Publications by authors named "Geoffrey I N Waterhouse"

Lithium (Li) metal batteries (LMBs) are promising for high-energy-density rechargeable batteries. However, Li dendrites formed by the reaction between highly active Li and non-aqueous electrolytes lead to safety concerns and rapid capacity decay. Developing a reliable solid-electrolyte interphase is critical for realizing high-rate and long-life LMBs, but remains technically challenging.

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Carbon nanomaterials show outstanding promise as electrocatalysts for hydrogen peroxide (HO) synthesis via the two-electron oxygen reduction reaction. However, carbon-based electrocatalysts that are capable of generating HO at industrial-level current densities (>300 mA cm) with high selectivity and long-term stability remain to be discovered. Herein, few-layer boron nanosheets are in-situ introduced into a porous carbon matrix, creating a metal-free electrocatalyst (B-C) with HO production rates of industrial relevance in neutral or alkaline media.

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Herein, conductive polyaniline (PANI) was chemically polymerized on the surface of a bismuth-based metal-organic framework (Bi-MOF) to form conductive PANI@Bi-MOF composites. FT-IR and PXRD measurements verified the successful production of PANI@Bi-MOF, whereas SEM, TEM, and EDAX mapping demonstrated that PANI was uniformly coated on the surface of Bi-MOF. The resulting PANI@Bi-MOF composites were characterized by cyclic voltammetry (CV and electrochemical impedance spectroscopy (EIS), then used to develop a sensitive electrochemical sensor for the detection of lead ions based on differential pulse anodic stripping voltammetry (DPASV).

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Electrochemical activation of dinitrogen (N) is notoriously challenging, typically yielding very low ammonia (NH) production rates. In this study, we present a continuous flow plasma-electrochemical reactor system for the direct conversion of nitrogen from air into ammonia. In our system, nitrogen molecules are first converted into a mixture of NO species in the plasma reactor, which are then fed into an electrochemical reactor.

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The electrochemical two-electron oxygen reduction reaction (2e ORR) offers a potentially cost-effective and eco-friendly route for the production of hydrogen peroxide (HO). However, the competing 4e ORR that converts oxygen to water limits the selectivity towards hydrogen peroxide. Accordingly, achieving highly selective HO production under low voltage conditions remains challenging.

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The development of efficient and stable electrocatalysts for water oxidation in acidic media is vital for the commercialization of the proton exchange membrane electrolyzers. In this work, we successfully construct Ru-O-Ir atomic interfaces for acidic oxygen evolution reaction (OER). The catalysts achieve overpotentials as low as 167, 300, and 390 mV at 10, 500, and 1500 mA cm in 0.

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Article Synopsis
  • Carbon dots (CDs) are a promising type of fluorescent nanomaterial known for their excellent optical characteristics, low toxicity, and high stability, making them useful in nanomedicine and energy applications.
  • Carbonized polymer dots (CPDs), a subtype of CDs, have tunable structures that enhance their optoelectronic properties, making them increasingly popular; however, their complex structure poses challenges in understanding their performance.
  • The research focuses on improving CPDs by controlling their core-shell structures to achieve desired properties, aiming for advanced applications in optoelectronics and energy through precise synthesis and modification techniques.
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Seawater electrolysis can generate carbon-neutral hydrogen but its efficiency is hindered by the low mass activity and poor stability of commercial catalysts at industrial current densities. Herein, Pt nanoclusters are loaded on nickel-iron-cobalt phosphide nanosheets, with the obtained Pt@NiFeCo-P electrocatalyst exhibiting excellent hydrogen evolution reaction (HER) activity and stability in alkaline seawater at ampere-level current densities. The catalyst delivers an ultralow HER overpotential of 19.

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Perilla essential oil (PLEO) offers benefits for food preservation and healthcare, yet its instability restricts its applications. In this study, chitosan (CS) and TiO used to prepare composite particles. TiO, after being modified with sodium laurate (SL), was successfully introduced at 0.

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Recent studies have shown that aqueous U(VI) ions can be transformed into U(VI) precipitates through electrocatalytic redox reactions for uranium recovery. However, there have been no reports of U(IV) solids, such as UO, using electrochemical methods under ambient conditions since low-valence states of uranium are typically oxidized to U(VI) by O or HO. Here we developed a secondary metal ion-induced strategy for electrocatalytic production of U(IV) solids from U(VI) solutions using a catalyst consisting of atomically dispersed gallium on hollow nitrogen-doped carbon capsules (Ga-N-C).

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  • Dual-atom catalysts (DACs), specifically dual-atom Fe catalysts (Fe/NC), have shown exceptional catalytic reactivity, but precise fabrication has been challenging.
  • A new synthesis method using in situ generated FeCl(g) dimers allows for better control over the Fe-Fe distance in the catalysts, leading to improved performance.
  • Research findings indicate that the optimal Fe-Fe distance enhances oxygen adsorption and subsequent reactions, significantly outperforming traditional catalysts like Pt/C.
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Removing trace amounts of acetylene (CH) from ethylene (CH)-rich gas mixtures is vital for the supply of high-purity CH to the chemical industry and plastics sector. However, selective removal of CH is challenging due to the similar physical and chemical properties of CH and CH. Here, we report a "single-molecule trap" strategy that utilizes electrostatic interactions between the one-dimensional (1D) channel of a covalent organic framework (denoted as COF-1) and CH molecules to massively enhance the adsorption selectivity toward CH over CH.

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Carbon dots (CDs), a type of nanoparticle with excellent optical properties, good biocompatibility, and small size, are finding increasing application across the fields of biology and biomedicine. In recent years, biomass-derived CDs with pharmacological activity (BP-CDs) derived from herbal medicines (HMs), HMs extracts and other natural products with demonstrated pharmaceutical activity have attracted particular attention. Herein, we review recent advances in the development of BP-CDs, covering the selection of biomass precursors, different methods used for the synthesis of BP-CDs from natural sources, and the purification of BP-CDs.

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Solid-state contact ion-selective electrodes (SC-ISEs) are an efficacious means of monitoring heavy metal contamination. Instability of the electrode potential is a key factor limiting their development, with biofouling in real water samples posing a significant challenge to maintaining stability. Therefore, addressing biofouling is crucial for optimizing solid-state ion-selective electrodes.

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Herein, a novel molecularly imprinted gel (MIG)-based electrochemical sensor equipped with hydrated zirconium oxide@hollow carbon spheres (ZrO(OH)@HCS) was developed for highly sensitive and selective detection of tert-butylhydroquinone (TBHQ) in foods. The MIG was synthesized by using L-histidine to rapidly cross-link cationic guar gum, acrylamide and TBHQ through intermolecular hydrogen bonds and electrostatic interactions at room temperature, which offered outstanding specific recognition performance for TBHQ. ZrO(OH)@HCS possessing excellent conductivity and water dispersibility was employed for signal amplification.

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Surface-enhanced Raman spectroscopy (SERS) detection platforms with high signal-to-noise ratio in the "biological-silent" region (1800-2800 cm) are presently being developed for sensing and imaging applications, overcoming the limitations of traditional SERS studies in the "fingerprint" region. Herein, a series of cyano-programmable Raman reporters (RRs) operating in the "biological-silent" region were designed based on 4-mercaptobenzonitrile derivatives and then embedded in core-shell Au@Ag nanostars using a "bottom-up" strategy to provide SERS enhancement and encapsulation protection. The approach enabled the "one-pot" readout interference-free detection of multiple bioamines (histamine, tyramine, and β-phenethylamine) based on aptamer-driven magnetic-induced technology.

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Improving the water stability of metal-organic frameworks (MOFs) is essential for their use in water pollution treatment and environmental remediation, though it remains technically challenging. Herein, we report a novel cationic MOF constructed with [ThO(OH)(COO)] units and [CoN·Cl] units possessing a ftw-type topology (denoted as ). itself exhibited poor water stability but excellent stability following a palladium(II) modulation strategy.

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Article Synopsis
  • Challenges in efficiently converting biomass-based aldehydes and alcohols to acids limit their broader application; this study presents a solution with a new catalyst.
  • The Pd/Ni(OH) catalyst achieves nearly 100% selectivity in producing 2,5-furandicarboxylic acid from 5-hydroxymethylfurfural, yielding 97.3% at a voltage of 0.6 V under standard conditions.
  • The catalyst's effectiveness is enhanced by its unique Ni-O-Pd interfaces, which promote reaction steps, prevent nanoparticle clumping, and maintain stability over 200 hours of continuous use.
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  • Near-infrared light-driven photocatalytic CO reduction (NIR-COPR) is a promising method for producing chemicals and fuels, but effective photocatalysts for this process are hard to develop.
  • A novel photocatalyst made of an anionic Ru complex within NiAl-layered double hydroxide nanosheets (NiAl-Ru-LDH) achieves efficient CO reduction with good selectivity and stability under 1200 nm light.
  • The catalyst works well due to the Ru complex lowering the band gap and facilitating electron transfer, while hydroxyl defects in the LDH enhance CO molecule adsorption and reduce energy barriers for the reaction.
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  • The study highlights the importance of the oxygen reduction reaction (ORR) in energy devices and introduces iron-cobalt phosphide nanoparticles (FeCoP) wrapped in a nitrogen-doped carbon framework (FeCoP@NC) as an effective electrocatalyst.
  • The FeCoP@NC catalyst shows impressive ORR performance, with a half-wave potential of 0.86 V and stability in alkaline conditions, surpassing commercial platinum catalysts and other noble-metal-free options.
  • Prototype zinc-air batteries utilizing FeCoP@NC demonstrate strong performance, featuring high open circuit voltages and power densities, with theoretical analyses indicating enhanced electron interacting benefits from the N-doped carbon encapsulation.
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NaTiO-based anodes show great promise for Na storage in sodium-ion batteries (SIBs), though the effect of NaTiO morphology on battery performance remains poorly understood. Herein, hydrothermal syntheses is used to prepare free-standing NaTiO nanosheets or NaTiO nanotubes on Ti foil substrates, with the structural and electrochemical properties of the resulting electrodes explored in detail. Results show that the NaTiO nanosheet electrode (NTO NSs) delivered superior performance in terms of reversible capacity, rate capability, and especially long-term durability in SIBs compared to its nanotube counterpart (NTO NTs).

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Theory-guided materials design is an effective strategy for designing catalysts with high intrinsic activity whilst minimizing the usage of expensive metals like platinum. As proof-of-concept, herein it demonstrates that using density functional theory (DFT) calculations and experimental validation that intermetallic PtCo alloy nanoparticles offer enhanced electrocatatalytic performance for the oxygen reduction reaction (ORR) compared to Pt nanoparticles. DFT calculations established that PtCo(111) surfaces possess better intrinsic ORR activity compared to Pt(111) surfaces, owing to the synergistic action of adjacent Pt and Co active sites which optimizes the binding strength of ORR intermediates to boost overall ORR kinetics.

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Foodborne pathogens result in a great harm to human, which is an urgent problem to be addressed. Herein, a novel cellulose-based packaging films with excellent anti-bacterial properties under visible light were prepared. A porphyrin-based covalent organic polymer (Por-COPs) was constructed, then covalently grafted onto dialdehyde cellulose (DAC).

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Herein, a novel surface enhanced Raman spectroscopy (SERS) aptasensor was developed for amantadine (AMD) detection, based on magnetite nanoparticles coated with polyethylenimine, silver nanoclusters and aptamers (FeO@PEI@AgNC-apt) as the capture probe and complementary DNA-modified gold nanorods (AuNRs@4-MPBA@Ag-c-DNA containing 4-mercaptophenylboric acid molecules) as the reporter probe. In the presence of AMD, the AMD and the reporter probe competed for the aptamer on the surface of the capture probe, resulting in the reporter probe detaching from the capture probe leading to a decrease in intensity of the SERS signal at 1067 cm for 4-MPBA. Under optimal conditions, a good linear relationship was established between the SERS intensity at 1067 cm and the logarithm of the AMD concentration over the range 10-10 mg L, with a LOD of 0.

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The monitoring of organic compounds in aquatic matrices poses challenges due to its complexity and time-intensive nature. To address these challenges, we introduce a novel approach utilizing a dual-channel mono (D) and comprehensive two-dimensional (D) gas chromatography coupled with time-of-flight mass spectrometry (GC × GC-TOFMS) system, integrated with a robotic pretreatment platform, for online monitoring of both volatile organic compounds (VOCs) and semivolatile organic compounds (SVOCs) in water matrices. Employing the robotic platform, we establish a suite of online liquid-liquid extraction (LLE) pretreatment processes for water samples, marking the first instance of such procedures.

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