that this novel chemosensor has the property of ratiometric detection of Zn2+ and Cd2+. The detection limit of HPU-10 sensing Zn2+ and Cd2+ is 0.319 and 0.965 μM, respectively. The sensing mechanism can be explained by (i) the decomposition of HPU-10 and (ii) the recombination of Zn2+ or Cd2+ with ligand forming 2HL--Zn2+ or 2HL--Cd2+, respectively. Moreover, the fluorescent sensor HPU-10 can detect the nitroaromatic compound 2, 4-DNP via a fluorescence quenching mechanism. The detection limits obtained from linear regression curve plots of 2, 4-DNP is calculated to be 1.69 μM. In addition, the possible use of the probe coated paper for tracing the target analytes has also been presented.]]> Fri 06 Aug 2021 13:39:40 AEST ]]>